Advancements in sensor technology have significantly enhanced atmospheric monitoring.Notably,metal oxide and carbon(MO_(x)/C)hybrids have gained attention for their exceptional sensitivity and room-temperature sensing...Advancements in sensor technology have significantly enhanced atmospheric monitoring.Notably,metal oxide and carbon(MO_(x)/C)hybrids have gained attention for their exceptional sensitivity and room-temperature sensing performance.However,previous methods of synthesizing MO_(x)/C composites suffer from problems,including inhomogeneity,aggregation,and challenges in micropatterning.Herein,we introduce a refined method that employs a metal–organic framework(MOF)as a precursor combined with direct laser writing.The inherent structure of MOFs ensures a uniform distribution of metal ions and organic linkers,yielding homogeneous MO_(x)/C structures.The laser processing facilitates precise micropatterning(<2μm,comparable to typical photolithography)of the MO_(x)/C crystals.The optimized MOF-derived MO_(x)/C sensor rapidly detected ethanol gas even at room temperature(105 and 18 s for response and recovery,respectively),with a broad range of sensing performance from 170 to 3,400 ppm and a high response value of up to 3,500%.Additionally,this sensor exhibited enhanced stability and thermal resilience compared to previous MOF-based counterparts.This research opens up promising avenues for practical applications in MOF-derived sensing devices.展开更多
The development of aqueous zinc ion battery cathode materials with high capacity and high magnification is still a challenge.Herein,porous vanadium oxide/carbon(p-VO_(x)@C,mainly VO_(2) with a small amount of V_(2)O_(...The development of aqueous zinc ion battery cathode materials with high capacity and high magnification is still a challenge.Herein,porous vanadium oxide/carbon(p-VO_(x)@C,mainly VO_(2) with a small amount of V_(2)O_(3)) core/shell microspheres with oxygen vacancies are facilely fabricated by using a vanadium-based metal-organic framework(MIL-100(V)) as a sacrificial template.This unique structure can improve the conductivity of the VO_(x),accelerate electrolyte diffusion,and suppress structural collapse during circulation.Subsequently,H_(2)O molecules are introduced into the interlayer of VO_(x) through a highly efficient in-situ electrochemical activation process,facilitating the intercalation and diffusion of zinc ions.After the activation,an optimal sample exhibits a high specific capacity of 464.3 mA h g^(-1) at0.2 A g^(-1) and 395.2 mA h g^(-1) at 10 A g^(-1),indicating excellent rate performance.Moreover,the optimal sample maintains a capacity retention of about 89.3% after 2500 cycles at 10 A g^(-1).Density functional theory calculation demonstrates that the presence of oxygen vacancies and intercalated water molecules can significantly reduce the diffusion barrier for zinc ions.In addition,it is proved that the storage of zinc ions in the cathode is achieved by reversible intercalation/extraction during the charge and discharge process through various ex-situ analysis technologies.This work demonstrates that the p-VO_(x)@C has great potential for applications in aqueous ZIBs after electrochemical activation.展开更多
Glycerol carbonate,an important glycerol value-added product,has been widely used as an active intermediate and inert solvent in the synthesis of cosmetics,detergents,chemical intermediates,polymers,and so on.The dire...Glycerol carbonate,an important glycerol value-added product,has been widely used as an active intermediate and inert solvent in the synthesis of cosmetics,detergents,chemical intermediates,polymers,and so on.The direct carbonylation from glycerol with CO_(2)is considered a promising route,but still tough work due to the thermodynamic stability and the kinetic inertness of CO_(2).In this work,highlyselective direct carbonylation of glycerol and CO_(2)into glycerol carbonate has been achieved over highly dispersed MgInCe-mixed metal oxides(MgInCe-MMO),which were prepared through the topological transformation derived from the MgInCe-layered double hydroxides(MgInCe-LDHs).By precisely modulating the surface basic-acidic properties and the oxygen vacancies,an efficient carbonylation of glycerol with CO_(2)has been achieved with a selectivity of up to>99%to glycerol carbonate.Deep investigation into the synergistic catalysis of base-acid sites and oxygen vacancies has been clarified.展开更多
Carbon monoxide(CO)and nitric oxide(NO)are signal molecules that enhance plant adaptation to environmental stimuli.Auxin is an essential phytohormone for plant growth and development.CO and NO play crucial roles in mo...Carbon monoxide(CO)and nitric oxide(NO)are signal molecules that enhance plant adaptation to environmental stimuli.Auxin is an essential phytohormone for plant growth and development.CO and NO play crucial roles in modulating the plant’s response to iron deficiency.Iron deficiency leads to an increase in the activity of heme oxygenase(HO)and the subsequent generation of CO.Additionally,it alters the polar subcellular distribution of Pin-Formed 1(PIN1)proteins,resulting in enhanced auxin transport.This alteration,in turn,leads to an increase in NO accumulation.Furthermore,iron deficiency enhances the activity of ferric chelate reductase(FCR),as well as the expression of the Fer-like iron deficiency-induced transcription factor 1(FIT)and the ferric reduction oxidase 2(FRO2)genes in plant roots.Overexpression of the long hypocotyl 1(HY1)gene,which encodes heme oxygenase,or the CO donor treatment resulted in enhanced basipetal auxin transport,higher FCR activity,and the expression of FIT and FRO2 genes under Fe deficiency.Here,a potential mechanism is proposed:CO and NO interact with auxin to address iron deficiency stress.CO alters auxin transport,enhancing its accumulation in roots and up-regulating key iron-related genes like FRO2 and IRT1.Elevated auxin levels affect NO signaling,leading to greater sensitivity in root development.This interplay promotes FCR activity,which is crucial for iron absorption.Together,these molecules enhance iron uptake and root growth,revealing a novel aspect of plant physiology in adapting to environmental stress.展开更多
Considering the serious electromagnetic wave(EMW)pollution problems and complex application condition,there is a pressing need to amalgamate multiple functionalities within a single substance.However,the effective int...Considering the serious electromagnetic wave(EMW)pollution problems and complex application condition,there is a pressing need to amalgamate multiple functionalities within a single substance.However,the effective integration of diverse functions into designed EMW absorption materials still faces the huge challenges.Herein,reduced graphene oxide/carbon foams(RGO/CFs)with two-dimensional/three-dimensional(2D/3D)van der Waals(vdWs)heterostructures were meticulously engineered and synthesized utilizing an efficient methodology involving freeze-drying,immersing absorption,secondary freeze-drying,followed by carbonization treatment.Thanks to their excellent linkage effect of amplified dielectric loss and optimized impedance matching,the designed 2D/3D RGO/CFs vdWs heterostructures demonstrated commendable EMW absorption performances,achieving a broad absorption bandwidth of 6.2 GHz and a reflection loss of-50.58 dB with the low matching thicknesses.Furthermore,the obtained 2D/3D RGO/CFs vdWs heterostructures also displayed the significant radar stealth properties,good corrosion resistance performances as well as outstanding thermal insulation capabilities,displaying the great potential in complex and variable environments.Accordingly,this work not only demonstrated a straightforward method for fabricating 2D/3D vdWs heterostructures,but also outlined a powerful mixeddimensional assembly strategy for engineering multifunctional foams for electromagnetic protection,aerospace and other complex conditions.展开更多
This study investigates the influence of electropolymerization conditions on the deposition of polypyrrole(PPy)onto cotton-derived carbon fiber(CF)modified with reduced graphene oxide(rGO)for supercapacitors applicati...This study investigates the influence of electropolymerization conditions on the deposition of polypyrrole(PPy)onto cotton-derived carbon fiber(CF)modified with reduced graphene oxide(rGO)for supercapacitors applications using an experimental/theorical approach.The surface modification of CF by rGO and/or by PPy electrodeposited at 10,25 and 50 mV s^(-1) was thoroughly examined physicochemical and electrochemically.Composite electrodes comprising CF-rGo-PPy,synthesized via electropolymerization at 25 mV s^(-1),demonstrated a remarkable increase in capacitance,showcasing~742 F g^(-1) compared to 153 F g^(-1) for CF.SEM,N_(2)-surface area,XPS,and TD-DFT approach revealed that the higher capacitance observed in CF-rGo-PPy electrodes underscores the influence of morphology and charged nitrogen species on the electrochemical performance of these modified electrodes.Notably,this electrode material achieves a specific capacitance retention of~96%of their initial capacitance after 10000 cycles at 0.5 A g^(-1) measured in a two-electrodes cell configuration.This work also discusses the influence of the scan rate used for pyrrole electropolymerization on the pseudocapacitance contribution of PPy and its possible effect on the porosity of the material.These results highlight the importance of appropriate electropolymerization conditions that allow obtaining the synergistic effect between CF,rGO and PPy.展开更多
The unabated carbon dioxide(CO_(2))emission into the atmosphere has exacerbated global climate change,resulting in extreme weather events,biodiversity loss,and an intensified greenhouse effect.To address these challen...The unabated carbon dioxide(CO_(2))emission into the atmosphere has exacerbated global climate change,resulting in extreme weather events,biodiversity loss,and an intensified greenhouse effect.To address these challenges and work toward carbon(C)neutrality and reduced CO_(2)emissions,the capture and utilization of CO_(2)have become imperative in both scientific research and industry.One cutting-edge approach to achieving efficient catalytic performance involves integrating green bioconversion and chemical conversion.This innovative strategy offers several advantages,including environmental friendliness,high efficiency,and multi-selectivity.This study provides a comprehensive review of existing technical routes for carbon sequestration(CS)and introduces two novel CS pathways:the electrochemicalbiological hybrid and artificial photosynthesis systems.It also thoroughly examines the synthesis of valuable Cnproducts from the two CS systems employing different catalysts and biocatalysts.As both systems heavily rely on electron transfer,direct and mediated electron transfer has been discussed and summarized in detail.Additionally,this study explores the conditions suitable for different catalysts and assesses the strengths and weaknesses of biocatalysts.We also explored the biocompatibility of the electrode materials and developed novel materials.These materials were specifically engineered to combine with enzymes or microbial cells to solve the biocompatibility problem,while improving the electron transfer efficiency of both.Furthermore,this review summarizes the relevant systems developed in recent years for manufacturing different products,along with their respective production efficiencies,providing a solid database for development in this direction.The novel chemical-biological combination proposed herein holds great promise for the future conversion of CO_(2)into advanced organic compounds.Additionally,it offers exciting prospects for utilizing CO_(2)in synthesizing a wide range of industrial products.Ultimately,the present study provides a unique perspective for achieving the vital goals of“peak shaving”and C-neutrality,contributing significantly to our collective efforts to combat climate change and its associated challenges.展开更多
Acorn production in oak(Quercus spp.)shows considerable inter-annual variation,known as masting,which provides a natural defence against seed predators but a highly-variable supply of acorns for uses such as in commer...Acorn production in oak(Quercus spp.)shows considerable inter-annual variation,known as masting,which provides a natural defence against seed predators but a highly-variable supply of acorns for uses such as in commercial tree planting each year.Anthropogenic emissions of greenhouse gases have been very widely reported to influence plant growth and seed or fruit size and quantity via the‘fertilisation effect’that leads to enhanced photosynthesis.To examine if acorn production in mature woodland communities will be affected by further increase in CO_(2),the contents of litter traps from a Free Air Carbon Enrichment(FACE)experiment in deciduous woodland in central England were analysed for numbers of flowers and acorns of pedunculate oak(Quercus robur L.)at different stages of development and their predation levels under ambient and elevated CO_(2) concentrations.Inter-annual variation in acorn numbers was considerable and cyclical between 2015 and 2021,with the greatest numbers of mature acorns in 2015,2017 and 2020 but almost none in 2018.The numbers of flowers,enlarged cups,immature acorns,empty acorn cups,and galls in the litter traps also varied amongst years;comparatively high numbers of enlarged cups were recorded in 2018,suggesting Q.robur at this site is a fruit maturation masting species(i.e.,the extent of abortion of pollinated flowers during acorn development affects mature acorn numbers greatly).Raising the atmospheric CO_(2) concentration by 150μL L^(−1),from early 2017,increased the numbers of immature acorns,and all acorn evidence(empty cups+immature acorns+mature acorns)detected in the litter traps compared to ambient controls by 2021,but did not consistently affect the numbers of flowers,enlarged cups,empty cups,or mature acorns.The number of flowers in the elevated CO_(2) plots’litter traps was greater in 2018 than 2017,one year after CO_(2) enrichment began,whereas numbers declined in ambient plots.Enrichment with CO_(2) also increased the number of oak knopper galls(Andricus quercuscalicis Burgsdorf).We conclude that elevated CO_(2) increased the occurrence of acorns developing from flowers,but the putative benefit to mature acorn numbers may have been hidden by excessive pre-and/or post-dispersal predation.There was no evidence that elevated CO_(2) altered masting behaviour.展开更多
Ethylene glycol(EG)plays a pivotal role as a primary raw material in the polyester industry,and the syngas-to-EG route has become a significant technical route in production.The carbon monoxide(CO)gas-phase catalytic ...Ethylene glycol(EG)plays a pivotal role as a primary raw material in the polyester industry,and the syngas-to-EG route has become a significant technical route in production.The carbon monoxide(CO)gas-phase catalytic coupling to synthesize dimethyl oxalate(DMO)is a crucial process in the syngas-to-EG route,whereby the composition of the reactor outlet exerts influence on the ultimate quality of the EG product and the energy consumption during the subsequent separation process.However,measuring product quality in real time or establishing accurate dynamic mechanism models is challenging.To effectively model the DMO synthesis process,this study proposes a hybrid modeling strategy that integrates process mechanisms and data-driven approaches.The CO gas-phase catalytic coupling mechanism model is developed based on intrinsic kinetics and material balance,while a long short-term memory(LSTM)neural network is employed to predict the macroscopic reaction rate by leveraging temporal relationships derived from archived measurements.The proposed model is trained semi-supervised to accommodate limited-label data scenarios,leveraging historical data.By integrating these predictions with the mechanism model,the hybrid modeling approach provides reliable and interpretable forecasts of mass fractions.Empirical investigations unequivocally validate the superiority of the proposed hybrid modeling approach over conventional data-driven models(DDMs)and other hybrid modeling techniques.展开更多
Urea generation through electrochemical CO_(2) and NO_(3)~-co-reduction reaction(CO_(2)NO_(3)RR)is still limited by either the low selectivity or yield rate of urea.Herein,we report copper carbonate hydroxide(Cu_2(OH)...Urea generation through electrochemical CO_(2) and NO_(3)~-co-reduction reaction(CO_(2)NO_(3)RR)is still limited by either the low selectivity or yield rate of urea.Herein,we report copper carbonate hydroxide(Cu_2(OH)_2CO_(3))as an efficient CO_(2)NO_(3)RR electrocatalyst with an impressive urea Faradaic efficiency of45.2%±2.1%and a high yield rate of 1564.5±145.2μg h~(-1)mg_(cat)~(-1).More importantly,H_(2) evolution is fully inhibited on this electrocatalyst over a wide potential range between-0.3 and-0.8 V versus reversible hydrogen electrode.Our thermodynamic simulation reveals that the first C-N coupling follows a unique pathway on Cu_2(OH)_2CO_(3) by combining the two intermediates,~*COOH and~*NHO.This work demonstrates that high selectivity and yield rate of urea can be simultaneously achieved on simple Cu-based electrocatalysts in CO_(2)NO_(3)RR,and provide guidance for rational design of more advanced catalysts.展开更多
Understanding the response of the Earth system to varying concentrations of carbon dioxide(CO_(2))is critical for projecting possible future climate change and for providing insight into mitigation and adaptation stra...Understanding the response of the Earth system to varying concentrations of carbon dioxide(CO_(2))is critical for projecting possible future climate change and for providing insight into mitigation and adaptation strategies in the near future.In this study,we generate a dataset by conducting an experiment involving carbon dioxide removal(CDR)—a potential way to suppress global warming—using the Chinese Academy of Sciences Earth System Model version 2.0(CASESM2.0).A preliminary evaluation is provided.The model is integrated from 200–340 years as a 1%yr^(−1) CO_(2) concentration increase experiment,and then to~478 years as a carbon dioxide removal experiment until CO_(2) returns to its original value.Finally,another 80 years is integrated in which CO_(2) is kept constant.Changes in the 2-m temperature,precipitation,sea surface temperature,ocean temperature,Atlantic meridional overturning circulation(AMOC),and sea surface height are all analyzed.In the ramp-up period,the global mean 2-m temperature and precipitation both increase while the AMOC weakens.Values of all the above variables change in the opposite direction in the ramp-down period,with a delayed peak relative to the CO_(2) peak.After CO_(2) returns to its original value,the global mean 2-m temperature is still~1 K higher than in the original state,and precipitation is~0.07 mm d^(–1) higher.At the end of the simulation,there is a~0.5°C increase in ocean temperature and a 1 Sv weakening of the AMOC.Our model simulation produces similar results to those of comparable experiments previously reported in the literature.展开更多
The well-developed coal electricity generation and coal chemical industries have led to huge carbon dioxide(CO_(2))emissions in the northeastern Ordos Basin.The geological storage of CO_(2) in saline aquifers is an ef...The well-developed coal electricity generation and coal chemical industries have led to huge carbon dioxide(CO_(2))emissions in the northeastern Ordos Basin.The geological storage of CO_(2) in saline aquifers is an effective backup way to achieve carbon neutrality.In this case,the potential of saline aquifers for CO_(2) storage serves as a critical basis for subsequent geological storage project.This study calculated the technical control capacities of CO_(2) of the saline aquifers in the fifth member of the Shiqianfeng Formation(the Qian-5 member)based on the statistical analysis of the logging and the drilling and core data from more than 200 wells in the northeastern Ordos Basin,as well as the sedimentary facies,formation lithology,and saline aquifer development patterns of the Qian-5 member.The results show that(1)the reservoirs of saline aquifers in the Qian-5 member,which comprise distributary channel sand bodies of deltaic plains,feature low porosities and permeabilities;(2)The study area hosts three NNE-directed saline aquifer zones,where saline aquifers generally have a single-layer thickness of 3‒8 m and a cumulative thickness of 8‒24 m;(3)The saline aquifers of the Qian-5 member have a total technical control capacity of CO_(2) of 119.25×10^(6) t.With the largest scale and the highest technical control capacity(accounting for 61%of the total technical control capacity),the Jinjie-Yulin saline aquifer zone is an important prospect area for the geological storage of CO_(2) in the saline aquifers of the Qian-5 member in the study area.展开更多
Despite the extensive application of advanced oxidation processes(AOPs)in water treatment,the efficiency of AOPs in eliminating various emerging contaminants such as halogenated antibiotics is constrained by a number ...Despite the extensive application of advanced oxidation processes(AOPs)in water treatment,the efficiency of AOPs in eliminating various emerging contaminants such as halogenated antibiotics is constrained by a number of factors.Halogen moieties exhibit strong resistance to oxidative radicals,affecting the dehalogenation and detoxification efficiencies.To address these limitations of AOPs,advanced reduction processes(ARPs)have been proposed.Herein,a novel nucleophilic reductant—namely,the carbon dioxide radical anion(CO_(2)^(·-))—is introduced for the simultaneous degradation,dehalogenation,and detoxification of florfenicol(FF),a typical halogenated antibiotic.The results demonstrate that FF is completely eliminated by CO_(2)^(·-),with approximately 100%of Cland 46%of Freleased after 120 min of treatment.Simultaneous detoxification is observed,which exhibits a linear response to the release of free inorganic halogen ions(R^(2)=0.97,p<0.01).The formation of halogen-free products is the primary reason for the superior detoxification performance of this method,in comparison with conventional hydroxyl-radical-based AOPs.Products identification and density functional theory(DFT)calculations reveal the underlying dehalogenation mechanism,in which the chlorine moiety of FF is more susceptible than other moieties to nucleophilic attack by CO_(2)^(·-).Moreover,CO_(2)^(·-)-based ARPs exhibit superior dehalogenation efficiencies(>75%)in degrading a series of halogenated antibiotics,including chloramphenicol(CAP),thiamphenicol(THA),diclofenac(DLF),triclosan(TCS),and ciprofloxacin(CIP).The system shows high tolerance to the pH of the solution and the presence of natural water constituents,and demonstrates an excellent degradation performance in actual groundwater,indicating the strong application potential of CO_(2)^(·-)-based ARPs in real life.Overall,this study elucidates the feasibility of CO_(2)^(·-)for the simultaneous degradation,dehalogenation,and detoxification of halogenated antibiotics and provides a promising method for their regulation during water or wastewater treatment.展开更多
The absolute partial and total cross sections for electron impact ionization of carbon monoxide are reported for electron energies from 350 eV to 8000 eV.The product ions(CO^(+),C^(+),O^(+),CO^(2+),C^(2+),and O^(2+))a...The absolute partial and total cross sections for electron impact ionization of carbon monoxide are reported for electron energies from 350 eV to 8000 eV.The product ions(CO^(+),C^(+),O^(+),CO^(2+),C^(2+),and O^(2+))are measured by employing an ion imaging mass spectrometer and two ion-pair dissociation channels(C^(+)+O^(+)and C^(2+)+O^(+))are identified.The absolute cross sections for producing individual ions and their total,as well as for the ion-pair dissociation channels are obtained by normalizing the data of CO^(+)to that of Ar^(+)from CO-Ar mixture target with a fixed 1:1 ratio.The overall errors are evaluated by considering various kinds of uncertainties.A comprehensive comparison is made with the available data,which shows a good agreement with each other over the energy ranges that are overlapped.This work presents new cross-section data with electron energies above 1000 eV.展开更多
Oxygenated carbon materials exhibit outstanding electrocatalytic performance in the production of hydrogen peroxide(H2O2)through a two-electron oxygen reduction reaction.The nature of the active functional group and u...Oxygenated carbon materials exhibit outstanding electrocatalytic performance in the production of hydrogen peroxide(H2O2)through a two-electron oxygen reduction reaction.The nature of the active functional group and underlying reaction mechanism,however,remain unclear.Here,a comprehensive workflow was established to identify the active sites from the numerous possible structures.The common hydroxyl group at the notched edge demonstrates a key role in the two-electron process.The local chemical environment weakens the binding of OOH intermediate to substrate while enhancing interaction with solution,thereby promoting the H_(2)O_(2)production.With increasing pH,the intramolecular hydrogen bond between OOH intermediate and hydroxyl decreases,facilitating OOH desorption.Furthermore,the rise in selectivity with increasing potential stems from the suppression of the four-electron process.The active site was further validated through experiments.Guided by theoretical understanding,optimal performance was achieved with high selectivity(>95%)and current density(2.06 mA/cm^(2))in experiment.展开更多
Water-quenched copper-nickel metallurgical slag enriched with olivine minerals exhibits promising potential for the production of CO_(2)-mineralized cementitious materials.In this work,copper-nickel slag-based cementi...Water-quenched copper-nickel metallurgical slag enriched with olivine minerals exhibits promising potential for the production of CO_(2)-mineralized cementitious materials.In this work,copper-nickel slag-based cementitious material(CNCM)was synthesized by using different chemical activation methods to enhance its hydration reactivity and CO_(2) mineralization capacity.Different water curing ages and carbonation conditions were explored related to their carbonation and mechanical properties development.Meanwhile,thermogravimetry differential scanning calorimetry and X-ray diffraction methods were applied to evaluate the CO_(2) adsorption amount and carbonation products of CNCM.Microstructure development of carbonated CNCM blocks was examined by backscattered electron imaging(BSE)with energy-dispersive X-ray spectrometry.Results showed that among the studied samples,the CNCM sample that was subjected to water curing for 3 d exhibited the highest CO_(2) sequestration amount of 8.51wt%at 80℃and 72 h while presenting the compressive strength of 39.07 MPa.This result indicated that 1 t of this CNCM can sequester 85.1 kg of CO_(2) and exhibit high compressive strength.Although the addition of citric acid did not improve strength development,it was beneficial to increase the CO_(2) diffusion and adsorption amount under the same carbonation conditions from BSE results.This work provides guidance for synthesizing CO_(2)-mineralized cementitious materials using large amounts of metallurgical slags containing olivine minerals.展开更多
Electrochemical reduction of CO_(2)(CO_(2)RR)has become a research hot spot in recent years in the context of carbon neutrality.HCOOH is one of the most promising products obtained by electrochemical reduction of CO_(...Electrochemical reduction of CO_(2)(CO_(2)RR)has become a research hot spot in recent years in the context of carbon neutrality.HCOOH is one of the most promising products obtained by electrochemical reduction of CO_(2) due to its high energy value as estimated by market price per energy unit and wide application in chemical industry.Biomass is the most abundant renewable resource in the natural world.Coupling biomass oxidative conversion with CO_(2)RR driven by renewable electricity would well achieve carbon negativity.In this work,we comprehensively reviewed the current research progress on CO_(2)RR to produce HCOOH and coupled system for conversion of biomass and its derivatives to produce value-added products.Sn-and Bi-based electrocatalysts are discussed for CO_(2)RR with regards to the structure of the catalyst and reaction mechanisms.Electro-oxidation reactions of biomass derived sugars,alcohols,furan aldehydes and even polymeric components of lignocellulose were reviewed as alternatives to replace oxygen evolution reaction(OER)in the conventional electrolysis process.It was recommended that to further improve the efficiency of the coupled system,future work should be focused on the development of more efficient and stable catalysts,careful design of the electrolytic cells for improving the mass transfer and development of environment-friendly processes for recovering the formed formate and biomass oxidation products.展开更多
The phase change of CO_(2) has a significant bearing on the siting, injection, and monitoring of storage. The phase state of CO_(2) is closely related to pressure. In the process of seismic exploration, the informatio...The phase change of CO_(2) has a significant bearing on the siting, injection, and monitoring of storage. The phase state of CO_(2) is closely related to pressure. In the process of seismic exploration, the information of formation pressure can be response in the seismic data. Therefore, it is possible to monitor the formation pressure using time-lapse seismic method. Apart from formation pressure, the information of porosity and CO_(2) saturation can be reflected in the seismic data. Here, based on the actual situation of the work area, a rockphysical model is proposed to address the feasibility of time-lapse seismic monitoring during CO_(2) storage in the anisotropic formation. The model takes into account the formation pressure, variety minerals composition, fracture, fluid inhomogeneous distribution, and anisotropy caused by horizontal layering of rock layers(or oriented alignment of minerals). From the proposed rockphysical model and the well-logging, cores and geological data at the target layer, the variation of P-wave and S-wave velocity with formation pressure after CO_(2) injection is calculated. And so are the effects of porosity and CO_(2) saturation. Finally, from anisotropic exact reflection coefficient equation, the reflection coefficients under different formation pressures are calculated. It is proved that the reflection coefficient varies with pressure. Compared with CO_(2) saturation, the pressure has a greater effect on the reflection coefficient. Through the convolution model, the seismic record is calculated. The seismic record shows the difference with different formation pressure. At present, in the marine CO_(2) sequestration monitoring domain, there is no study involving the effect of formation pressure changes on seismic records in seafloor anisotropic formation. This study can provide a basis for the inversion of reservoir parameters in anisotropic seafloor CO_(2) reservoirs.展开更多
In the carbonate industry,deep decarbonization strategies are necessary to effectively remediate CO_(2).These strategies mainly include both sustainable energy supplies and the conversion of CO_(2)in downstream proces...In the carbonate industry,deep decarbonization strategies are necessary to effectively remediate CO_(2).These strategies mainly include both sustainable energy supplies and the conversion of CO_(2)in downstream processes.This study developed a coupled process of biomass chemical looping H2 production and reductive calcination of CaCO_(3).Firstly,a mass and energy balance of the coupled process was established in Aspen Plus.Following this,process optimization and energy integration were implemented to provide optimized operation conditions.Lastly,a life cycle assessment was carried out to assess the carbon footprint of the coupled process.Results reveal that the decomposition temperature of CaCO_(3)in an H_(2)atmosphere can be reduced to 780℃(generally around 900℃),and the conversion of CO_(2)from CaCO_(3)decomposition reached 81.33%with an H2:CO ratio of 2.49 in gaseous products.By optimizing systemic energy through heat integration,an energy efficiency of 86.30%was achieved.Additionally,the carbon footprint analysis revealed that the process with energy integration had a low global warming potential(GWP)of-2.624 kg·kg^(-1)(CO_(2)/CaO).Conclusively,this work performed a systematic analysis of introducing biomass-derived H_(2)into CaCO_(3)calcination and demonstrated the positive role of reductive calcination using green H_(2)in mitigating CO_(2)emissions within the carbonate industry.展开更多
Drip irrigation and flood irrigation are major irrigation methods for maize crops in the Hetao Irrigation District,Inner Mongolia Autonomous Region,China.This research delves into the effects of these irrigation metho...Drip irrigation and flood irrigation are major irrigation methods for maize crops in the Hetao Irrigation District,Inner Mongolia Autonomous Region,China.This research delves into the effects of these irrigation methods on carbon dioxide(CO_(2))exchange and crop growth in this region.The experimental site was divided into drip and flood irrigation zones.The irrigation schedules of this study aligned with the local commonly used irrigation schedule.We employed a developed chamber system to measure the diurnal CO_(2)exchange of maize plants during various growth stages under both drip and flood irrigation methods.From May to September in 2020 and 2021,two sets of repeated experiments were conducted.In each experiment,a total of nine measurements of CO_(2)exchange were performed to obtain carbon exchange data at different growth stages of maize crop.During each CO_(2)exchange measurement event,CO_(2)flux data were collected every two hours over a day-long period to capture the diurnal variations in CO_(2)exchange.During each CO_(2)exchange measurement event,the biological parameters(aboveground biomass and crop growth rate)of maize and environmental parameters(including air humidity,air temperature,precipitation,soil water content,and photosynthetically active radiation)were measured.The results indicated a V-shaped trend in net ecosystem CO_(2)exchange in daytime,reducing slowly at night,while the net assimilation rate(net primary productivity)exhibited a contrasting trend.Notably,compared with flood irrigation,drip irrigation demonstrated significantly higher average daily soil CO_(2)emission and greater average daily CO_(2)absorption by maize plants.Consequently,within the maize ecosystem,drip irrigation appeared more conducive to absorbing atmospheric CO_(2).Furthermore,drip irrigation demonstrated a faster crop growth rate and increased aboveground biomass compared with flood irrigation.A strong linear relationship existed between leaf area index and light utilization efficiency,irrespective of the irrigation method.Notably,drip irrigation displayed superior light use efficiency compared with flood irrigation.The final yield results corroborated these findings,indicating that drip irrigation yielded higher harvest index and overall yield than flood irrigation.The results of this study provide a basis for the selection of optimal irrigation methods commonly used in the Hetao Irrigation District.This research also serves as a reference for future irrigation studies that consider measurements of both carbon emissions and yield simultaneously.展开更多
基金supported by the National Research Foundation of Korea(NRF)grants funded by the Ministry of Science and ICT(MSIT)(RS-2023-00251283,and 2022M3D1A2083618)by the Ministry of Education(2020R1A6A1A03040516).
文摘Advancements in sensor technology have significantly enhanced atmospheric monitoring.Notably,metal oxide and carbon(MO_(x)/C)hybrids have gained attention for their exceptional sensitivity and room-temperature sensing performance.However,previous methods of synthesizing MO_(x)/C composites suffer from problems,including inhomogeneity,aggregation,and challenges in micropatterning.Herein,we introduce a refined method that employs a metal–organic framework(MOF)as a precursor combined with direct laser writing.The inherent structure of MOFs ensures a uniform distribution of metal ions and organic linkers,yielding homogeneous MO_(x)/C structures.The laser processing facilitates precise micropatterning(<2μm,comparable to typical photolithography)of the MO_(x)/C crystals.The optimized MOF-derived MO_(x)/C sensor rapidly detected ethanol gas even at room temperature(105 and 18 s for response and recovery,respectively),with a broad range of sensing performance from 170 to 3,400 ppm and a high response value of up to 3,500%.Additionally,this sensor exhibited enhanced stability and thermal resilience compared to previous MOF-based counterparts.This research opens up promising avenues for practical applications in MOF-derived sensing devices.
基金supported by the National Natural Science Foundation of China(Nos.92163118,51972234)。
文摘The development of aqueous zinc ion battery cathode materials with high capacity and high magnification is still a challenge.Herein,porous vanadium oxide/carbon(p-VO_(x)@C,mainly VO_(2) with a small amount of V_(2)O_(3)) core/shell microspheres with oxygen vacancies are facilely fabricated by using a vanadium-based metal-organic framework(MIL-100(V)) as a sacrificial template.This unique structure can improve the conductivity of the VO_(x),accelerate electrolyte diffusion,and suppress structural collapse during circulation.Subsequently,H_(2)O molecules are introduced into the interlayer of VO_(x) through a highly efficient in-situ electrochemical activation process,facilitating the intercalation and diffusion of zinc ions.After the activation,an optimal sample exhibits a high specific capacity of 464.3 mA h g^(-1) at0.2 A g^(-1) and 395.2 mA h g^(-1) at 10 A g^(-1),indicating excellent rate performance.Moreover,the optimal sample maintains a capacity retention of about 89.3% after 2500 cycles at 10 A g^(-1).Density functional theory calculation demonstrates that the presence of oxygen vacancies and intercalated water molecules can significantly reduce the diffusion barrier for zinc ions.In addition,it is proved that the storage of zinc ions in the cathode is achieved by reversible intercalation/extraction during the charge and discharge process through various ex-situ analysis technologies.This work demonstrates that the p-VO_(x)@C has great potential for applications in aqueous ZIBs after electrochemical activation.
基金Financial support from the National Key Research and Development Program of China(2022YFB3805602)the National Natural Science Foundation of China(22138001,22288102)the Fundamental Research Funds for the Central Universities。
文摘Glycerol carbonate,an important glycerol value-added product,has been widely used as an active intermediate and inert solvent in the synthesis of cosmetics,detergents,chemical intermediates,polymers,and so on.The direct carbonylation from glycerol with CO_(2)is considered a promising route,but still tough work due to the thermodynamic stability and the kinetic inertness of CO_(2).In this work,highlyselective direct carbonylation of glycerol and CO_(2)into glycerol carbonate has been achieved over highly dispersed MgInCe-mixed metal oxides(MgInCe-MMO),which were prepared through the topological transformation derived from the MgInCe-layered double hydroxides(MgInCe-LDHs).By precisely modulating the surface basic-acidic properties and the oxygen vacancies,an efficient carbonylation of glycerol with CO_(2)has been achieved with a selectivity of up to>99%to glycerol carbonate.Deep investigation into the synergistic catalysis of base-acid sites and oxygen vacancies has been clarified.
基金Open Project of Jiangsu Key Laboratory for Eco-Agricultural Biotechnology around Hongze Lake,Grant Number HZHLAB2201.
文摘Carbon monoxide(CO)and nitric oxide(NO)are signal molecules that enhance plant adaptation to environmental stimuli.Auxin is an essential phytohormone for plant growth and development.CO and NO play crucial roles in modulating the plant’s response to iron deficiency.Iron deficiency leads to an increase in the activity of heme oxygenase(HO)and the subsequent generation of CO.Additionally,it alters the polar subcellular distribution of Pin-Formed 1(PIN1)proteins,resulting in enhanced auxin transport.This alteration,in turn,leads to an increase in NO accumulation.Furthermore,iron deficiency enhances the activity of ferric chelate reductase(FCR),as well as the expression of the Fer-like iron deficiency-induced transcription factor 1(FIT)and the ferric reduction oxidase 2(FRO2)genes in plant roots.Overexpression of the long hypocotyl 1(HY1)gene,which encodes heme oxygenase,or the CO donor treatment resulted in enhanced basipetal auxin transport,higher FCR activity,and the expression of FIT and FRO2 genes under Fe deficiency.Here,a potential mechanism is proposed:CO and NO interact with auxin to address iron deficiency stress.CO alters auxin transport,enhancing its accumulation in roots and up-regulating key iron-related genes like FRO2 and IRT1.Elevated auxin levels affect NO signaling,leading to greater sensitivity in root development.This interplay promotes FCR activity,which is crucial for iron absorption.Together,these molecules enhance iron uptake and root growth,revealing a novel aspect of plant physiology in adapting to environmental stress.
基金provided by Guizhou Provincial Science and Technology Projects for Platform and Talent Team Plan(GCC[2023]007)Fok Ying Tung Education Foundation(171095)National Natural Science Foundation of China(11964006).
文摘Considering the serious electromagnetic wave(EMW)pollution problems and complex application condition,there is a pressing need to amalgamate multiple functionalities within a single substance.However,the effective integration of diverse functions into designed EMW absorption materials still faces the huge challenges.Herein,reduced graphene oxide/carbon foams(RGO/CFs)with two-dimensional/three-dimensional(2D/3D)van der Waals(vdWs)heterostructures were meticulously engineered and synthesized utilizing an efficient methodology involving freeze-drying,immersing absorption,secondary freeze-drying,followed by carbonization treatment.Thanks to their excellent linkage effect of amplified dielectric loss and optimized impedance matching,the designed 2D/3D RGO/CFs vdWs heterostructures demonstrated commendable EMW absorption performances,achieving a broad absorption bandwidth of 6.2 GHz and a reflection loss of-50.58 dB with the low matching thicknesses.Furthermore,the obtained 2D/3D RGO/CFs vdWs heterostructures also displayed the significant radar stealth properties,good corrosion resistance performances as well as outstanding thermal insulation capabilities,displaying the great potential in complex and variable environments.Accordingly,this work not only demonstrated a straightforward method for fabricating 2D/3D vdWs heterostructures,but also outlined a powerful mixeddimensional assembly strategy for engineering multifunctional foams for electromagnetic protection,aerospace and other complex conditions.
基金CONCYTEC and PROCIENCIA agencies from Peru in the framework of the call for Basic Research Projects2019-01[contract number401-2019-FONDECYT].
文摘This study investigates the influence of electropolymerization conditions on the deposition of polypyrrole(PPy)onto cotton-derived carbon fiber(CF)modified with reduced graphene oxide(rGO)for supercapacitors applications using an experimental/theorical approach.The surface modification of CF by rGO and/or by PPy electrodeposited at 10,25 and 50 mV s^(-1) was thoroughly examined physicochemical and electrochemically.Composite electrodes comprising CF-rGo-PPy,synthesized via electropolymerization at 25 mV s^(-1),demonstrated a remarkable increase in capacitance,showcasing~742 F g^(-1) compared to 153 F g^(-1) for CF.SEM,N_(2)-surface area,XPS,and TD-DFT approach revealed that the higher capacitance observed in CF-rGo-PPy electrodes underscores the influence of morphology and charged nitrogen species on the electrochemical performance of these modified electrodes.Notably,this electrode material achieves a specific capacitance retention of~96%of their initial capacitance after 10000 cycles at 0.5 A g^(-1) measured in a two-electrodes cell configuration.This work also discusses the influence of the scan rate used for pyrrole electropolymerization on the pseudocapacitance contribution of PPy and its possible effect on the porosity of the material.These results highlight the importance of appropriate electropolymerization conditions that allow obtaining the synergistic effect between CF,rGO and PPy.
基金supported by the National Key R&D Program of China(2018YFA0901700)the National Natural Science Foundation of China(31970038,22278241)+1 种基金a grant from the Institute Guo Qiang,Tsinghua University(2021GQG1016)the Department of Chemical Engineering-i BHE Joint Cooperation Fund。
文摘The unabated carbon dioxide(CO_(2))emission into the atmosphere has exacerbated global climate change,resulting in extreme weather events,biodiversity loss,and an intensified greenhouse effect.To address these challenges and work toward carbon(C)neutrality and reduced CO_(2)emissions,the capture and utilization of CO_(2)have become imperative in both scientific research and industry.One cutting-edge approach to achieving efficient catalytic performance involves integrating green bioconversion and chemical conversion.This innovative strategy offers several advantages,including environmental friendliness,high efficiency,and multi-selectivity.This study provides a comprehensive review of existing technical routes for carbon sequestration(CS)and introduces two novel CS pathways:the electrochemicalbiological hybrid and artificial photosynthesis systems.It also thoroughly examines the synthesis of valuable Cnproducts from the two CS systems employing different catalysts and biocatalysts.As both systems heavily rely on electron transfer,direct and mediated electron transfer has been discussed and summarized in detail.Additionally,this study explores the conditions suitable for different catalysts and assesses the strengths and weaknesses of biocatalysts.We also explored the biocompatibility of the electrode materials and developed novel materials.These materials were specifically engineered to combine with enzymes or microbial cells to solve the biocompatibility problem,while improving the electron transfer efficiency of both.Furthermore,this review summarizes the relevant systems developed in recent years for manufacturing different products,along with their respective production efficiencies,providing a solid database for development in this direction.The novel chemical-biological combination proposed herein holds great promise for the future conversion of CO_(2)into advanced organic compounds.Additionally,it offers exciting prospects for utilizing CO_(2)in synthesizing a wide range of industrial products.Ultimately,the present study provides a unique perspective for achieving the vital goals of“peak shaving”and C-neutrality,contributing significantly to our collective efforts to combat climate change and its associated challenges.
基金supported by Future Trees Trust,The Patsy Wood Trust,Scottish Forestry Trust,Aitchinson Tait Trust,and Action Oak for fundingsupport from the UK Natural Environment Research Council (NE/S015833/1 (QUINTUS))+1 种基金support from the JABBS Trust,Norbury Park Estate,The John Horseman Trust,Ecological Continuity Trust,and the University of BirminghamAccess to BIFoR Core Data was funded by Royal Society University Research Fellowship URFR1191326
文摘Acorn production in oak(Quercus spp.)shows considerable inter-annual variation,known as masting,which provides a natural defence against seed predators but a highly-variable supply of acorns for uses such as in commercial tree planting each year.Anthropogenic emissions of greenhouse gases have been very widely reported to influence plant growth and seed or fruit size and quantity via the‘fertilisation effect’that leads to enhanced photosynthesis.To examine if acorn production in mature woodland communities will be affected by further increase in CO_(2),the contents of litter traps from a Free Air Carbon Enrichment(FACE)experiment in deciduous woodland in central England were analysed for numbers of flowers and acorns of pedunculate oak(Quercus robur L.)at different stages of development and their predation levels under ambient and elevated CO_(2) concentrations.Inter-annual variation in acorn numbers was considerable and cyclical between 2015 and 2021,with the greatest numbers of mature acorns in 2015,2017 and 2020 but almost none in 2018.The numbers of flowers,enlarged cups,immature acorns,empty acorn cups,and galls in the litter traps also varied amongst years;comparatively high numbers of enlarged cups were recorded in 2018,suggesting Q.robur at this site is a fruit maturation masting species(i.e.,the extent of abortion of pollinated flowers during acorn development affects mature acorn numbers greatly).Raising the atmospheric CO_(2) concentration by 150μL L^(−1),from early 2017,increased the numbers of immature acorns,and all acorn evidence(empty cups+immature acorns+mature acorns)detected in the litter traps compared to ambient controls by 2021,but did not consistently affect the numbers of flowers,enlarged cups,empty cups,or mature acorns.The number of flowers in the elevated CO_(2) plots’litter traps was greater in 2018 than 2017,one year after CO_(2) enrichment began,whereas numbers declined in ambient plots.Enrichment with CO_(2) also increased the number of oak knopper galls(Andricus quercuscalicis Burgsdorf).We conclude that elevated CO_(2) increased the occurrence of acorns developing from flowers,but the putative benefit to mature acorn numbers may have been hidden by excessive pre-and/or post-dispersal predation.There was no evidence that elevated CO_(2) altered masting behaviour.
基金supported in part by the National Key Research and Development Program of China(2022YFB3305300)the National Natural Science Foundation of China(62173178).
文摘Ethylene glycol(EG)plays a pivotal role as a primary raw material in the polyester industry,and the syngas-to-EG route has become a significant technical route in production.The carbon monoxide(CO)gas-phase catalytic coupling to synthesize dimethyl oxalate(DMO)is a crucial process in the syngas-to-EG route,whereby the composition of the reactor outlet exerts influence on the ultimate quality of the EG product and the energy consumption during the subsequent separation process.However,measuring product quality in real time or establishing accurate dynamic mechanism models is challenging.To effectively model the DMO synthesis process,this study proposes a hybrid modeling strategy that integrates process mechanisms and data-driven approaches.The CO gas-phase catalytic coupling mechanism model is developed based on intrinsic kinetics and material balance,while a long short-term memory(LSTM)neural network is employed to predict the macroscopic reaction rate by leveraging temporal relationships derived from archived measurements.The proposed model is trained semi-supervised to accommodate limited-label data scenarios,leveraging historical data.By integrating these predictions with the mechanism model,the hybrid modeling approach provides reliable and interpretable forecasts of mass fractions.Empirical investigations unequivocally validate the superiority of the proposed hybrid modeling approach over conventional data-driven models(DDMs)and other hybrid modeling techniques.
基金supported by the Research Grants Council(26206115,16304821 and 16309418)the Southern Marine Science and Engineering Guangdong Laboratory(Guangzhou)(SMSEGL20SC01)+2 种基金the Innovation and Technology Commission(grant no.ITC-CNERC14EG03)of the Hong Kong Special Administrative Regionthe Hong Kong Postdoctoral Fellowship Scheme(HKUST PDFS2021-4S12 and HKUST PDFS2021-6S08)the support from the Shenzhen fundamental research funding(JCYJ20210324115809026,20200925154115001,JCYJ20200109141216566)。
文摘Urea generation through electrochemical CO_(2) and NO_(3)~-co-reduction reaction(CO_(2)NO_(3)RR)is still limited by either the low selectivity or yield rate of urea.Herein,we report copper carbonate hydroxide(Cu_2(OH)_2CO_(3))as an efficient CO_(2)NO_(3)RR electrocatalyst with an impressive urea Faradaic efficiency of45.2%±2.1%and a high yield rate of 1564.5±145.2μg h~(-1)mg_(cat)~(-1).More importantly,H_(2) evolution is fully inhibited on this electrocatalyst over a wide potential range between-0.3 and-0.8 V versus reversible hydrogen electrode.Our thermodynamic simulation reveals that the first C-N coupling follows a unique pathway on Cu_2(OH)_2CO_(3) by combining the two intermediates,~*COOH and~*NHO.This work demonstrates that high selectivity and yield rate of urea can be simultaneously achieved on simple Cu-based electrocatalysts in CO_(2)NO_(3)RR,and provide guidance for rational design of more advanced catalysts.
基金jointly supported by the National Key Research and Development Program of China (Grant No. 2022YFC3105000)the Youth Innovation Promotion Association of CAS (2022074)+3 种基金the National Natural Science Foundation of China (Grant Nos. 42005123, 42275173 and 41706028)the National Key Research and Development Program of China(2022YFE0106500)the 7th Youth Talent Support Project of Ningxia Hui Autonomous Region Association for Science and TechnologyNational Key Scientific and Technological Infrastructure project ‘‘Earth System Science Numerical Simulator Facility’’(EarthLab) for supporting the simulations in this study
文摘Understanding the response of the Earth system to varying concentrations of carbon dioxide(CO_(2))is critical for projecting possible future climate change and for providing insight into mitigation and adaptation strategies in the near future.In this study,we generate a dataset by conducting an experiment involving carbon dioxide removal(CDR)—a potential way to suppress global warming—using the Chinese Academy of Sciences Earth System Model version 2.0(CASESM2.0).A preliminary evaluation is provided.The model is integrated from 200–340 years as a 1%yr^(−1) CO_(2) concentration increase experiment,and then to~478 years as a carbon dioxide removal experiment until CO_(2) returns to its original value.Finally,another 80 years is integrated in which CO_(2) is kept constant.Changes in the 2-m temperature,precipitation,sea surface temperature,ocean temperature,Atlantic meridional overturning circulation(AMOC),and sea surface height are all analyzed.In the ramp-up period,the global mean 2-m temperature and precipitation both increase while the AMOC weakens.Values of all the above variables change in the opposite direction in the ramp-down period,with a delayed peak relative to the CO_(2) peak.After CO_(2) returns to its original value,the global mean 2-m temperature is still~1 K higher than in the original state,and precipitation is~0.07 mm d^(–1) higher.At the end of the simulation,there is a~0.5°C increase in ocean temperature and a 1 Sv weakening of the AMOC.Our model simulation produces similar results to those of comparable experiments previously reported in the literature.
基金funded by the Top 10 key scientific and technological projects of CHN Energy in 2021 entitled Research and Demonstration of Technology for Carbon Dioxide Capture and Energy Recycling Utilization(GJNYKJ[2021]No.128,No.:GJNY-21-51)the Carbon Neutrality College(Yulin)Northwest University project entitled Design and research of large-scale CCUS cluster construction in Yulin area,Shaanxi Province(YL2022-38-01).
文摘The well-developed coal electricity generation and coal chemical industries have led to huge carbon dioxide(CO_(2))emissions in the northeastern Ordos Basin.The geological storage of CO_(2) in saline aquifers is an effective backup way to achieve carbon neutrality.In this case,the potential of saline aquifers for CO_(2) storage serves as a critical basis for subsequent geological storage project.This study calculated the technical control capacities of CO_(2) of the saline aquifers in the fifth member of the Shiqianfeng Formation(the Qian-5 member)based on the statistical analysis of the logging and the drilling and core data from more than 200 wells in the northeastern Ordos Basin,as well as the sedimentary facies,formation lithology,and saline aquifer development patterns of the Qian-5 member.The results show that(1)the reservoirs of saline aquifers in the Qian-5 member,which comprise distributary channel sand bodies of deltaic plains,feature low porosities and permeabilities;(2)The study area hosts three NNE-directed saline aquifer zones,where saline aquifers generally have a single-layer thickness of 3‒8 m and a cumulative thickness of 8‒24 m;(3)The saline aquifers of the Qian-5 member have a total technical control capacity of CO_(2) of 119.25×10^(6) t.With the largest scale and the highest technical control capacity(accounting for 61%of the total technical control capacity),the Jinjie-Yulin saline aquifer zone is an important prospect area for the geological storage of CO_(2) in the saline aquifers of the Qian-5 member in the study area.
基金financially supported by the National Natural Science Foundation of China(22176059,21777042,and 22076045)the authors would also like to acknowledge support from the Science and Technology Commission of Shanghai Municipality’s Yangfan Special Project(23YF1408400)the Fundamental Research Funds for the Central Universities.
文摘Despite the extensive application of advanced oxidation processes(AOPs)in water treatment,the efficiency of AOPs in eliminating various emerging contaminants such as halogenated antibiotics is constrained by a number of factors.Halogen moieties exhibit strong resistance to oxidative radicals,affecting the dehalogenation and detoxification efficiencies.To address these limitations of AOPs,advanced reduction processes(ARPs)have been proposed.Herein,a novel nucleophilic reductant—namely,the carbon dioxide radical anion(CO_(2)^(·-))—is introduced for the simultaneous degradation,dehalogenation,and detoxification of florfenicol(FF),a typical halogenated antibiotic.The results demonstrate that FF is completely eliminated by CO_(2)^(·-),with approximately 100%of Cland 46%of Freleased after 120 min of treatment.Simultaneous detoxification is observed,which exhibits a linear response to the release of free inorganic halogen ions(R^(2)=0.97,p<0.01).The formation of halogen-free products is the primary reason for the superior detoxification performance of this method,in comparison with conventional hydroxyl-radical-based AOPs.Products identification and density functional theory(DFT)calculations reveal the underlying dehalogenation mechanism,in which the chlorine moiety of FF is more susceptible than other moieties to nucleophilic attack by CO_(2)^(·-).Moreover,CO_(2)^(·-)-based ARPs exhibit superior dehalogenation efficiencies(>75%)in degrading a series of halogenated antibiotics,including chloramphenicol(CAP),thiamphenicol(THA),diclofenac(DLF),triclosan(TCS),and ciprofloxacin(CIP).The system shows high tolerance to the pH of the solution and the presence of natural water constituents,and demonstrates an excellent degradation performance in actual groundwater,indicating the strong application potential of CO_(2)^(·-)-based ARPs in real life.Overall,this study elucidates the feasibility of CO_(2)^(·-)for the simultaneous degradation,dehalogenation,and detoxification of halogenated antibiotics and provides a promising method for their regulation during water or wastewater treatment.
基金Project supported by the National Key Research and Development Program of China (Grant No.2022YFA1602502)the National Natural Science Foundation of China (Grant No.12127804)the Strategic Priority Research Program of the Chinese Academy of Sciences (Grant Nos.XDB34000000)。
文摘The absolute partial and total cross sections for electron impact ionization of carbon monoxide are reported for electron energies from 350 eV to 8000 eV.The product ions(CO^(+),C^(+),O^(+),CO^(2+),C^(2+),and O^(2+))are measured by employing an ion imaging mass spectrometer and two ion-pair dissociation channels(C^(+)+O^(+)and C^(2+)+O^(+))are identified.The absolute cross sections for producing individual ions and their total,as well as for the ion-pair dissociation channels are obtained by normalizing the data of CO^(+)to that of Ar^(+)from CO-Ar mixture target with a fixed 1:1 ratio.The overall errors are evaluated by considering various kinds of uncertainties.A comprehensive comparison is made with the available data,which shows a good agreement with each other over the energy ranges that are overlapped.This work presents new cross-section data with electron energies above 1000 eV.
基金supported by the National Natural Science Foundation of China(No.52171022,No.22105214)Zhejiang Provincial Natural Science Foundation of China(Grant No.LXR22B030001)+3 种基金Fujian Institute of Innovation and Chinese Academy of Sciences.K.C.Wong Education Foundation(GJTD-2019-13)the National Key Research and Development Program of China(2019YFB2203400)Ningbo Yongjiang Talent Introduction Programme(2021A-036-B)NingBo S&T Innovation 2025 Major Special Programme(No:2020z059)and the“111 Project”(B20030).
文摘Oxygenated carbon materials exhibit outstanding electrocatalytic performance in the production of hydrogen peroxide(H2O2)through a two-electron oxygen reduction reaction.The nature of the active functional group and underlying reaction mechanism,however,remain unclear.Here,a comprehensive workflow was established to identify the active sites from the numerous possible structures.The common hydroxyl group at the notched edge demonstrates a key role in the two-electron process.The local chemical environment weakens the binding of OOH intermediate to substrate while enhancing interaction with solution,thereby promoting the H_(2)O_(2)production.With increasing pH,the intramolecular hydrogen bond between OOH intermediate and hydroxyl decreases,facilitating OOH desorption.Furthermore,the rise in selectivity with increasing potential stems from the suppression of the four-electron process.The active site was further validated through experiments.Guided by theoretical understanding,optimal performance was achieved with high selectivity(>95%)and current density(2.06 mA/cm^(2))in experiment.
基金supported by the Intergovernmental International Science and Technology Innovation Cooperation Key Project of the National Key Research and Development Program of China (No.2022YFE0135100)the National Natural Science Foundation of China (No.52072171)+1 种基金the Beijing Nova Program (No.20220484057)the Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD).
文摘Water-quenched copper-nickel metallurgical slag enriched with olivine minerals exhibits promising potential for the production of CO_(2)-mineralized cementitious materials.In this work,copper-nickel slag-based cementitious material(CNCM)was synthesized by using different chemical activation methods to enhance its hydration reactivity and CO_(2) mineralization capacity.Different water curing ages and carbonation conditions were explored related to their carbonation and mechanical properties development.Meanwhile,thermogravimetry differential scanning calorimetry and X-ray diffraction methods were applied to evaluate the CO_(2) adsorption amount and carbonation products of CNCM.Microstructure development of carbonated CNCM blocks was examined by backscattered electron imaging(BSE)with energy-dispersive X-ray spectrometry.Results showed that among the studied samples,the CNCM sample that was subjected to water curing for 3 d exhibited the highest CO_(2) sequestration amount of 8.51wt%at 80℃and 72 h while presenting the compressive strength of 39.07 MPa.This result indicated that 1 t of this CNCM can sequester 85.1 kg of CO_(2) and exhibit high compressive strength.Although the addition of citric acid did not improve strength development,it was beneficial to increase the CO_(2) diffusion and adsorption amount under the same carbonation conditions from BSE results.This work provides guidance for synthesizing CO_(2)-mineralized cementitious materials using large amounts of metallurgical slags containing olivine minerals.
基金supported by the National Key R&D Program of China(2022YFA2105900)the National Natural Science Foundation of China(No.22178197)。
文摘Electrochemical reduction of CO_(2)(CO_(2)RR)has become a research hot spot in recent years in the context of carbon neutrality.HCOOH is one of the most promising products obtained by electrochemical reduction of CO_(2) due to its high energy value as estimated by market price per energy unit and wide application in chemical industry.Biomass is the most abundant renewable resource in the natural world.Coupling biomass oxidative conversion with CO_(2)RR driven by renewable electricity would well achieve carbon negativity.In this work,we comprehensively reviewed the current research progress on CO_(2)RR to produce HCOOH and coupled system for conversion of biomass and its derivatives to produce value-added products.Sn-and Bi-based electrocatalysts are discussed for CO_(2)RR with regards to the structure of the catalyst and reaction mechanisms.Electro-oxidation reactions of biomass derived sugars,alcohols,furan aldehydes and even polymeric components of lignocellulose were reviewed as alternatives to replace oxygen evolution reaction(OER)in the conventional electrolysis process.It was recommended that to further improve the efficiency of the coupled system,future work should be focused on the development of more efficient and stable catalysts,careful design of the electrolytic cells for improving the mass transfer and development of environment-friendly processes for recovering the formed formate and biomass oxidation products.
文摘The phase change of CO_(2) has a significant bearing on the siting, injection, and monitoring of storage. The phase state of CO_(2) is closely related to pressure. In the process of seismic exploration, the information of formation pressure can be response in the seismic data. Therefore, it is possible to monitor the formation pressure using time-lapse seismic method. Apart from formation pressure, the information of porosity and CO_(2) saturation can be reflected in the seismic data. Here, based on the actual situation of the work area, a rockphysical model is proposed to address the feasibility of time-lapse seismic monitoring during CO_(2) storage in the anisotropic formation. The model takes into account the formation pressure, variety minerals composition, fracture, fluid inhomogeneous distribution, and anisotropy caused by horizontal layering of rock layers(or oriented alignment of minerals). From the proposed rockphysical model and the well-logging, cores and geological data at the target layer, the variation of P-wave and S-wave velocity with formation pressure after CO_(2) injection is calculated. And so are the effects of porosity and CO_(2) saturation. Finally, from anisotropic exact reflection coefficient equation, the reflection coefficients under different formation pressures are calculated. It is proved that the reflection coefficient varies with pressure. Compared with CO_(2) saturation, the pressure has a greater effect on the reflection coefficient. Through the convolution model, the seismic record is calculated. The seismic record shows the difference with different formation pressure. At present, in the marine CO_(2) sequestration monitoring domain, there is no study involving the effect of formation pressure changes on seismic records in seafloor anisotropic formation. This study can provide a basis for the inversion of reservoir parameters in anisotropic seafloor CO_(2) reservoirs.
基金support from the National Natural Science Foundation of China(21978128,91934302)partial support from the State Key Laboratory of Materials-oriented Chemical Engineering(ZK202006)also acknowledged.Additionallysupported by the“Cultivation Program for The Excellent Doctoral Dissertation of Nanjing Tech University(3800124701)”.
文摘In the carbonate industry,deep decarbonization strategies are necessary to effectively remediate CO_(2).These strategies mainly include both sustainable energy supplies and the conversion of CO_(2)in downstream processes.This study developed a coupled process of biomass chemical looping H2 production and reductive calcination of CaCO_(3).Firstly,a mass and energy balance of the coupled process was established in Aspen Plus.Following this,process optimization and energy integration were implemented to provide optimized operation conditions.Lastly,a life cycle assessment was carried out to assess the carbon footprint of the coupled process.Results reveal that the decomposition temperature of CaCO_(3)in an H_(2)atmosphere can be reduced to 780℃(generally around 900℃),and the conversion of CO_(2)from CaCO_(3)decomposition reached 81.33%with an H2:CO ratio of 2.49 in gaseous products.By optimizing systemic energy through heat integration,an energy efficiency of 86.30%was achieved.Additionally,the carbon footprint analysis revealed that the process with energy integration had a low global warming potential(GWP)of-2.624 kg·kg^(-1)(CO_(2)/CaO).Conclusively,this work performed a systematic analysis of introducing biomass-derived H_(2)into CaCO_(3)calcination and demonstrated the positive role of reductive calcination using green H_(2)in mitigating CO_(2)emissions within the carbonate industry.
基金supported by the Shandong Province Natural Science Foundation Youth Branch(ZR2023QC157)the National Natural Science Foundation of China(51979233)+1 种基金the Key Research and Development Project of Shaanxi Province(2022KW-47,2022NY-220)the Heze University Doctoral Research Fund(XY21BS24,XY22BS17).
文摘Drip irrigation and flood irrigation are major irrigation methods for maize crops in the Hetao Irrigation District,Inner Mongolia Autonomous Region,China.This research delves into the effects of these irrigation methods on carbon dioxide(CO_(2))exchange and crop growth in this region.The experimental site was divided into drip and flood irrigation zones.The irrigation schedules of this study aligned with the local commonly used irrigation schedule.We employed a developed chamber system to measure the diurnal CO_(2)exchange of maize plants during various growth stages under both drip and flood irrigation methods.From May to September in 2020 and 2021,two sets of repeated experiments were conducted.In each experiment,a total of nine measurements of CO_(2)exchange were performed to obtain carbon exchange data at different growth stages of maize crop.During each CO_(2)exchange measurement event,CO_(2)flux data were collected every two hours over a day-long period to capture the diurnal variations in CO_(2)exchange.During each CO_(2)exchange measurement event,the biological parameters(aboveground biomass and crop growth rate)of maize and environmental parameters(including air humidity,air temperature,precipitation,soil water content,and photosynthetically active radiation)were measured.The results indicated a V-shaped trend in net ecosystem CO_(2)exchange in daytime,reducing slowly at night,while the net assimilation rate(net primary productivity)exhibited a contrasting trend.Notably,compared with flood irrigation,drip irrigation demonstrated significantly higher average daily soil CO_(2)emission and greater average daily CO_(2)absorption by maize plants.Consequently,within the maize ecosystem,drip irrigation appeared more conducive to absorbing atmospheric CO_(2).Furthermore,drip irrigation demonstrated a faster crop growth rate and increased aboveground biomass compared with flood irrigation.A strong linear relationship existed between leaf area index and light utilization efficiency,irrespective of the irrigation method.Notably,drip irrigation displayed superior light use efficiency compared with flood irrigation.The final yield results corroborated these findings,indicating that drip irrigation yielded higher harvest index and overall yield than flood irrigation.The results of this study provide a basis for the selection of optimal irrigation methods commonly used in the Hetao Irrigation District.This research also serves as a reference for future irrigation studies that consider measurements of both carbon emissions and yield simultaneously.