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 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
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
As a common precursor for supercritical CO_(2)(scCO_(2))deposition techniques,solubility data of organometallic complexes in scCO_(2)is crucial for the preparation of nanocomposites.Recently,metal acetylacetonates hav...As a common precursor for supercritical CO_(2)(scCO_(2))deposition techniques,solubility data of organometallic complexes in scCO_(2)is crucial for the preparation of nanocomposites.Recently,metal acetylacetonates have shown great potential for the preparation of single-atom catalytic materials.In this study,the solubilities of iron(Ⅲ)acetylacetonate(Fe(acac)3)and nickel(Ⅱ)acetylacetonate(Ni(acac)2)were measured at the temperature from 313.15 to 333.15 K and in the pressure range of 9.5–25.2 MPa to accumulate new solubility data.Solubility was measured using a static weight loss method.The semi-empirical models proposed by Chrastil and Sung et al.were used to correlate the solubility data of Fe(acac)3 and Ni(acac)2.The equations obtained can be used to predict the solubility of the same system in the experimental range.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
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
Production of light olefins from CO_(2), the primary greenhouse gases, is of great importance to mitigate the adverse effects of CO_(2) emission on environment and to supply the value-added products from nonpetroleum ...Production of light olefins from CO_(2), the primary greenhouse gases, is of great importance to mitigate the adverse effects of CO_(2) emission on environment and to supply the value-added products from nonpetroleum resource. However, development of robust catalyst with controllable selectivity and stability remains a challenge. Herein, we report that Zn-promoted Fe catalyst can boost the stable and selective production of light olefins from CO_(2). Specifically, the Zn-promoted Fe exhibits a highly stable activity and olefin selectivity over 200 h time-on-stream compared to the unpromoted Fe catalyst, primarily owing to the preservation of active χ-Fe_(5)C_(2) phase. Structural characterizations of the spent catalysts suggest that Zn substantially regulates the content of iron carbide on the surface and suppresses the reoxidation of bulk iron carbide during the reaction. DFT calculations confirm that adsorption of surface carbon atoms and graphene-like carbonaceous species are not thermochemically favored on Zn-promoted Fe catalyst. Carbon deposition by CAC coupling reactions of two surface carbon atoms and dehydrogenation of CH intermediate are also inhibited. Furthermore, the effects of Zn on antioxidation of iron carbide were also investigated. Zn favored the hydrogenation of surface adsorbed oxygen atoms to H_(2)O and the desorption of H_(2)O, which reduces the possibility of surface carbide being oxidized by the chemisorbed oxygen.展开更多
Mixed metal oxide(MMO) represents a critical class of materials that can allow for obtaining a dynamic interface between its components:reduced metal and its metal oxide counterpart during an electrocatalytic reaction...Mixed metal oxide(MMO) represents a critical class of materials that can allow for obtaining a dynamic interface between its components:reduced metal and its metal oxide counterpart during an electrocatalytic reaction.Here,a synthetic method utilizing a MOF-derived micro/mesoporous carbon as a template to prepare sub-2 nm MMO catalysts for CO_(2) electro reduction is reported.Starting from the zeolite imidazolate framework(ZIF-8),the pyrolyzed derivatives were used to synthesize sub-2 nm Pd-Ni MMO with different compositions.The Ni-rich(Pd_(20)-Ni_(80)/ZC) catalyst exhibits unexpectedly superior performance for CO production with an improved Faradaic efficiency(FE) of 95.3% at the current density of 200 mA cm^(-2) at-0.56 V vs.reversible hydrogen electrode(RHE) compared to other Pd-Ni compositions.X-ray photoelectron spectroscopy(XPS) analysis confirms the presence of Ni^(2+) and Pd^(2+) in all compositions,demonstrating the presence of MMO.Density functional theory(DFT) calculation reveals that the lower CO binding energy on the surface of the Pd_(20)-Ni_(80) cluster eases CO desorption,thus increasing its production.This work provides a general synthetic strategy for MMO electrocatalysts and can pave a new way for screening multimetallic catalysts with a dynamic electrochemical interface.展开更多
Through our newly-developed "chemical vapor deposition integrated process (ISVD-IP)'" using carbon OlOXlae (t..u2) as me raw matenal and only carbon source introduced, CO2 could be catalytically activated and c...Through our newly-developed "chemical vapor deposition integrated process (ISVD-IP)'" using carbon OlOXlae (t..u2) as me raw matenal and only carbon source introduced, CO2 could be catalytically activated and converted to a new solid-form product, i.e., carbon nanotubes (CO2-derived) at a quite high yield (the single-pass carbon yield in the solid-form carbon-product produced from CO2 catalytic capture and conversion was more than 30% at a single-pass carbon-base). For comparison, when only pure carbon dioxide was introduced using the conventional CVD method without integrated process, no solid-form carbon-material product could be formed. In the addition of saturated steam at room temperature in the feed for CVD, there were much more end-opening carbon nano-tubes produced, at a slightly higher carbon yield. These inspiring works opened a remarkable and alternative new approach for carbon dioxide catalytic capture to solid-form product, comparing with that of CO2 sequestration (CCS) or CO2 mineralization (solidification), etc. As a result, there was much less body volume and almost no greenhouse effect for this solid-form carbon-material than those of primitive carbon dioxide.展开更多
1 Introduction Nowadays, green chemistry has received increased attention. The use of water and scCO2 as a solvent or reagent is an important field for organic reactions and green chemistry both in laboratory and indu...1 Introduction Nowadays, green chemistry has received increased attention. The use of water and scCO2 as a solvent or reagent is an important field for organic reactions and green chemistry both in laboratory and industry.展开更多
Copolymerization of carbon dioxide with epichlorohydrin was successfully carried out by usingNd(P_(204))_3-Al(i-Bu)_3 as catalyst (P_(204))=(RO)_2 POO--,R=CH_3 (CH_2),CH(C_2H_5) CH_2--). Addi-tion of carbonyl compound...Copolymerization of carbon dioxide with epichlorohydrin was successfully carried out by usingNd(P_(204))_3-Al(i-Bu)_3 as catalyst (P_(204))=(RO)_2 POO--,R=CH_3 (CH_2),CH(C_2H_5) CH_2--). Addi-tion of carbonyl compounds into the catalyst decreased the carbon dioxide content of the copoly-mer to some extent. Compared to nonpolar solvents, ethereal and moderate polar solvents werefavourable to obtaining higher carbon dioxide content copolymer. The coincidence of these resultswith the assumed copolymerization scheme clearly indicated that the copolymerization proceeds via coordinate anionic mechanism.展开更多
The catalyzation of CoTPP for electrocarboxylation of alkyl halides, alkenes and ketones with CO_2 are studied. The electrocarboxylation of these organic compounds with CO_2 in the presenec of catalyst can occur at mo...The catalyzation of CoTPP for electrocarboxylation of alkyl halides, alkenes and ketones with CO_2 are studied. The electrocarboxylation of these organic compounds with CO_2 in the presenec of catalyst can occur at more positive potential than that of no catalyst. The products of electrocarboxylation were identified by UV, IR and GC-MS. The electrocarboxylation mechanisms of different organic compounds are discussed.展开更多
The development history of carbon capture,utilization and storage for enhanced oil recovery(CCUS-EOR)in China is comprehensively reviewed,which consists of three stages:research and exploration,field test and industri...The development history of carbon capture,utilization and storage for enhanced oil recovery(CCUS-EOR)in China is comprehensively reviewed,which consists of three stages:research and exploration,field test and industrial application.The breakthrough understanding of CO_(2) flooding mechanism and field practice in recent years and the corresponding supporting technical achievements of CCUS-EOR project are systematically described.The future development prospects are also pointed out.After nearly 60 years of exploration,the theory of CO_(2) flooding and storage suitable for continental sedimentary reservoirs in China has been innovatively developed.It is suggested that C7–C15 are also important components affecting miscibility of CO_(2) and crude oil.The mechanism of rapid recovery of formation energy by CO_(2) and significant improvement of block productivity and recovery factor has been verified in field tests.The CCUS-EOR reservoir engineering design technology for continental sedimentary reservoir is established.The technology of reservoir engineering parameter design and well spacing optimization has been developed,which focuses on maintaining miscibility to improve oil displacement efficiency and uniform displacement to improve sweep efficiency.The technology of CO_(2) capture,injection and production process,whole-system anticorrosion,storage monitoring and other whole-process supporting technologies have been initially formed.In order to realize the efficient utilization and permanent storage of CO_(2),it is necessary to take the oil reservoir in the oil-water transition zone into consideration,realize the large-scale CO_(2) flooding and storage in the area from single reservoir to the overall structural control system.The oil reservoir in the oil-water transition zone is developed by stable gravity flooding of injecting CO_(2) from structural highs.The research on the storage technology such as the conversion of residual oil and CO_(2) into methane needs to be carried out.展开更多
Molten carbonate is an excellent electrolyte for the electrochemical reduction of CO_(2)to carbonaceous materials.However,the electrolyte–electrode-reaction relationship has not been well understood.Herein,we propose...Molten carbonate is an excellent electrolyte for the electrochemical reduction of CO_(2)to carbonaceous materials.However,the electrolyte–electrode-reaction relationship has not been well understood.Herein,we propose a general descriptor,the CO_(2)activity,to reveal the electrolyte–electrode-reaction relationship by thermodynamic calculations and experimental studies.Experimental studies agree well with theoretical predictions that both cations(Li^(+),Ca^(2+),Sr^(2+)and Ba^(2+))and anions(BO_(2)^(-),Ti_(5)O_(14)^(8-),SiO_(3)^(2-))can modulate the CO_(2)activity to control both cathode and anode reactions in a typical molten carbonate electrolyzer in terms of tuning reaction products and overpotentials.In this regard,the reduction of CO_(3)^(2-)can be interpreted as the direct reduction of CO_(2)generated from the dissociated CO_(3)^(2-),and the CO_(2)activity can be used as a general descriptor to predict the electrode reaction in molten carbonate.Overall,the CO_(2)activity descriptor unlocks the electrolyte–electrode-reaction relationship,thereby providing fundamental insights into guiding molten carbonate CO_(2)electrolysis.展开更多
The excessive use of nonrenewable energy has brought about serious greenhouse effect.Converting CO_(2) into high-value-added chemicals is undoubtedly the best choice to solve energy problems.Due to the excellent cost-...The excessive use of nonrenewable energy has brought about serious greenhouse effect.Converting CO_(2) into high-value-added chemicals is undoubtedly the best choice to solve energy problems.Due to the excellent cost-effectiveness and dramatic catalytic performance,nickel-based catalysts have been considered as the most promising candidates for the electrocatalytic CO_(2) reduction reaction(eCO_(2)RR).In this work,the electrocatalytic reduction mechanism of CO_(2) over Ni-based materials is reviewed.The strategies to improve the eCO_(2)RR performance are emphasized.Moreover,the research on Ni-based materials for syngas generation is briefly summarized.Finally,the prospects of nickel-based materials in the eCO_(2)RR are provided with the hope of improving transition-metal-based electrocatalysts for eCO_(2)RR in the future.展开更多
CO_(2) electrolysis with solid oxide electrolytic cells(SOECs)using intermittently available renewable energy has potential applications for carbon neutrality and energy storage.In this study,a pulsed current strategy...CO_(2) electrolysis with solid oxide electrolytic cells(SOECs)using intermittently available renewable energy has potential applications for carbon neutrality and energy storage.In this study,a pulsed current strategy is used to replicate intermittent energy availability,and the stability and conversion rate of the cyclic operation by a large-scale flat-tube SOEC are studied.One hundred cycles under pulsed current ranging from -100 to -300 mA/cm^(2) with a total operating time of about 800 h were carried out.The results show that after 100 cycles,the cell voltage attenuates by 0.041%/cycle in the high current stage of−300 mA/cm^(2),indicating that the lifetime of the cell can reach up to about 500 cycles.The total CO_(2) conversion rate reached 52%,which is close to the theoretical value of 54.3% at -300 mA/cm^(2),and the calculated efficiency approached 98.2%,assuming heat recycling.This study illustrates the significant advantages of SOEC in efficient electrochemical energy conversion,carbon emission mitigation,and seasonal energy storage.展开更多
Micro-interface intensified reactor(MIR)can be applied in series/parallel in the absorption of CO_(2)in industrial gases by Na_(2)CO_(3)due to the ability to produce large numbers of stable microbubbles.This work focu...Micro-interface intensified reactor(MIR)can be applied in series/parallel in the absorption of CO_(2)in industrial gases by Na_(2)CO_(3)due to the ability to produce large numbers of stable microbubbles.This work focuses on the variation pattern of mass transfer characteristics parameters of the reaction gas in Na_(2)CO_(3) solution under the influence of different solution properties and operating parameters in the reaction of CO_(2)absorption by Na2CO3.The mass transfer characteristics parameters include bubble Sauter mean diameter,gas holdup,interfacial area,liquid side mass transfer coefficient,and liquid side volume mass transfer coefficient kLa.The solution properties and operating parameters include Na2CO3 concentration(0.05–2.0 mol·L^(-1)),superficial gas velocity(0.00221–0.01989 m·s^(-1)),superficial liquid velocity(0.00332–0.02984 m·s^(-1)),and ionic strength(1.42456–1.59588 mol·kg^(-1)).And volumetric mass transfer coeffi-cients kLa and superficial reaction rates r of the MIR and the bubble column reactor are compared in the reaction of sodium carbonate absorption of carbon dioxide,and the former shows a greater improvement under different solution properties and operating parameters.The enhanced role of MIR in mass transfer in non-homogeneous reactions is verified and the feasibility of industrial practical applications of MIR is demonstrated.展开更多
Although biomass-derived carbon(biochar)has been widely used in the energy field,the relation between the carbonization condition and the physical/chemical property of the product remains elusive.Here,we revealed the ...Although biomass-derived carbon(biochar)has been widely used in the energy field,the relation between the carbonization condition and the physical/chemical property of the product remains elusive.Here,we revealed the carbonization condition's effect on the morphology,surface property,and electrochemical performance of the obtained carbon.An open slit pore structure with shower-puff-like nanoparticles can be obtained by finely tuning the carbonization temperature,and its unique pore structure and surface properties enable the Li–O_(2) battery with cycling longevity(221 cycles with 99.8%Coulombic efficiency at 0.2 mA cm^(−2) and controlled discharge–charge depths of 500 mAh g^(−1))and high capacity(16,334 mAh g^(−1) at 0.02 mA cm^(−2)).This work provides a greater understanding of the mechanism of the biochar carbonization procedure under various pyrolysis conditions,paving the way for future study of energy storage devices.展开更多
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 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.
基金financial support from the National Key Research and Development Program of China(2020YFA0710202)the National Natural Science Foundation of China(21978043,U1662130)+1 种基金Inner Mongolia University of Technology Scientific Research Initial Funding(DC2300001240)Talent Introduction Support Project of Inner Mongolia(DC2300001426).
文摘As a common precursor for supercritical CO_(2)(scCO_(2))deposition techniques,solubility data of organometallic complexes in scCO_(2)is crucial for the preparation of nanocomposites.Recently,metal acetylacetonates have shown great potential for the preparation of single-atom catalytic materials.In this study,the solubilities of iron(Ⅲ)acetylacetonate(Fe(acac)3)and nickel(Ⅱ)acetylacetonate(Ni(acac)2)were measured at the temperature from 313.15 to 333.15 K and in the pressure range of 9.5–25.2 MPa to accumulate new solubility data.Solubility was measured using a static weight loss method.The semi-empirical models proposed by Chrastil and Sung et al.were used to correlate the solubility data of Fe(acac)3 and Ni(acac)2.The equations obtained can be used to predict the solubility of the same system in the experimental range.
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the funding support from Shanghai Sailing Program (19YF1411000)National Natural Science Foundation of China (21878080, 21808058)Ningxia Science Foundation (2019AAC03282)。
文摘Production of light olefins from CO_(2), the primary greenhouse gases, is of great importance to mitigate the adverse effects of CO_(2) emission on environment and to supply the value-added products from nonpetroleum resource. However, development of robust catalyst with controllable selectivity and stability remains a challenge. Herein, we report that Zn-promoted Fe catalyst can boost the stable and selective production of light olefins from CO_(2). Specifically, the Zn-promoted Fe exhibits a highly stable activity and olefin selectivity over 200 h time-on-stream compared to the unpromoted Fe catalyst, primarily owing to the preservation of active χ-Fe_(5)C_(2) phase. Structural characterizations of the spent catalysts suggest that Zn substantially regulates the content of iron carbide on the surface and suppresses the reoxidation of bulk iron carbide during the reaction. DFT calculations confirm that adsorption of surface carbon atoms and graphene-like carbonaceous species are not thermochemically favored on Zn-promoted Fe catalyst. Carbon deposition by CAC coupling reactions of two surface carbon atoms and dehydrogenation of CH intermediate are also inhibited. Furthermore, the effects of Zn on antioxidation of iron carbide were also investigated. Zn favored the hydrogenation of surface adsorbed oxygen atoms to H_(2)O and the desorption of H_(2)O, which reduces the possibility of surface carbide being oxidized by the chemisorbed oxygen.
基金supported by the National Research Foundation of Korea (NRF) Grant funded by the Korean Government (MSIT) (RS-2023-00210114)supported by the National Research Foundation of Korea (NRF) grant funded by the Korea government (MSIT) (NRF-2021R1C1C1004264 and NRF2021R1A4A1032114)+1 种基金supported by the National Research Foundation of Korea (NRF) Grant funded by the Korean Government (MSIT) (NRF-2022R1A4A1019296)supported by the National R&D Program through the National Research Foundation of Korea (NRF), funded by the Ministry of Science and ICT (2021M3D1A2051636)。
文摘Mixed metal oxide(MMO) represents a critical class of materials that can allow for obtaining a dynamic interface between its components:reduced metal and its metal oxide counterpart during an electrocatalytic reaction.Here,a synthetic method utilizing a MOF-derived micro/mesoporous carbon as a template to prepare sub-2 nm MMO catalysts for CO_(2) electro reduction is reported.Starting from the zeolite imidazolate framework(ZIF-8),the pyrolyzed derivatives were used to synthesize sub-2 nm Pd-Ni MMO with different compositions.The Ni-rich(Pd_(20)-Ni_(80)/ZC) catalyst exhibits unexpectedly superior performance for CO production with an improved Faradaic efficiency(FE) of 95.3% at the current density of 200 mA cm^(-2) at-0.56 V vs.reversible hydrogen electrode(RHE) compared to other Pd-Ni compositions.X-ray photoelectron spectroscopy(XPS) analysis confirms the presence of Ni^(2+) and Pd^(2+) in all compositions,demonstrating the presence of MMO.Density functional theory(DFT) calculation reveals that the lower CO binding energy on the surface of the Pd_(20)-Ni_(80) cluster eases CO desorption,thus increasing its production.This work provides a general synthetic strategy for MMO electrocatalysts and can pave a new way for screening multimetallic catalysts with a dynamic electrochemical interface.
基金the National 973 Program of Ministry of Sciences and Technologies of China(2011CB201202)the National Natural Science Foundation of China(20776089)
文摘Through our newly-developed "chemical vapor deposition integrated process (ISVD-IP)'" using carbon OlOXlae (t..u2) as me raw matenal and only carbon source introduced, CO2 could be catalytically activated and converted to a new solid-form product, i.e., carbon nanotubes (CO2-derived) at a quite high yield (the single-pass carbon yield in the solid-form carbon-product produced from CO2 catalytic capture and conversion was more than 30% at a single-pass carbon-base). For comparison, when only pure carbon dioxide was introduced using the conventional CVD method without integrated process, no solid-form carbon-material product could be formed. In the addition of saturated steam at room temperature in the feed for CVD, there were much more end-opening carbon nano-tubes produced, at a slightly higher carbon yield. These inspiring works opened a remarkable and alternative new approach for carbon dioxide catalytic capture to solid-form product, comparing with that of CO2 sequestration (CCS) or CO2 mineralization (solidification), etc. As a result, there was much less body volume and almost no greenhouse effect for this solid-form carbon-material than those of primitive carbon dioxide.
基金the National Natural Science Foundation of China(Nos.20332030,20572027,20625205 and 20772034)Natural Science Foundation of Guangdong Province,China(No.07118070).
文摘1 Introduction Nowadays, green chemistry has received increased attention. The use of water and scCO2 as a solvent or reagent is an important field for organic reactions and green chemistry both in laboratory and industry.
文摘Copolymerization of carbon dioxide with epichlorohydrin was successfully carried out by usingNd(P_(204))_3-Al(i-Bu)_3 as catalyst (P_(204))=(RO)_2 POO--,R=CH_3 (CH_2),CH(C_2H_5) CH_2--). Addi-tion of carbonyl compounds into the catalyst decreased the carbon dioxide content of the copoly-mer to some extent. Compared to nonpolar solvents, ethereal and moderate polar solvents werefavourable to obtaining higher carbon dioxide content copolymer. The coincidence of these resultswith the assumed copolymerization scheme clearly indicated that the copolymerization proceeds via coordinate anionic mechanism.
基金This work is supported by the National Natural Science Foundation of China
文摘The catalyzation of CoTPP for electrocarboxylation of alkyl halides, alkenes and ketones with CO_2 are studied. The electrocarboxylation of these organic compounds with CO_2 in the presenec of catalyst can occur at more positive potential than that of no catalyst. The products of electrocarboxylation were identified by UV, IR and GC-MS. The electrocarboxylation mechanisms of different organic compounds are discussed.
基金Supported by the China National Science and Technology Major Project(2016ZX05016).
文摘The development history of carbon capture,utilization and storage for enhanced oil recovery(CCUS-EOR)in China is comprehensively reviewed,which consists of three stages:research and exploration,field test and industrial application.The breakthrough understanding of CO_(2) flooding mechanism and field practice in recent years and the corresponding supporting technical achievements of CCUS-EOR project are systematically described.The future development prospects are also pointed out.After nearly 60 years of exploration,the theory of CO_(2) flooding and storage suitable for continental sedimentary reservoirs in China has been innovatively developed.It is suggested that C7–C15 are also important components affecting miscibility of CO_(2) and crude oil.The mechanism of rapid recovery of formation energy by CO_(2) and significant improvement of block productivity and recovery factor has been verified in field tests.The CCUS-EOR reservoir engineering design technology for continental sedimentary reservoir is established.The technology of reservoir engineering parameter design and well spacing optimization has been developed,which focuses on maintaining miscibility to improve oil displacement efficiency and uniform displacement to improve sweep efficiency.The technology of CO_(2) capture,injection and production process,whole-system anticorrosion,storage monitoring and other whole-process supporting technologies have been initially formed.In order to realize the efficient utilization and permanent storage of CO_(2),it is necessary to take the oil reservoir in the oil-water transition zone into consideration,realize the large-scale CO_(2) flooding and storage in the area from single reservoir to the overall structural control system.The oil reservoir in the oil-water transition zone is developed by stable gravity flooding of injecting CO_(2) from structural highs.The research on the storage technology such as the conversion of residual oil and CO_(2) into methane needs to be carried out.
基金funded by National Natural Science Foun-dation of China(No.52031008,21673162).
文摘Molten carbonate is an excellent electrolyte for the electrochemical reduction of CO_(2)to carbonaceous materials.However,the electrolyte–electrode-reaction relationship has not been well understood.Herein,we propose a general descriptor,the CO_(2)activity,to reveal the electrolyte–electrode-reaction relationship by thermodynamic calculations and experimental studies.Experimental studies agree well with theoretical predictions that both cations(Li^(+),Ca^(2+),Sr^(2+)and Ba^(2+))and anions(BO_(2)^(-),Ti_(5)O_(14)^(8-),SiO_(3)^(2-))can modulate the CO_(2)activity to control both cathode and anode reactions in a typical molten carbonate electrolyzer in terms of tuning reaction products and overpotentials.In this regard,the reduction of CO_(3)^(2-)can be interpreted as the direct reduction of CO_(2)generated from the dissociated CO_(3)^(2-),and the CO_(2)activity can be used as a general descriptor to predict the electrode reaction in molten carbonate.Overall,the CO_(2)activity descriptor unlocks the electrolyte–electrode-reaction relationship,thereby providing fundamental insights into guiding molten carbonate CO_(2)electrolysis.
基金support from the National Natural Science Foundation of China(52072389,52311530113)the Science and Technology Commission of Shanghai Municipality(22DZ1205600,20520760900)+2 种基金the Program of Shanghai Academic Research Leader(20XD1424300)for financial support.The authors also would like to express their gratitude to Tangshan Basic Research Funding Projects(23130210E),Hebei Province High-level Talent(Postdoctor)Funding Project(B2022003025)Key R&D projects of North China University of Science and Technology(ZD-ST-202301)Tangshan Talent Funding Project(A202202007)for their financial support.
文摘The excessive use of nonrenewable energy has brought about serious greenhouse effect.Converting CO_(2) into high-value-added chemicals is undoubtedly the best choice to solve energy problems.Due to the excellent cost-effectiveness and dramatic catalytic performance,nickel-based catalysts have been considered as the most promising candidates for the electrocatalytic CO_(2) reduction reaction(eCO_(2)RR).In this work,the electrocatalytic reduction mechanism of CO_(2) over Ni-based materials is reviewed.The strategies to improve the eCO_(2)RR performance are emphasized.Moreover,the research on Ni-based materials for syngas generation is briefly summarized.Finally,the prospects of nickel-based materials in the eCO_(2)RR are provided with the hope of improving transition-metal-based electrocatalysts for eCO_(2)RR in the future.
基金National Key Research&Development Project,Grant/Award Number:2017YFE0129300Ningbo Science and Technology Innovation 2025 Major Project,Grant/Award Numbers:2019B10046,2020Z107+2 种基金Zhejiang Provincial Key R&D Program,Grant/Award Number:2021C01101National Natural Science Foundation of China,Grant/Award Numbers:U20A20251,11932005The from 0 to 1 Innovative Program of CAS,Grant/Award Number:ZDBS-LY-JSC021。
文摘CO_(2) electrolysis with solid oxide electrolytic cells(SOECs)using intermittently available renewable energy has potential applications for carbon neutrality and energy storage.In this study,a pulsed current strategy is used to replicate intermittent energy availability,and the stability and conversion rate of the cyclic operation by a large-scale flat-tube SOEC are studied.One hundred cycles under pulsed current ranging from -100 to -300 mA/cm^(2) with a total operating time of about 800 h were carried out.The results show that after 100 cycles,the cell voltage attenuates by 0.041%/cycle in the high current stage of−300 mA/cm^(2),indicating that the lifetime of the cell can reach up to about 500 cycles.The total CO_(2) conversion rate reached 52%,which is close to the theoretical value of 54.3% at -300 mA/cm^(2),and the calculated efficiency approached 98.2%,assuming heat recycling.This study illustrates the significant advantages of SOEC in efficient electrochemical energy conversion,carbon emission mitigation,and seasonal energy storage.
基金Natural Science Foundation of Jiangsu Province(BK20210185)National Natural Science Foundation of China(22278202).
文摘Micro-interface intensified reactor(MIR)can be applied in series/parallel in the absorption of CO_(2)in industrial gases by Na_(2)CO_(3)due to the ability to produce large numbers of stable microbubbles.This work focuses on the variation pattern of mass transfer characteristics parameters of the reaction gas in Na_(2)CO_(3) solution under the influence of different solution properties and operating parameters in the reaction of CO_(2)absorption by Na2CO3.The mass transfer characteristics parameters include bubble Sauter mean diameter,gas holdup,interfacial area,liquid side mass transfer coefficient,and liquid side volume mass transfer coefficient kLa.The solution properties and operating parameters include Na2CO3 concentration(0.05–2.0 mol·L^(-1)),superficial gas velocity(0.00221–0.01989 m·s^(-1)),superficial liquid velocity(0.00332–0.02984 m·s^(-1)),and ionic strength(1.42456–1.59588 mol·kg^(-1)).And volumetric mass transfer coeffi-cients kLa and superficial reaction rates r of the MIR and the bubble column reactor are compared in the reaction of sodium carbonate absorption of carbon dioxide,and the former shows a greater improvement under different solution properties and operating parameters.The enhanced role of MIR in mass transfer in non-homogeneous reactions is verified and the feasibility of industrial practical applications of MIR is demonstrated.
基金supported by the National Natural Science Foundation of China(NSFC No.22179005)the BIT Research and Innovation Promoting Project(Grant No.2022YCXY008)supported by Cunzhong Zhang at the Beijing Institute of Technology.
文摘Although biomass-derived carbon(biochar)has been widely used in the energy field,the relation between the carbonization condition and the physical/chemical property of the product remains elusive.Here,we revealed the carbonization condition's effect on the morphology,surface property,and electrochemical performance of the obtained carbon.An open slit pore structure with shower-puff-like nanoparticles can be obtained by finely tuning the carbonization temperature,and its unique pore structure and surface properties enable the Li–O_(2) battery with cycling longevity(221 cycles with 99.8%Coulombic efficiency at 0.2 mA cm^(−2) and controlled discharge–charge depths of 500 mAh g^(−1))and high capacity(16,334 mAh g^(−1) at 0.02 mA cm^(−2)).This work provides a greater understanding of the mechanism of the biochar carbonization procedure under various pyrolysis conditions,paving the way for future study of energy storage devices.