Ordered porous cabon with a 2-D hexagonal structure,high specific surface area and large pore volume was synthesized through a twostep heating method using tri-block copolymer as template and phenolic resin as carbon ...Ordered porous cabon with a 2-D hexagonal structure,high specific surface area and large pore volume was synthesized through a twostep heating method using tri-block copolymer as template and phenolic resin as carbon precursor.The results indicated the electrochemical performance of the sulfur/carbon composites prepared with the ordered porous carbon was significantly affected by the pore structure of the carbon.Both the specific capacity and cycling stability of the sulfur/carbon composites were improved using the bimodal micro/meso-porous carbon frameworks with high surface area.Its initial discharge capacity can be as high as 1200 mAh·g-1 at a current density of 167.5 mA·g-1The improved capacity retention was obtained during the cell cycling as well.展开更多
The demand on low-carbon emission fabrication technologies for energy storage materials is increasing dramatically with the global interest on carbon neutrality.As a promising active material for metal-sulfur batterie...The demand on low-carbon emission fabrication technologies for energy storage materials is increasing dramatically with the global interest on carbon neutrality.As a promising active material for metal-sulfur batteries,sulfur is of great interest due to its high-energy-density and abundance.However,there is a lack of industry-friendly and low-carbon fabrication strategies for high-performance sulfur-based active particles,which,however,is in critical need by their practical success.Herein,based on a hail-inspired sulfur nano-storm(HSN)technology developed in our lab,we report an energy-saving,solvent-free strategy for producing core-shell sulfur/carbon electrode particles(CNT@AC-S)in minutes.The fabrication of the CNT@AC-S electrode particles only involves low-cost sulfur blocks,commercial carbon nanotubes(CNT)and activated carbon(AC)micro-particles with high specific surface area.Based on the above core-shell CNT@AC-S particles,sulfur cathode with a high sulfur-loading of 9.2 mg cm^(-2) delivers a stable area capacity of 6.6 mAh cm^(-2) over 100 cycles.Furthermore,even for sulfur cathode with a super-high sulfur content(72 wt%over the whole electrode),it still delivers a high area capacity of 9 mAh cm^(-2) over50 cycles in a quasi-lean electrolyte condition.In a nutshell,this study brings a green and industryfriendly fabrication strategy for cost-effective production of rationally designed S-rich electrode particles.展开更多
Aqueous zinc-sulfur batteries at room temperature hold great potential for next-generation energy storage technology due to their low cost,safety and high energy density.However,slow reaction kinetics and high activat...Aqueous zinc-sulfur batteries at room temperature hold great potential for next-generation energy storage technology due to their low cost,safety and high energy density.However,slow reaction kinetics and high activation energy at the sulfur cathode pose great challenges for the practical applications.Herein,biomass-derived carbon with single-atomic cobalt sites(MMPC-Co)is synthesized as the cathode in Zn-S batteries.The catalysis of single-atom Co sites greatly promotes the transform of cathode electrolyte interface(CEI)on the cathode surface,while offering accelerated charge transfer rate for high conversion reversibility and large electrochemical surface area(ECSA)for high electrocatalytic current.Furthermore,the rich pore structure not only physically limits sulfur loss,but also accelerates the transport of zinc ions.In addition,the large pore volume of MMPC-Co is able to relieve the stress effect caused by the volume expansion of Zn S during charge/discharge cycles,thereby maintaining the stability of electrode structure.Consequently,the sulfur cathode maintains a high specific capacity of 729.96 m A h g^(-1)after 500 cycles at4 A g^(-1),which is much better than most cathode materials reported in the literature.This work provides new insights into the design and development of room-temperature aqueous Zn-S batteries.展开更多
Understanding the adsorption interactions between carbon materials and sulfur compounds has far-reaching impacts,in addition to their well-known important role in energy storage and conversion,such as lithium-ion batt...Understanding the adsorption interactions between carbon materials and sulfur compounds has far-reaching impacts,in addition to their well-known important role in energy storage and conversion,such as lithium-ion batteries.In this paper,properties of intrinsic B or Si single-atom doped,and B-Si codoped graphene(GR)and graphdiyne(GDY)were investigated by using density functional theory-based calculations,in which the optimal doping configurations were explored for potential applications in adsorbing sulfur compounds.Results showed that both B or Si single-atom doping and B-Si codoping could substantially enhance the electron transport properties of GR and GDY,improving their surface activity.Notably,B and Si atoms displayed synergistic effects for the codoped configurations,where B-Si codoped GR/GDY exhibited much better performance in the adsorption of sulfurcontaining chemicals than single-atom doped systems.In addition,results demonstrated that,after B-Si codoping,the adsorption energy and charge transfer amounts of GDY with sulfur compounds were much larger than those of GR,indicating that B-Si codoped GDY might be a favorable material for more effectively interacting with sulfur reagents.展开更多
Transition metal-nitrogen-carbon(M-N-C)as a promising substitute for the conventional noble metalbased catalyst still suffers from low activity and durability for oxygen reduction reaction(ORR)in proton exchange membr...Transition metal-nitrogen-carbon(M-N-C)as a promising substitute for the conventional noble metalbased catalyst still suffers from low activity and durability for oxygen reduction reaction(ORR)in proton exchange membrane fuel cells(PEMFCs).To tackle the issue,herein,a new type of sulfur-doped ironnitrogen-hard carbon(S-Fe-N-HC)nanosheets with high activity and durability in acid media were developed by using a newly synthesized precursor of amide-based polymer with Fe ions based on copolymerizing two monomers of 2,5-thiophene dicarboxylic acid(TDA)as S source and 1,8-diaminonaphthalene(DAN)as N source via an amination reaction.The as-synthesized S-Fe-N-HC features highly dispersed atomic Fe Nxmoieties embedded into rich thiophene-S doped hard carbon nanosheets filled with highly twisted graphite-like microcrystals,which is distinguished from the majority of M-N-C with soft or graphitic carbon structures.These unique characteristics endow S-Fe-N-HC with high ORR activity and outstanding durability in 0.5 M H_(2)SO_(4).Its initial half-wave potential is 0.80 V and the corresponding loss is only 21 m V after 30,000 cycles.Meanwhile,its practical PEMFC performance is a maximum power output of 628.0 mW cm^(-2)and a slight power density loss is 83.0 m W cm^(-2)after 200-cycle practical operation.Additionally,theoretical calculation shows that the activity of Fe Nxmoieties on ORR can be further enhanced by sulfur doping at meta-site near FeN_(4)C.These results evidently demonstrate that the dual effect of hard carbon substrate and S doping derived from the precursor platform of amid-polymers can effectively enhance the activity and durability of Fe-N-C catalysts,providing a new guidance for developing advanced M-N-C catalysts for ORR.展开更多
Hydrogen sulfide(H_(2)S)is an industrial exhausted gas that is highly toxic to humans and the environment.Combining desulfurization and fabrication of cathode materials for lithium-sulfur batteries(LSBs)can solve this...Hydrogen sulfide(H_(2)S)is an industrial exhausted gas that is highly toxic to humans and the environment.Combining desulfurization and fabrication of cathode materials for lithium-sulfur batteries(LSBs)can solve this issue with a double benefit.Herein,the amino-functionalized lotus root-like carbon nanofibers(NH_(2)-PLCNFs)are prepared by the amination of electrospinning carbon nanofibers under dielectric barrier discharge plasma.Selective catalytic oxidation of H_(2)S to elemental sulfur(S)is achieved over the metalfree NH_(2)-PLCNFs catalyst,and the obtained composite S@NH_(2)-PLCNFs is further used as cathode in LSBs.NH_(2)-PLCNFs enable efficient desulfurization(removal capacity as high as 3.46 g H_(2)S g^(−1) catalyst)and strongly covalent stabilization of S on modified carbon nanofibers.LSBs equipped with S@NH_(2)-PLCNFs deliver a high specific capacity of 705.8 mA h g^(−1) at 1 C after 1000 cycles based on the spatial confinement and the covalent stabilization of electroactive materials on amino-functionalized porous carbon matrix.It is revealed that S@NH_(2)-PLCNFs obtained by this kind of chemical vapor deposition leads to a more homogeneous S distribution and superior electrochemical performance to the sample S/NH_(2)-PLCNF-M prepared by the traditional molten infusion.This work opens a new avenue for the combination of environment protection and energy storage.展开更多
Room-temperature sodium–sulfur(RT/Na–S)batteries are regarded as promising large-scale stationary energy storage systems owing to their high energy density and low cost as well as the earth-abundant reserves of sodi...Room-temperature sodium–sulfur(RT/Na–S)batteries are regarded as promising large-scale stationary energy storage systems owing to their high energy density and low cost as well as the earth-abundant reserves of sodium and sulfur.However,the diffusion of polysulfides and sluggish kinetics of conversion reactions are still major challenges for their application.Herein,we developed a powerful and functional separator to inhibit the shuttle effect by coating a lightweight three-dimensional cellulose nanofiber-derived carbon aerogel on a glass fiber separator(denoted NSCA@GF).The hierarchical porous structures,favorable electronic conductivity,and three-dimensional interconnected network of N,S-codoped carbon aerogel endow a multifunctional separator with strong polysulfide anchoring capability and fast reaction kinetics of polysulfide conversion,which can act as the barrier layer and an expanded current collector to increase sulfur utilization.Moreover,the hetero-doped N/S sites are believed to strengthen polysulfide anchoring capability via chemisorption and accelerate the redox kinetics of polysulfide conversion,which is confirmed from experimental and theoretical results.As a result,the assembled Na–S coin cells with the NSCA@GF separator showed a high reversible capacity(788.8 mAh g^(−1) at 0.1 C after 100 cycles)and superior cycling stability(only 0.059%capacity decay per cycle over 1000 cycles at 1 C),thereby demonstrating the significant potential for application in high-performance RT/Na–S batteries.展开更多
The development of simple and effective strategies to prepare electrocatalysts,which possess unique and stable structures comprised of metal/nonmetallic atoms for oxygen reduction reaction(ORR)and oxygen evolution rea...The development of simple and effective strategies to prepare electrocatalysts,which possess unique and stable structures comprised of metal/nonmetallic atoms for oxygen reduction reaction(ORR)and oxygen evolution reaction(OER),is currently an urgent issue.Herein,an efficient bifunctional electrocatalyst featured by ultralong N,S-doped carbon nano-hollow-sphere chains about 1300 nm with encapsulated Co nanoparticles(Co-CNHSCs)is developed.The multifunctional catalytic properties of Co together with the heteroatom-induced charge redistribution(i.e.,modulating the electronic structure of the active site)result in superior catalytic activities toward OER and ORR in alkaline media.The optimized catalyst Co-CNHSC-3 displays an outstanding electrocatalytic ability for ORR and OER,a high specific capacity of 1023.6 mAh gZn^(-1),and excellent reversibility after 80 h at 10mA cm^(-2)in a Zn-air battery system.This work presents a new strategy for the design and synthesis of efficient multifunctional carbon-based catalysts for energy storage and conversion devices.展开更多
Carbon materials are effective substitutes for Pt counter electrodes(CEs) in dye-sensitized solar cells(DSSCs). However, many of these materials, such as carbon nanotubes and graphene, are expensive and require comple...Carbon materials are effective substitutes for Pt counter electrodes(CEs) in dye-sensitized solar cells(DSSCs). However, many of these materials, such as carbon nanotubes and graphene, are expensive and require complex preparation process. Herein, waste lignin, recycled from hazardous black liquors,is used to create oxygen-nitrogen-sulfur codoped carbon microspheres for use in DSSC CEs through the facile process of low-temperature preoxidation and high-temperature self-activation. The large number of ester bonds formed by preoxidation increase the degree of cross-linking of the lignin chains, leading to the formation of highly disordered carbon with ample defect sites during pyrolysis. The presence of organic O/N/S components in the waste lignin results in high O/N/S doping of the pyrolysed carbon,which increases the electrolyte ion adsorption and accelerates the electron transfer at the CE/electrolyte interface, as confirmed by density functional theory(DFT) calculations. The presence of inorganic impurities enables the construction of a hierarchical micropore-rich carbon structure through the etching effect during self-activation, which can provide abundant catalytically active sites for the reversible adsorption/desorption of electrolyte ions. Under these synergistic effects, the DSSCs that use this novel carbon CE achieve a quite high power-conversion efficiency of 9.22%. To the best of our knowledge, the value is a new record reported so far for biomass-carbon-based DSSCs.展开更多
Carbonaceous materials are considered as ideal anode for potassium ion batteries(PIBs)due to their abundant resources and stable physical and chemical properties.However,improvements of reversible capacity and cycle p...Carbonaceous materials are considered as ideal anode for potassium ion batteries(PIBs)due to their abundant resources and stable physical and chemical properties.However,improvements of reversible capacity and cycle performance are still needed,aiming to the practical application.Herein,S/N/O tridoped carbon(SNOC)nanospheres are prepared by in-situ vulcanized polybenzoxazine.The S/N/O tridoped carbon matrix provides abundant active sites for potassium ion adsorption and effectively improves potassium storage capacity.Moreover,the SNOC nanospheres possess large carbon interlayer spacing and high specific surface area,which broaden the diffusion pathway of potassium ions and accelerate the electron transfer speed,resulting in excellent rate performance.As an anode for PIBs,SNOC shows attractive rate performance(438.5 mA h g^(-1) at 50 mA g^(-1) and 174.5 mA h g^(-1) at2000 mA g^(-1)),ultra-high reversible capacity(397.4 mA h g^(-1) at 100 mA g^(-1) after 700 cycles)and ultra-long cycling life(218.9 mA h g^(-1) at 2000 mA g^(-1) after 7300 cycles,123.1 mA h g^(-1) at3000 mA g^(-1) after 16500 cycles and full cell runs for 4000 cycles).Density functional theory calculation confirms that S/N/O tri-doping enhances the adsorption and diffusion of potassium ions,and in-situ Fourier-transform infrared explores explored the potassium storage mechanism of SNOC.展开更多
As the need for high-energy–density batteries continues to grow, lithium-sulfur(Li–S) batteries have become a highly promising next-generation energy solution due to their low cost and exceptional energy density com...As the need for high-energy–density batteries continues to grow, lithium-sulfur(Li–S) batteries have become a highly promising next-generation energy solution due to their low cost and exceptional energy density compared to commercially available Li-ion batteries. Research into carbon-based sulfur hosts for Li–S batteries has been ongoing for over two decades, leading to a significant number of publications and patents.However, the commercialization of Li–S batteries has yet to be realized. This can be attributed, in part, to the instability of the Li metal anode. However, even when considering just the cathode side, there is still no consensus on whether carbon-based hosts will prove to be the best sulfur hosts for the industrialization of Li–S batteries. Recently, there has been controversy surrounding the use of carbon-based materials as the ideal sulfur hosts for practical applications of Li–S batteries under high sulfur loading and lean electrolyte conditions. To address this question, it is important to review the results of research into carbon-based hosts, assess their strengths and weaknesses, and provide a clear perspective. This review systematically evaluates the merits and mechanisms of various strategies for developing carbon-based host materials for high sulfur loading and lean electrolyte conditions. The review covers structural design and functional optimization strategies in detail, providing a comprehensive understanding of the development of sulfur hosts. The review also describes the use of efficient machine learning methods for investigating Li–S batteries. Finally, the outlook section lists and discusses current trends, challenges, and uncertainties surrounding carbon-based hosts, and concludes by presenting our standpoint and perspective on the subject.展开更多
In this study,we isolated and cultured phytoplankton along the coast of China and measured the cellular carbon,nitrogen,and sulfur contents under four temperatures.The results showed that the contents of the cellular ...In this study,we isolated and cultured phytoplankton along the coast of China and measured the cellular carbon,nitrogen,and sulfur contents under four temperatures.The results showed that the contents of the cellular elements varied widely among different phytoplankton.We found that temperature is one of the important factors affecting the carbon,nitrogen,and sulfur contents in phytoplankton cells;however,the degree of influence of temperature is different for different kinds of phytoplankton.By measuring the nitrogen content in cells,we found that the C:N ratio indirectly measured in the experiment fluctuated in the range of 3.50-8.97,and the average C:N ratio was 5.52.In this experiment,we accurately measured the cell elemental contents at different temperatures and transformed the cell count results into carbon,nitrogen,and sulfur contents to express the biomass.This method ensures that the contribution of species that are small in number but with a large cell volume in biomass is considered.Moreover,this method comprehensively considers the interspecific differences of species and the uneven distribution of elements in phytoplankton cells,which is of significance in the estimation of marine carbon and nitrogen budget.The distribution of nitrogen content in marine phytoplankton can well indicate the marine eutrophication caused by human activities.Climate change can affect the community structure and element composition of marine phytoplankton,meanwhile marine carbon and nitrogen element can regulate the climate to a certain extent.展开更多
Due to low cost,high capacity,and high energy density,lithium–sulfur(Li–S)batteries have attracted much attention;however,their cycling performance was largely limited by the poor redox kinetics and low sulfur utili...Due to low cost,high capacity,and high energy density,lithium–sulfur(Li–S)batteries have attracted much attention;however,their cycling performance was largely limited by the poor redox kinetics and low sulfur utilization.Herein,predicted by density functional theory calculations,single‐atomic Co‐B2N2 site‐imbedded boron and nitrogen co‐doped carbon nanotubes(SA‐Co/BNC)were designed to accomplish high sulfur loading,fast kinetic,and long service period Li–S batteries.Experiments proved that Co‐B2N2 atomic sites can effectively catalyze lithium polysulfide conversion.Therefore,the electrodes delivered a specific capacity of 1106 mAh g−1 at 0.2 C after 100 cycles and exhibited an outstanding cycle performance over 1000 cycles at 1 C with a decay rate of 0.032%per cycle.Our study offers a new strategy to couple the combined effect of nanocarriers and single‐atomic catalysts in novel coordination environments for high‐performance Li–S batteries.展开更多
Exploring carbon emission effects based on the evolution of residents’ dietary structure to achieve the carbon neutrality goal and mitigate climate change is an important task.This study took China as the research ob...Exploring carbon emission effects based on the evolution of residents’ dietary structure to achieve the carbon neutrality goal and mitigate climate change is an important task.This study took China as the research object(data excluding Hong Kong,Macao and Taiwan) and used the carbon emission coefficient method to quantitatively measure the food carbon emissions from 1987–2020,then analyzed the carbon emission effects under the evolution of dietary structure.The results showed that during the study period,the Chinese dietary structure gradually changed to a high-carbon consumption pattern.The dietary structure of urban residents developed to a balanced one,while that of rural residents developed to a high-quality one.During the study period,the per capita food carbon emissions and total food consumption of Chinese showed an increasing trend.The per capita food carbon emissions of residents in urban and rural showed an overall upward trend.The total food carbon emissions in urban increased significantly,while that in rural increased first and then decreased.The influence of beef and mutton on carbon emissions is the highest in dietary structure.Compared with the balanced dietary pattern,the food carbon emissions of Chinese residents had not yet reached the peak,but were evolving to a high-carbon consumption pattern.展开更多
CO_(2)is one of the most important greenhouse gases(GHGs)in the earth’s atmosphere.Since the industrial era,anthropogenic activities have emitted excessive quantities of GHGs into the atmosphere,resulting in climate ...CO_(2)is one of the most important greenhouse gases(GHGs)in the earth’s atmosphere.Since the industrial era,anthropogenic activities have emitted excessive quantities of GHGs into the atmosphere,resulting in climate warming since the 1950s and leading to an increased frequency of extreme weather and climate events.In 2020,China committed to striving for carbon neutrality by 2060.This commitment and China’s consequent actions will result in significant changes in global and regional anthropogenic carbon emissions and therefore require timely,comprehensive,and objective monitoring and verification support(MVS)systems.The MVS approach relies on the top-down assimilation and inversion of atmospheric CO_(2)concentrations,as recommended by the Intergovernmental Panel on Climate Change(IPCC)Inventory Guidelines in 2019.However,the regional high-resolution assimilation and inversion method is still in its initial stage of development.Here,we have constructed an inverse system for carbon sources and sinks at the kilometer level by coupling proper orthogonal decomposition(POD)with four-dimensional variational(4DVar)data assimilation based on the weather research and forecasting-greenhouse gas(WRF-GHG)model.Our China Carbon Monito ring and Verification Support at the Regional level(CCMVS-R)system can continuously assimilate information on atmospheric CO_(2)and other related information and realize the inversion of regional and local anthropogenic carbon emissions and natural terrestrial ecosystem carbon exchange.Atmospheric CO_(2)data were collected from six ground-based monito ring sites in Shanxi Province,China to verify the inversion effect of regio nal anthropogenic carbon emissions by setting ideal and real experiments using a two-layer nesting method(at 27 and 9 km).The uncertainty of the simulated atmospheric CO_(2)decreased significantly,with a root-mean-square error of CO_(2)concentration values between the ideal value and the simulated after assimilation was close to 0.The total anthropogenic carbon emissions in Shanxi Province in 2019 from the assimilated inversions were approximately 28.6%(17%-38%)higher than the mean of five emission inventories using the bottomup method,showing that the top-down CCMVS-R system can obtain more comprehensive information on anthropogenic carbon emissions.展开更多
The overall performance of metal catalysts can be efficiently adjusted by modifying carbon carriers with different valence sulfur precursors.The wet impregnation technique successfully prepared carbon material carrier...The overall performance of metal catalysts can be efficiently adjusted by modifying carbon carriers with different valence sulfur precursors.The wet impregnation technique successfully prepared carbon material carriers doped with varying sources of sulfur(Na_(2)SO_(4),NaHSO_(3),Na_(2)S·9H_(2)O).Palladium carbon catalysts doped with different sulfur precursors had been prepared with the aid of the liquid-phase reduction method of the selective hydrogenation of o-chloronitrobenzene(o-CNB)to o-chloroaniline(o-CAN).The catalyst prepared for Na_(2)S·9H_(2)O as a precursor has excellent performance,and the selectivity for o-CAN is more than 99.9%at 100%conversion.In addition,the characterization results show that with the decrease of S valence,the electronic effect between S and Pd increases,and the outer electron shift of Pd increases,which reduces the adsorption and dissociation ability of Pd to hydrogen,resulting in excellent selectivity.The effects provided a good idea for the hydrogenation of o-CNB and a different point of view on sulfur doping in a variety of hydrogenation reactions.展开更多
Bifunctional hybrid anodes(BHAs),which are both a high-performance active host material for lithium-ion storage as well as a guiding agent for homogeneous lithium metal nucleation and growth,exhibit significant potent...Bifunctional hybrid anodes(BHAs),which are both a high-performance active host material for lithium-ion storage as well as a guiding agent for homogeneous lithium metal nucleation and growth,exhibit significant potential as anodes for next-generation high-energy-density lithium-ion batteries(LIBs).In this study,sulfur-doped hard carbon nanosphere assemblies(S-HCNAs)were prepared through a hydrothermal treatment of a liquid organic precursor,followed by high-temperature thermal annealing with elemental sulfur for application as BHAs for LIBs.In a carbonate-based electrolyte containing fluoroethylene carbonate additive,the S-HCNAs showed high lithium-ion storage capacities in sloping as well as plateau voltage sections,good rate capabilities,and stable cyclabilities.In addition,high average Coulombic efficiencies(CEs)of~96.9%were achieved for dual lithium-ion and lithium metal storage cycles.In the LIB full-cell tests with typical NCM811 cathodes,the S-HCNA-based BHAs containing~400 mA h g^(−1) of excess lithium led to high energy and power densities of~500Wh kg^(−1) and~1695Wkg^(−1),respectively,and a stable cycling performance with~100%CEs was achieved.展开更多
Chinese cabbage(Brassica rapa ssp. pekinensis) has a long cultivation history and is one of the vegetable crops with the largest cultivation area in China. However, salt stress severely damages photosynthesis and horm...Chinese cabbage(Brassica rapa ssp. pekinensis) has a long cultivation history and is one of the vegetable crops with the largest cultivation area in China. However, salt stress severely damages photosynthesis and hormone metabolism, nutritional balances, and results in ion toxicity in plants. To better understand the mechanisms of salt-induced growth inhibition in Chinese cabbage, RNA-seq and physiological index determination were conducted to explore the impacts of salt stress on carbon cycle metabolism and photosynthesis in Chinese cabbage. Here, we found that the number of thylakoids and grana lamellae and the content of starch granules and chlorophyll in the leaves of Chinese cabbage under salt stress showed a time-dependent response, first increasing and then decreasing. Chinese cabbage increased the transcript levels of genes related to the photosynthetic apparatus and carbon metabolism under salt stress, probably in an attempt to alleviate damage to the photosynthetic system and enhance CO_(2) fixation and energy metabolism. The transcription of genes related to starch and sucrose synthesis and degradation were also enhanced;this might have been an attempt to maintain intracellular osmotic pressure by increasing soluble sugar concentrations. Soluble sugars could also be used as potential reactive oxygen species(ROS) scavengers, in concert with peroxidase(POD)enzymes, to eliminate ROS that accumulate during metabolic processes. Our study characterizes the synergistic response network of carbon metabolism and photosynthesis under salt stress.展开更多
The metal-organic framework(MOF)derived Ni–Co–C–N composite alloys(NiCCZ)were“embedded”inside the carbon cloth(CC)strands as opposed to the popular idea of growing them upward to realize ultrastable energy storag...The metal-organic framework(MOF)derived Ni–Co–C–N composite alloys(NiCCZ)were“embedded”inside the carbon cloth(CC)strands as opposed to the popular idea of growing them upward to realize ultrastable energy storage and conversion application.The NiCCZ was then oxygen functionalized,facilitating the next step of stoichiometric sulfur anion diffusion during hydrothermal sulfurization,generating a flower-like metal hydroxysulfide structure(NiCCZOS)with strong partial implantation inside CC.Thus obtained NiCCZOS shows an excellent capacity when tested as a supercapacitor electrode in a three-electrode configuration.Moreover,when paired with the biomass-derived nitrogen-rich activated carbon,the asymmetric supercapacitor device shows almost 100%capacity retention even after 45,000 charge–discharge cycles with remarkable energy density(59.4 Wh kg^(-1)/263.8μWh cm^(–2))owing to a uniquely designed cathode.Furthermore,the same electrode performed as an excellent bifunctional water-splitting electrocatalyst with an overpotential of 271 mV for oxygen evolution reaction(OER)and 168.4 mV for hydrogen evolution reaction(HER)at 10 mA cm−2 current density along with 30 h of unhinged chronopotentiometric stability performance for both HER and OER.Hence,a unique metal chalcogenide composite electrode/substrate configuration has been proposed as a highly stable electrode material for flexible energy storage and conversion applications.展开更多
Enzyme-induced carbonate precipitation(EICP)is an emanating,eco-friendly and potentially sound technique that has presented promise in various geotechnical applications.However,the durability and microscopic character...Enzyme-induced carbonate precipitation(EICP)is an emanating,eco-friendly and potentially sound technique that has presented promise in various geotechnical applications.However,the durability and microscopic characteristics of EICP-treated specimens against the impact of drying-wetting(D-W)cycles is under-explored yet.This study investigates the evolution of mechanical behavior and pore charac-teristics of EICP-treated sea sand subjected to D-W cycles.The uniaxial compressive strength(UCS)tests,synchrotron radiation micro-computed tomography(micro-CT),and three-dimensional(3D)recon-struction of CT images were performed to study the multiscale evolution characteristics of EICP-reinforced sea sand under the effect of D-W cycles.The potential correlations between microstructure characteristics and macro-mechanical property deterioration were investigated using gray relational analysis(GRA).Results showed that the UCS of EICP-treated specimens decreases by 63.7% after 15 D-W cycles.The proportion of mesopores gradually decreases whereas the proportion of macropores in-creases due to the exfoliated calcium carbonate with increasing number of D-W cycles.The micro-structure in EICP-reinforced sea sand was gradually disintegrated,resulting in increasing pore size and development of pore shape from ellipsoidal to columnar and branched.The gray relational degree suggested that the weight loss rate and UCS deterioration were attributed to the development of branched pores with a size of 100-1000 m m under the action of D-W cycles.Overall,the results in this study provide a useful guidancee for the long-term stability and evolution characteristics of EICP-reinforced sea sand under D-W weathering conditions.展开更多
基金supported by the National High Technology Research and Development Program of China(863 Program)the Strategic Priority Research Program of the Chinese Academy of Sciences
文摘Ordered porous cabon with a 2-D hexagonal structure,high specific surface area and large pore volume was synthesized through a twostep heating method using tri-block copolymer as template and phenolic resin as carbon precursor.The results indicated the electrochemical performance of the sulfur/carbon composites prepared with the ordered porous carbon was significantly affected by the pore structure of the carbon.Both the specific capacity and cycling stability of the sulfur/carbon composites were improved using the bimodal micro/meso-porous carbon frameworks with high surface area.Its initial discharge capacity can be as high as 1200 mAh·g-1 at a current density of 167.5 mA·g-1The improved capacity retention was obtained during the cell cycling as well.
基金supported by the Double First-Class Construction Funds of Sichuan University and National Natural Science Foundation of China(NNSFC)financial support from the National Science Foundation of China(51873126,51422305,51721091)。
文摘The demand on low-carbon emission fabrication technologies for energy storage materials is increasing dramatically with the global interest on carbon neutrality.As a promising active material for metal-sulfur batteries,sulfur is of great interest due to its high-energy-density and abundance.However,there is a lack of industry-friendly and low-carbon fabrication strategies for high-performance sulfur-based active particles,which,however,is in critical need by their practical success.Herein,based on a hail-inspired sulfur nano-storm(HSN)technology developed in our lab,we report an energy-saving,solvent-free strategy for producing core-shell sulfur/carbon electrode particles(CNT@AC-S)in minutes.The fabrication of the CNT@AC-S electrode particles only involves low-cost sulfur blocks,commercial carbon nanotubes(CNT)and activated carbon(AC)micro-particles with high specific surface area.Based on the above core-shell CNT@AC-S particles,sulfur cathode with a high sulfur-loading of 9.2 mg cm^(-2) delivers a stable area capacity of 6.6 mAh cm^(-2) over 100 cycles.Furthermore,even for sulfur cathode with a super-high sulfur content(72 wt%over the whole electrode),it still delivers a high area capacity of 9 mAh cm^(-2) over50 cycles in a quasi-lean electrolyte condition.In a nutshell,this study brings a green and industryfriendly fabrication strategy for cost-effective production of rationally designed S-rich electrode particles.
基金the financial support from the National Natural Science Foundation of China,China(No.52172058)。
文摘Aqueous zinc-sulfur batteries at room temperature hold great potential for next-generation energy storage technology due to their low cost,safety and high energy density.However,slow reaction kinetics and high activation energy at the sulfur cathode pose great challenges for the practical applications.Herein,biomass-derived carbon with single-atomic cobalt sites(MMPC-Co)is synthesized as the cathode in Zn-S batteries.The catalysis of single-atom Co sites greatly promotes the transform of cathode electrolyte interface(CEI)on the cathode surface,while offering accelerated charge transfer rate for high conversion reversibility and large electrochemical surface area(ECSA)for high electrocatalytic current.Furthermore,the rich pore structure not only physically limits sulfur loss,but also accelerates the transport of zinc ions.In addition,the large pore volume of MMPC-Co is able to relieve the stress effect caused by the volume expansion of Zn S during charge/discharge cycles,thereby maintaining the stability of electrode structure.Consequently,the sulfur cathode maintains a high specific capacity of 729.96 m A h g^(-1)after 500 cycles at4 A g^(-1),which is much better than most cathode materials reported in the literature.This work provides new insights into the design and development of room-temperature aqueous Zn-S batteries.
基金the support of the National Natural Science Foundation of China(Grant No.51472074).
文摘Understanding the adsorption interactions between carbon materials and sulfur compounds has far-reaching impacts,in addition to their well-known important role in energy storage and conversion,such as lithium-ion batteries.In this paper,properties of intrinsic B or Si single-atom doped,and B-Si codoped graphene(GR)and graphdiyne(GDY)were investigated by using density functional theory-based calculations,in which the optimal doping configurations were explored for potential applications in adsorbing sulfur compounds.Results showed that both B or Si single-atom doping and B-Si codoping could substantially enhance the electron transport properties of GR and GDY,improving their surface activity.Notably,B and Si atoms displayed synergistic effects for the codoped configurations,where B-Si codoped GR/GDY exhibited much better performance in the adsorption of sulfurcontaining chemicals than single-atom doped systems.In addition,results demonstrated that,after B-Si codoping,the adsorption energy and charge transfer amounts of GDY with sulfur compounds were much larger than those of GR,indicating that B-Si codoped GDY might be a favorable material for more effectively interacting with sulfur reagents.
基金finically supported by the National Natural Science Foundation of China(22075055)the Guangxi Science and Technology Project(AB16380030)。
文摘Transition metal-nitrogen-carbon(M-N-C)as a promising substitute for the conventional noble metalbased catalyst still suffers from low activity and durability for oxygen reduction reaction(ORR)in proton exchange membrane fuel cells(PEMFCs).To tackle the issue,herein,a new type of sulfur-doped ironnitrogen-hard carbon(S-Fe-N-HC)nanosheets with high activity and durability in acid media were developed by using a newly synthesized precursor of amide-based polymer with Fe ions based on copolymerizing two monomers of 2,5-thiophene dicarboxylic acid(TDA)as S source and 1,8-diaminonaphthalene(DAN)as N source via an amination reaction.The as-synthesized S-Fe-N-HC features highly dispersed atomic Fe Nxmoieties embedded into rich thiophene-S doped hard carbon nanosheets filled with highly twisted graphite-like microcrystals,which is distinguished from the majority of M-N-C with soft or graphitic carbon structures.These unique characteristics endow S-Fe-N-HC with high ORR activity and outstanding durability in 0.5 M H_(2)SO_(4).Its initial half-wave potential is 0.80 V and the corresponding loss is only 21 m V after 30,000 cycles.Meanwhile,its practical PEMFC performance is a maximum power output of 628.0 mW cm^(-2)and a slight power density loss is 83.0 m W cm^(-2)after 200-cycle practical operation.Additionally,theoretical calculation shows that the activity of Fe Nxmoieties on ORR can be further enhanced by sulfur doping at meta-site near FeN_(4)C.These results evidently demonstrate that the dual effect of hard carbon substrate and S doping derived from the precursor platform of amid-polymers can effectively enhance the activity and durability of Fe-N-C catalysts,providing a new guidance for developing advanced M-N-C catalysts for ORR.
基金financial support from projects funded by the National Natural Science Foundation of China(22179017,52172038).
文摘Hydrogen sulfide(H_(2)S)is an industrial exhausted gas that is highly toxic to humans and the environment.Combining desulfurization and fabrication of cathode materials for lithium-sulfur batteries(LSBs)can solve this issue with a double benefit.Herein,the amino-functionalized lotus root-like carbon nanofibers(NH_(2)-PLCNFs)are prepared by the amination of electrospinning carbon nanofibers under dielectric barrier discharge plasma.Selective catalytic oxidation of H_(2)S to elemental sulfur(S)is achieved over the metalfree NH_(2)-PLCNFs catalyst,and the obtained composite S@NH_(2)-PLCNFs is further used as cathode in LSBs.NH_(2)-PLCNFs enable efficient desulfurization(removal capacity as high as 3.46 g H_(2)S g^(−1) catalyst)and strongly covalent stabilization of S on modified carbon nanofibers.LSBs equipped with S@NH_(2)-PLCNFs deliver a high specific capacity of 705.8 mA h g^(−1) at 1 C after 1000 cycles based on the spatial confinement and the covalent stabilization of electroactive materials on amino-functionalized porous carbon matrix.It is revealed that S@NH_(2)-PLCNFs obtained by this kind of chemical vapor deposition leads to a more homogeneous S distribution and superior electrochemical performance to the sample S/NH_(2)-PLCNF-M prepared by the traditional molten infusion.This work opens a new avenue for the combination of environment protection and energy storage.
基金support of the Guangdong Basic and Applied Basic Research Foundation(grant nos.2020A1515110705 and 2021A1515110245)the China Postdoctoral Science Foundation(grant nos.2020M682711 and 2020M682710)+2 种基金the National Program for Support of Topnotch Young Professionals(grant no.x2qsA4210090)the National Natural Science Foundation of China(grant no.31971614)the State Key Laboratory of Pulp and Paper Engineering(grant no.2020C03).
文摘Room-temperature sodium–sulfur(RT/Na–S)batteries are regarded as promising large-scale stationary energy storage systems owing to their high energy density and low cost as well as the earth-abundant reserves of sodium and sulfur.However,the diffusion of polysulfides and sluggish kinetics of conversion reactions are still major challenges for their application.Herein,we developed a powerful and functional separator to inhibit the shuttle effect by coating a lightweight three-dimensional cellulose nanofiber-derived carbon aerogel on a glass fiber separator(denoted NSCA@GF).The hierarchical porous structures,favorable electronic conductivity,and three-dimensional interconnected network of N,S-codoped carbon aerogel endow a multifunctional separator with strong polysulfide anchoring capability and fast reaction kinetics of polysulfide conversion,which can act as the barrier layer and an expanded current collector to increase sulfur utilization.Moreover,the hetero-doped N/S sites are believed to strengthen polysulfide anchoring capability via chemisorption and accelerate the redox kinetics of polysulfide conversion,which is confirmed from experimental and theoretical results.As a result,the assembled Na–S coin cells with the NSCA@GF separator showed a high reversible capacity(788.8 mAh g^(−1) at 0.1 C after 100 cycles)and superior cycling stability(only 0.059%capacity decay per cycle over 1000 cycles at 1 C),thereby demonstrating the significant potential for application in high-performance RT/Na–S batteries.
基金Collaborative Innovation Center of Suzhou Nano Science and TechnologyNational Natural Science Foundation of China,Grant/Award Numbers:21773163,22271203+3 种基金EPSRC for an Overseas Travel Grant,Grant/Award Number:EP/R023816/1State Key Laboratory of Organometallic Chemistry of Shanghai Institute of Organic Chemistry,Grant/Award Number:KF2021005Priority Academic Program Development of Jiangsu Higher Education InstitutionsProject of Scientific and Technologic Infrastructure of Suzhou,Grant/Award Number:SZS201905。
文摘The development of simple and effective strategies to prepare electrocatalysts,which possess unique and stable structures comprised of metal/nonmetallic atoms for oxygen reduction reaction(ORR)and oxygen evolution reaction(OER),is currently an urgent issue.Herein,an efficient bifunctional electrocatalyst featured by ultralong N,S-doped carbon nano-hollow-sphere chains about 1300 nm with encapsulated Co nanoparticles(Co-CNHSCs)is developed.The multifunctional catalytic properties of Co together with the heteroatom-induced charge redistribution(i.e.,modulating the electronic structure of the active site)result in superior catalytic activities toward OER and ORR in alkaline media.The optimized catalyst Co-CNHSC-3 displays an outstanding electrocatalytic ability for ORR and OER,a high specific capacity of 1023.6 mAh gZn^(-1),and excellent reversibility after 80 h at 10mA cm^(-2)in a Zn-air battery system.This work presents a new strategy for the design and synthesis of efficient multifunctional carbon-based catalysts for energy storage and conversion devices.
基金supported by the National Natural Science Foundation of China (31890771 and 31901249)the Young Elite Scientists Sponsorship Program by CAST (2019QNRC001)+3 种基金the Hunan Provincial Technical Innovation Platform and Talent Program in Science and Technology (2020RC3041)the Training Program for Excellent Young Innovators of Changsha (kq2106056)the Hunan Provincial Natural Science Foundation of China (2022JJ30079)the Postgraduate Technology Innovation Project of Central South University of Forestry and Technology (2022CX02017)。
文摘Carbon materials are effective substitutes for Pt counter electrodes(CEs) in dye-sensitized solar cells(DSSCs). However, many of these materials, such as carbon nanotubes and graphene, are expensive and require complex preparation process. Herein, waste lignin, recycled from hazardous black liquors,is used to create oxygen-nitrogen-sulfur codoped carbon microspheres for use in DSSC CEs through the facile process of low-temperature preoxidation and high-temperature self-activation. The large number of ester bonds formed by preoxidation increase the degree of cross-linking of the lignin chains, leading to the formation of highly disordered carbon with ample defect sites during pyrolysis. The presence of organic O/N/S components in the waste lignin results in high O/N/S doping of the pyrolysed carbon,which increases the electrolyte ion adsorption and accelerates the electron transfer at the CE/electrolyte interface, as confirmed by density functional theory(DFT) calculations. The presence of inorganic impurities enables the construction of a hierarchical micropore-rich carbon structure through the etching effect during self-activation, which can provide abundant catalytically active sites for the reversible adsorption/desorption of electrolyte ions. Under these synergistic effects, the DSSCs that use this novel carbon CE achieve a quite high power-conversion efficiency of 9.22%. To the best of our knowledge, the value is a new record reported so far for biomass-carbon-based DSSCs.
基金financially supported by the National Natural Science Foundation of China(21975069 and 21872045)the Key Project of Research and Development Plan of Hunan Province(2019SK2071)+1 种基金the Natural Science Foundation of Hunan Province,China(2020JJ4169)the State Key Laboratory of Heavy Oil Processing,China University of Petroleum,Development and Reform Commission of Hunan Province。
文摘Carbonaceous materials are considered as ideal anode for potassium ion batteries(PIBs)due to their abundant resources and stable physical and chemical properties.However,improvements of reversible capacity and cycle performance are still needed,aiming to the practical application.Herein,S/N/O tridoped carbon(SNOC)nanospheres are prepared by in-situ vulcanized polybenzoxazine.The S/N/O tridoped carbon matrix provides abundant active sites for potassium ion adsorption and effectively improves potassium storage capacity.Moreover,the SNOC nanospheres possess large carbon interlayer spacing and high specific surface area,which broaden the diffusion pathway of potassium ions and accelerate the electron transfer speed,resulting in excellent rate performance.As an anode for PIBs,SNOC shows attractive rate performance(438.5 mA h g^(-1) at 50 mA g^(-1) and 174.5 mA h g^(-1) at2000 mA g^(-1)),ultra-high reversible capacity(397.4 mA h g^(-1) at 100 mA g^(-1) after 700 cycles)and ultra-long cycling life(218.9 mA h g^(-1) at 2000 mA g^(-1) after 7300 cycles,123.1 mA h g^(-1) at3000 mA g^(-1) after 16500 cycles and full cell runs for 4000 cycles).Density functional theory calculation confirms that S/N/O tri-doping enhances the adsorption and diffusion of potassium ions,and in-situ Fourier-transform infrared explores explored the potassium storage mechanism of SNOC.
基金support from EPSRC-New Investigator Award 2020 (EP/V002260/1)The Faraday Institute-Battery Study and Seed Research Project (FIRG052)+2 种基金The Royal Society-International Exchanges 2021 Cost Share (NSFC)(IECNSFC211074)the China Scholarship Council (CSC, No. 201806130168)the International Postdoctoral Exchange Fellowship Program (Grant No. PC2022020)
文摘As the need for high-energy–density batteries continues to grow, lithium-sulfur(Li–S) batteries have become a highly promising next-generation energy solution due to their low cost and exceptional energy density compared to commercially available Li-ion batteries. Research into carbon-based sulfur hosts for Li–S batteries has been ongoing for over two decades, leading to a significant number of publications and patents.However, the commercialization of Li–S batteries has yet to be realized. This can be attributed, in part, to the instability of the Li metal anode. However, even when considering just the cathode side, there is still no consensus on whether carbon-based hosts will prove to be the best sulfur hosts for the industrialization of Li–S batteries. Recently, there has been controversy surrounding the use of carbon-based materials as the ideal sulfur hosts for practical applications of Li–S batteries under high sulfur loading and lean electrolyte conditions. To address this question, it is important to review the results of research into carbon-based hosts, assess their strengths and weaknesses, and provide a clear perspective. This review systematically evaluates the merits and mechanisms of various strategies for developing carbon-based host materials for high sulfur loading and lean electrolyte conditions. The review covers structural design and functional optimization strategies in detail, providing a comprehensive understanding of the development of sulfur hosts. The review also describes the use of efficient machine learning methods for investigating Li–S batteries. Finally, the outlook section lists and discusses current trends, challenges, and uncertainties surrounding carbon-based hosts, and concludes by presenting our standpoint and perspective on the subject.
基金supported by the National Natural Science Foundation of China-Shandong Joint Foundation(No.U1806211)。
文摘In this study,we isolated and cultured phytoplankton along the coast of China and measured the cellular carbon,nitrogen,and sulfur contents under four temperatures.The results showed that the contents of the cellular elements varied widely among different phytoplankton.We found that temperature is one of the important factors affecting the carbon,nitrogen,and sulfur contents in phytoplankton cells;however,the degree of influence of temperature is different for different kinds of phytoplankton.By measuring the nitrogen content in cells,we found that the C:N ratio indirectly measured in the experiment fluctuated in the range of 3.50-8.97,and the average C:N ratio was 5.52.In this experiment,we accurately measured the cell elemental contents at different temperatures and transformed the cell count results into carbon,nitrogen,and sulfur contents to express the biomass.This method ensures that the contribution of species that are small in number but with a large cell volume in biomass is considered.Moreover,this method comprehensively considers the interspecific differences of species and the uneven distribution of elements in phytoplankton cells,which is of significance in the estimation of marine carbon and nitrogen budget.The distribution of nitrogen content in marine phytoplankton can well indicate the marine eutrophication caused by human activities.Climate change can affect the community structure and element composition of marine phytoplankton,meanwhile marine carbon and nitrogen element can regulate the climate to a certain extent.
基金Yunnan Expert Workstation,Grant/Award Number:202005AF150028Program for the Outstanding Young Talents of Hebei Province,China,Grant/Award Number:YGZ+6 种基金Guangdong Innovative and Entrepreneurial Team Program,Grant/Award Number:2016ZT06C517Guangdong Science and Technology Department,Grant/Award Number:2020B0909030004National Natural Science Foundation of China,Grant/Award Numbers:21601136,22075211,52071125Outstanding Youth Project of Guangdong Natural Science Foundation,Grant/Award Number:2021B1515020051Natural Science Foundation of Hebei Province,China,Grant/Award Numbers:B2020202052,B2021202028,E2020202071Chunhui Project of Ministry of Education of the People's Republic of China,Grant/Award Number:Z2017010Science and Technology Program of Guangzhou,Grant/Award Number:2019050001。
文摘Due to low cost,high capacity,and high energy density,lithium–sulfur(Li–S)batteries have attracted much attention;however,their cycling performance was largely limited by the poor redox kinetics and low sulfur utilization.Herein,predicted by density functional theory calculations,single‐atomic Co‐B2N2 site‐imbedded boron and nitrogen co‐doped carbon nanotubes(SA‐Co/BNC)were designed to accomplish high sulfur loading,fast kinetic,and long service period Li–S batteries.Experiments proved that Co‐B2N2 atomic sites can effectively catalyze lithium polysulfide conversion.Therefore,the electrodes delivered a specific capacity of 1106 mAh g−1 at 0.2 C after 100 cycles and exhibited an outstanding cycle performance over 1000 cycles at 1 C with a decay rate of 0.032%per cycle.Our study offers a new strategy to couple the combined effect of nanocarriers and single‐atomic catalysts in novel coordination environments for high‐performance Li–S batteries.
基金Under the auspices of National Natural Science Foundation of China(No.42171230)。
文摘Exploring carbon emission effects based on the evolution of residents’ dietary structure to achieve the carbon neutrality goal and mitigate climate change is an important task.This study took China as the research object(data excluding Hong Kong,Macao and Taiwan) and used the carbon emission coefficient method to quantitatively measure the food carbon emissions from 1987–2020,then analyzed the carbon emission effects under the evolution of dietary structure.The results showed that during the study period,the Chinese dietary structure gradually changed to a high-carbon consumption pattern.The dietary structure of urban residents developed to a balanced one,while that of rural residents developed to a high-quality one.During the study period,the per capita food carbon emissions and total food consumption of Chinese showed an increasing trend.The per capita food carbon emissions of residents in urban and rural showed an overall upward trend.The total food carbon emissions in urban increased significantly,while that in rural increased first and then decreased.The influence of beef and mutton on carbon emissions is the highest in dietary structure.Compared with the balanced dietary pattern,the food carbon emissions of Chinese residents had not yet reached the peak,but were evolving to a high-carbon consumption pattern.
基金supported by the General Project of Top-Design of Multi-Scale Nature-Social ModelsData Support and Decision Support System for NSFC Carbon Neutrality Major Project(42341202)the Basic Scientific Research Fund of the Chinese Academy of Meteorological Sciences(2021Z014)。
文摘CO_(2)is one of the most important greenhouse gases(GHGs)in the earth’s atmosphere.Since the industrial era,anthropogenic activities have emitted excessive quantities of GHGs into the atmosphere,resulting in climate warming since the 1950s and leading to an increased frequency of extreme weather and climate events.In 2020,China committed to striving for carbon neutrality by 2060.This commitment and China’s consequent actions will result in significant changes in global and regional anthropogenic carbon emissions and therefore require timely,comprehensive,and objective monitoring and verification support(MVS)systems.The MVS approach relies on the top-down assimilation and inversion of atmospheric CO_(2)concentrations,as recommended by the Intergovernmental Panel on Climate Change(IPCC)Inventory Guidelines in 2019.However,the regional high-resolution assimilation and inversion method is still in its initial stage of development.Here,we have constructed an inverse system for carbon sources and sinks at the kilometer level by coupling proper orthogonal decomposition(POD)with four-dimensional variational(4DVar)data assimilation based on the weather research and forecasting-greenhouse gas(WRF-GHG)model.Our China Carbon Monito ring and Verification Support at the Regional level(CCMVS-R)system can continuously assimilate information on atmospheric CO_(2)and other related information and realize the inversion of regional and local anthropogenic carbon emissions and natural terrestrial ecosystem carbon exchange.Atmospheric CO_(2)data were collected from six ground-based monito ring sites in Shanxi Province,China to verify the inversion effect of regio nal anthropogenic carbon emissions by setting ideal and real experiments using a two-layer nesting method(at 27 and 9 km).The uncertainty of the simulated atmospheric CO_(2)decreased significantly,with a root-mean-square error of CO_(2)concentration values between the ideal value and the simulated after assimilation was close to 0.The total anthropogenic carbon emissions in Shanxi Province in 2019 from the assimilated inversions were approximately 28.6%(17%-38%)higher than the mean of five emission inventories using the bottomup method,showing that the top-down CCMVS-R system can obtain more comprehensive information on anthropogenic carbon emissions.
基金financially supported by the National Natural Science Foundation of China(22078292,22008212,U20A20119,21776258)。
文摘The overall performance of metal catalysts can be efficiently adjusted by modifying carbon carriers with different valence sulfur precursors.The wet impregnation technique successfully prepared carbon material carriers doped with varying sources of sulfur(Na_(2)SO_(4),NaHSO_(3),Na_(2)S·9H_(2)O).Palladium carbon catalysts doped with different sulfur precursors had been prepared with the aid of the liquid-phase reduction method of the selective hydrogenation of o-chloronitrobenzene(o-CNB)to o-chloroaniline(o-CAN).The catalyst prepared for Na_(2)S·9H_(2)O as a precursor has excellent performance,and the selectivity for o-CAN is more than 99.9%at 100%conversion.In addition,the characterization results show that with the decrease of S valence,the electronic effect between S and Pd increases,and the outer electron shift of Pd increases,which reduces the adsorption and dissociation ability of Pd to hydrogen,resulting in excellent selectivity.The effects provided a good idea for the hydrogenation of o-CNB and a different point of view on sulfur doping in a variety of hydrogenation reactions.
基金supported by the Basic Science Research Program through the National Research Foundation of Korea(NRF)funded by the Ministry of Education(NRF-2019R1A2C1084836 and NRF-2021R1A4A2001403)supported by 2018 Research Grant(PoINT)from Kangwon National University。
文摘Bifunctional hybrid anodes(BHAs),which are both a high-performance active host material for lithium-ion storage as well as a guiding agent for homogeneous lithium metal nucleation and growth,exhibit significant potential as anodes for next-generation high-energy-density lithium-ion batteries(LIBs).In this study,sulfur-doped hard carbon nanosphere assemblies(S-HCNAs)were prepared through a hydrothermal treatment of a liquid organic precursor,followed by high-temperature thermal annealing with elemental sulfur for application as BHAs for LIBs.In a carbonate-based electrolyte containing fluoroethylene carbonate additive,the S-HCNAs showed high lithium-ion storage capacities in sloping as well as plateau voltage sections,good rate capabilities,and stable cyclabilities.In addition,high average Coulombic efficiencies(CEs)of~96.9%were achieved for dual lithium-ion and lithium metal storage cycles.In the LIB full-cell tests with typical NCM811 cathodes,the S-HCNA-based BHAs containing~400 mA h g^(−1) of excess lithium led to high energy and power densities of~500Wh kg^(−1) and~1695Wkg^(−1),respectively,and a stable cycling performance with~100%CEs was achieved.
基金financially supported by the Natural Science Foundation of Hebei Province-Innovation Group Research Project(Grant No.C2020204111)the National Natural Science Foundation of China(Grant No.31930098)+3 种基金the Science Fund for Distinguished Young Scholars of Hebei Province(Grant No.C2021204049)the Hebei Province Outstanding Youth Fund(Grant No.BJ2021024)the Hebei Provincial Key Research Projects(21326344D)Hebei International Joint Research Base of Modern Agricultural Biotechnology.
文摘Chinese cabbage(Brassica rapa ssp. pekinensis) has a long cultivation history and is one of the vegetable crops with the largest cultivation area in China. However, salt stress severely damages photosynthesis and hormone metabolism, nutritional balances, and results in ion toxicity in plants. To better understand the mechanisms of salt-induced growth inhibition in Chinese cabbage, RNA-seq and physiological index determination were conducted to explore the impacts of salt stress on carbon cycle metabolism and photosynthesis in Chinese cabbage. Here, we found that the number of thylakoids and grana lamellae and the content of starch granules and chlorophyll in the leaves of Chinese cabbage under salt stress showed a time-dependent response, first increasing and then decreasing. Chinese cabbage increased the transcript levels of genes related to the photosynthetic apparatus and carbon metabolism under salt stress, probably in an attempt to alleviate damage to the photosynthetic system and enhance CO_(2) fixation and energy metabolism. The transcription of genes related to starch and sucrose synthesis and degradation were also enhanced;this might have been an attempt to maintain intracellular osmotic pressure by increasing soluble sugar concentrations. Soluble sugars could also be used as potential reactive oxygen species(ROS) scavengers, in concert with peroxidase(POD)enzymes, to eliminate ROS that accumulate during metabolic processes. Our study characterizes the synergistic response network of carbon metabolism and photosynthesis under salt stress.
基金supported by the Basic Science Research Program through the National Research Foundation of Korea(NRF)grant funded by the Korean government(MSIT)(2021R1A4A2000934).
文摘The metal-organic framework(MOF)derived Ni–Co–C–N composite alloys(NiCCZ)were“embedded”inside the carbon cloth(CC)strands as opposed to the popular idea of growing them upward to realize ultrastable energy storage and conversion application.The NiCCZ was then oxygen functionalized,facilitating the next step of stoichiometric sulfur anion diffusion during hydrothermal sulfurization,generating a flower-like metal hydroxysulfide structure(NiCCZOS)with strong partial implantation inside CC.Thus obtained NiCCZOS shows an excellent capacity when tested as a supercapacitor electrode in a three-electrode configuration.Moreover,when paired with the biomass-derived nitrogen-rich activated carbon,the asymmetric supercapacitor device shows almost 100%capacity retention even after 45,000 charge–discharge cycles with remarkable energy density(59.4 Wh kg^(-1)/263.8μWh cm^(–2))owing to a uniquely designed cathode.Furthermore,the same electrode performed as an excellent bifunctional water-splitting electrocatalyst with an overpotential of 271 mV for oxygen evolution reaction(OER)and 168.4 mV for hydrogen evolution reaction(HER)at 10 mA cm−2 current density along with 30 h of unhinged chronopotentiometric stability performance for both HER and OER.Hence,a unique metal chalcogenide composite electrode/substrate configuration has been proposed as a highly stable electrode material for flexible energy storage and conversion applications.
基金The authors gratefully acknowledge the financial support of National NaturalScience Foundation of China(Grant No.41972276)Natural Science Foundation of Fujian Province,China(Grant No.2020J06013)"Foal Eagle Program"Youth Top-notch Talent Project of Fujian Province,China(Grant No.00387088).
文摘Enzyme-induced carbonate precipitation(EICP)is an emanating,eco-friendly and potentially sound technique that has presented promise in various geotechnical applications.However,the durability and microscopic characteristics of EICP-treated specimens against the impact of drying-wetting(D-W)cycles is under-explored yet.This study investigates the evolution of mechanical behavior and pore charac-teristics of EICP-treated sea sand subjected to D-W cycles.The uniaxial compressive strength(UCS)tests,synchrotron radiation micro-computed tomography(micro-CT),and three-dimensional(3D)recon-struction of CT images were performed to study the multiscale evolution characteristics of EICP-reinforced sea sand under the effect of D-W cycles.The potential correlations between microstructure characteristics and macro-mechanical property deterioration were investigated using gray relational analysis(GRA).Results showed that the UCS of EICP-treated specimens decreases by 63.7% after 15 D-W cycles.The proportion of mesopores gradually decreases whereas the proportion of macropores in-creases due to the exfoliated calcium carbonate with increasing number of D-W cycles.The micro-structure in EICP-reinforced sea sand was gradually disintegrated,resulting in increasing pore size and development of pore shape from ellipsoidal to columnar and branched.The gray relational degree suggested that the weight loss rate and UCS deterioration were attributed to the development of branched pores with a size of 100-1000 m m under the action of D-W cycles.Overall,the results in this study provide a useful guidancee for the long-term stability and evolution characteristics of EICP-reinforced sea sand under D-W weathering conditions.