Countries around the world have been making efforts to reduce pollutant emissions. However, the response of global black carbon(BC) aging to emission changes remains unclear. Using the Community Atmosphere Model versi...Countries around the world have been making efforts to reduce pollutant emissions. However, the response of global black carbon(BC) aging to emission changes remains unclear. Using the Community Atmosphere Model version 6 with a machine-learning-integrated four-mode version of the Modal Aerosol Module, we quantify global BC aging responses to emission reductions for 2011–2018 and for 2050 and 2100 under carbon neutrality. During 2011–18, global trends in BC aging degree(mass ratio of coatings to BC, R_(BC)) exhibited marked regional disparities, with a significant increase in China(5.4% yr^(-1)), which contrasts with minimal changes in the USA, Europe, and India. The divergence is attributed to opposing trends in secondary organic aerosol(SOA) and sulfate coatings, driven by regional changes in the emission ratios of corresponding coating precursors to BC(volatile organic compounds-VOCs/BC and SO_(2)/BC). Projections under carbon neutrality reveal that R_(BC) will increase globally by 47%(118%) in 2050(2100), with strong convergent increases expected across major source regions. The R_(BC) increase, primarily driven by enhanced SOA coatings due to sharper BC reductions relative to VOCs, will enhance the global BC mass absorption cross-section(MAC) by 11%(17%) in 2050(2100).Consequently, although the global BC burden will decline sharply by 60%(76%), the enhanced MAC partially offsets the magnitude of the decline in the BC direct radiative effect, resulting in the moderation of global BC DRE decreases to 88%(92%) of the BC burden reductions in 2050(2100). This study highlights the globally enhanced BC aging and light absorption capacity under carbon neutrality, thereby partly offsetting the impact of BC direct emission reductions on future changes in BC radiative effects globally.展开更多
Under the backdrop of“Carbon Peak and Carbon Neutrality”(dual carbon)goal in China,the methane-carbon dioxide reforming reaction has attracted considerable attention due to its environmental benefits of converting t...Under the backdrop of“Carbon Peak and Carbon Neutrality”(dual carbon)goal in China,the methane-carbon dioxide reforming reaction has attracted considerable attention due to its environmental benefits of converting two greenhouse gases(methane and carbon dioxide)into syngas and its promising industrial applications.Nickel(Ni)-based catalysts,with high catalytic activity,low cost,and abundant resources,are considered ideal candidates for industrial applications.In this article,three reaction kinetic models were briefly introduced,namely the Power-Law(PL)model,the Eley-Rideal(ER)model,and the Langmuir-Hinshelwood-Hougen-Watson(LHHW)model.Based on the LHHW model,the reaction kinetics and mechanisms of different catalytic systems were systematically discussed,including the properties of supports,the doping of noble metals and transition metals,the role of promoters,and the influence of the geometric and electronic structures of Ni on the reaction mechanism.Furthermore,the kinetics of carbon deposition and elimination on various catalysts were analyzed.Based on the reaction rate expressions for carbon elimination,the reasons for the high activity of transition metal iron(Fe)-doped catalysts and core-shell structured catalysts in carbon elimination were explained.Based on the detailed collation and comparative analysis of the reaction mechanisms and kinetic characteristics across diverse Ni-based catalytic systems,a theoretical guidance for the designing of high-performance catalysts was provided in this work.展开更多
Vanadium redox flow batteries(VRFBs)are a means of large-scale energy storage due to their excellent scalability,safety,long cycling life,and decoupled power and energy capacities.However,the slow redox kinetics of va...Vanadium redox flow batteries(VRFBs)are a means of large-scale energy storage due to their excellent scalability,safety,long cycling life,and decoupled power and energy capacities.However,the slow redox kinetics of vanadium species on conventional carbon electrodes remains a major limitation to their performance.We investigated the deposition of carbon black,carbon nanotubes,and electrochemically exfoliated graphene(Exf-Gr)onto thermally-activated carbon paper(ACP)by spray coating to increase the electrode electrocatalytic activity.The modified electrodes were characterized using scanning electron microscopy,X-ray diffraction,Raman spectroscopy,X-ray photoelectron microscopy,and surface area analysis,while their electrochemical properties were evaluated by cyclic voltammetry,electrochemical impedance spectroscopy,and singlecell VRFB testing.Among the modified electrodes,Exf-Gr/ACP had the best performance,achieving a 2.9-fold reduction in charge transfer resistance compared to pristine ACP and delivering 2.5 times the discharge capacity in single-cell tests.This improvement is attributed to Exf-Gr’s high surface area,favorable catalytic activity,and excellent dispersion on the ACP substrate.Surface modification with electrochemically exfoliated graphene is a highly effective strategy for improving the electrode performance in VRFB systems,with significant implications for large-scale energy storage.展开更多
Biological nitrogen fixation(BNF)and photosynthetic carbon fixation underpin food production and climate mitigation,yet natural systems are constrained by oxygen sensitivity,high energy demand,and inefficient catalyst...Biological nitrogen fixation(BNF)and photosynthetic carbon fixation underpin food production and climate mitigation,yet natural systems are constrained by oxygen sensitivity,high energy demand,and inefficient catalysts.This review synthesizes advances that recast these processes as engineering targets and proposes a conceptual roadmap that bridges synthetic symbioses with the synthetic biology of enzymes and pathways.For BNF,progress spans cross-kingdom strategies—from refactoring nif gene sets and targeting nitrogenase assembly to eukaryotic organelles,to engineering plant-associated diazotrophs,rhizosphere control circuits,and emerging nodule-like microenvironments.For carbon assimilation,new-to-nature CO_(2)-fixation modules and photorespiratory bypasses illustrate how pathway redesign and alternative carboxylases can circumvent key Calvin–Benson–Bassham limitations,and expanding photosynthetic light capture offers additional leverage.Across these domains,we extract common design principles:(i)nitrogenase output is increasingly governed by carbon/energy supply and electron delivery as much as by oxygen protection;(ii)robust function requires compartment-aware enzyme–chassis coordination,substrate channeling,and dynamic regulation using sensors and control circuits;and(iii)scalable implementation may benefit from distributing metabolic labor across engineered consortia rather than forcing all functions into a single host.We discuss enabling technologies—including AI-guided protein design and directed evolution,cell-free prototyping,chassis toolkits,and materials/bioelectrochemical interfaces—that can accelerate design–build–test–learn cycles and reduce barriers to deployment.Together,these insights define a path toward integrated nitrogen and carbon fixation systems for low-emission agriculture and biomanufacturing.展开更多
In this study,melamine and cyanuric acid were used as precursors to form supramolecular crystals via hydrogen-bond-assisted self-assembly followed by hydrothermal treatment.Subsequent high-temperature calcination yiel...In this study,melamine and cyanuric acid were used as precursors to form supramolecular crystals via hydrogen-bond-assisted self-assembly followed by hydrothermal treatment.Subsequent high-temperature calcination yielded a novel brush-like three-dimensional carbon nitride.The brush-like 3D architecture was found to expose more accessible active sites,markedly accelerate electron transfer,and suppress the recombination of photogenerated charge carriers.The resulting superoxide(O_(2)^(-·))and hydroxyl(·OH)radicals generated via electron reduction were identified as the key reactive species in the photocatalytic process.Moreover,the surface of the brush-like structure is enriched with nitrogen vacancies,which enhance the catalyst’s ability to harvest visible light.The photocatalytic performance of the brush-like CNS-650 catalyst was evaluated for rhodamine B(RhB)degradation.Under red-light irradiation(660 nm),its degradation rate was 7.4 times higher than that of bulk CN.This work provides valuable insights into the design and application of efficient metal-free 3D photocatalysts.展开更多
Pitch is an excellent precursor for the production of hard carbon,with pre-oxidation crucial process in the fabrication.The structural changes in the different molecular components of pitch during thermochemical treat...Pitch is an excellent precursor for the production of hard carbon,with pre-oxidation crucial process in the fabrication.The structural changes in the different molecular components of pitch during thermochemical treatment are a key factor in determining the sodium-ion storage of pitchbased hard carbon anodes.We investigated the effects of the different molecular structures in the asphaltene precursor,including aromatic rings and aliphatic chains,on the sodiumion storage behavior of the resulting carbon.We found that polar oxygen functional groups limit the steric hindrance caused by the aromatic rings in pitch,and thus facilitate the introduction of cross-linked structures.During high-temperature carbonization,aromatic rings form a rigid carbon framework that prevents the rearrangement of ordered carbon layers,leading to a short-range disordered carbon structure and promotes the production of closed pores.For example,a material prepared from asphaltene,which contains a large number of oxygen-containing functional groups and macromolecular aromatic rings,using pre-oxidation at 300℃ and carbonization at 1200℃ had a reversible capacity of 316.7 mAh g^(−1) when used as the anode for sodium ion batteries.Our research provides a theoretical basis for the selection of raw materials for the development of high-quality pitch-based hard carbons.展开更多
Zinc-ion supercapacitors(ZISCs)have received considerable interest for energy storage because of their low cost,high safety,and minimal environmental impact.However,they have a low energy density and poor cycling perf...Zinc-ion supercapacitors(ZISCs)have received considerable interest for energy storage because of their low cost,high safety,and minimal environmental impact.However,they have a low energy density and poor cycling performance.The design of a better cathode material is needed to overcome these limitations.A simple method was used to synthesize binder-free electrochemically exfoliated carbon paper(EECP)which modifies the surface of the paper by introducing oxygen functional groups and thus improves its pseudocapacitance.When used in a Zn-ion supercapacitor(ZISC),an EECPbased cathode provides a large surface area and quick charge transfer.As a result,the ZISC had remarkable charge storage properties and had a dominant capacitive-type charge storage mechanism with 78.8%retention of capacity at 10 mV/s of the total storage.Furthermore,at 1 A/g,the EECP electrode had a maximum capacitance of 252.5 F/g.The EECP electrode retained 81.7%of its capacitance after 10000 cycles,indicating its promise for use in the growing renewable energy sector.A ZISC was also constructed using EECP as the positive electrode and Zn as the negative electrode with a 1 mol L^(−1) ZnSO_(4) electrolyte.It had a capacitance of 186.22 F/g at 1 A/g and a 97.01%retention rate after 10000 cycles.It also had an excellent energy density of 46.6 Wh/kg at a power density of 500.4 W/kg.The material is therefore suitable for use in high-rate next-generation ZISCs.展开更多
Carbon-based materials have gained significant attention in anticancer treatment because of their exceptional biocompatibility,yet critical challenges persist in establishing definitive correlations between their poro...Carbon-based materials have gained significant attention in anticancer treatment because of their exceptional biocompatibility,yet critical challenges persist in establishing definitive correlations between their porous structures and functional performance.We report the use of a silica template to guide pore formation in the design of mesoporous carbon spheres(mC)with tailored pore structures for improved combined photothermal-chemotherapy.The mesopore size of mC has been adjusted by kinetic control of the resin polymerization and silica hydrolysis.Structural characterization showed that 4.4 nm mesopores enabled an exceptional gemcitabine loading of 228 mg g^(−1) and a sustained pH/thermal dual-responsive release with>70%drug release under near-infrared(NIR)irradiation.Finite element analysis demonstrated pore size-dependent heat transfer dynamics,with the improved mC achieving a superior photothermal conversion efficiency of 62%by a combination of N-doping and defect engineering.In vitro evaluations confirmed outstanding biocompatibility with>95%cell viability at 200μg mL^(−1) and potent tumor suppression in pancreatic and biliary cancer models with an~5%cell viability at 25μg mL^(−1) where combined therapy showed a 3.7-fold increased cytotoxicity over monotherapy.The improved structure of mC facilitated cascade therapeutic effects with enhanced tumor permeability derived from NIR-triggered hyperthermia and prolonged therapeutic exposure due to pH-responsive drug release.This pore engineering strategy establishes a structure-function process for next-generation theranostic platforms,addressing the critical limitations of conventional pancreatic and biliary cancer therapies through spatiotemporal control of multimodal treatment.展开更多
The development of materials with excellent microwave absorption(MWA)and electromagnetic interference(EMI)shielding performances has currently received attention.Herein,mesophase pitch-based carbon foam(MPCF)with 3D i...The development of materials with excellent microwave absorption(MWA)and electromagnetic interference(EMI)shielding performances has currently received attention.Herein,mesophase pitch-based carbon foam(MPCF)with 3D interconnected pore structure was prepared through the high pressure pyrolysis of mesophase coal tar pitch.It is found that the 3D interconnected cellular pores of MPCF facilitate multiple reflections of electromagnetic waves,which results in the minimum reflection loss(RLmin)value of MPCF reaches-37.84 dB with the effective absorption bandwidth(EAB)of 5.44 GHz at a thickness of 2.70 mm,and the total average electromagnetic shielding effectiveness(SE_(T))under 3.00 mm thickness achieves 26.52 dB in X-band.Subsequently,MPCF is activated by KOH to obtain activated carbon foam(A-MPCF).The average SE_(T)of A-MPCF achieves 103.00 dB for abundant nanopores on the pore cell walls,which leads to a transition from the multiple reflections of electromagnetic waves on the walls to diffuse reflection.Unfortunately,the reflection coefficient(R)of A-MPCF increases from 0.78 to 0.90.To reduce the R value,Fe_(3)O_(4)/A-MPCF was fabricated via the in situ growth of nano Fe_(3)O_(4)on A-MPCF.Consequently,the R value of Fe_(3)O_(4)/A-MPCF was reduced from 0.90 to 0.74,whereas the MWA performance was only slightly decreased.This work proposes a simple strategy for simultaneously adjusting MWA and EMI shielding performances of materials.展开更多
Lithium–sulfur(Li–S)batteries are promisingcandidates for next-generation energy storagegiven their high energy density and potential low cost.Chemically activated carbon(CAC)is often used fortheir cathodes,because ...Lithium–sulfur(Li–S)batteries are promisingcandidates for next-generation energy storagegiven their high energy density and potential low cost.Chemically activated carbon(CAC)is often used fortheir cathodes,because it has a high specific surfacearea for sulfur loading.We have developed a pressurizedphysical activation(PPA)method that producedan activated carbon(PPAC)with a high specific surfacearea comparable to that of CAC.The pore structure of PPAC could be changed and its use as a cathode material for Li–Sbatteries was investigated.Battery tests at different capacity rates(C-rates)showed that it had a much improved high-rate performancewith a discharge capacity of 900 mAh/(g of sulfur)at 1 C,in contrast to only 600 mAh/(g of sulfur)for CAC.Porestructure analyses showed that PPAC prepared at a high activation temperature(1000℃)had unusual channel-like mesoporesbetween the microdomains that are the basic structural units of artificial carbon materials.These are connected to microporesdeveloped in each microdomain,and deliver ions from the surroundings to the internal pores and vice versa.The well-developedmicropores and mesopores of PPAC respectively ensured the high adsorption of lithium polysulfides and a high rate ofion diffusion.Compared to CAC,PPAC is a high-performance,low-cost cathode material that is promising for use in futureLi–S batteries.展开更多
CO_(2) capture and utilization(CCU)technologies have been recognized as crucial strategies for mitigating global warming,reducing carbon emission,and promoting resource circularity.As such,the design and development o...CO_(2) capture and utilization(CCU)technologies have been recognized as crucial strategies for mitigating global warming,reducing carbon emission,and promoting resource circularity.As such,the design and development of related materials have attracted considerable research attention.Carbon-based materials,characterized by tunable pore structures,abundant active sites,high specific surface area,and excellent chemical stability,demonstrate significant potential for applications in CO_(2) capture and utilization.This review systematically analyzes the adsorption behaviors and performance variations of typical carbon materials,including activated carbon,porous carbon,graphene,and carbon nanotubes during CO_(2) capture processes.Concerning CO_(2) utilization,emphasis is placed on recent advances in the catalytic applications of carbon-based materials in key reactions such as methanation,reverse water-gas shift,dry reforming of methane,and alcohol synthesis.Moreover,the benefits and drawbacks of carbon materials in terms of CO_(2) adsorption capacity,catalytic activity,and stability are thoroughly evaluated,and their potential applications in integrated CO_(2) capture and utilization technologies are discussed.Finally,key strategies for enhancing the performance of carbonaceous materials through structural modulation and surface modification are elucidated.This review aims to provide theoretical guidance for the future development and large-scale implementation of carbon-based materials in CCU technologies.展开更多
Ship operations are crucial to global trade,and their decarbonization is essential to mitigate climate change.This study evaluates the economic viability of existing and emerging decarbonization technologies in mariti...Ship operations are crucial to global trade,and their decarbonization is essential to mitigate climate change.This study evaluates the economic viability of existing and emerging decarbonization technologies in maritime shipping using the levelized cost of energy methodology.It includes a detailed comparative analysis based on essential criteria and sensitivity assessments to highlight the economic impacts of technological advancements.Key factors influencing total costs include fuel costs,carbon pricing,and energy demands for carbon capture.The findings reveal that methanol is more cost-effective than heavy fuel oil(HFO)when priced below 3000 CNY/t,assuming HFO costs 4400 CNY/t.Additionally,methanol with post-combustion carbon capture is less expensive than pre-combustion carbon capture.When carbon prices rise above 480 CNY/t,carbon capture technologies prove more economical than purchasing carbon emission allowances for HFO and liquefied natural gas.Enhanc-ing the use of exhaust gas waste heat is recommended for cost savings.Post-combustion carbon capture also shows greater efficiency,requiring about 1.1 GJ/t less energy than pre-combustion methods,leading to lower overall costs.Future research should focus on market mechanisms to stabilize fuel prices and develop less energy-intensive carbon capture technologies.This study offers critical insights into effective decarbonization strategies for advancing global maritime trade in the present and future.展开更多
Despite their high theoretical capacity and energy density,lithiumsulfur(Li–S)batteries still face challenges such as soluble lithium polysulfides(LiPSs)shuttling and sluggish redox kinetics.In this work,we used a no...Despite their high theoretical capacity and energy density,lithiumsulfur(Li–S)batteries still face challenges such as soluble lithium polysulfides(LiPSs)shuttling and sluggish redox kinetics.In this work,we used a novel MoS_(2)-Mo_(2)C heterostructure anchored on a carbon sponge(CS)as a Li_(2)S host to solve these problems.A simple hydrothermal process following carbothermal reduction was used to construct the MoS_(2)-Mo_(2)C heterostructure,enabling control of the phases and integration of MoS_(2) and Mo_(2)C.Structural characterization confirmed the coherent interface of the heterostructure with a precise orientation relationship between the two phases and their uniform distribution.An evaluation of the adsorption and catalytic performance of the material showed that it has an exceptional LiPSs adsorption capacity with faster conversion from Li_(2)S_(4) to Li_(2)S_(2).Density functional theory calculations further confirmed these results.As a result,the cathode had a high initial discharge capacity of 693 mAh g^(−1) at 0.2 C and achieved stable cycling at 2 C for 500 cycles with a low decay rate of 0.107%per cycle.The heterostructure design,coupled with the macroporous CS framework,effectively prevented the shuttling and increased sulfur utilization,offering a promising way to produce practical high-energydensity Li–S batteries.展开更多
The effects of nitrogen(N)deposition on forest soil organic carbon(SOC)are largely unclear,likely due to the divergent responses of particulate(POC)and mineral-associated carbon(MAOC).Conventional understory inorganic...The effects of nitrogen(N)deposition on forest soil organic carbon(SOC)are largely unclear,likely due to the divergent responses of particulate(POC)and mineral-associated carbon(MAOC).Conventional understory inorganic N(UIN)additions neglect canopy processes and the impacts of organic N,potentially misevaluating N deposition effects.This study was conducted in a long-term N addition experiment established in a Moso bamboo forest,which included six treatments combining canopy and understory N additions with organic(urea glycine)and inorganic(NH_(4)NO_(3))forms at a rate of 50 kg N·ha^(-1)·yr^(-1).Litterbags were installed for a two-year decomposition experiment and collected at quarterly intervals,together with concurrent soil sampling under litterbags at 0–10 cm depth.We aimed to examine the effects of canopy vs.understory N addition and organic vs.inorganic N form on soil POC and MAOC concentrations.Our results showed that canopy N additions significantly reduced POC(ased POC-15.9%)but did not affect MAOC(P>0.05).Conversely,understory N additions significantly incre(30.9%)and decreased MAOC(and fungal diversity(FuD),-28.9%).Canopy N additions decreased POC by enhancing peroxidase activity while understory N additions promoted POC by inhibiting litter decomposition.Additionally,understory N addition-induced soil acidification decreased soil Ca^(2+)concentration,microbial carbon use efficiency,and bacterial necromass C,as well as the release of litter water-soluble compounds,thereby inhibiting MAOC.Moreover,nitrogen forms(organic vs.inorganic)had no effect on SOC fractions.Our findings underscore that canopy and understory N addition approaches differentially regulate SOC fractions by altering litter decomposition–microbial–mineral interactions,and the understory approach may overestimate soil POC gain and MAOC loss driven by atmospheric N deposition.展开更多
基金supported by the National Natural Science Foundation of China (42505149,41925023,U2342223,42105069,and 91744208)the China Postdoctoral Science Foundation (2025M770303)+1 种基金the Fundamental Research Funds for the Central Universities (14380230)the Jiangsu Funding Program for Excellent Postdoctoral Talent,and Jiangsu Collaborative Innovation Center of Climate Change。
文摘Countries around the world have been making efforts to reduce pollutant emissions. However, the response of global black carbon(BC) aging to emission changes remains unclear. Using the Community Atmosphere Model version 6 with a machine-learning-integrated four-mode version of the Modal Aerosol Module, we quantify global BC aging responses to emission reductions for 2011–2018 and for 2050 and 2100 under carbon neutrality. During 2011–18, global trends in BC aging degree(mass ratio of coatings to BC, R_(BC)) exhibited marked regional disparities, with a significant increase in China(5.4% yr^(-1)), which contrasts with minimal changes in the USA, Europe, and India. The divergence is attributed to opposing trends in secondary organic aerosol(SOA) and sulfate coatings, driven by regional changes in the emission ratios of corresponding coating precursors to BC(volatile organic compounds-VOCs/BC and SO_(2)/BC). Projections under carbon neutrality reveal that R_(BC) will increase globally by 47%(118%) in 2050(2100), with strong convergent increases expected across major source regions. The R_(BC) increase, primarily driven by enhanced SOA coatings due to sharper BC reductions relative to VOCs, will enhance the global BC mass absorption cross-section(MAC) by 11%(17%) in 2050(2100).Consequently, although the global BC burden will decline sharply by 60%(76%), the enhanced MAC partially offsets the magnitude of the decline in the BC direct radiative effect, resulting in the moderation of global BC DRE decreases to 88%(92%) of the BC burden reductions in 2050(2100). This study highlights the globally enhanced BC aging and light absorption capacity under carbon neutrality, thereby partly offsetting the impact of BC direct emission reductions on future changes in BC radiative effects globally.
基金Supported by Innovation Capability Support Program of Shaanxi(2024RS-CXTD-53,2024ZC-KJXX-096)the Key R&D Program of Shaanxi Province(2022QCY-LL-69)Xi’an Science and Technology Project(24GXFW0089)。
文摘Under the backdrop of“Carbon Peak and Carbon Neutrality”(dual carbon)goal in China,the methane-carbon dioxide reforming reaction has attracted considerable attention due to its environmental benefits of converting two greenhouse gases(methane and carbon dioxide)into syngas and its promising industrial applications.Nickel(Ni)-based catalysts,with high catalytic activity,low cost,and abundant resources,are considered ideal candidates for industrial applications.In this article,three reaction kinetic models were briefly introduced,namely the Power-Law(PL)model,the Eley-Rideal(ER)model,and the Langmuir-Hinshelwood-Hougen-Watson(LHHW)model.Based on the LHHW model,the reaction kinetics and mechanisms of different catalytic systems were systematically discussed,including the properties of supports,the doping of noble metals and transition metals,the role of promoters,and the influence of the geometric and electronic structures of Ni on the reaction mechanism.Furthermore,the kinetics of carbon deposition and elimination on various catalysts were analyzed.Based on the reaction rate expressions for carbon elimination,the reasons for the high activity of transition metal iron(Fe)-doped catalysts and core-shell structured catalysts in carbon elimination were explained.Based on the detailed collation and comparative analysis of the reaction mechanisms and kinetic characteristics across diverse Ni-based catalytic systems,a theoretical guidance for the designing of high-performance catalysts was provided in this work.
基金supported by the University of Seoul’s 2025 Research Fund.
文摘Vanadium redox flow batteries(VRFBs)are a means of large-scale energy storage due to their excellent scalability,safety,long cycling life,and decoupled power and energy capacities.However,the slow redox kinetics of vanadium species on conventional carbon electrodes remains a major limitation to their performance.We investigated the deposition of carbon black,carbon nanotubes,and electrochemically exfoliated graphene(Exf-Gr)onto thermally-activated carbon paper(ACP)by spray coating to increase the electrode electrocatalytic activity.The modified electrodes were characterized using scanning electron microscopy,X-ray diffraction,Raman spectroscopy,X-ray photoelectron microscopy,and surface area analysis,while their electrochemical properties were evaluated by cyclic voltammetry,electrochemical impedance spectroscopy,and singlecell VRFB testing.Among the modified electrodes,Exf-Gr/ACP had the best performance,achieving a 2.9-fold reduction in charge transfer resistance compared to pristine ACP and delivering 2.5 times the discharge capacity in single-cell tests.This improvement is attributed to Exf-Gr’s high surface area,favorable catalytic activity,and excellent dispersion on the ACP substrate.Surface modification with electrochemically exfoliated graphene is a highly effective strategy for improving the electrode performance in VRFB systems,with significant implications for large-scale energy storage.
基金supported by the funds of the Ministry of Science and Technology of China(2019YFA0904700)the National Natural Science Foundation of China(32471477)to Cheng Qi.
文摘Biological nitrogen fixation(BNF)and photosynthetic carbon fixation underpin food production and climate mitigation,yet natural systems are constrained by oxygen sensitivity,high energy demand,and inefficient catalysts.This review synthesizes advances that recast these processes as engineering targets and proposes a conceptual roadmap that bridges synthetic symbioses with the synthetic biology of enzymes and pathways.For BNF,progress spans cross-kingdom strategies—from refactoring nif gene sets and targeting nitrogenase assembly to eukaryotic organelles,to engineering plant-associated diazotrophs,rhizosphere control circuits,and emerging nodule-like microenvironments.For carbon assimilation,new-to-nature CO_(2)-fixation modules and photorespiratory bypasses illustrate how pathway redesign and alternative carboxylases can circumvent key Calvin–Benson–Bassham limitations,and expanding photosynthetic light capture offers additional leverage.Across these domains,we extract common design principles:(i)nitrogenase output is increasingly governed by carbon/energy supply and electron delivery as much as by oxygen protection;(ii)robust function requires compartment-aware enzyme–chassis coordination,substrate channeling,and dynamic regulation using sensors and control circuits;and(iii)scalable implementation may benefit from distributing metabolic labor across engineered consortia rather than forcing all functions into a single host.We discuss enabling technologies—including AI-guided protein design and directed evolution,cell-free prototyping,chassis toolkits,and materials/bioelectrochemical interfaces—that can accelerate design–build–test–learn cycles and reduce barriers to deployment.Together,these insights define a path toward integrated nitrogen and carbon fixation systems for low-emission agriculture and biomanufacturing.
基金Supported by the National Natural Science Foundation of China(Grant 22578376,52374283)the Natural Science Foundation of Jiangsu Province(Grant BK20240332)。
文摘In this study,melamine and cyanuric acid were used as precursors to form supramolecular crystals via hydrogen-bond-assisted self-assembly followed by hydrothermal treatment.Subsequent high-temperature calcination yielded a novel brush-like three-dimensional carbon nitride.The brush-like 3D architecture was found to expose more accessible active sites,markedly accelerate electron transfer,and suppress the recombination of photogenerated charge carriers.The resulting superoxide(O_(2)^(-·))and hydroxyl(·OH)radicals generated via electron reduction were identified as the key reactive species in the photocatalytic process.Moreover,the surface of the brush-like structure is enriched with nitrogen vacancies,which enhance the catalyst’s ability to harvest visible light.The photocatalytic performance of the brush-like CNS-650 catalyst was evaluated for rhodamine B(RhB)degradation.Under red-light irradiation(660 nm),its degradation rate was 7.4 times higher than that of bulk CN.This work provides valuable insights into the design and application of efficient metal-free 3D photocatalysts.
文摘Pitch is an excellent precursor for the production of hard carbon,with pre-oxidation crucial process in the fabrication.The structural changes in the different molecular components of pitch during thermochemical treatment are a key factor in determining the sodium-ion storage of pitchbased hard carbon anodes.We investigated the effects of the different molecular structures in the asphaltene precursor,including aromatic rings and aliphatic chains,on the sodiumion storage behavior of the resulting carbon.We found that polar oxygen functional groups limit the steric hindrance caused by the aromatic rings in pitch,and thus facilitate the introduction of cross-linked structures.During high-temperature carbonization,aromatic rings form a rigid carbon framework that prevents the rearrangement of ordered carbon layers,leading to a short-range disordered carbon structure and promotes the production of closed pores.For example,a material prepared from asphaltene,which contains a large number of oxygen-containing functional groups and macromolecular aromatic rings,using pre-oxidation at 300℃ and carbonization at 1200℃ had a reversible capacity of 316.7 mAh g^(−1) when used as the anode for sodium ion batteries.Our research provides a theoretical basis for the selection of raw materials for the development of high-quality pitch-based hard carbons.
基金supported by National Natural Science Foundation of China(52472194)the Deanship of Research and Graduate Studies at King Khalid University through Large Research Project(RGP-2/687/46).
文摘Zinc-ion supercapacitors(ZISCs)have received considerable interest for energy storage because of their low cost,high safety,and minimal environmental impact.However,they have a low energy density and poor cycling performance.The design of a better cathode material is needed to overcome these limitations.A simple method was used to synthesize binder-free electrochemically exfoliated carbon paper(EECP)which modifies the surface of the paper by introducing oxygen functional groups and thus improves its pseudocapacitance.When used in a Zn-ion supercapacitor(ZISC),an EECPbased cathode provides a large surface area and quick charge transfer.As a result,the ZISC had remarkable charge storage properties and had a dominant capacitive-type charge storage mechanism with 78.8%retention of capacity at 10 mV/s of the total storage.Furthermore,at 1 A/g,the EECP electrode had a maximum capacitance of 252.5 F/g.The EECP electrode retained 81.7%of its capacitance after 10000 cycles,indicating its promise for use in the growing renewable energy sector.A ZISC was also constructed using EECP as the positive electrode and Zn as the negative electrode with a 1 mol L^(−1) ZnSO_(4) electrolyte.It had a capacitance of 186.22 F/g at 1 A/g and a 97.01%retention rate after 10000 cycles.It also had an excellent energy density of 46.6 Wh/kg at a power density of 500.4 W/kg.The material is therefore suitable for use in high-rate next-generation ZISCs.
文摘Carbon-based materials have gained significant attention in anticancer treatment because of their exceptional biocompatibility,yet critical challenges persist in establishing definitive correlations between their porous structures and functional performance.We report the use of a silica template to guide pore formation in the design of mesoporous carbon spheres(mC)with tailored pore structures for improved combined photothermal-chemotherapy.The mesopore size of mC has been adjusted by kinetic control of the resin polymerization and silica hydrolysis.Structural characterization showed that 4.4 nm mesopores enabled an exceptional gemcitabine loading of 228 mg g^(−1) and a sustained pH/thermal dual-responsive release with>70%drug release under near-infrared(NIR)irradiation.Finite element analysis demonstrated pore size-dependent heat transfer dynamics,with the improved mC achieving a superior photothermal conversion efficiency of 62%by a combination of N-doping and defect engineering.In vitro evaluations confirmed outstanding biocompatibility with>95%cell viability at 200μg mL^(−1) and potent tumor suppression in pancreatic and biliary cancer models with an~5%cell viability at 25μg mL^(−1) where combined therapy showed a 3.7-fold increased cytotoxicity over monotherapy.The improved structure of mC facilitated cascade therapeutic effects with enhanced tumor permeability derived from NIR-triggered hyperthermia and prolonged therapeutic exposure due to pH-responsive drug release.This pore engineering strategy establishes a structure-function process for next-generation theranostic platforms,addressing the critical limitations of conventional pancreatic and biliary cancer therapies through spatiotemporal control of multimodal treatment.
基金Supported by the National Natural Science Foundation of China(22378181).
文摘The development of materials with excellent microwave absorption(MWA)and electromagnetic interference(EMI)shielding performances has currently received attention.Herein,mesophase pitch-based carbon foam(MPCF)with 3D interconnected pore structure was prepared through the high pressure pyrolysis of mesophase coal tar pitch.It is found that the 3D interconnected cellular pores of MPCF facilitate multiple reflections of electromagnetic waves,which results in the minimum reflection loss(RLmin)value of MPCF reaches-37.84 dB with the effective absorption bandwidth(EAB)of 5.44 GHz at a thickness of 2.70 mm,and the total average electromagnetic shielding effectiveness(SE_(T))under 3.00 mm thickness achieves 26.52 dB in X-band.Subsequently,MPCF is activated by KOH to obtain activated carbon foam(A-MPCF).The average SE_(T)of A-MPCF achieves 103.00 dB for abundant nanopores on the pore cell walls,which leads to a transition from the multiple reflections of electromagnetic waves on the walls to diffuse reflection.Unfortunately,the reflection coefficient(R)of A-MPCF increases from 0.78 to 0.90.To reduce the R value,Fe_(3)O_(4)/A-MPCF was fabricated via the in situ growth of nano Fe_(3)O_(4)on A-MPCF.Consequently,the R value of Fe_(3)O_(4)/A-MPCF was reduced from 0.90 to 0.74,whereas the MWA performance was only slightly decreased.This work proposes a simple strategy for simultaneously adjusting MWA and EMI shielding performances of materials.
文摘Lithium–sulfur(Li–S)batteries are promisingcandidates for next-generation energy storagegiven their high energy density and potential low cost.Chemically activated carbon(CAC)is often used fortheir cathodes,because it has a high specific surfacearea for sulfur loading.We have developed a pressurizedphysical activation(PPA)method that producedan activated carbon(PPAC)with a high specific surfacearea comparable to that of CAC.The pore structure of PPAC could be changed and its use as a cathode material for Li–Sbatteries was investigated.Battery tests at different capacity rates(C-rates)showed that it had a much improved high-rate performancewith a discharge capacity of 900 mAh/(g of sulfur)at 1 C,in contrast to only 600 mAh/(g of sulfur)for CAC.Porestructure analyses showed that PPAC prepared at a high activation temperature(1000℃)had unusual channel-like mesoporesbetween the microdomains that are the basic structural units of artificial carbon materials.These are connected to microporesdeveloped in each microdomain,and deliver ions from the surroundings to the internal pores and vice versa.The well-developedmicropores and mesopores of PPAC respectively ensured the high adsorption of lithium polysulfides and a high rate ofion diffusion.Compared to CAC,PPAC is a high-performance,low-cost cathode material that is promising for use in futureLi–S batteries.
基金Supported by National Key R&D Program of China(2025YFE0109700)the National Natural Science Foundation of China(52106150)。
文摘CO_(2) capture and utilization(CCU)technologies have been recognized as crucial strategies for mitigating global warming,reducing carbon emission,and promoting resource circularity.As such,the design and development of related materials have attracted considerable research attention.Carbon-based materials,characterized by tunable pore structures,abundant active sites,high specific surface area,and excellent chemical stability,demonstrate significant potential for applications in CO_(2) capture and utilization.This review systematically analyzes the adsorption behaviors and performance variations of typical carbon materials,including activated carbon,porous carbon,graphene,and carbon nanotubes during CO_(2) capture processes.Concerning CO_(2) utilization,emphasis is placed on recent advances in the catalytic applications of carbon-based materials in key reactions such as methanation,reverse water-gas shift,dry reforming of methane,and alcohol synthesis.Moreover,the benefits and drawbacks of carbon materials in terms of CO_(2) adsorption capacity,catalytic activity,and stability are thoroughly evaluated,and their potential applications in integrated CO_(2) capture and utilization technologies are discussed.Finally,key strategies for enhancing the performance of carbonaceous materials through structural modulation and surface modification are elucidated.This review aims to provide theoretical guidance for the future development and large-scale implementation of carbon-based materials in CCU technologies.
基金supported by the National Key R&D Program of China(No.2022YFC3701500)the Key R&D Plan Projects of Zhejiang Province(No.2024SSYS0072)Zhejiang Provincial Natural Science Foundation(No.LDT23E0601).
文摘Ship operations are crucial to global trade,and their decarbonization is essential to mitigate climate change.This study evaluates the economic viability of existing and emerging decarbonization technologies in maritime shipping using the levelized cost of energy methodology.It includes a detailed comparative analysis based on essential criteria and sensitivity assessments to highlight the economic impacts of technological advancements.Key factors influencing total costs include fuel costs,carbon pricing,and energy demands for carbon capture.The findings reveal that methanol is more cost-effective than heavy fuel oil(HFO)when priced below 3000 CNY/t,assuming HFO costs 4400 CNY/t.Additionally,methanol with post-combustion carbon capture is less expensive than pre-combustion carbon capture.When carbon prices rise above 480 CNY/t,carbon capture technologies prove more economical than purchasing carbon emission allowances for HFO and liquefied natural gas.Enhanc-ing the use of exhaust gas waste heat is recommended for cost savings.Post-combustion carbon capture also shows greater efficiency,requiring about 1.1 GJ/t less energy than pre-combustion methods,leading to lower overall costs.Future research should focus on market mechanisms to stabilize fuel prices and develop less energy-intensive carbon capture technologies.This study offers critical insights into effective decarbonization strategies for advancing global maritime trade in the present and future.
文摘Despite their high theoretical capacity and energy density,lithiumsulfur(Li–S)batteries still face challenges such as soluble lithium polysulfides(LiPSs)shuttling and sluggish redox kinetics.In this work,we used a novel MoS_(2)-Mo_(2)C heterostructure anchored on a carbon sponge(CS)as a Li_(2)S host to solve these problems.A simple hydrothermal process following carbothermal reduction was used to construct the MoS_(2)-Mo_(2)C heterostructure,enabling control of the phases and integration of MoS_(2) and Mo_(2)C.Structural characterization confirmed the coherent interface of the heterostructure with a precise orientation relationship between the two phases and their uniform distribution.An evaluation of the adsorption and catalytic performance of the material showed that it has an exceptional LiPSs adsorption capacity with faster conversion from Li_(2)S_(4) to Li_(2)S_(2).Density functional theory calculations further confirmed these results.As a result,the cathode had a high initial discharge capacity of 693 mAh g^(−1) at 0.2 C and achieved stable cycling at 2 C for 500 cycles with a low decay rate of 0.107%per cycle.The heterostructure design,coupled with the macroporous CS framework,effectively prevented the shuttling and increased sulfur utilization,offering a promising way to produce practical high-energydensity Li–S batteries.
文摘The effects of nitrogen(N)deposition on forest soil organic carbon(SOC)are largely unclear,likely due to the divergent responses of particulate(POC)and mineral-associated carbon(MAOC).Conventional understory inorganic N(UIN)additions neglect canopy processes and the impacts of organic N,potentially misevaluating N deposition effects.This study was conducted in a long-term N addition experiment established in a Moso bamboo forest,which included six treatments combining canopy and understory N additions with organic(urea glycine)and inorganic(NH_(4)NO_(3))forms at a rate of 50 kg N·ha^(-1)·yr^(-1).Litterbags were installed for a two-year decomposition experiment and collected at quarterly intervals,together with concurrent soil sampling under litterbags at 0–10 cm depth.We aimed to examine the effects of canopy vs.understory N addition and organic vs.inorganic N form on soil POC and MAOC concentrations.Our results showed that canopy N additions significantly reduced POC(ased POC-15.9%)but did not affect MAOC(P>0.05).Conversely,understory N additions significantly incre(30.9%)and decreased MAOC(and fungal diversity(FuD),-28.9%).Canopy N additions decreased POC by enhancing peroxidase activity while understory N additions promoted POC by inhibiting litter decomposition.Additionally,understory N addition-induced soil acidification decreased soil Ca^(2+)concentration,microbial carbon use efficiency,and bacterial necromass C,as well as the release of litter water-soluble compounds,thereby inhibiting MAOC.Moreover,nitrogen forms(organic vs.inorganic)had no effect on SOC fractions.Our findings underscore that canopy and understory N addition approaches differentially regulate SOC fractions by altering litter decomposition–microbial–mineral interactions,and the understory approach may overestimate soil POC gain and MAOC loss driven by atmospheric N deposition.
