MnO_(2) stands out among cathode materials for aqueous zinc-ion batteries(AZIBs)high capacity and voltage,it has poor stability and slow Zn^(2+) kinetics.Herein,we propose a dual-regulation strategy integrating copper...MnO_(2) stands out among cathode materials for aqueous zinc-ion batteries(AZIBs)high capacity and voltage,it has poor stability and slow Zn^(2+) kinetics.Herein,we propose a dual-regulation strategy integrating copper doping and carbon-based confinement.Residual carbon(RC),derived from acid-washed coal gasification fine slag(CGFS),serves as a conductive and porous framework for the directional growth of Cu-doped MnO_(2) nanowires(CMO@RC).The synergistic modulation of Cu-induced electronic structure tuning and carbon confinement induced mechanical/electrical stabilization significantly enhances Zn^(2+) transport and electrochemical performance.CMO@RC achieves a high capacity of 563 mA·h·g^(−1) at 0.1 A·g^(−1) and maintains 106%after 1000 cycles at 1 A·g^(−1).Kinetic analyses confirm the dual-path Zn^(2+) diffusion and accelerated reaction kinetics,while DFT calculations reveal that Cu doping enhances Mn 3d orbital hybridization and electron interaction with carbon,elevating the density of states near the Fermi level and reducing charge transfer barriers.Furthermore,pouch cell testing demonstrates outstanding flexibility and mechanical resilience.This study provides a cost-effective and scalable strategy for high-performance AZIBs,leveraging both experimental and theoretical validations.展开更多
For rechargeable aqueous zinc-ion batteries(ZIBs),the design of nanocomposites comprised of electrochemically active materials and carbon materials with novel structures has great prom-ise in addressing the issue of e...For rechargeable aqueous zinc-ion batteries(ZIBs),the design of nanocomposites comprised of electrochemically active materials and carbon materials with novel structures has great prom-ise in addressing the issue of electrical conductivity and structural stability in the electrode materials during electrochemical cycling.We report the production of a novel flexible electrode material,by anchoring MnO_(2) nanosheets on a B,N co-doped carbon nanotube ar-ray(BNCNTs)grown on carbon cloth(BNCNTs@MnO_(2)),which was fabricated by in-situ pyrolysis and hydrothermal growth.The generated BNCNTs were strongly bonded to the surface of the car-bon fibers in the carbon cloth which provides both excellent elec-tron transport and ion diffusion,and improves the stability and dur-ability of the cathode.Importantly,the BNCNTs offer more active sites for the hydrothermal growth of MnO_(2),ensuring a uniform dis-tribution.Electrochemical tests show that BNCNTs@MnO_(2) delivers a high specific capacity of 310.7 mAh g^(−1) at 0.1 A g^(−1),along with excellent rate capability and outstanding cycling stability,with a 79.7% capacity retention after 8000 cycles at 3 A g^(−1).展开更多
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
Rational developing high-performance and economically efficient dual-functional oxygen electrocatalysts to drive the lumberly reactivity rates of oxygen reduction reaction(ORR)and oxygen evolution reaction(OER)in Zn-a...Rational developing high-performance and economically efficient dual-functional oxygen electrocatalysts to drive the lumberly reactivity rates of oxygen reduction reaction(ORR)and oxygen evolution reaction(OER)in Zn-air batteries is highly attractive,yet remains conceptually challenging.Herein,Ni/MnO heterostructure nanosheets and nanoparticles firmly anchored onto the N-doped carbon nanofibers(noted as Ni/MnO@N-C NS/NFs)for efficient bifunctional ORR/OER electrocatalysis are designed and realized through a facile electrospinning-pyrolysis-etching strategy.The epitaxial in situ grown Ni/MnO with enriched oxygen vacancies stimulated the charge redistribution in their coupling regions,which effectively optimizes the adsorption/desorption of O-related intermediates in ORR/OER.Benefiting from the Ni/MnO heterostructure moieties and the unique two-dimensional/one-dimensional(2D/1D)superstructure of carbon support with abundantly dispersive active species,the resultant Ni/MnO@N-C NS/NFs deliver robust ORR activity and OER property(an overpotential of 306 mV to obtain 10 mA·cm^(-2))with a smaller potential gap(ΔE=0.77 V)in alkaline electrolyte.More significantly,practical zinc-air battery building with Ni/MnO@N-C NS/NFs delivers a higher open circuit voltage,excellent output power density,and prominent durability with stable charging and discharging cycle life.The present work demonstrates a crucial understanding of building advanced heterostructure electrocatalysts with enriched oxygen vacancies for metal-air batteries application.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
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
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
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
Soil organic carbon(SOC)dynamics significantly influence ecosystem carbon source-sink balance,particularly in agroecosystems.However,uncertainty remains regarding optimal land use types for maximizing farmland carbon ...Soil organic carbon(SOC)dynamics significantly influence ecosystem carbon source-sink balance,particularly in agroecosystems.However,uncertainty remains regarding optimal land use types for maximizing farmland carbon storage across different soil types,and identifying effective land management practices for enhanced carbon accumulation is essential for reducing agricultural emissions and strengthening carbon sinks.This study examined SOC variations in eastern Yunnan’s subtropical highlands(2,132 sites),analyzing topsoil(0–20 cm)across five land uses(dryland,irrigated land,forestland,grassland and plantation)of five soil types(red,yellow,yellowbrown,brown,purple).The investigation explored relationships between SOC and edaphic factors(26 elements)to determine SOC influencing factors.The study area demonstrated a mean SOC content of 27.78 g kg^(–1),with distinct spatial heterogeneity characterized by lower values in the southwestern sector and higher concentrations in the northeastern region.Brown soils displayed the highest SOC content(P<0.05),followed by yellow-brown then red,yellow,and purple soils.Irrigation significantly enhanced SOC storage,particularly in brown soils where irrigated land contained 2.2-,2.4-,and 1.6-times higher SOC than forestland,grassland,and dryland,respectively.Similar irrigation benefits occurred in purple,yellow,and yellow-brown soils,indicating moisture limitation as the primary SOC constraint.Notably,SOC exhibited strong positive correlations with nitrogen,sulfur,and selenium.Nitrogen fertilization demonstrated dual benefits:enhancing SOC sequestration and promoting Se enrichment in crops,potentially supporting specialty agriculture.Although land use impacts on SOC varied across soil types(P>0.05),irrigation consistently emerged as the optimal management for carbon sink enhancement.These findings suggest that targeted water management could effectively reduce farmland carbon emissions in moisture-limited subtropical highlands.Strategic nitrogen application offers co-benefits for soil fertility and selenium biofortification,providing practical pathways for climate-smart agriculture in similar ecoregions.展开更多
To elucidate the effect of calcite-regulated activated carbon(AC)structure on low-temperature denitrification performance of SCR catalysts,this work prepared a series of Mn-Ce/De-AC-xCaCO_(3)(x is the calcite content ...To elucidate the effect of calcite-regulated activated carbon(AC)structure on low-temperature denitrification performance of SCR catalysts,this work prepared a series of Mn-Ce/De-AC-xCaCO_(3)(x is the calcite content in coal)catalysts were prepared by the incipient wetness impregnation method,followed by acid washing to remove calcium-containing minerals.Comprehensive characterization and low-temperature denitrification tests revealed that calcite-induced structural modulation of coal-derived AC significantly enhances catalytic activity.Specifically,NO conversion increased from 88.3%of Mn-Ce/De-AC to 91.7%of Mn-Ce/De-AC-1CaCO_(3)(210℃).The improved SCR denitrification activity results from the enhancement of physicochemical properties including higher Mn^(4+)content and Ce^(4+)/Ce^(3+)ratio,an abundance of chemisorbed oxygen and acidic sites,which could strengthen the SCR reaction pathways(richer NH_(3)activated species and bidentate nitrate active species).Therefore,NO removal is enhanced.展开更多
Understanding the dynamics of vegetation carbon sequestration(VCS)is essential for regional carbon neutrality strategies.This study revealed the spatiotemporal patterns of VCS and its relationship with anthropogenic c...Understanding the dynamics of vegetation carbon sequestration(VCS)is essential for regional carbon neutrality strategies.This study revealed the spatiotemporal patterns of VCS and its relationship with anthropogenic carbon emissions(ACEs)in Shandong Province,China during 2000-2020,and identified the sensitivity factors affecting VCS.The results show that:1)VCS increased consistently from 193.45 million t to 256.41 million t,with high values areas concentrated in the central,northeastern,and southeastern mountainous and hilly regions,while low values were found in water bodies and urban built-up areas.At the city level,Linyi,Yantai,Binzhou,and Jinan experienced the most significant rises-reaching up to 243000 t/yr.At the county level,Pingdu,Qixia,and Yiyuan also showed substantial growth,each exceeding 30400 t/yr.2)Digital Elevation Molde(DEM)was identified as the dominant natural factor influencing VCS distribution,while land use optimization measures,especially afforestation and farmland conversion in sloped terrain,were the primary human drivers of VCS increase.3)Urbanization and carbon neutrality were not mutually exclusive.While urban expansion locally reduced VCS,rural emigration enhanced carbon sinks in surrounding areas,partially offsetting urban losses.This compensatory mechanism supported VCS increases in nearly all cities and 90% of counties.Nevertheless,with ACEs continuing to rise and the offset ratio by VCS declining,achieving carbon neutrality requires regional strategies that integrate with accelerated energy conservation,emission reduction technologies,and energy transition.These findings provide a scientific basis for decomposing carbon neutrality targets across cities and counties in Shandong and a reference for developing localized land use policies in similar regions.展开更多
Sodium-based dual-ion batteries(SDIBs)have been attracting increasing attention in recent years owing to their low cost,environmental benignancy,and high operating voltage.However,the sluggish ion kinetics of conventi...Sodium-based dual-ion batteries(SDIBs)have been attracting increasing attention in recent years owing to their low cost,environmental benignancy,and high operating voltage.However,the sluggish ion kinetics of conventional carbon anodes that cannot match the fast capacitive anion intercalation behavior of graphite cathodes constraints on improving power density of SDIBs.Herein,we present an ingenious carbon microdomain engineering strategy to fabricate high-performance carbon anode with ion-mediated high-activity nitrogen species and molecular-scale closed-pore architectures.Experimental characterizations and theoretical investigations demonstrate that Zn^(2+)-mediated structural engineering tailors oxidized nitrogen species,which proficiently accelerate the sodium-ion desolvation kinetics;meanwhile the acetate-mediated pore-forming process modulates closed pores,which synergistically afford abundant sodium storage sites for high plateau-region capacity.As a result,the optimized microdomain engineered carbon material(MEC_(3))tailored with the optimal amount of zinc acetate demonstrates an outstanding plateau-region capacity of 253 mAh g^(-1)even at 1 C,among the highest reported values.Consequently,the MEC_(3)||expanded graphite dual-ion battery exhibits an unprecedented cycling stability at high current rate,maintaining 80.6%capacity retention after 10,000 cycles at 10 C,among the best reports.This microdomain engineering strategy provides a new design principle for overcoming kinetic limitations of carbonaceous materials in plateau-dominated sodium storage systems.展开更多
We proposed a strategy to address the issue by synthesizing MnO with half-filled 3 d electron orbitals.That is,MnO nanocubes with an edge length of 61.82 nm were successfully prepared through electros-pinning and one-...We proposed a strategy to address the issue by synthesizing MnO with half-filled 3 d electron orbitals.That is,MnO nanocubes with an edge length of 61.82 nm were successfully prepared through electros-pinning and one-step pyrolysis as the cathode electrode for Li-O_(2)batteries.It is observed that the intermediate LiMnO_(4)rather than Li_(2)O_(2)is formed when LiO_(2)interactes with MnO(111)during the discharge process.It is precisely because of LiMnO_(4)that reduces its charge overpotential to 0.29 V.The novel reaction mechanism dominated by LiMnO_(4)further facilitates the lower charge overpotential,thereby enhancing the energy efficiency of the batteries.展开更多
Porous carbon microspheres are widely regarded as a superior CO_(2) adsorbent due to their exceptional efficiency and affordability.However,better adsorption performance is very attractive for porous carbon microspher...Porous carbon microspheres are widely regarded as a superior CO_(2) adsorbent due to their exceptional efficiency and affordability.However,better adsorption performance is very attractive for porous carbon microspheres.And modification of the pore structure is one of the effective strategies.In this study,multi-cavity mesoporous carbon microspheres were successfully synthesized by the synergistic method of soft and hard templates,during which a phenolic resin with superior thermal stability was employed as the carbon precursor and a mixture of silica sol and F108 as the mesoporous template.Carbon microspheres with multi-cavity mesoporous structures were prepared,and all the samples showed highly even mesopores,with diameters around 12 nm.The diameter of these microspheres decreased from 396.8 nm to about 182.5 nm with the increase of silica sol.After CO_(2) activation,these novel carbon microspheres(APCF0.5-S1.75)demonstrated high specific surface area(983.3 m^(2)/g)and remarkable CO_(2) uptake of 4.93 mmol/g at 0℃ and1 bar.This could be attributed to the unique multi-cavity structure,which offers uniform mesoporous pore channels,minimal CO_(2) transport of and a greater number of active sites for CO_(2) adsorption.展开更多
基金support from the Key projects of scientific research projects of universities in Anhui Province(2024AH050360).
文摘MnO_(2) stands out among cathode materials for aqueous zinc-ion batteries(AZIBs)high capacity and voltage,it has poor stability and slow Zn^(2+) kinetics.Herein,we propose a dual-regulation strategy integrating copper doping and carbon-based confinement.Residual carbon(RC),derived from acid-washed coal gasification fine slag(CGFS),serves as a conductive and porous framework for the directional growth of Cu-doped MnO_(2) nanowires(CMO@RC).The synergistic modulation of Cu-induced electronic structure tuning and carbon confinement induced mechanical/electrical stabilization significantly enhances Zn^(2+) transport and electrochemical performance.CMO@RC achieves a high capacity of 563 mA·h·g^(−1) at 0.1 A·g^(−1) and maintains 106%after 1000 cycles at 1 A·g^(−1).Kinetic analyses confirm the dual-path Zn^(2+) diffusion and accelerated reaction kinetics,while DFT calculations reveal that Cu doping enhances Mn 3d orbital hybridization and electron interaction with carbon,elevating the density of states near the Fermi level and reducing charge transfer barriers.Furthermore,pouch cell testing demonstrates outstanding flexibility and mechanical resilience.This study provides a cost-effective and scalable strategy for high-performance AZIBs,leveraging both experimental and theoretical validations.
基金financial support from projects funded by the National Natural Science Foundation of China(52172038,22179017)the National Key Research and Development Program of China(2022YFB4101600,2022YFB4101601)。
文摘For rechargeable aqueous zinc-ion batteries(ZIBs),the design of nanocomposites comprised of electrochemically active materials and carbon materials with novel structures has great prom-ise in addressing the issue of electrical conductivity and structural stability in the electrode materials during electrochemical cycling.We report the production of a novel flexible electrode material,by anchoring MnO_(2) nanosheets on a B,N co-doped carbon nanotube ar-ray(BNCNTs)grown on carbon cloth(BNCNTs@MnO_(2)),which was fabricated by in-situ pyrolysis and hydrothermal growth.The generated BNCNTs were strongly bonded to the surface of the car-bon fibers in the carbon cloth which provides both excellent elec-tron transport and ion diffusion,and improves the stability and dur-ability of the cathode.Importantly,the BNCNTs offer more active sites for the hydrothermal growth of MnO_(2),ensuring a uniform dis-tribution.Electrochemical tests show that BNCNTs@MnO_(2) delivers a high specific capacity of 310.7 mAh g^(−1) at 0.1 A g^(−1),along with excellent rate capability and outstanding cycling stability,with a 79.7% capacity retention after 8000 cycles at 3 A g^(−1).
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 the National Natural Science Foundation of China(No.22302096)the Natural Science Foundation of Jiangsu Higher Education Institutions of China(Nos.23KJB150039 and 24KJB150026)+1 种基金Natural Science Foundation of Zhejiang Province(No.LQ24E040002)the Natural Science Foundation of Huzhou City(No.2023YZ18).
文摘Rational developing high-performance and economically efficient dual-functional oxygen electrocatalysts to drive the lumberly reactivity rates of oxygen reduction reaction(ORR)and oxygen evolution reaction(OER)in Zn-air batteries is highly attractive,yet remains conceptually challenging.Herein,Ni/MnO heterostructure nanosheets and nanoparticles firmly anchored onto the N-doped carbon nanofibers(noted as Ni/MnO@N-C NS/NFs)for efficient bifunctional ORR/OER electrocatalysis are designed and realized through a facile electrospinning-pyrolysis-etching strategy.The epitaxial in situ grown Ni/MnO with enriched oxygen vacancies stimulated the charge redistribution in their coupling regions,which effectively optimizes the adsorption/desorption of O-related intermediates in ORR/OER.Benefiting from the Ni/MnO heterostructure moieties and the unique two-dimensional/one-dimensional(2D/1D)superstructure of carbon support with abundantly dispersive active species,the resultant Ni/MnO@N-C NS/NFs deliver robust ORR activity and OER property(an overpotential of 306 mV to obtain 10 mA·cm^(-2))with a smaller potential gap(ΔE=0.77 V)in alkaline electrolyte.More significantly,practical zinc-air battery building with Ni/MnO@N-C NS/NFs delivers a higher open circuit voltage,excellent output power density,and prominent durability with stable charging and discharging cycle life.The present work demonstrates a crucial understanding of building advanced heterostructure electrocatalysts with enriched oxygen vacancies for metal-air batteries application.
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.
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.
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.
基金funded by the Yunnan Provincial Key Programs for Basic Research Project,China(202301AS070087)the Yunnan Provincial R&D Program,China(202405AF140014 and 202302AO370015)the National Natural Science Foundation of China(42307058).
文摘Soil organic carbon(SOC)dynamics significantly influence ecosystem carbon source-sink balance,particularly in agroecosystems.However,uncertainty remains regarding optimal land use types for maximizing farmland carbon storage across different soil types,and identifying effective land management practices for enhanced carbon accumulation is essential for reducing agricultural emissions and strengthening carbon sinks.This study examined SOC variations in eastern Yunnan’s subtropical highlands(2,132 sites),analyzing topsoil(0–20 cm)across five land uses(dryland,irrigated land,forestland,grassland and plantation)of five soil types(red,yellow,yellowbrown,brown,purple).The investigation explored relationships between SOC and edaphic factors(26 elements)to determine SOC influencing factors.The study area demonstrated a mean SOC content of 27.78 g kg^(–1),with distinct spatial heterogeneity characterized by lower values in the southwestern sector and higher concentrations in the northeastern region.Brown soils displayed the highest SOC content(P<0.05),followed by yellow-brown then red,yellow,and purple soils.Irrigation significantly enhanced SOC storage,particularly in brown soils where irrigated land contained 2.2-,2.4-,and 1.6-times higher SOC than forestland,grassland,and dryland,respectively.Similar irrigation benefits occurred in purple,yellow,and yellow-brown soils,indicating moisture limitation as the primary SOC constraint.Notably,SOC exhibited strong positive correlations with nitrogen,sulfur,and selenium.Nitrogen fertilization demonstrated dual benefits:enhancing SOC sequestration and promoting Se enrichment in crops,potentially supporting specialty agriculture.Although land use impacts on SOC varied across soil types(P>0.05),irrigation consistently emerged as the optimal management for carbon sink enhancement.These findings suggest that targeted water management could effectively reduce farmland carbon emissions in moisture-limited subtropical highlands.Strategic nitrogen application offers co-benefits for soil fertility and selenium biofortification,providing practical pathways for climate-smart agriculture in similar ecoregions.
基金Supported by the Science and Technology Cooperation and Exchange special project of Cooperation of Shanxi Province(202404041101014)the Fundamental Research Program of Shanxi Province(202403021212333)+3 种基金the Joint Funds of the National Natural Science Foundation of China(U24A20555)the Lvliang Key R&D of University-Local Cooperation(2023XDHZ10)the Initiation Fund for Doctoral Research of Taiyuan University of Science and Technology(20242026)the Outstanding Doctor Funding Award of Shanxi Province(20242080).
文摘To elucidate the effect of calcite-regulated activated carbon(AC)structure on low-temperature denitrification performance of SCR catalysts,this work prepared a series of Mn-Ce/De-AC-xCaCO_(3)(x is the calcite content in coal)catalysts were prepared by the incipient wetness impregnation method,followed by acid washing to remove calcium-containing minerals.Comprehensive characterization and low-temperature denitrification tests revealed that calcite-induced structural modulation of coal-derived AC significantly enhances catalytic activity.Specifically,NO conversion increased from 88.3%of Mn-Ce/De-AC to 91.7%of Mn-Ce/De-AC-1CaCO_(3)(210℃).The improved SCR denitrification activity results from the enhancement of physicochemical properties including higher Mn^(4+)content and Ce^(4+)/Ce^(3+)ratio,an abundance of chemisorbed oxygen and acidic sites,which could strengthen the SCR reaction pathways(richer NH_(3)activated species and bidentate nitrate active species).Therefore,NO removal is enhanced.
基金Under the auspices of the National Natural Science Foundation of China(No.42476247,42461015)the Open Research Fund of Key Laboratory of Coastal Science and Integrated Management,Ministry of Natural Resources(No.2024COSIM01)Guangxi Science and Technology Base and Talent Special Project(No.GuikeAD23026194)。
文摘Understanding the dynamics of vegetation carbon sequestration(VCS)is essential for regional carbon neutrality strategies.This study revealed the spatiotemporal patterns of VCS and its relationship with anthropogenic carbon emissions(ACEs)in Shandong Province,China during 2000-2020,and identified the sensitivity factors affecting VCS.The results show that:1)VCS increased consistently from 193.45 million t to 256.41 million t,with high values areas concentrated in the central,northeastern,and southeastern mountainous and hilly regions,while low values were found in water bodies and urban built-up areas.At the city level,Linyi,Yantai,Binzhou,and Jinan experienced the most significant rises-reaching up to 243000 t/yr.At the county level,Pingdu,Qixia,and Yiyuan also showed substantial growth,each exceeding 30400 t/yr.2)Digital Elevation Molde(DEM)was identified as the dominant natural factor influencing VCS distribution,while land use optimization measures,especially afforestation and farmland conversion in sloped terrain,were the primary human drivers of VCS increase.3)Urbanization and carbon neutrality were not mutually exclusive.While urban expansion locally reduced VCS,rural emigration enhanced carbon sinks in surrounding areas,partially offsetting urban losses.This compensatory mechanism supported VCS increases in nearly all cities and 90% of counties.Nevertheless,with ACEs continuing to rise and the offset ratio by VCS declining,achieving carbon neutrality requires regional strategies that integrate with accelerated energy conservation,emission reduction technologies,and energy transition.These findings provide a scientific basis for decomposing carbon neutrality targets across cities and counties in Shandong and a reference for developing localized land use policies in similar regions.
基金support from the National Key R&D Program of China(2022YFB2402600)the National Natural Science Foundation of China(52125105,52572282,52472269,52273312,22309200)+3 种基金Guangdong Basic and Applied Basic Research Foundation(2024A1515010201,2024A1515012379,2024A1515011670,2023A1515011519)Guangdong Special Support Program Outstanding Young Talents in Science and Technology Innovation(2021TQ05L894)Shenzhen Science and Technology Planning Project(JSGG20220831104004008,SGDX20230116092055008,KCXST20221021111606016)the NSRF via the Program Management Unit for Human Resources&Institutional Development,Research and Innovation(B49G680115).
文摘Sodium-based dual-ion batteries(SDIBs)have been attracting increasing attention in recent years owing to their low cost,environmental benignancy,and high operating voltage.However,the sluggish ion kinetics of conventional carbon anodes that cannot match the fast capacitive anion intercalation behavior of graphite cathodes constraints on improving power density of SDIBs.Herein,we present an ingenious carbon microdomain engineering strategy to fabricate high-performance carbon anode with ion-mediated high-activity nitrogen species and molecular-scale closed-pore architectures.Experimental characterizations and theoretical investigations demonstrate that Zn^(2+)-mediated structural engineering tailors oxidized nitrogen species,which proficiently accelerate the sodium-ion desolvation kinetics;meanwhile the acetate-mediated pore-forming process modulates closed pores,which synergistically afford abundant sodium storage sites for high plateau-region capacity.As a result,the optimized microdomain engineered carbon material(MEC_(3))tailored with the optimal amount of zinc acetate demonstrates an outstanding plateau-region capacity of 253 mAh g^(-1)even at 1 C,among the highest reported values.Consequently,the MEC_(3)||expanded graphite dual-ion battery exhibits an unprecedented cycling stability at high current rate,maintaining 80.6%capacity retention after 10,000 cycles at 10 C,among the best reports.This microdomain engineering strategy provides a new design principle for overcoming kinetic limitations of carbonaceous materials in plateau-dominated sodium storage systems.
基金Funded by the National Natural Science Foundation of China(No.22075035)the Technology Planning Project of Liaoning Province(No.2020JH2/10700008)the Dalian Science and Technology Innovation Fund Project(No.2022JJ11CG005)。
文摘We proposed a strategy to address the issue by synthesizing MnO with half-filled 3 d electron orbitals.That is,MnO nanocubes with an edge length of 61.82 nm were successfully prepared through electros-pinning and one-step pyrolysis as the cathode electrode for Li-O_(2)batteries.It is observed that the intermediate LiMnO_(4)rather than Li_(2)O_(2)is formed when LiO_(2)interactes with MnO(111)during the discharge process.It is precisely because of LiMnO_(4)that reduces its charge overpotential to 0.29 V.The novel reaction mechanism dominated by LiMnO_(4)further facilitates the lower charge overpotential,thereby enhancing the energy efficiency of the batteries.
基金supported by the National Key R&D Program of China(No.2021YFB3501102).
文摘Porous carbon microspheres are widely regarded as a superior CO_(2) adsorbent due to their exceptional efficiency and affordability.However,better adsorption performance is very attractive for porous carbon microspheres.And modification of the pore structure is one of the effective strategies.In this study,multi-cavity mesoporous carbon microspheres were successfully synthesized by the synergistic method of soft and hard templates,during which a phenolic resin with superior thermal stability was employed as the carbon precursor and a mixture of silica sol and F108 as the mesoporous template.Carbon microspheres with multi-cavity mesoporous structures were prepared,and all the samples showed highly even mesopores,with diameters around 12 nm.The diameter of these microspheres decreased from 396.8 nm to about 182.5 nm with the increase of silica sol.After CO_(2) activation,these novel carbon microspheres(APCF0.5-S1.75)demonstrated high specific surface area(983.3 m^(2)/g)and remarkable CO_(2) uptake of 4.93 mmol/g at 0℃ and1 bar.This could be attributed to the unique multi-cavity structure,which offers uniform mesoporous pore channels,minimal CO_(2) transport of and a greater number of active sites for CO_(2) adsorption.
