Photoelectrochemical CO_(2)reduction to multi-carbon products fuels remains challenged by inefficient C–C coupling and competing proton reduction reaction.Herein,we designed a cationic covalent organic framework(COF+...Photoelectrochemical CO_(2)reduction to multi-carbon products fuels remains challenged by inefficient C–C coupling and competing proton reduction reaction.Herein,we designed a cationic covalent organic framework(COF+)to create an electrostatic microenvironment that synergizes with CuPt alloy nanoparticles for selective ethylene/ethane production.By spatially decoupling CO_(2)enrichment from proton exclusion,the COF^(+)/CuPt interface simultaneously facilitates CO_(2)accessibility while impeding H+migration,suppressing the hydrogen evolution reaction(HER).This unique microenvironment stabilizes key anionic intermediates(*COO^(−),*OCCO^(−))and promotes*CO dimerization,steering electron transfer toward C–C coupling.The optimized system achieves a record-high Faradaic efficiency of 51.5%±5.3%for ethane and 10.6%±2.5%for ethylene with a total C2+yield exceeding 62%at−0.25 V vs.RHE and high stability(>300 min),representing the highest performance for photoelectrochemical CO_(2)reduction to ethane.The combined analyses of in situ spectroscopy and theoretical calculations reveal that electrostatic field effects lower the energy barrier for*OCCO formation while accelerating hydrogenation kinetics.Therefore,this work demonstrates that microenvironment modification of the active site by cationic covalent organic framework is a versatile strategy for solar-driven CO_(2)conversion into value-added hydrocarbons.展开更多
The bidirectional convergence of artificial intelligence and nanophotonics drives photonic technologies toward unprecedented levels of intelligence and efficiency,fundamentally reshaping their design paradigms and app...The bidirectional convergence of artificial intelligence and nanophotonics drives photonic technologies toward unprecedented levels of intelligence and efficiency,fundamentally reshaping their design paradigms and application boundaries.With its powerful data-driven and nonlinear optimization capabilities,artificial intelligence has become a powerful tool for optical design,enabling the inverse design of nanophotonics devices while accelerating the forward computation of electromagnetic responses.Conversely,nanophotonics provides a wave-based computational platform,giving rise to novel optical neural networks that achieve high-speed parallel computing and efficient information processing.This paper reviews the latest progress in the bidirectional field of artificial intelligence and nanophotonics,analyzes the basic principles of various applications from a universal perspective,comprehensively evaluates the advantages and limitations of different research methods,and makes a forwardlooking outlook on the bidirectional integration of artificial intelligence and nanophotonics,focusing on analyzing future development trends,potential applications,and challenges.The deep integration of artificial intelligence and nanophotonics is ushering in a new era for photonic technologies,offering unparalleled opportunities for fundamental research and industrial applications.展开更多
The electrochemical CO_(2) reduction reaction(eCO_(2)RR),producing gaseous C_(2+)products such as ethylene(C_(2)H_(4)),represents a sustainable strategy to mitigate the greenhouse effect.Inspired by the promotion effe...The electrochemical CO_(2) reduction reaction(eCO_(2)RR),producing gaseous C_(2+)products such as ethylene(C_(2)H_(4)),represents a sustainable strategy to mitigate the greenhouse effect.Inspired by the promotion effect of the cyano group(-C≡N) for C-C coupling in organic chemistry,several cyano-containing organocatalysts have been found to be capable of directly converting CO_(2) into C_(2)H_(4) with-C≡N as the active center during the eCO_(2)RR.The selectivity of C_(2)H_(4) for the representative catalyst,metal-free dicyandiamide(DCD),reached 27.6 % after partial hydrogenation in KHCO_(3) solution.In addition,its selectivity can be further improved to 57.7 % when coupled with oriented Cu crystals.The experimental and computational results collectively reveal that charge redistribution between Cu{100} and DCD promotes the partial hydrogenation of the cyano group and lays the foundation for the reduced energy barrier for the CO_(2) reduction on-C≡N.This study breaks the limitations of traditional metal/metal oxide-based catalysts by using cyano-containing organocatalysts for direct C_(2+) product generation,expanding the eCO_(2)RR catalyst library.In addition,this research elucidates the role of charge redistribution and cyano group hydrogenation in lowering reaction barriers,providing fundamental guidance for the design of new organocatalysts.展开更多
Copper complexes inspired by O_(2)-activating enzymes have been widely investigated as molecular water oxidation catalysts,capable of facile and reversible O─O bond formation and cleavage under mild conditions.In thi...Copper complexes inspired by O_(2)-activating enzymes have been widely investigated as molecular water oxidation catalysts,capable of facile and reversible O─O bond formation and cleavage under mild conditions.In this study,two copper phenanthroline complexes,namely,Cu(phen)and Cu(dophen),exhibit high turnover frequencies(TOFs)of 74±13 and(5.66±0.29)×10^(3)s^(−1)for water oxidation,respectively.Moreover,amino acid-functionalized carbon dots(CDs)were used to support the adhesion of the[Cu]complexes onto the electrode,significantly enhancing the TOFs of(2.80±0.12)×10^(3)and(4.11±0.24)×10^(4)s^(−1),respectively,exceeding the activity of photosystem Ⅱ in nature.Remarkably,the amino acid-functionalized CDs provide a secondary sphere that mimics the catalytic microenvironment of the copper centre,which promotes proton-coupled electron transfer and O─O bond formation.Finally,the photovoltaic-electrolysis(PVE)system was established using CDs-supported Cu catalysts and commercial silicon solar panels,achieving a high solar-to-hydrogen efficiency of 11.59%under the illumination of AM 1.5 G.This represents the most efficient solar-driven water splitting system based on copper-based catalysts to date,introducing the biomimetic secondary sphere to a“proton-rocking”process for water oxidation catalysis and application of the PVE system.展开更多
Al-based TiC particle-reinforced composites with varying TiC concentrations were fabricated through semi-continuous casting.The effects of TiC particles on the alloys’microstructure,grain boundary segregation,and mec...Al-based TiC particle-reinforced composites with varying TiC concentrations were fabricated through semi-continuous casting.The effects of TiC particles on the alloys’microstructure,grain boundary segregation,and mechanical properties were systematically analyzed.Moreover,the mechanisms by which TiC particles contribute to grain refinement,suppression of grain boundary segregation,and enhancement of hardness and wear resistance were discussed.The results demonstrate that TiC particles act as heterogeneous nucleation sites forα-Al within the Al-Cu-Mn alloys,leading to a refinement of grain size.As the TiC particle’s content increases,the grain size of the alloy drops at first and then elevates,transitioning from coarse dendritic crystals to fine equiaxed grains.At a TiC content of 1.3wt.%,the alloy exhibits the smallest grain size,reducing from 139±42μm without TiC to 90±38μm.Beyond this concentration,grain coarsening is observed.The incorporation of TiC particles effectively mitigates Cu segregation at grain boundaries,thereby enhancing the homogeneity of the Al-Cu-Mn matrix alloys.Additionally,the addition of TiC particles promotes hardness and wear resistance.Both hardness and wear resistance exhibit an initial increase followed by a decrease with increasing TiC content from 0 to 1.8wt.%.展开更多
The cell fate of primordial germ cell(PGC)in zebrafish is pre-determined by maternally deposited germ plasm,which is packaged into ribonucleoprotein complex in oocytes and inherited into PGC-fated cells in embryos.How...The cell fate of primordial germ cell(PGC)in zebrafish is pre-determined by maternally deposited germ plasm,which is packaged into ribonucleoprotein complex in oocytes and inherited into PGC-fated cells in embryos.However,the maternal factors regulating the assembly of germ plasm and PGC development remain poorly understood.In this study,we report that the maternal transcription factor Znf706 regulates the assembly of germ plasm factors into a granule-like structure localized perinuclearly in PGC during migration.Maternal and zygotic mutants of znf706 exhibit deficient germ plasm scattering at the early embryonic stage,decreased PGC numbers with some mislocation during PGC migration,and a lower female ratio in adulthood.Notably,the implementation of Znf706 CUT&Tag and RNA-seq on immature oocytes uncovers that Znf706 in stage I oocytes may promote transcription of several mitochondrial genes in addition to other functions.Hence,we propose that Znf706 is implicated in germ plasm assembly and PGC development in zebrafish.展开更多
Hydrogen is a critical renewable energy source in the energy transition.However,water electrolysis,which is the primary technique for achieving large-scale and low-carbon hydrogen production,still suffers from high pr...Hydrogen is a critical renewable energy source in the energy transition.However,water electrolysis,which is the primary technique for achieving large-scale and low-carbon hydrogen production,still suffers from high production costs and energy consumption.The key is to develop highly efficient electrochemical water splitting catalysts.In recent years,the preparation of electrocatalysts via plasma treatment has gained recognition for its rapid,eco-friendly,and controllable properties,especially in the optimization of nano-microstructure.This review comprehensively summarizes the impact of plasma treatment on the nano-microstructure of water electrolysis catalysts,encompassing dispersion enhancement,morphology modulation,surface functionalization,defect construction,and element doping.These impacts on the nano-microstructure increase the surface area,modify the pore structure,introduce active sites,and regulate the electronic environment,thereby promoting the water splitting performance of electrocatalysts.Finally,the remaining challenges and potential opportunities are discussed for the future development of plasma treatment.This review would be a valuable reference for plasmaassisted electrocatalyst synthesis and mechanism understanding in plasma impact on nano-microstructure.展开更多
Microgrids (MGs) and active distribution networks (ADNs) are important platforms for distributed energy resource (DER) consumption. The increasing penetration of DERs has motivated the development ADNs coupled with MG...Microgrids (MGs) and active distribution networks (ADNs) are important platforms for distributed energy resource (DER) consumption. The increasing penetration of DERs has motivated the development ADNs coupled with MGs. This paper proposes a distributedco-optimization method for peer-to-peer (P2P) energy trading and network operation for an ADN integrated with multiple microgrids(MMGs). A framework that optimizes P2P energy trading among MMGs and ADN operations was first established. Subsequently, anenergy management model that aims to minimize the operation and energy trading costs was constructed for each MG. Accordingly, theMMGs’ cooperative game model was established based on Nash bargaining theory to incentivize each stakeholder to participate in P2Penergy trading, and a distributed solution method based on the alternating direction method of multipliers was developed. Moreover, analgorithm that adjusts the amount of energy trading between the ADN and MG is proposed to ensure safe operation of the distributionnetwork. With the communication between the MG and ADN, the MMGs’ P2P trading and ADN operations are optimized in a coordinated manner. Finally, numerical simulations were conducted to verify the accuracy and effectiveness of the proposed method.展开更多
基金financial support from the National Natural Science Foundation of China(No.52273187)the Guangdong Basic and Applied Basic Research Foundation(2022A1515110372,2023A1515011306,2023A1515240077)+1 种基金the National Key Research and Development Program of China(2022YFA1502900)the Guangdong-Hong Kong Joint Laboratory for Preparation and Application of Ordered Structural Materials of Guangdong Province(2023B1212120011).
文摘Photoelectrochemical CO_(2)reduction to multi-carbon products fuels remains challenged by inefficient C–C coupling and competing proton reduction reaction.Herein,we designed a cationic covalent organic framework(COF+)to create an electrostatic microenvironment that synergizes with CuPt alloy nanoparticles for selective ethylene/ethane production.By spatially decoupling CO_(2)enrichment from proton exclusion,the COF^(+)/CuPt interface simultaneously facilitates CO_(2)accessibility while impeding H+migration,suppressing the hydrogen evolution reaction(HER).This unique microenvironment stabilizes key anionic intermediates(*COO^(−),*OCCO^(−))and promotes*CO dimerization,steering electron transfer toward C–C coupling.The optimized system achieves a record-high Faradaic efficiency of 51.5%±5.3%for ethane and 10.6%±2.5%for ethylene with a total C2+yield exceeding 62%at−0.25 V vs.RHE and high stability(>300 min),representing the highest performance for photoelectrochemical CO_(2)reduction to ethane.The combined analyses of in situ spectroscopy and theoretical calculations reveal that electrostatic field effects lower the energy barrier for*OCCO formation while accelerating hydrogenation kinetics.Therefore,this work demonstrates that microenvironment modification of the active site by cationic covalent organic framework is a versatile strategy for solar-driven CO_(2)conversion into value-added hydrocarbons.
基金supported by the National Key R&D Program of China(Grant No.2024YFB3614600)the National Natural Science Foundation of China(Grant No.52402185)+1 种基金Guangzhou Basic and Applied Basic Research Foundation(Grant No.2025A1515011800)Shenzhen Science and Technology Program(Grant No.JCYJ20241202123712017)。
文摘The bidirectional convergence of artificial intelligence and nanophotonics drives photonic technologies toward unprecedented levels of intelligence and efficiency,fundamentally reshaping their design paradigms and application boundaries.With its powerful data-driven and nonlinear optimization capabilities,artificial intelligence has become a powerful tool for optical design,enabling the inverse design of nanophotonics devices while accelerating the forward computation of electromagnetic responses.Conversely,nanophotonics provides a wave-based computational platform,giving rise to novel optical neural networks that achieve high-speed parallel computing and efficient information processing.This paper reviews the latest progress in the bidirectional field of artificial intelligence and nanophotonics,analyzes the basic principles of various applications from a universal perspective,comprehensively evaluates the advantages and limitations of different research methods,and makes a forwardlooking outlook on the bidirectional integration of artificial intelligence and nanophotonics,focusing on analyzing future development trends,potential applications,and challenges.The deep integration of artificial intelligence and nanophotonics is ushering in a new era for photonic technologies,offering unparalleled opportunities for fundamental research and industrial applications.
基金financial support provided by the National Natural Science Foundation of China (52472304)。
文摘The electrochemical CO_(2) reduction reaction(eCO_(2)RR),producing gaseous C_(2+)products such as ethylene(C_(2)H_(4)),represents a sustainable strategy to mitigate the greenhouse effect.Inspired by the promotion effect of the cyano group(-C≡N) for C-C coupling in organic chemistry,several cyano-containing organocatalysts have been found to be capable of directly converting CO_(2) into C_(2)H_(4) with-C≡N as the active center during the eCO_(2)RR.The selectivity of C_(2)H_(4) for the representative catalyst,metal-free dicyandiamide(DCD),reached 27.6 % after partial hydrogenation in KHCO_(3) solution.In addition,its selectivity can be further improved to 57.7 % when coupled with oriented Cu crystals.The experimental and computational results collectively reveal that charge redistribution between Cu{100} and DCD promotes the partial hydrogenation of the cyano group and lays the foundation for the reduced energy barrier for the CO_(2) reduction on-C≡N.This study breaks the limitations of traditional metal/metal oxide-based catalysts by using cyano-containing organocatalysts for direct C_(2+) product generation,expanding the eCO_(2)RR catalyst library.In addition,this research elucidates the role of charge redistribution and cyano group hydrogenation in lowering reaction barriers,providing fundamental guidance for the design of new organocatalysts.
基金supported by the National Natural Science Foundation of China(No.52273187)National Key R&D Program of China(2021YFA1500800)+1 种基金Guangdong Basic and Applied Basic Research Foundation(2022A1515110372,2023A1515011306,2023A1515240077)Guangdong-Hong Kong Joint Laboratory for Preparation and Application of Ordered Structural Materials of Guangdong Province(2023B1212120011)。
文摘Copper complexes inspired by O_(2)-activating enzymes have been widely investigated as molecular water oxidation catalysts,capable of facile and reversible O─O bond formation and cleavage under mild conditions.In this study,two copper phenanthroline complexes,namely,Cu(phen)and Cu(dophen),exhibit high turnover frequencies(TOFs)of 74±13 and(5.66±0.29)×10^(3)s^(−1)for water oxidation,respectively.Moreover,amino acid-functionalized carbon dots(CDs)were used to support the adhesion of the[Cu]complexes onto the electrode,significantly enhancing the TOFs of(2.80±0.12)×10^(3)and(4.11±0.24)×10^(4)s^(−1),respectively,exceeding the activity of photosystem Ⅱ in nature.Remarkably,the amino acid-functionalized CDs provide a secondary sphere that mimics the catalytic microenvironment of the copper centre,which promotes proton-coupled electron transfer and O─O bond formation.Finally,the photovoltaic-electrolysis(PVE)system was established using CDs-supported Cu catalysts and commercial silicon solar panels,achieving a high solar-to-hydrogen efficiency of 11.59%under the illumination of AM 1.5 G.This represents the most efficient solar-driven water splitting system based on copper-based catalysts to date,introducing the biomimetic secondary sphere to a“proton-rocking”process for water oxidation catalysis and application of the PVE system.
基金supported by the Advanced Materials-National Science and Technology Major Project(Grant No.2025ZD0611400).
文摘Al-based TiC particle-reinforced composites with varying TiC concentrations were fabricated through semi-continuous casting.The effects of TiC particles on the alloys’microstructure,grain boundary segregation,and mechanical properties were systematically analyzed.Moreover,the mechanisms by which TiC particles contribute to grain refinement,suppression of grain boundary segregation,and enhancement of hardness and wear resistance were discussed.The results demonstrate that TiC particles act as heterogeneous nucleation sites forα-Al within the Al-Cu-Mn alloys,leading to a refinement of grain size.As the TiC particle’s content increases,the grain size of the alloy drops at first and then elevates,transitioning from coarse dendritic crystals to fine equiaxed grains.At a TiC content of 1.3wt.%,the alloy exhibits the smallest grain size,reducing from 139±42μm without TiC to 90±38μm.Beyond this concentration,grain coarsening is observed.The incorporation of TiC particles effectively mitigates Cu segregation at grain boundaries,thereby enhancing the homogeneity of the Al-Cu-Mn matrix alloys.Additionally,the addition of TiC particles promotes hardness and wear resistance.Both hardness and wear resistance exhibit an initial increase followed by a decrease with increasing TiC content from 0 to 1.8wt.%.
基金supported by the National Natural Science Foundation of China(31988101 to A.M.)the National Key Research and Development Program of China(2023YFA1800300 to X.W.and 2018YFC1003304 to A.M.)the Yunnan Provincial Science and Technology Project at Southwest United Graduate School(202302A0370011 to A.M.).
文摘The cell fate of primordial germ cell(PGC)in zebrafish is pre-determined by maternally deposited germ plasm,which is packaged into ribonucleoprotein complex in oocytes and inherited into PGC-fated cells in embryos.However,the maternal factors regulating the assembly of germ plasm and PGC development remain poorly understood.In this study,we report that the maternal transcription factor Znf706 regulates the assembly of germ plasm factors into a granule-like structure localized perinuclearly in PGC during migration.Maternal and zygotic mutants of znf706 exhibit deficient germ plasm scattering at the early embryonic stage,decreased PGC numbers with some mislocation during PGC migration,and a lower female ratio in adulthood.Notably,the implementation of Znf706 CUT&Tag and RNA-seq on immature oocytes uncovers that Znf706 in stage I oocytes may promote transcription of several mitochondrial genes in addition to other functions.Hence,we propose that Znf706 is implicated in germ plasm assembly and PGC development in zebrafish.
基金supported by the National Key Research and Development Program of China(2021YFB4000405).
文摘Hydrogen is a critical renewable energy source in the energy transition.However,water electrolysis,which is the primary technique for achieving large-scale and low-carbon hydrogen production,still suffers from high production costs and energy consumption.The key is to develop highly efficient electrochemical water splitting catalysts.In recent years,the preparation of electrocatalysts via plasma treatment has gained recognition for its rapid,eco-friendly,and controllable properties,especially in the optimization of nano-microstructure.This review comprehensively summarizes the impact of plasma treatment on the nano-microstructure of water electrolysis catalysts,encompassing dispersion enhancement,morphology modulation,surface functionalization,defect construction,and element doping.These impacts on the nano-microstructure increase the surface area,modify the pore structure,introduce active sites,and regulate the electronic environment,thereby promoting the water splitting performance of electrocatalysts.Finally,the remaining challenges and potential opportunities are discussed for the future development of plasma treatment.This review would be a valuable reference for plasmaassisted electrocatalyst synthesis and mechanism understanding in plasma impact on nano-microstructure.
基金supported by the State Key Laboratory of Technology and Equipment for Defense against Power System Operational Risks Program(grant number SGNR0000KJJS2302139).
文摘Microgrids (MGs) and active distribution networks (ADNs) are important platforms for distributed energy resource (DER) consumption. The increasing penetration of DERs has motivated the development ADNs coupled with MGs. This paper proposes a distributedco-optimization method for peer-to-peer (P2P) energy trading and network operation for an ADN integrated with multiple microgrids(MMGs). A framework that optimizes P2P energy trading among MMGs and ADN operations was first established. Subsequently, anenergy management model that aims to minimize the operation and energy trading costs was constructed for each MG. Accordingly, theMMGs’ cooperative game model was established based on Nash bargaining theory to incentivize each stakeholder to participate in P2Penergy trading, and a distributed solution method based on the alternating direction method of multipliers was developed. Moreover, analgorithm that adjusts the amount of energy trading between the ADN and MG is proposed to ensure safe operation of the distributionnetwork. With the communication between the MG and ADN, the MMGs’ P2P trading and ADN operations are optimized in a coordinated manner. Finally, numerical simulations were conducted to verify the accuracy and effectiveness of the proposed method.
