Ruthenium(Ru)-based electrocatalysts show great promise as substitutes for platinum(Pt)for the alkaline hydrogen evolution reaction(HER)because of their efficient water dissociation capabilities.Nevertheless,the stron...Ruthenium(Ru)-based electrocatalysts show great promise as substitutes for platinum(Pt)for the alkaline hydrogen evolution reaction(HER)because of their efficient water dissociation capabilities.Nevertheless,the strong adsorption of Ru-OH intermediates(Ru-OHad)blocks the active site,leading to unsatisfactory HER performance.In this study,we report a universal ligand-exchange strategy for synthesizing a MOF-on-MOF-derived FeP-CoP heterostructure-anchored Ru single-atom site catalyst(Ru-FeP-CoP/NPC).The obtained catalyst shows a low overpotential(28 mV at 10 mA cm^(-2))and a high mass activity(9.29 A mg^(-1) at 100 mV),surpassing the performance of commercial Pt/C by a factor of 46.Theoretical studies show that regulating the local charge distribution of Ru single-atom sites could alleviate surrounding OH-blockages,accelerating water dissociation and facilitating hydrogen adsorption/desorption,thus enhancing HER activity.This work aims to inspire further design of highly active and durable electrocatalysts with tailored electronic properties for high-purity hydrogen production.展开更多
Mechanical overloading and aging are two essential factors for osteoarthritis(OA)development.Mitochondria have been identified as a mechano-transducer situated between extracellular mechanical signals and chondrocyte ...Mechanical overloading and aging are two essential factors for osteoarthritis(OA)development.Mitochondria have been identified as a mechano-transducer situated between extracellular mechanical signals and chondrocyte biology,but their roles and the associated mechanisms in mechanical stress-associated chondrocyte senescence and OA have not been elucidated.展开更多
Developing efficient and durable hydrogen evolution reaction(HER)electrocatalysts is one of the most important issues for the commercialization of seawater electrolysis,but it remains challenging.Here,we report a CeO_...Developing efficient and durable hydrogen evolution reaction(HER)electrocatalysts is one of the most important issues for the commercialization of seawater electrolysis,but it remains challenging.Here,we report a CeO_(2)-CoP nanoneedle array catalyst loaded on Ti mesh(CeO_(2)-CoP/TM)with workfunction-induced directional charge transport properties.The CeO_(2)-CoP/TM catalyst showed superior HER catalytic activity and stability,with over potentials of 41 and 60 mV to attain 10 mA cm^(-2),in 1 M KOH and 1 M KOH+seawater electrolyte,respectively.Experimental results and theoretical calculations reveal that the work function drives the charge transfer from CeO_(2)to CoP,which effectively balances the electronic density of CoP and CeO_(2),optimizes the d-band center,and accelerates the water activation kinetics,thus enhancing the HER activity.The solar-driven water electrolysis device displays a high and stable solar-to-hydrogen conversion efficiency of 19.6%.This study offers a work function-induced directional charge transport strategy to design efficient and durable catalysts for hydrogen production.展开更多
Electrocatalytic water splitting is the most directly available route to generate renewable and sustainable hydrogen.Here,we report the design of a composite material in which arrays of square pillar-like NiMoO4nanoro...Electrocatalytic water splitting is the most directly available route to generate renewable and sustainable hydrogen.Here,we report the design of a composite material in which arrays of square pillar-like NiMoO4nanorods coated with N,P-doped carbon layers are uniformly contained in numerous nested nanoparticle structures.The catalysts have superior catalytic activity,requiring only 59 mV and 187 mV for HER and OER to attain a current density of 10 mA/cm^(2),respectively.The assembled two-electrode electrolytic cell required a voltage of 1.48 V to reach 10 mA/cm^(2),along with excellent long-term stability.Theoretical calculations reveal that electrons aggregate and redistribute at the heterogeneous interface,with the d-band centers of the Ni and Fe atoms being positively shifted compared to the Fermi level,effectively optimizing the adsorption of intermediates and reducing the Gibbs free energy,thus accelerating the catalytic process.Meanwhile,an integrated solar-driven water-splitting system demonstrated a high and stable solar-to-hydrogen efficiency of 18.20%.This work provides new possibilities for developing non-precious metal-based bifunctional electrocatalysts for large-scale water splitting applications.展开更多
Crystallinity and crystal structure greatly influence the photocatalytic behavior of photocatalysts.Pristine g-C3N4 produced by traditional thermal-induced polycondensation reaction bears low crystallinity and thus po...Crystallinity and crystal structure greatly influence the photocatalytic behavior of photocatalysts.Pristine g-C3N4 produced by traditional thermal-induced polycondensation reaction bears low crystallinity and thus poor photoactivity,which originates from the incomplete polymerization of the precursor containing amine groups,abundant hydrogen bonds,and unreacted amino,as well as cyanide functional groups in the skeleton.During photocatalytic process,these residual functional groups often work as electron trap sites,which may hinder the transfer of electrons on the plane,resulting in low photoactivity.Fortunately,crystalline carbon nitride(CCN)was reported as a promising photocatalyst because its increased crystallinity not only reduces the number of carriers recombination centers,but also increases charge conductivity and improves light utilization due to extendedπ-conjugated systems and delocalizedπ-electrons.As such,we summarize the recent studies on CCN-based photocatalysts for the photoactivity enhancement.Firstly,the unique structure and properties of CCN materials are presented.Next,the preparation methods and modification strategies are well outlined.We also sum up the applications of CCN-based materials in the environmental purification and energy fields.Finally,this review concerning CNN materials ends with prospects and challenges in the obtainment of high crystallinity by effective techniques,and the deep understanding of photocatalytic mechanism.展开更多
The use of generative adversarial network(GAN)-based models for the conditional generation of image semantic segmentation has shown promising results in recent years.However,there are still some limitations,including ...The use of generative adversarial network(GAN)-based models for the conditional generation of image semantic segmentation has shown promising results in recent years.However,there are still some limitations,including limited diversity of image style,distortion of detailed texture,unbalanced color tone,and lengthy training time.To address these issues,we propose an asymmetric pre-training and fine-tuning(APF)-GAN model.展开更多
基金supported by the National Natural Science Foundation of China(22369025)Yunnan Applied Basic Research Projects(202201AT070095,202301AT070098,202301AT070107,202401AT070438,202401AT070433)+2 种基金the 3rd Professional Degree Graduate Practice Innovation Project of Yunnan University(ZC-23235291,ZC-23234269,KC-23236398,KC-23234063)the Education Reform Research Project of Yunnan University(No.2021Z06)the Xingdian Talent Program of Yunnan Province,and the Yunnan Revitalization Talent Support Program.
文摘Ruthenium(Ru)-based electrocatalysts show great promise as substitutes for platinum(Pt)for the alkaline hydrogen evolution reaction(HER)because of their efficient water dissociation capabilities.Nevertheless,the strong adsorption of Ru-OH intermediates(Ru-OHad)blocks the active site,leading to unsatisfactory HER performance.In this study,we report a universal ligand-exchange strategy for synthesizing a MOF-on-MOF-derived FeP-CoP heterostructure-anchored Ru single-atom site catalyst(Ru-FeP-CoP/NPC).The obtained catalyst shows a low overpotential(28 mV at 10 mA cm^(-2))and a high mass activity(9.29 A mg^(-1) at 100 mV),surpassing the performance of commercial Pt/C by a factor of 46.Theoretical studies show that regulating the local charge distribution of Ru single-atom sites could alleviate surrounding OH-blockages,accelerating water dissociation and facilitating hydrogen adsorption/desorption,thus enhancing HER activity.This work aims to inspire further design of highly active and durable electrocatalysts with tailored electronic properties for high-purity hydrogen production.
基金supported by grants from Natural Science Foundation of China grant No 82172491 (CN)National Natural Science Funds for Excellent Young Scholar No 82322044 (CN)+2 种基金National Key Research and Development Program of China (2022YFC3601902)Youth Talent Support Programme of Guangdong Provincial Association for Science and Technology (SKXRC202308)State-funded postdoctoral researcher program No GZC20231062 (CN)。
文摘Mechanical overloading and aging are two essential factors for osteoarthritis(OA)development.Mitochondria have been identified as a mechano-transducer situated between extracellular mechanical signals and chondrocyte biology,but their roles and the associated mechanisms in mechanical stress-associated chondrocyte senescence and OA have not been elucidated.
基金financially supported by the National Natural Science Foundation of China(22369025)the Yunnan Applied Basic Research Projects(202201AT070095,202301AT070098)+2 种基金the Scientific Research Fund Project of Yunnan Provincial Department of Education(2023Y0262)the Education Reform Research Project of Yunnan University(2021Z06)the Yunnan Revitalization Talent Support Program。
文摘Developing efficient and durable hydrogen evolution reaction(HER)electrocatalysts is one of the most important issues for the commercialization of seawater electrolysis,but it remains challenging.Here,we report a CeO_(2)-CoP nanoneedle array catalyst loaded on Ti mesh(CeO_(2)-CoP/TM)with workfunction-induced directional charge transport properties.The CeO_(2)-CoP/TM catalyst showed superior HER catalytic activity and stability,with over potentials of 41 and 60 mV to attain 10 mA cm^(-2),in 1 M KOH and 1 M KOH+seawater electrolyte,respectively.Experimental results and theoretical calculations reveal that the work function drives the charge transfer from CeO_(2)to CoP,which effectively balances the electronic density of CoP and CeO_(2),optimizes the d-band center,and accelerates the water activation kinetics,thus enhancing the HER activity.The solar-driven water electrolysis device displays a high and stable solar-to-hydrogen conversion efficiency of 19.6%.This study offers a work function-induced directional charge transport strategy to design efficient and durable catalysts for hydrogen production.
基金financially supported by Yunnan Applied Basic Research Projects(Nos.202001BB050006,202201AT070095)Scientific Research Fund Project of Yunnan Provincial Department of Education(No.2023Y0262)Education Reform Research Project of Yunnan University(No.2021Z06)。
文摘Electrocatalytic water splitting is the most directly available route to generate renewable and sustainable hydrogen.Here,we report the design of a composite material in which arrays of square pillar-like NiMoO4nanorods coated with N,P-doped carbon layers are uniformly contained in numerous nested nanoparticle structures.The catalysts have superior catalytic activity,requiring only 59 mV and 187 mV for HER and OER to attain a current density of 10 mA/cm^(2),respectively.The assembled two-electrode electrolytic cell required a voltage of 1.48 V to reach 10 mA/cm^(2),along with excellent long-term stability.Theoretical calculations reveal that electrons aggregate and redistribute at the heterogeneous interface,with the d-band centers of the Ni and Fe atoms being positively shifted compared to the Fermi level,effectively optimizing the adsorption of intermediates and reducing the Gibbs free energy,thus accelerating the catalytic process.Meanwhile,an integrated solar-driven water-splitting system demonstrated a high and stable solar-to-hydrogen efficiency of 18.20%.This work provides new possibilities for developing non-precious metal-based bifunctional electrocatalysts for large-scale water splitting applications.
基金the National Natural Science Foundation of China(Nos.52370109,22022608,21876113,22176127,21261140333,and 92034301)China Postdoctoral Science Foundation(No.2022M710830)+9 种基金Venture and Innovation Support Program for Chongqing Overseas Returnees(No.cx2022005)the Natural Science Foundation Project of CQ CSTC(No.CSTB2022NSCQ-MSX0035)National Key Research and Development Program of China(No.2020YFA0211004)the Shanghai Engineering Research Center of Green Energy Chemical Engineering(No.18DZ2254200)“111”Innovation and Talent Recruitment Base on Photochemical and Energy Materials(No.D18020)Shanghai Government(Nos.22010503400,18SG41,and YDZX20213100003002)Shanghai Sailing Program(No.22YF1430400)Research Project of Chongqing Education Commission Foundation(No.KJQN201800826)Science and Technology Research Program of Chongqing Municipal Education Commission of China(No.KJZD-K202100801)Post-doctoral Program Funded by Chongqing,and Chongqing University Innovation Research Group project(No.CXQT21023).
文摘Crystallinity and crystal structure greatly influence the photocatalytic behavior of photocatalysts.Pristine g-C3N4 produced by traditional thermal-induced polycondensation reaction bears low crystallinity and thus poor photoactivity,which originates from the incomplete polymerization of the precursor containing amine groups,abundant hydrogen bonds,and unreacted amino,as well as cyanide functional groups in the skeleton.During photocatalytic process,these residual functional groups often work as electron trap sites,which may hinder the transfer of electrons on the plane,resulting in low photoactivity.Fortunately,crystalline carbon nitride(CCN)was reported as a promising photocatalyst because its increased crystallinity not only reduces the number of carriers recombination centers,but also increases charge conductivity and improves light utilization due to extendedπ-conjugated systems and delocalizedπ-electrons.As such,we summarize the recent studies on CCN-based photocatalysts for the photoactivity enhancement.Firstly,the unique structure and properties of CCN materials are presented.Next,the preparation methods and modification strategies are well outlined.We also sum up the applications of CCN-based materials in the environmental purification and energy fields.Finally,this review concerning CNN materials ends with prospects and challenges in the obtainment of high crystallinity by effective techniques,and the deep understanding of photocatalytic mechanism.
基金This work was supported by the Fundamental Research Funds for the Central Universities 07063233084the Young Scientists Fund of the National Natural Science Foundation of China(Grant No.62206134)the Tianjin Key Laboratory of Visual Computing and Intelligent Perception(VCIP).Computation is supported by the Supercomputing Center of Nankai University(NKSC).
文摘The use of generative adversarial network(GAN)-based models for the conditional generation of image semantic segmentation has shown promising results in recent years.However,there are still some limitations,including limited diversity of image style,distortion of detailed texture,unbalanced color tone,and lengthy training time.To address these issues,we propose an asymmetric pre-training and fine-tuning(APF)-GAN model.
