Solar-driven photoelectrochemical(PEC)water splitting systems are highly promising for converting solar energy into clean and sustainable chemical energy.In such PEC systems,an integrated photoelectrode incorporates a...Solar-driven photoelectrochemical(PEC)water splitting systems are highly promising for converting solar energy into clean and sustainable chemical energy.In such PEC systems,an integrated photoelectrode incorporates a light harvester for absorbing solar energy,an interlayer for transporting photogenerated charge carriers,and a co-catalyst for triggering redox reactions.Thus,understanding the correlations between the intrinsic structural properties and functions of the photoelectrodes is crucial.Here we critically examine various 2D layered photoanodes/photocathodes,including graphitic carbon nitrides,transition metal dichalcogenides,layered double hydroxides,layered bismuth oxyhalide nanosheets,and MXenes,combined with advanced nanocarbons(carbon dots,carbon nanotubes,graphene,and graphdiyne)as co-catalysts to assemble integrated photoelectrodes for oxygen evolution/hydrogen evolution reactions.The fundamental principles of PEC water splitting and physicochemical properties of photoelectrodes and the associated catalytic reactions are analyzed.Elaborate strategies for the assembly of 2D photoelectrodes with nanocarbons to enhance the PEC performances are introduced.The mechanisms of interplay of 2D photoelectrodes and nanocarbon co-catalysts are further discussed.The challenges and opportunities in the field are identified to guide future research for maximizing the conversion efficiency of PEC water splitting.展开更多
Electroreduction of CO_(2)shows great potential for global CO_(2)utilization and uptake when collaborated with renewable electricity.Recent advances have been achieved in fundamental understanding and electrocatalyst ...Electroreduction of CO_(2)shows great potential for global CO_(2)utilization and uptake when collaborated with renewable electricity.Recent advances have been achieved in fundamental understanding and electrocatalyst development for CO_(2)electroreduction.We think this research area has progressed to the stage where significant efforts can focus on translating the obtained knowledge to the development of largescale electrolyzers,which have the potential to accelerate the transition of the current energy system into a sustainable and zero-carbon emission energy structure.In this perspective paper,we first critically evaluate the advancement of vapor-feed devices that use CO_(2)as reactants,from the point of view of industry applications.Then,by carefully comparing their performance to the state-of-the-art water electrolyzers which are well-established technology providing realistic performance targets,we looped back and discussed the remaining challenges including electrode catalysts,reaction conditions,mass transporting,membrane,device durability,operation mode,and so on.Finally,we provide perspectives on the challenges and suggest opportunities for generating fundamental knowledge and achieving technological progress toward the development of practical CO_(2)electrolyzers for the goal of building lowcarbon or/and net carbon-free economies.展开更多
Differential electrochemical mass spectrometry(DEMS)is one of the most powerful techniques for both the mechanistic and kinetic study of complicated electrocatalytic reactions.It can provide information on the nature ...Differential electrochemical mass spectrometry(DEMS)is one of the most powerful techniques for both the mechanistic and kinetic study of complicated electrocatalytic reactions.It can provide information on the nature and yields of the products generated,their production rate,and the structure-activity relationship between the electrocatalysts and the target reactions.The precise calibration of the mass signal is a prerequisite for the accurate evaluation of reaction kinetics.In this work,we use the oxidation reactions of CO and HCOOH to demonstrate how certain conditions,such as the flow rate and solution composition,affect the collection efficiency and ionization probability of the species to be detected.These parameters can affect the determination of the mass calibration constant and the accuracy of the subsequent quantitative DEMS analysis.We show the relationship between the mass calibration constant and the flow rate,and provide strategies for eliminating this and the related problems.展开更多
Metal-organic frameworks(MOFs)have been developed as an ideal platform for exploration of the relationship between intrinsic structure and catalytic activity,but the limited catalytic activity and stability has hamper...Metal-organic frameworks(MOFs)have been developed as an ideal platform for exploration of the relationship between intrinsic structure and catalytic activity,but the limited catalytic activity and stability has hampered their practical use in water splitting.Herein,we develop a bond length adjustment strategy for optimizing naphthalene-based MOFs that synthesized by acid etching Co-naphthalenedicarboxylic acid-based MOFs(donated as AE-CoNDA)to serve as efficient catalyst for water splitting.AE-CoNDA exhibits a low overpotential of 260 mV to reach 10 mA cm^(−2)and a small Tafel slope of 62 mV dec^(−1)with excellent stability over 100 h.After integrated AE-CoNDA onto BiVO_(4),photocurrent density of 4.3 mA cm^(−2)is achieved at 1.23 V.Experimental investigations demonstrate that the stretched Co-O bond length was found to optimize the orbitals hybridization of Co 3d and O 2p,which accounts for the fast kinetics and high activity.Theoretical calculations reveal that the stretched Co-O bond length strengthens the adsorption of oxygen-contained intermediates at the Co active sites for highly efficient water splitting.展开更多
Objective To explore the influence of oxidized high-density lipoprotein （oxHDL） on the maturation and migration of bone marrow-derived dendritic cells （BMDCs） from C57BL/6J mice. Methods The C57BL/6J mice bone ma...Objective To explore the influence of oxidized high-density lipoprotein （oxHDL） on the maturation and migration of bone marrow-derived dendritic cells （BMDCs） from C57BL/6J mice. Methods The C57BL/6J mice bone marrow cell suspension was prepared and purified. Recombinant granulocyte-macrophage colony-stimulating factor （rmGM-CSF） and recombinant interleukin-4 （rmlL-4） were used to promote monocytes to differentiate and suppress lymphocytes. Then 50μg/mL oxHDL was added to stimulate BMDCs, using 50μg/mL high-density lipoprotein （HDL） as homologous protein control, PBS as negative control, and 1 μg/mL lipopolysaccharide （LPS） as positive control. The CD86 and MHCII expression rates were detected with fluorescence-activated cell sorting （FACS）. Liquid scintillation counting （LSC） was used in mixed lymphocyte reactions （MLRs） to reflect the ability of BMDCs in stimulating the proliferation of homologous T cells, Levels of cytokines IL-12 and IL-10 were detected by ELISA. The cell migration was evaluated with the transwell system. Results Compared with PBS group, the expressions of CD86 and MHCII, counts per minute of MLRs, secretion of IL-12 and IL-10, and number of migrated cells in oxHDL group and LPS group significantly increased （all P 〈 0.05）, while the increment was less in oxHDL group than LPS group. The number of migrated cells in oxHDL group was about twice of that in HDL group. Conclusion OxHDL may promote the maturation and migration of BMDCs in vitro.展开更多
为便于深水双层整体式管道终端(Pipeline End Termination,PLET)的安装设计,以海洋石油201船的舷侧下放装置和南海某项目为基础,研究双层整体式PLET舷侧安装的悬挂和下放两个关键阶段的安装分析模型和主要参数。对比悬挂分析等效单层管...为便于深水双层整体式管道终端(Pipeline End Termination,PLET)的安装设计,以海洋石油201船的舷侧下放装置和南海某项目为基础,研究双层整体式PLET舷侧安装的悬挂和下放两个关键阶段的安装分析模型和主要参数。对比悬挂分析等效单层管模型与双层管模型,结果表明此2种建模方法均适用。双层管模型相关接触参数(接触刚度、接触面积、锚固件位置)对海底管道受力影响较小且能输出内外管接触载荷,较适用于安装设计。在下放过程中,管道载荷对PLET的重心位置和附加质量水动力系数较为敏感,在安装设计中需关注。展开更多
基金the support from the National Natural Science Foundation of China(21878271,51702284,21878270,and 21961160742)the Zhejiang Provincial Natural Science Foundation of China(LR19B060002)+8 种基金the Fundamental Research Funds for the Central Universitiesthe Startup Foundation for Hundred-Talent Program of Zhejiang Universitythe Leading Innovative and Entrepreneur Team Introduction Program of Zhejiang(2019R01006)Key Laboratory of Marine Materials and Related Technologies,CASZhejiang Key Laboratory of Marine Materials and Protective Technologies(2020K10)the support of the NSFC 21501138the Natural Science Foundation of Hubei Province(2019CFB556)Science Research Foundation of Wuhan Institute of Technology(K2019039)the Australian Research Council(ARC)and QUT Centre for Materials Science for partial support.
文摘Solar-driven photoelectrochemical(PEC)water splitting systems are highly promising for converting solar energy into clean and sustainable chemical energy.In such PEC systems,an integrated photoelectrode incorporates a light harvester for absorbing solar energy,an interlayer for transporting photogenerated charge carriers,and a co-catalyst for triggering redox reactions.Thus,understanding the correlations between the intrinsic structural properties and functions of the photoelectrodes is crucial.Here we critically examine various 2D layered photoanodes/photocathodes,including graphitic carbon nitrides,transition metal dichalcogenides,layered double hydroxides,layered bismuth oxyhalide nanosheets,and MXenes,combined with advanced nanocarbons(carbon dots,carbon nanotubes,graphene,and graphdiyne)as co-catalysts to assemble integrated photoelectrodes for oxygen evolution/hydrogen evolution reactions.The fundamental principles of PEC water splitting and physicochemical properties of photoelectrodes and the associated catalytic reactions are analyzed.Elaborate strategies for the assembly of 2D photoelectrodes with nanocarbons to enhance the PEC performances are introduced.The mechanisms of interplay of 2D photoelectrodes and nanocarbon co-catalysts are further discussed.The challenges and opportunities in the field are identified to guide future research for maximizing the conversion efficiency of PEC water splitting.
基金financially supported by the Zhejiang Energy Group Co.,Ltd.(ZNKJ-2021-111)Zhejiang Province key research and development program(2022C03040)。
文摘Electroreduction of CO_(2)shows great potential for global CO_(2)utilization and uptake when collaborated with renewable electricity.Recent advances have been achieved in fundamental understanding and electrocatalyst development for CO_(2)electroreduction.We think this research area has progressed to the stage where significant efforts can focus on translating the obtained knowledge to the development of largescale electrolyzers,which have the potential to accelerate the transition of the current energy system into a sustainable and zero-carbon emission energy structure.In this perspective paper,we first critically evaluate the advancement of vapor-feed devices that use CO_(2)as reactants,from the point of view of industry applications.Then,by carefully comparing their performance to the state-of-the-art water electrolyzers which are well-established technology providing realistic performance targets,we looped back and discussed the remaining challenges including electrode catalysts,reaction conditions,mass transporting,membrane,device durability,operation mode,and so on.Finally,we provide perspectives on the challenges and suggest opportunities for generating fundamental knowledge and achieving technological progress toward the development of practical CO_(2)electrolyzers for the goal of building lowcarbon or/and net carbon-free economies.
基金supported by the National Natural Science Foundation of China(no.21872132,21832004,91545124)the 973 Program from the Ministry of Science and Technology of China(no.2015CB932301)。
文摘Differential electrochemical mass spectrometry(DEMS)is one of the most powerful techniques for both the mechanistic and kinetic study of complicated electrocatalytic reactions.It can provide information on the nature and yields of the products generated,their production rate,and the structure-activity relationship between the electrocatalysts and the target reactions.The precise calibration of the mass signal is a prerequisite for the accurate evaluation of reaction kinetics.In this work,we use the oxidation reactions of CO and HCOOH to demonstrate how certain conditions,such as the flow rate and solution composition,affect the collection efficiency and ionization probability of the species to be detected.These parameters can affect the determination of the mass calibration constant and the accuracy of the subsequent quantitative DEMS analysis.We show the relationship between the mass calibration constant and the flow rate,and provide strategies for eliminating this and the related problems.
基金supported by the National Key Research and Development Program of China (2022YFB4002100)the development project of Zhejiang Province's "Jianbing" and "Lingyan" (2023C01226)+4 种基金the National Natural Science Foundation of China (22278364, U22A20432, 22238008, 22211530045, and 22178308)the Fundamental Research Funds for the Central Universities (226-2022-00044 and 226-2022-00055)the Science Foundation of Donghai Laboratory (DH-2022ZY0009)the Startup Foundation for Hundred-Talent Program of Zhejiang UniversityScientific Research Fund of Zhejiang Provincial Education Department.
文摘Metal-organic frameworks(MOFs)have been developed as an ideal platform for exploration of the relationship between intrinsic structure and catalytic activity,but the limited catalytic activity and stability has hampered their practical use in water splitting.Herein,we develop a bond length adjustment strategy for optimizing naphthalene-based MOFs that synthesized by acid etching Co-naphthalenedicarboxylic acid-based MOFs(donated as AE-CoNDA)to serve as efficient catalyst for water splitting.AE-CoNDA exhibits a low overpotential of 260 mV to reach 10 mA cm^(−2)and a small Tafel slope of 62 mV dec^(−1)with excellent stability over 100 h.After integrated AE-CoNDA onto BiVO_(4),photocurrent density of 4.3 mA cm^(−2)is achieved at 1.23 V.Experimental investigations demonstrate that the stretched Co-O bond length was found to optimize the orbitals hybridization of Co 3d and O 2p,which accounts for the fast kinetics and high activity.Theoretical calculations reveal that the stretched Co-O bond length strengthens the adsorption of oxygen-contained intermediates at the Co active sites for highly efficient water splitting.
基金Supported by the Foundation of Hunan Educational Committee (06C692)
文摘Objective To explore the influence of oxidized high-density lipoprotein （oxHDL） on the maturation and migration of bone marrow-derived dendritic cells （BMDCs） from C57BL/6J mice. Methods The C57BL/6J mice bone marrow cell suspension was prepared and purified. Recombinant granulocyte-macrophage colony-stimulating factor （rmGM-CSF） and recombinant interleukin-4 （rmlL-4） were used to promote monocytes to differentiate and suppress lymphocytes. Then 50μg/mL oxHDL was added to stimulate BMDCs, using 50μg/mL high-density lipoprotein （HDL） as homologous protein control, PBS as negative control, and 1 μg/mL lipopolysaccharide （LPS） as positive control. The CD86 and MHCII expression rates were detected with fluorescence-activated cell sorting （FACS）. Liquid scintillation counting （LSC） was used in mixed lymphocyte reactions （MLRs） to reflect the ability of BMDCs in stimulating the proliferation of homologous T cells, Levels of cytokines IL-12 and IL-10 were detected by ELISA. The cell migration was evaluated with the transwell system. Results Compared with PBS group, the expressions of CD86 and MHCII, counts per minute of MLRs, secretion of IL-12 and IL-10, and number of migrated cells in oxHDL group and LPS group significantly increased （all P 〈 0.05）, while the increment was less in oxHDL group than LPS group. The number of migrated cells in oxHDL group was about twice of that in HDL group. Conclusion OxHDL may promote the maturation and migration of BMDCs in vitro.
文摘为便于深水双层整体式管道终端(Pipeline End Termination,PLET)的安装设计,以海洋石油201船的舷侧下放装置和南海某项目为基础,研究双层整体式PLET舷侧安装的悬挂和下放两个关键阶段的安装分析模型和主要参数。对比悬挂分析等效单层管模型与双层管模型,结果表明此2种建模方法均适用。双层管模型相关接触参数(接触刚度、接触面积、锚固件位置)对海底管道受力影响较小且能输出内外管接触载荷,较适用于安装设计。在下放过程中,管道载荷对PLET的重心位置和附加质量水动力系数较为敏感,在安装设计中需关注。
