Over the past few decades,the design and development of carbon materials have occurred at a rapid pace.In particular,these porous graphene-like carbon nitride materials have received considerable attention due to thei...Over the past few decades,the design and development of carbon materials have occurred at a rapid pace.In particular,these porous graphene-like carbon nitride materials have received considerable attention due to their superior structures and performances in the energy transformation field.In this review,nitrogenated holey two-dimensional graphene and polymeric carbon nitride will be discussed in depth.The structural properties,synthetic methods,and applications including electrocatalytic reactions,such as hydrogen evolution reaction,oxygen reduction reaction,oxygen evolution reaction,and nitrogen reduction reaction,will be presented in detail.Finally,we will present the outlooks on the current obstacles to the development of carbon nitride materials.This comprehensive understanding will help guide and motivate researchers to develop and modify carbon nitride materials with better properties in the future.展开更多
Design and synthesis of noble-metal-free bifunctional catalysts for efficient and robust electrochemical water splitting are of significant importance in developing clean and renewable energy sources for sustainable e...Design and synthesis of noble-metal-free bifunctional catalysts for efficient and robust electrochemical water splitting are of significant importance in developing clean and renewable energy sources for sustainable energy consumption.Herein,a simple three-step strategy is reported to construct cobalt-iron nitride/alloy nanosheets on nickel foam(CoFe-NA/NF)as a bifunctional catalyst for both hydrogen evolution reaction(HER)and oxygen evolution reaction(OER).The electrocatalyst with optimized composition(CoFe-NA2/NF)can achieve ultralow overpotentials of 73 mV and 250 mV for HER and OER,respectively,at a current density of 10 mA cm^(-2) in 1 M KOH.Notably,the electrolyzer based on this electrocatalyst is able to boost the overall water splitting with a cell voltage of 1.564 V to deliver 10 mA cm^(-2) for at least 50 h without obvious performance decay.Furthermore,our experiment and theoretical calculation demonstrate that the combination of cobalt-iron nitride and alloy can have low hydrogen adsorption energy and facilitate water dissociation during HER.In addition,the surface reconstruction introduces metal oxyhydroxides to optimize the OER process.Our work may pave a new pathway to design bifunctional catalysts for overall water splitting.展开更多
Printable mesoscopic perovskite solar cells(PM-PSCs)possess notable merits in terms of cost-effectiveness,easy manufacturing,and large scale applications.Nevertheless,the absence of a hole transport layer contributes ...Printable mesoscopic perovskite solar cells(PM-PSCs)possess notable merits in terms of cost-effectiveness,easy manufacturing,and large scale applications.Nevertheless,the absence of a hole transport layer contributes to the exacerbation of carrier recombination,and the defects between the perovskite and electron transport layer(ETL)interfaces significantly decrease the efficiency of the devices.In this study,a bifunctional surface passivation approach is proposed by applying a thioacetamide(TAA)surfactant on the mesoporous TiO_(2)interface.The results demonstrate that TAA molecules could interact with TiO_(2),thereby diminishing the oxygen vacancy defects.Additionally,the amino group and sulfur atoms in TAA molecules act as Lewis base to effectively passivate the uncoordinated Pb^(2+)in perovskite and improve the morphology of perovskite,and decrease the trap-state density of perovskite.The TAA passivation mechanism improves the alignment of energy levels between TiO_(2)and perovskite,facilitating electron transport and reducing carrier recombination.Consequently,the TAA-passivated device achieved a champion power conversion efficiency(PCE)of 17.86%with a high fill factor(FF)of 79.16%and an open-circuit voltage(V_(OC))of 0.971 V.This investigation presents a feasible strategy for interfacial passivation of the ETL to further improve the efficiency of PM-PSCs.展开更多
Single atom catalyst(SAC)refers to a novel catalyst with the active metal atoms individually anchored on the support.Single atom catalysts present the unique appeal due to the high atomic availability and specific act...Single atom catalyst(SAC)refers to a novel catalyst with the active metal atoms individually anchored on the support.Single atom catalysts present the unique appeal due to the high atomic availability and specific activity,as well as the high pathway selectivity.Herein,we summarized the classification,preparation,characterization,and application of single atom catalysts.Finally,the current bottlenecks and the outlooks of the SAC research are discussed.展开更多
基金The authors acknowledge the financial support from the National Natural Science Foundation of China(22001228)the“Double-First Class”University Construction Project(C176220100022 and C176220100042)+2 种基金the Major Science and Technology Project of Precious Metal Materials Genetic Engineering in Yunnan Province(2019ZE001-1 and 202002AB080001)the International Joint Research Center for Advanced Energy Materials of Yunnan Province(202003AE140001)Guangzhi Hu is grateful to the Double Tops Joint Fund of the Yunnan Science and Technology Bureau and Yunnan University(2019FY003025).
文摘Over the past few decades,the design and development of carbon materials have occurred at a rapid pace.In particular,these porous graphene-like carbon nitride materials have received considerable attention due to their superior structures and performances in the energy transformation field.In this review,nitrogenated holey two-dimensional graphene and polymeric carbon nitride will be discussed in depth.The structural properties,synthetic methods,and applications including electrocatalytic reactions,such as hydrogen evolution reaction,oxygen reduction reaction,oxygen evolution reaction,and nitrogen reduction reaction,will be presented in detail.Finally,we will present the outlooks on the current obstacles to the development of carbon nitride materials.This comprehensive understanding will help guide and motivate researchers to develop and modify carbon nitride materials with better properties in the future.
基金supported by the Science and Technology Development Fund from Macao SAR(FDCT)(0102/2019/A2,0035/2019/AGJ,0154/2019/A3,0081/2019/AMJ,and 0033/2019/AMJ)Multi-Year Research Grants(MYRG2017-00027-FST and MYRG2018-00003-IAPME)from Research&Development Office at University of Macao。
文摘Design and synthesis of noble-metal-free bifunctional catalysts for efficient and robust electrochemical water splitting are of significant importance in developing clean and renewable energy sources for sustainable energy consumption.Herein,a simple three-step strategy is reported to construct cobalt-iron nitride/alloy nanosheets on nickel foam(CoFe-NA/NF)as a bifunctional catalyst for both hydrogen evolution reaction(HER)and oxygen evolution reaction(OER).The electrocatalyst with optimized composition(CoFe-NA2/NF)can achieve ultralow overpotentials of 73 mV and 250 mV for HER and OER,respectively,at a current density of 10 mA cm^(-2) in 1 M KOH.Notably,the electrolyzer based on this electrocatalyst is able to boost the overall water splitting with a cell voltage of 1.564 V to deliver 10 mA cm^(-2) for at least 50 h without obvious performance decay.Furthermore,our experiment and theoretical calculation demonstrate that the combination of cobalt-iron nitride and alloy can have low hydrogen adsorption energy and facilitate water dissociation during HER.In addition,the surface reconstruction introduces metal oxyhydroxides to optimize the OER process.Our work may pave a new pathway to design bifunctional catalysts for overall water splitting.
基金funded by the Yunnan Yunling Scholars Project,the National Natural Science Foundation of China(No.51562038)the Young-Middle-Aged Academic and Technical Leaders Reserve Talent Project in Yunnan Province(No.202005AC160015)the Yunnan Basic Applied Research Project(No.202101AT070013).
文摘Printable mesoscopic perovskite solar cells(PM-PSCs)possess notable merits in terms of cost-effectiveness,easy manufacturing,and large scale applications.Nevertheless,the absence of a hole transport layer contributes to the exacerbation of carrier recombination,and the defects between the perovskite and electron transport layer(ETL)interfaces significantly decrease the efficiency of the devices.In this study,a bifunctional surface passivation approach is proposed by applying a thioacetamide(TAA)surfactant on the mesoporous TiO_(2)interface.The results demonstrate that TAA molecules could interact with TiO_(2),thereby diminishing the oxygen vacancy defects.Additionally,the amino group and sulfur atoms in TAA molecules act as Lewis base to effectively passivate the uncoordinated Pb^(2+)in perovskite and improve the morphology of perovskite,and decrease the trap-state density of perovskite.The TAA passivation mechanism improves the alignment of energy levels between TiO_(2)and perovskite,facilitating electron transport and reducing carrier recombination.Consequently,the TAA-passivated device achieved a champion power conversion efficiency(PCE)of 17.86%with a high fill factor(FF)of 79.16%and an open-circuit voltage(V_(OC))of 0.971 V.This investigation presents a feasible strategy for interfacial passivation of the ETL to further improve the efficiency of PM-PSCs.
基金the financial support from the National Natural Science Foundation of China(No.22001228)“Double-First Class”University Construction Project(Nos.C176220100022 and C176220100042)+1 种基金Major Science and Technology Project of Precious Metal Materials Genetic Engineering in Yunnan Province(Nos.2019ZE001-1,202002AB080001-6)the Yunnan Science and Technology Bureau and Yunnan University(No.2019FY003025)。
文摘Single atom catalyst(SAC)refers to a novel catalyst with the active metal atoms individually anchored on the support.Single atom catalysts present the unique appeal due to the high atomic availability and specific activity,as well as the high pathway selectivity.Herein,we summarized the classification,preparation,characterization,and application of single atom catalysts.Finally,the current bottlenecks and the outlooks of the SAC research are discussed.