Cu-based MOFs,i.e.,HKUST-1,etc.,have been pertinently chosen as the pristine materials for CO_(2) ER due to the unique ability of copper for generation hydrocarbon fuel.However,the limited conductivity and stability b...Cu-based MOFs,i.e.,HKUST-1,etc.,have been pertinently chosen as the pristine materials for CO_(2) ER due to the unique ability of copper for generation hydrocarbon fuel.However,the limited conductivity and stability become the stumbling-block that prevents the development of it.The exploring of MOFsderived M-C materials starts a new chapter for the MOFs precursors,which provides a remarkable electronic connection between carbon matrix and metals/metal oxides.N-doped M-N-C with extensive M-N sites scattering into the carbon matrix are more popular because of their impressive contribution to catalytic activity and specific product selectivity.Nevertheless,Cu-N-C system remained undeveloped up to now.The lack of ideal precursor,the sensitivity of Cu to be oxidized,and the difficulties in the synthesis of small size Cu nanoparticles are thus known as the main barriers to the development of Cu-N-C electrocatalysts.Herein,a nitrogen-rich Cu-BTT MOF is employed for the derivation of N-doped Cu-N-CT composite electrocatalysts by the pyrolyze method.High-temperature pyrolysis product of Cu-N-C1100exhibits the best catalytic activity for productions of CO(-0.6 V vs.RHE,jCO=0.4 mA/cm^(2))and HCOOH(-0.9 V vs.RHE,jHCOOH=1.4 mA/cm^(2)).展开更多
In this study,through direct pyrolysis of a nitrogen-rich metal-organic framework of Fe-BTT at different temperatures and followed by acid treatment,we prepared a series of Fe–N–CT(T=800–1000°C)composite catal...In this study,through direct pyrolysis of a nitrogen-rich metal-organic framework of Fe-BTT at different temperatures and followed by acid treatment,we prepared a series of Fe–N–CT(T=800–1000°C)composite catalysts with uniform cubic morphology and homogeneously distributed active sites.Acid leaching leads to the removal of excess Fe NPs and the exposure of more pyridinic N and porphyrin-like Fe–Nx sites and creates a higher specific surface area.Structural and electrochemical performance test results showed that Fe–N–C900catalyst exhibited the highest selectivity for CO product at–1.2 V vs.Ag/AgCl,with 496 m V of overpotential and 86.8%of Faraday efficiency,as well as excellent long-term stability,due to the good inheritance from rich-N Fe–BTT precursor.展开更多
基金supported by the National Natural Science Foundation of China(20171169)Six Talent Peaks Project in Jiangsu Province(No.2017-XNY-043)+1 种基金the projects funded by the High-Level Personnel Support Program of Yang-Zhou Universitythe Priority Academic Program Development of Jiangsu Higher Education Institutions。
文摘Cu-based MOFs,i.e.,HKUST-1,etc.,have been pertinently chosen as the pristine materials for CO_(2) ER due to the unique ability of copper for generation hydrocarbon fuel.However,the limited conductivity and stability become the stumbling-block that prevents the development of it.The exploring of MOFsderived M-C materials starts a new chapter for the MOFs precursors,which provides a remarkable electronic connection between carbon matrix and metals/metal oxides.N-doped M-N-C with extensive M-N sites scattering into the carbon matrix are more popular because of their impressive contribution to catalytic activity and specific product selectivity.Nevertheless,Cu-N-C system remained undeveloped up to now.The lack of ideal precursor,the sensitivity of Cu to be oxidized,and the difficulties in the synthesis of small size Cu nanoparticles are thus known as the main barriers to the development of Cu-N-C electrocatalysts.Herein,a nitrogen-rich Cu-BTT MOF is employed for the derivation of N-doped Cu-N-CT composite electrocatalysts by the pyrolyze method.High-temperature pyrolysis product of Cu-N-C1100exhibits the best catalytic activity for productions of CO(-0.6 V vs.RHE,jCO=0.4 mA/cm^(2))and HCOOH(-0.9 V vs.RHE,jHCOOH=1.4 mA/cm^(2)).
基金supported by the National Natural Science Foundation of China(No.21671169)the Priority Academic Program Development of Jiangsu Higher Education Institutions。
文摘In this study,through direct pyrolysis of a nitrogen-rich metal-organic framework of Fe-BTT at different temperatures and followed by acid treatment,we prepared a series of Fe–N–CT(T=800–1000°C)composite catalysts with uniform cubic morphology and homogeneously distributed active sites.Acid leaching leads to the removal of excess Fe NPs and the exposure of more pyridinic N and porphyrin-like Fe–Nx sites and creates a higher specific surface area.Structural and electrochemical performance test results showed that Fe–N–C900catalyst exhibited the highest selectivity for CO product at–1.2 V vs.Ag/AgCl,with 496 m V of overpotential and 86.8%of Faraday efficiency,as well as excellent long-term stability,due to the good inheritance from rich-N Fe–BTT precursor.