Nitrogen-rich zeolitic imidazolate frameworks(ZIFs)are ideal precursors for the synthesis of metal single atoms anchored on N-doped carbon.However,the microporous structures of conventional ZIFs lead to low mass trans...Nitrogen-rich zeolitic imidazolate frameworks(ZIFs)are ideal precursors for the synthesis of metal single atoms anchored on N-doped carbon.However,the microporous structures of conventional ZIFs lead to low mass transfer efficiency and low metal utilization of their derivatives.Here,we construct a composite of Co single atoms anchored on nitrogen-doped carbon with a three-dimensional ordered macroporous structure(Co-SA/3DOM-NC)by two-step pyrolysis of ordered macro/microporous ZnCo-ZIF.Co-SA/3DOM-NC shows high activity in the oxidative esterification of furfural,achieving a 99%yield of methyl 2-furoate under mild reaction conditions,which is significantly superior to the microporous and the Conanoparticle counterparts.The high activity of Co-SA/3DOM-NC should be attributed to the CoN4 centers with high intrinsic activity and the ordered macroporous structure,promoting the mass transfer of reactants and accessibility of active sites.展开更多
基金supported by the National Natural Science Foundation of China(No.21825802,22138003,and 22108083)the Fundamental Research Funds for the Central Universities(No.2022ZYGXZR017 and 2022ZYGXZR108)+5 种基金the Foundation of Advanced Catalytic Engineering Research Center of the Ministry of Education(No.2020AC006)the State Key Laboratory of Pulp and Paper Engineering(No.2022C04 and 2022ZD05)the Guangdong Pearl River Talents Program(No.2021ZT09Z109 and 2021QN02C8)the Natural Science Foundation of Guangdong Province(No.2017A030312005 and 2022A1515012575)the Guangdong Basic and Applied Basic Research Foundation(No.2021A1515110413)the Science and Technology Program of Guangzhou(No.202201010118)。
文摘Nitrogen-rich zeolitic imidazolate frameworks(ZIFs)are ideal precursors for the synthesis of metal single atoms anchored on N-doped carbon.However,the microporous structures of conventional ZIFs lead to low mass transfer efficiency and low metal utilization of their derivatives.Here,we construct a composite of Co single atoms anchored on nitrogen-doped carbon with a three-dimensional ordered macroporous structure(Co-SA/3DOM-NC)by two-step pyrolysis of ordered macro/microporous ZnCo-ZIF.Co-SA/3DOM-NC shows high activity in the oxidative esterification of furfural,achieving a 99%yield of methyl 2-furoate under mild reaction conditions,which is significantly superior to the microporous and the Conanoparticle counterparts.The high activity of Co-SA/3DOM-NC should be attributed to the CoN4 centers with high intrinsic activity and the ordered macroporous structure,promoting the mass transfer of reactants and accessibility of active sites.
