文献类型：期刊文献

英文题名：Construction of Single Ni Atom-Immobilized ZIF-8 with Ordered Hierarchical Pore Structures for Selective CO2 Photoreduction

作者：Liu, Zhiguo[1,2];Chen, Ziyu[1,2];Li, Mingyang[1,2];Li, Jiaying[1,2];Zhuang, Weijie[1,2];Yang, Xiao[1,2];Wu, Shiqun[1,2];Zhang, Jinlong[1,2,3]

机构：[1]East China Univ Sci & Technol, Shanghai Engn Res Ctr Multimedia Environm Catalysi, Sch Chem & Mol Engn, Key Lab Adv Mat, Shanghai 200237, Peoples R China;[2]East China Univ Sci & Technol, Feringa Nobel Prize Scientist Joint Res Ctr, Frontiers Sci Ctr Mat Biol & Dynam Chem, Sch Chem & Mol Engn,Joint Int Res Lab Precis Chem, Shanghai 200237, Peoples R China;[3]Yancheng Inst Technol, Sch Chem & Chem Engn, Yancheng 224051, Peoples R China

年份：2023

卷号：13

期号：10

起止页码：6630

外文期刊名：ACS CATALYSIS

收录：;EI(收录号：20232114116654);WOS:【SCI-EXPANDED(收录号:WOS:000994333000001)】；

基金：This work was supported by the National Key Research and Development Program of China (2022YFE0107900 and 2022YFB3803600) , the National Natural Science Foundation of China (21972040, 21673073, and 22202070) , the Innovation Program of Shanghai Municipal Education Commission (2021-01-07-00-02-E00106) , the Science and Technology Commission of Shanghai Municipality (22230780200 and 20DZ2250400) , the Project supported by Shanghai Municipal Science and Technology Major Project (2018SHZDZX03) , the Program of Introducing Talents of Discipline to Universities (nos. B20031 and B16017) , the Postdoctoral Innovative Talent Support Program (BX20220107) , the Shanghai Rising-Star Program (22YF1410200) , and the Fundamental Research Funds for the Central Universities (222201717003) .

语种：英文

外文关键词：CO2 photoreduction; hierarchical porous material; Ni single atom; ZIF-8; inhibition of water reduction

摘要：The rational construction of single-atom-modified porous metal-organic frameworks (MOFs) for efficient CO2 photoconversion is a promising avenue, yet the one that poses a significant challenge. In this study, we demonstrate the successful construction of a Ni single-atom-immobilized ZIF-8 with an ordered hierarchical (macro-micro) pore structure for highly efficient photocatalytic CO2 reduction to CO. The interpenetrated macroporous structure in microporous ZIF-8 is built up by employing polystyrene (PS) opal as a hard template, while the high stability of the framework is achieved through the double-solvent-induced crystallization. The hierarchical porous structure enables rapid mass transport and strong adsorption of CO2, while Ni single atoms as active sites and electron-trapping sites optimize the reaction energy and hinder the competitive H2 evolution. As a result, the Ni single-atom-immobilized hierarchical porous ZIF-8 achieves high stability and an activity of 4.2 mmol g-1 h-1 for CO yield with an electronic selectivity of 94%, which shows a 47-fold CO yield of that for ZIF-8. This work highlights the significance of constructing a hierarchical porous structure of MOFs and single-atom-active sites to improve the activity and selectivity of CO2 photoreduction for realizing carbon neutralization.