文献类型：期刊文献

英文题名：Platinum Single Atoms Anchored on a Covalent Organic Framework: Boosting Active Sites for Photocatalytic Hydrogen Evolution

作者：Dong, Pengyu[1];Wang, Yan[2];Zhang, Aicaijun[2];Cheng, Ting[1];Xi, Xinguo[2];Zhang, Jinlong[3]

机构：[1]Yancheng Inst Technol, Key Lab Adv Technol Environm Protect Jiangsu Prov, Yancheng 224051, Peoples R China;[2]Yancheng Inst Technol, Sch Chem & Chem Engn, Yancheng 224051, Peoples R China;[3]East China Univ Sci & Technol, Key Lab Adv Mat & Inst Fine Chem, Sch Chem & Mol Engn, Shanghai Engn Res Ctr Multimedia Environm Catalys, Shanghai 200237, Peoples R China

年份：2021

卷号：11

期号：21

起止页码：13266

外文期刊名：ACS CATALYSIS

收录：;EI(收录号：20214611145427);WOS:【SCI-EXPANDED(收录号:WOS:000716773800041)】；

基金：This work is financially supported by the National Natural Science Foundation of China (Grant nos. 51772258, 21403184, and 21972040), the Qinglan Project of Jiangsu Province, Scientific Research and Practical Innovation Project for Graduate Students in Jiangsu Province (No. KYCX20_2965), Innovation Program of Shanghai Municipal Education Commission (2021-01-07-00-02-E00106), the Science and Technology Commission of Shanghai Municipality (20DZ2250400), and Joint Open Fund of Jiangsu Collaborative Innovation Center for Ecological Building Material and Environmental Protection Equipment and Key Laboratory for Advanced Technology in Environmental Protection of Jiangsu Province (JH201805). The authors thank the Analysis & Testing Center of Yancheng Institute of Technology for support.

语种：英文

外文关键词：heterogeneous photocatalysis; covalent organic frameworks; single-atom Pt; hydrogen evolution; visible-light-driven; coordination site construction

摘要：It is of great importance to explore and achieve a more effective approach toward the controllable synthesis of single-atom-based photocatalysts with high metal content and long-term durability. Herein, single-atom platinum (Pt) with high loading content anchored on the pore walls of two-dimensional beta-ketoenamine-linked covalent organic frameworks (TpPa-1-COF) is presented. Aided by advanced characterization techniques of aberration-corrected high-angle annular dark-field scanning transmission electron microscopy (AC HAADF-STEM) and X-ray absorption fine structure (XAFS) spectroscopy, it has been demonstrated that atomically dispersed Pt is formed on the TpPa-1-COF support through a six-coordinated C3N-Pt-Cl-2 species. The optimized Pt-1@TpPa-1 catalyst exhibits a high photocatalytic H-2 evolution rate of 719 mu mol g(-1) h(-1) under visible-light irradiation, a high actual Pt loading content of 0.72 wt %, and a large turnover frequency (TOF) of 19.5 h(-1), with activity equivalent to 3.9 and 48 times higher than those of Pt nanoparticles/TpPa-1 and bare TpPa-1, respectively. The improved photocatalytic per formance for H-2 evolution is ascribed to the effective photogenerated charge separation and migration and well-dispersed active sites of single-atom Pt. Moreover, density functional theory (DFT) calculations further reveal the role of Pt single atoms in the enhanced photocatalytic activity for H-2 evolution. Overall, this work provides some inspiration for designing single-atom-based photocatalysts with outstanding stability and efficiency using COFs as the support.