文献类型：期刊文献

英文题名：Development of Crystalline Covalent Triazine Frameworks to Enable In Situ Preparation of Single-Atom Ni-N3-C for Efficient Electrochemical CO2 Reduction

作者：Yang, Na[1,2];Yang, Lan[3];Zhu, Xiang[1,2];Zhao, Peiqing[1,2];Liu, Honglai[3];Xia, Chungu[1,2];Dai, Sheng[4];Tian, Chengcheng[5]

机构：[1]Chinese Acad Sci, Suzhou Res Inst, State Key Lab Oxo Synth & Select Oxidat, Lanzhou Inst Chem Phys, Suzhou 215000, Peoples R China;[2]Univ Chinese Acad Sci, Beijing 101408, Peoples R China;[3]East China Univ Sci & Technol, Sch Chem Engn, State Key Lab Chem Engn, Shanghai 200237, Peoples R China;[4]Oak Ridge Natl Lab, Chem Sci Div, Oak Ridge, TN 37831 USA;[5]East China Univ Sci & Technol, Sch Resources & Environm Engn, Shanghai 200237, Peoples R China

年份：2022

卷号：4

期号：11

起止页码：2143

外文期刊名：ACS MATERIALS LETTERS

收录：;EI(收录号：20224112866881);WOS:【SCI-EXPANDED(收录号:WOS:000898512400001)】；

基金：X.Z. thanks the financial support from the National Program for Young Talents of China, Foundation research project of Jiangsu Province (Y91266JZQ1), National Natural Science Foundation of China (E00966GZQ2 and E00966GMS1). C.T. was supported by Shanghai International Science and Technology Cooperation Project (20230710700). The research was also supported financially by the National Natural Science Foundation of China (52170109). S.D. (discussion of the results) was supported by U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division.

语种：英文

外文关键词：Carbon dioxide - Carbon monoxide - Chlorine compounds - Nickel compounds - Zinc chloride

摘要：The synthesis of highly crystalline covalent triazine frameworks (CTFs) with fully conjugated nitrogen-enriched architectures is a long-term challenging subject. Herein, a solvent-and catalyst-free approach was implemented for the first time to create crystalline CTFs based on a new trimerization of amidine-type monomers. A highly crystalline triazine-linked polymer with a specific surface area of 255 m(2) g(-1) was achieved, whereas additional aldehydes were no longer required. Furthermore, an in situ transformation strategy was developed by exploring a molten salt (ZnCl2) to promote this new condensation, so as to convert as-obtained CTFs into isolated single-atom catalysts (SACs). Interestingly, the usage of ZnCl2 not only enables a crystalline CTF with a significantly enhanced surface area, up to 663 m(2) g(-1) but also provides a means of realizing atomically dispersed nickel (Ni) catalysts with unique Ni-N-3-C sites. As a result, the resulting SAC exhibits efficient electrochemical carbon dioxide (CO2) reduction performance, where a maximum Faradaic efficiency for carbon monoxide (CO) production of 97.5% at -0.52 V (vs. reversible hydrogen electrode, RHE) and an excellent turnover frequency (3192 h(-1)) with a current density of 23.32 mA cm(-2) at -1.02 V can be obtained, respectively. We anticipate our findings will facilitate new possibilities for the development of crystalline porous organic frameworks and SACs for various catalysis.