Zheng Zhiqiang, Wang Zhongqiang, Xue Yurui, He Feng, Li Yuliang
Science Center for Material Creation and Energy Conversion, School of Chemistry and Chemical Engineering, Institute of Frontier and Interdisciplinary Science, Shandong University, Jinan 250100, P.R. China.
CAS Key Laboratory of Organic Solids, Beijing National laboratory for Molecular Sciences (BNLMS), CAS Research/Education Center for Excellence in Molecular Science, Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, P.R. China.
ACS Mater Au. 2021 Aug 7;1(2):107-115. doi: 10.1021/acsmaterialsau.1c00012. eCollection 2021 Nov 10.
The conversion of carbon dioxide (CO) into organic carbonates under ambient temperatures and pressures with high conversion and selectivity still faces a great challenge. The zerovalent atomic catalysts (ACs), featuring accurate structure and valence states, provide a new and accurate model system for catalysis. Herein we developed a general preadsorption-reduction strategy to synthesize zerovalent cobalt AC on graphdiyne (Co/GDY). The Co/GDY ACs were used for efficient and selective CO fixation. We were surprised to find that Co/GDY ACs reached nearly 100% conversion at 80 °C and 1 atm in CO fixation and with a significantly high turnover frequency (TOF) of 3024.8 h, which is almost several orders larger than that of benchmarked catalysts. Such high conversion and selectivity represent the advantages of emerging catalysts.
在环境温度和压力下将二氧化碳（CO₂）高效且选择性地转化为有机碳酸盐仍然面临巨大挑战。零价原子催化剂（ACs）具有精确的结构和价态，为催化提供了一个全新且精确的模型体系。在此，我们开发了一种通用的预吸附-还原策略，以在石墨炔（Co/GDY）上合成零价钴原子催化剂。Co/GDY原子催化剂被用于高效且选择性地固定CO₂。我们惊讶地发现，在CO₂固定反应中，Co/GDY原子催化剂在80℃和1个大气压下转化率接近100%，并且具有高达3024.8 h⁻¹的周转频率（TOF），这几乎比基准催化剂高出几个数量级。如此高的转化率和选择性体现了新型催化剂的优势。
