文献类型：期刊文献

英文题名：Structure-Property-Energetics Relationship of Organosulfide Capture Using Cu(I)/Cu(II)-BTC Edited by Valence Engineering

作者：Chen, Yuxiang[1];Wang, Dan[1];Jiang, Hao[1];Tan, Jialun[1];An, Yang[1];Chen, Yonghao[1];Wu, Yuan[1];Sun, Hui[1,2];Shen, Benxian[1,2];Zhao, Jigang[1,2];Liu, Jichang[1,2];Ling, Hao[1,2];Wu, Di[3,4,5];Han, Xiao[1];Xu, Sixin[1]

机构：[1]East China Univ Sci & Technol, Petr Proc Res Ctr, Sch Chem Engn, Shanghai 200237, Peoples R China;[2]East China Univ Sci & Technol, Int Joint Res Ctr Green Energy Chem Engn, Shanghai 200237, Peoples R China;[3]Washington State Univ, Alexandra Navrotsky Inst Expt Thermodynam, Pullman, WA 99163 USA;[4]Washington State Univ, Gene & Linda Voiland Sch Chem Engn & Bioengn Mat, Washington, WA 99163 USA;[5]Washington State Univ, Dept Chem, Pullman, WA 99163 USA

年份：2021

卷号：60

期号：1

起止页码：371

外文期刊名：INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH

收录：;EI(收录号：20210209762945);WOS:【SCI-EXPANDED(收录号:WOS:000611072000030)】；

基金：This work is financially supported by the National Natural Science Foundation of China (grants 91634112 and 21878097) and the Natural Science Foundation of Shanghai (grant 16ZR1408100). D.W. acknowledges the institutional funds from the Gene and Linda Voiland School of Chemical Engineering and Bioengineering and the Alexandra Navrotsky Institute for Experimental Thermodynamics at Washington State University.

语种：英文

外文关键词：Copper compounds - Density functional theory - Extended X ray absorption fine structure spectroscopy - Computation theory - Sulfur compounds - X ray absorption near edge structure spectroscopy - Sodium compounds - X ray absorption - Coordination reactions

摘要：Valence engineering of copper (Cu) within functional materials is effective to tune the performance and energetics of catalysts and sorbents. Here, by precisely controlling the Cu(II)/Cu(I) ratio employing Na2S2O3 as the reduction agent, we synthesized a family of copper-1,3,5-benzenetricarboxylic acid (Cu-BTC) sorbents for organosulfur compound capture. Integrated X-ray absorption fine structure and density functional theory studies suggest that the atomic-level, short-range order changes caused by Cu reduction lead to simultaneous stability, affinity, and pore topology evolutions in Cu(I)/Cu(II)-BTC, which govern the sorption capacity and binding energetics of dimethyl disulfide capture. This multiscale fundamental study with both experimental and computational results highlights the power of coordination chemistry on materials engineering on atomic level.