Insights on selective Pb adsorption via O 2p orbit in UiO-66 containing rich-zirconium vacancies  

作　　者：Yu-Hang Li Shuai Gao Lu Zhang Hanchun Chen Chong-Chen Wang Haodong Ji 

机构地区：[1]Eco-environment and Resource Efficiency Research Laboratory,School of Environment and Energy,Peking University Shenzhen Graduate School,Shenzhen 518055,China [2]Beijing Key Laboratory of Functional Materials for Building Structure and Environment Remediation,School of Environment and Energy Engineering,Beijing University of Civil Engineering and Architecture,Beijing 100044,Chin

出　　处：《Chinese Chemical Letters》2024年第8期357-361,共5页中国化学快报（英文版）

基　　金：supports from the National Natural Science Foundation of China(NSFC,No.52100069);the Shenzhen Science and Technology Program(No.JCYJ20220531093205013);the 2023 Shenzhen Sustainable Supporting Funds for Colleges and Universities(No.20231121170027002)are greatly acknowledged.

摘　　要：Herein,we constructed defective UiO-66 with rich Zr vacancy structure model,in which the defective structure was verified by various characterizations.Also,the Pb adsorption experiments affirmed that defective UiO-66 could display better adsorption and selective adsorption ability than that of perfect UiO-66.The results of partial density of states(PDOS)and Mulliken charge population indicated that the blue shift of O 2p and Zr 4d orbit induced the electron rearrangement of atoms closed to the bonding sites,while the positive charge number of Zr atoms decreased than before.Combining with the expansion of pore size,Pb atom was more inclined to transfer and bond with unsaturated coordination oxygens.More significantly,quantitative structure-activity relationships(QSARs)demonstrated that selective capture of Pb instead of Zn,Cu,Cd and Hg displayed by defective UiO-66 was determined jointly by bond strength,adsorption energy and electron transfer.This work provided some theoretical direction for the purpose of the fabrication of adsorbent and the investigation of mechanism.

关 键 词：Selective adsorption Heavy metal Density functional theory UiO-66 Zr vacancies 

分 类 号：O647.33[理学—物理化学] X703[理学—化学]