Atomically synergistic bimetallic pair sites in a dual-cluster-based MOF for ultrafast degradation of chemical warfare agent simulants  

作　　者：Zhi-Bing Sun Qian-You Wang Cai Li Man Cao Jing-Zheng Zhang Jie Wu 

机构地区：[1]Henan Key Laboratory of Special Functional Molecular Materials,Ministry of Education,and College of Chemistry,Zhengzhou University,Zhengzhou 450001,China [2]Zhengzhou Research Institute,Beijing Institute of Technology,Zhengzhou 450000,China

出　　处：《Nano Research》2025年第2期940-948,共9页纳米研究(英文版)

基　　金：This work was supported by the National Natural Science Foundation of China(No.22175155);the opening project of the State Key Laboratory of Explosion Science and Technology(Beijing Institute of Technology)(No.KFJJ22-05M);the Science and Technology on Applied Physical Chemistry Laboratory,China(No.6142602230302).

摘　　要：Metal clusters represent a promising class of catalysts for various reactions,but the simultaneous improvement of their stability and catalytic activity is a longstanding challenge.Herein,we created a stable dual-cluster metal-organic framework(MOF)that featured atomically synergistic bimetallic pair sites colocalized within sub nanometer pockets.The pair sites,consisting of Ni and Mo sites respectively originating from defective MOF and Polyoxometalate(POM)clusters,were rationally constructed by size-matched ligand exchange.The as-obtained dual-cluster MOF(MnMo_(6)-lg-PCN-601)exhibited superior catalytic activity,rate performance(t_(1/2)<1 min,TOF=140 min^(-1)),and stability toward the degradation of the chemical warfare agent simulant 2-chloroethyl ethyl sulfide(CEES).In-situ Fourier transform infrared(FTIR)studies and density functional theory(DFT)calculations demonstrated that the atomic synergy between colocalized pair sites favored the adsorption and activation of the CEES substrate,moreover,it also promoted H_(2)O_(2) decomposition for the selective oxidation of CEES.Our work opens a new avenue for the construction of stable metal clusters with high catalytic activity for application in various multi-substrate reactions.

关 键 词：metal-organic frameworks metal clusters synergistic catalysis degradation of chemical warfare agent(CWA) 

分 类 号：O64[理学—物理化学]