Ultrafine PdRu Nanoparticles Immobilized in Metal-Organic Frameworks for Efficient Fluorophenol Hydrodefluorination under Mild Aqueous Conditions  

作　　者：Wenqian Yang Qinglin Liu Jun Yang Jiahui Xian Yinle Li Guangqin Li Cheng-Yong Su 

机构地区：[1]State Key Laboratory of Optoelectronic Materials and Technologies,MOE Laboratory of Bioinorganic and Synthetic Chemistry,Lehn Institute of Functional Materials,School of Chemistry Sun Yat-Sen University,Guangzhou 510006

出　　处：《CCS Chemistry》2022年第7期2276-2285,共10页中国化学会会刊（英文）

基　　金：supported by the National Key R&D Program of China(no.2018YFA0108300);the Overseas High-level Talents Plan of China and Guangdong Province,the Fundamental Research Funds for the Central Universities;the Program for Guangdong Introducing Innovative and Entrepreneurial Teams(no.2017Z T07C069);Local Innovative and Research Teams Project of Guangdong Pearl River Talents Program(no.2017BT01C161);the NSFC Projects(nos.22075321,21821003,21890380,and 21905315).

摘　　要：Fluorinated organic compounds are of great importance to modern industries,while their release to the environment is inevitable,causing extreme environmental pollution and the subsequent hazardous effect on ecosystems.This is because the degradation of fluorinated compounds under mild conditions remains a challenging task due to the strong C-F bond strength.In this study,we report preparation of PdRu@MIL-101 through immobilizing ultrafine PdRu alloy nanoparticles with a mean diameter of∼2 nminto the metal-organic framework(MOF),MIL-101(Cr),which was highly active and stable in the hydrodefluorination of 4-fluorophenol(4-FP)under mild aqueous conditions.The optimized catalyst Pd0.5Ru0.5@MIL-101 achieved impressive hydrogenation performance with a 98.5% conversion of 4-FP and a 97.7% selectivity of cyclohexanol,much better than the single metal-doped Pd@MIL-101 and Ru@MIL-101 catalysts.The excellent catalytic behavior contributed to the synergistic effect of combining the PdRu alloying effect and the MOF nanospace confinement effect,providing a promising strategy to develop highly efficient hydrodefluorination catalysts to assist environmental restoration and green ecology.

关 键 词：PdRu ultrafine nanoparticles PdRu alloy metal-organic frameworks HYDRODEFLUORINATION synergistic effect 

分 类 号：O64[理学—物理化学]