Synergy of metal-support interaction and positive Pd species promoting efficient C-CI bond activation on Pd-based Ce-MOF-derived catalysts  

作　　者：Xiao-Jie Hu Yu-Han Sun Ling-Yue Liu Dan-Jun Mao Shou-Rong Zheng 

机构地区：[1]State Key Laboratory of Pollution Control and Resource Reuse,School of the Environment,Nanjing University,Nanjing 210023,China [2]Department of Applied Biology and Chemical Technology,The Hong Kong Polytechnic University,Hong Kong 999077,Hong Kong,China

出　　处：《Rare Metals》2024年第11期5835-5847,共13页稀有金属（英文版）

基　　金：financially supported by the National Natural Science Foundation of China(Nos.21976086 and 22002059)。

摘　　要：Monochloroacetic acid(MCAA)is identified as a highly carcinogenic disinfection by-product in chlorinated drinking water.In this study,a series of CeO_(2)-supported Pd catalysts(Pd/MCeO_(2))were synthesized through one-step calcination of Pd-loaded Ce-UiO-66-BDC(CeMOF),and the liquid-phase catalytic hydrodechlorination of MCA A was explored using these catalysts.For comparison,Pd/CeO_(2)catalysts were additionally synthesized using the conventional impregnation method.The characterization results reveal that the catalysts exhibit strong metal-support interaction,leading to high Pd dispersion and Pd^(n+)content.Additionally,the calcination temperature significantly influences catalytic performance,with the catalyst calcined at 500℃(Pd/MCeO_(2)-500)demonstrating the highest catalytic activity and achieving complete dechlorination of MCA A within 50 min.Furthermore,it is found that the catalytic MCAA hydrodechlorination using the catalysts adheres to the Langmuir-Hinshelwood model.Accordingly,low reaction pH is favorable for the catalytic hydrodechlorination of MCAA,enhancing MCAA adsorption on the catalyst surface due to the electrostatic interaction between MCAA and the catalyst surface.Theoretical results suggest that the presence of Pd^(n+)efficiently facilitates MCAA adsorption and C-Cl cleavage,thus significantly enhancing the liquid-phase catalytic hydrodechlorination.

关 键 词：Ce-UiO-66-BDC One-step calcination Metal-support interaction Liquid-phase catalytic hydrodechlorination Monochloroacetic acid 

分 类 号：O643.36[理学—物理化学]