RuO_(x)分散性导致的活性氧异化与氯苯氧化相关性  

Correlation between chlorobenzene oxidation and active oxygen species induced by the dispersity of RuO_(x)

作　　者：陈曦[1,2] 贾子良 王梦雪 王鹏 季鑫佟[1] 乔昕茹 郭冬瑞 梁美生 CHEN Xi;JIA Zi-liang;WANG Meng-xue;WANG Peng;JI Xin-tong;QIAO Xin-ru;GUO Dong-rui;LIANG Mei-sheng(College of Environment and Ecology,Taiyuan University of Technology,Jinzhong 030600,China;Shanxi Academy of Eco-Environmental Planning and Technology,Taiyuan 030009,China)

机构地区：[1]太原理工大学环境与生态学院,山西晋中030600 [2]山西省生态环境规划和技术研究院,山西太原030009

出　　处：《中国环境科学》2025年第4期1820-1832,共13页China Environmental Science

基　　金：国家自然科学基金(22376156);山西省基础研究计划项目(202203021211140);太原市生态环境局委托项目(RH2400000291)。

摘　　要：在相同的催化剂载体TiCeO_(x)和贵金属含量下,利用Ru^(3+)浸渍还原(自下而上)和Ru胶体溶液热扩散(自上而下)两种方法制备具有不同分散性的贵金属负载型催化剂.其中Ru^(3+)浸渍还原法制备的催化剂RuTiCeO_(x)-N中,Ru物种以RuO_(x)纳米团簇的形式存在;Ru胶体溶液热扩散法制备的催化剂RuTiCeO_(x)-A中,Ru物种以单原子分散的形式存在.Ru物种不同的分散状态导致其参与氯苯(CB)氧化反应的活性氧物种和酸性位点的差异性,其中RuTiCeO_(x)-N中的主要活性氧物种为化学吸附氧,RuTiCeO_(x)-A中的主要活性氧物种为表面晶格氧.CB的化学吸附诱使活性氧物种转变为羟基(-OH)官能团参与催化反应.在活性氧物种和强弱多种酸性位的共同作用下,RuTiCeO_(x)-A催化剂表现出了优异的活性和稳定性,CB在300℃可以完全转化,且可以维持24h而不失活.TiCeO_(x)bimetallic catalysts were prepared as catalyst carries.And the Ru-supported catalysts with different dispersions were synthesized by the methods of Ru^(3+)impregnation reduction(bottom to up)and Ru colloid solution thermal diffusion(top to down)methods.In the catalyst RuTiCeO_(x)-N prepared by Ru^(3+)immersion reduction method,Ru species exist in the form of RuO_(x)nanoclusters.In the catalyst RuTiCeO_(x)-A prepared by Ru colloid solution thermal diffusion,Ru species exist in the form of single-atom dispersion.The different dispersion states of Ru species lead to the difference of active oxygen species and acid sites involved in chlorobenzene(CB)oxidation.Chemisorbed oxygen and surface lattice oxygen could be the dominating active oxygen species for RuTiCeO_(x)-N and RuTiCeO_(x)-A,respectively.And due to the chemisorption of CB,that could be transformed into hydroxyl radical(-OH)to be involved in the catalytic reaction.Catalyst RuTiCeO_(x)-A performed better with the complete conversion of CB at 300℃and 24h of durability test without deactivation.That could be attributed to the synergy between its resulted active oxygen species and multiple acid sites(strong and weak).

关 键 词：催化剂载体 贵金属 团簇 单原子分散 氧物种 羟基 

分 类 号：X511[环境科学与工程—环境工程]