Constructing Bridge Hydroxyl Groups on the Ru/MOx/HZSM-5 (M = W, Mo) Catalysts to Promote the Hydrolysis Oxidation of Multicomponent VOCs

IF 11.3 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL 环境科学与技术 Pub Date : 2024-12-24 DOI:10.1021/acs.est.4c09649
Linke Wu, Yuxi Liu, Xiaohui Yu, Ruyi Gao, Yiwen Jia, Qinpei Sun, Ying Feng, Lin Jing, Zhiquan Hou, Jiguang Deng, Hongxing Dai
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Abstract

Chlorinated and oxygenated volatile organic compounds (CVOCs and OVOCs) pose a significant threat to human health. Catalytic oxidation effectively removes these pollutants, but catalyst deactivation is a challenge. Our study focused on the hydrolysis oxidation of chlorobenzene (CB) and ethyl acetate (EA) over Ru/MOx/HZSM-5 (M = W, Mo). It was found that doping MoOx to the catalyst increased the structural hydroxyl amount and balanced surface acidity, thus significantly improving the catalytic stability, with Ru/MoOx/HZSM-5 exhibiting a better activity for CB and EA oxidation (T90% = 438 and 276 °C at space velocity = 20,000 mL g–1 h–1, respectively). Water vapor introduction considerably promoted hydrolysis oxidation and protected the active sites from being poisoned by cumulative chlorine. The synergistic interaction of the Mo–O(H)–Al structure in Ru/MoOx/HZSM-5 with the Si–OH–Al structure promotes the activation of H2O to form bridging hydroxyl groups, which provide a proton-rich environment for hydrolysis oxidation. It was also found that dissociated H2O reacted with adsorbed oxygen species to form highly active *OOH, accelerating the deep oxidation of intermediates. We believe that the present study can provide a unique strategy for the effective elimination of multicomponent VOCs under complex conditions.

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Ru/MOx/HZSM-5 (M = W, Mo)催化剂上构建桥羟基促进多组分VOCs水解氧化
氯化和含氧挥发性有机化合物(CVOCs和OVOCs)对人类健康构成重大威胁。催化氧化可以有效地去除这些污染物,但催化剂的失活是一个挑战。研究了Ru/MOx/HZSM-5 (M = W, Mo)对氯苯(CB)和乙酸乙酯(EA)的水解氧化反应。结果发现,在催化剂中掺杂MoOx增加了结构羟基的数量,平衡了表面酸度,从而显著提高了催化稳定性,Ru/MoOx/HZSM-5对CB和EA的氧化活性较好(T90% = 438和276℃,空速= 20,000 mL g-1 h-1)。水蒸气的引入大大促进了水解氧化,保护了活性位点不受累积氯的毒害。Ru/MoOx/HZSM-5中Mo-O (H) -Al结构与Si-OH-Al结构的协同作用促进了H2O的活化,形成桥接羟基,为水解氧化提供了富含质子的环境。还发现解离的H2O与吸附的氧原子反应生成高活性的*OOH,加速中间体的深度氧化。我们相信,本研究可以为在复杂条件下有效消除多组分VOCs提供一种独特的策略。
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来源期刊
环境科学与技术
环境科学与技术 环境科学-工程:环境
CiteScore
17.50
自引率
9.60%
发文量
12359
审稿时长
2.8 months
期刊介绍: Environmental Science & Technology (ES&T) is a co-sponsored academic and technical magazine by the Hubei Provincial Environmental Protection Bureau and the Hubei Provincial Academy of Environmental Sciences. Environmental Science & Technology (ES&T) holds the status of Chinese core journals, scientific papers source journals of China, Chinese Science Citation Database source journals, and Chinese Academic Journal Comprehensive Evaluation Database source journals. This publication focuses on the academic field of environmental protection, featuring articles related to environmental protection and technical advancements.
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