Robust Ru/Ce@Co Catalyst with an Optimized Support Structure for Propane Oxidation.

IF 10.8 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL 环境科学与技术 Pub Date : 2024-07-03 DOI:10.1021/acs.est.4c03449
Aiyong Wang, Jiajia Ding, Mingqi Li, Peiyao Song, Zhiyuan Zhao, Yanglong Guo, Yun Guo, Li Wang, Qiguang Dai, Wangcheng Zhan
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Abstract

Short carbon chain alkanes, as typical volatile organic compounds (VOCs), have molecular structural stability and low molecular polarity, leading to an enormous challenge in the catalytic oxidation of propane. Although Ru-based catalysts exhibit a surprisingly high activity for the catalytic oxidation of propane to CO2 and H2O, active RuOx species are partially oxidized and sintered during the oxidation reaction, leading to a decrease in catalytic activity and significantly inhibiting their application in industrial processes. Herein, the Ru/Ce@Co catalyst is synthesized with a specific structure, in which cerium dioxide is dispersed in a thin layer on the surface of Co3O4, and Ru nanoparticles fall preferentially on cerium oxide with high dispersity. Compared with the Ru/CeO2 and Ru/Co3O4 catalysts, the Ru/Ce@Co catalyst demonstrates excellent catalytic activity and stability for the oxidation of propane, even under severe operating conditions, such as recycling reaction, high space velocity, a certain degree of moisture, and high temperature. Benefiting from this particular structure, the Ru/Ce@Co (5:95) catalyst with more Ce3+ species leads to the Ru species being anchored more firmly on the CeO2 surface with a low-valent state and has a strong potential for adsorption and activation of propane and oxygen, which is beneficial for RuOx species with high activity and stability. This work provides a novel strategy for designing high-efficiency Ru-based catalysts for the catalytic combustion of short carbon alkanes.

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具有优化支撑结构的强效 Ru/Ce@Co 催化剂用于丙烷氧化。
短碳链烷烃作为典型的挥发性有机化合物(VOC),具有分子结构稳定和分子极性低的特点,这给丙烷的催化氧化带来了巨大挑战。虽然 Ru 基催化剂在催化丙烷氧化为 CO2 和 H2O 的过程中表现出惊人的高活性,但活性 RuOx 物种在氧化反应过程中部分被氧化和烧结,导致催化活性降低,极大地阻碍了其在工业过程中的应用。本文合成了具有特殊结构的 Ru/Ce@Co 催化剂,二氧化铈以薄层形式分散在 Co3O4 表面,纳米 Ru 粒子优先落在氧化铈上,分散度高。与 Ru/CeO2 和 Ru/Co3O4 催化剂相比,Ru/Ce@Co 催化剂在丙烷氧化过程中表现出优异的催化活性和稳定性,即使在循环反应、高空间速度、一定湿度和高温等苛刻的操作条件下也是如此。得益于这种特殊的结构,Ru/Ce@Co(5:95)催化剂中含有更多的 Ce3+ 物种,从而使 Ru 物种以低价态更牢固地固定在 CeO2 表面,具有吸附和活化丙烷和氧气的强大潜力,有利于 RuOx 物种具有高活性和稳定性。这项工作为设计用于催化燃烧短碳烷烃的高效 Ru 基催化剂提供了一种新策略。
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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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