Fabrication of Highly Dispersed Ru Catalysts on CeO2 for Efficient C3H6 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 : 2024-09-26 DOI:10.1021/acs.est.4c07159

Bifeng Zhang, Jiawei Yang, Yibo Mu, Xiaoyu Ji, Yandi Cai, Nan Jiang, Shaohua Xie, Qiuhui Qian, Fudong Liu, Wei Tan, Lin Dong

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Abstract

Emissions of volatile organic compounds (VOCs) threaten both the environment and human health. To realize the elimination of VOCs, Ru/CeO₂ catalysts have been intensively investigated and applied. Although it has been widely acknowledged that the catalytic performance of platinum group metal catalysts was highly determined by their dispersion and coordination environment, the most reactive structures on Ru/CeO₂ catalysts for VOCs oxidation are still ambiguous. In this work, starting from Ce-BTC (BTC = 1,3,5-benzenetricarboxylic acid) materials, atomically dispersed Ru catalysts and agglomerated Ru catalysts were successfully created via one-step hydrothermal method (Ru-CeO₂-BTC) and conventional incipient wetness impregnation method (Ru/CeO₂-BTC), respectively. In a typical model reaction of C₃H₆ oxidation, atomically dispersed Ru^δ+ species with the formation of abundant Ru–O–Ce linkages on Ru-CeO₂-BTC were found to perform much better than agglomerated RuO_x species on Ru/CeO₂-BTC. Further characterizations and mechanism study disclosed that Ru-CeO₂-BTC catalyst with atomically dispersed Ru ions and more superior low temperature redox performance compared to Ru/CeO₂-BTC could better facilitate the adsorption/activation of C₃H₆ and the decomposition/desorption of intermediates, thus exhibiting superior C₃H₆ oxidation activity. This work elucidated the reactive sites on Ru/CeO₂ catalysts in the C₃H₆ oxidation reaction and provided insightful guidance for designing efficient Ru/CeO₂ catalysts to eliminate VOCs.

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在 CeO2 上制备高度分散的 Ru 催化剂以实现 C3H6 的高效氧化

挥发性有机化合物（VOCs）的排放威胁着环境和人类健康。为了消除挥发性有机化合物，人们对 Ru/CeO2 催化剂进行了深入研究和应用。尽管人们普遍认为铂族金属催化剂的催化性能在很大程度上取决于其分散和配位环境，但 Ru/CeO2 催化剂氧化 VOCs 的最强反应结构仍不明确。本研究以 Ce-BTC（BTC = 1,3,5-苯三羧酸）材料为起点，分别通过一步水热法（Ru-CeO2-BTC）和传统萌发湿法浸渍法（Ru/CeO2-BTC）成功制备了原子分散型 Ru 催化剂和团聚型 Ru 催化剂。在典型的 C3H6 氧化模型反应中，发现原子分散的 Ruδ+ 物种在 Ru-CeO2-BTC 上形成了丰富的 Ru-O-Ce 连接，其性能远远优于 Ru/CeO2-BTC 上团聚的 RuOx 物种。进一步的表征和机理研究发现，与 Ru/CeO2-BTC 相比，Ru-CeO2-BTC 催化剂上的 Ru 离子原子分散，低温氧化还原性能更优，能更好地促进 C3H6 的吸附/活化和中间产物的分解/解吸，从而表现出更高的 C3H6 氧化活性。这项工作阐明了 Ru/CeO2 催化剂在 C3H6 氧化反应中的反应位点，为设计高效的 Ru/CeO2 催化剂消除挥发性有机化合物提供了深刻的指导。

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来源期刊

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.