Shaohua Xie, Yue Lu, Kailong Ye, Wei Tan, Sufeng Cao, Chunying Wang, Daekun Kim, Xing Zhang, Jeremia Loukusa, Yaobin Li, Yan Zhang, Lu Ma, Steven N Ehrlich, Nebojsa S Marinkovic, Jiguang Deng, Maria Flytzani-Stephanopoulos, Fudong Liu
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引用次数: 0
摘要
在缺乏足够缺陷的载体上有效合成和应用单原子催化剂仍然是环境催化领域的一大挑战。在此,我们提出了一种通用的缺陷富集策略,通过 H2 还原预处理来增加 CeO2 基载体的表面缺陷。与未进行缺陷富集的相应催化剂相比,由缺陷 CeO2 基支撑物(包括 CeO2、CeZrOx 和 CeO2/Al2O3 (CA))支撑的铂催化剂在还原活化时表现出更高的铂分散性和一氧化碳氧化活性。具体来说,铂以嵌入单原子的形式存在于具有富集表面缺陷(CA-HD)的 CA 载体上,在此基础上,通过还原活化可获得嵌入铂簇(PtC)的高活性催化剂,其底层铂原子取代了 CeO2 表面晶格中的 Ce 阳离子。嵌入的 PtC 能更好地促进 CO 的吸附,并促进 PtC-CeO2 界面上 O2 的活化,从而使活化后的 Pt/CA-HD 催化剂具有更高的低温 CO 氧化活性。
Enhancing the Carbon Monoxide Oxidation Performance through Surface Defect Enrichment of Ceria-Based Supports for Platinum Catalyst.
Effective synthesis and application of single-atom catalysts on supports lacking enough defects remain a significant challenge in environmental catalysis. Herein, we present a universal defect-enrichment strategy to increase the surface defects of CeO2-based supports through H2 reduction pretreatment. The Pt catalysts supported by defective CeO2-based supports, including CeO2, CeZrOx, and CeO2/Al2O3 (CA), exhibit much higher Pt dispersion and CO oxidation activity upon reduction activation compared to their counterpart catalysts without defect enrichment. Specifically, Pt is present as embedded single atoms on the CA support with enriched surface defects (CA-HD) based on which the highly active catalyst showing embedded Pt clusters (PtC) with the bottom layer of Pt atoms substituting the Ce cations in the CeO2 surface lattice can be obtained through reduction activation. Embedded PtC can better facilitate CO adsorption and promote O2 activation at PtC-CeO2 interfaces, thereby contributing to the superior low-temperature CO oxidation activity of the Pt/CA-HD catalyst after activation.
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.