Effect of A-Site Defects on the Catalytic Activity of Perovskite LaCoO3: Insights from the Electronic Structure

IF 11.3 1区化学 Q1 CHEMISTRY, PHYSICAL

ACS Catalysis Pub Date : 2025-01-17 DOI:10.1021/acscatal.4c06142

Hanlin Chen, Xiaoliang Liang, Zijuan You, Fuding Tan, Jingwen Zhou, Xiaoju Lin, Meiqin Chen, Peng Liu, Yiping Yang, Suhua Wang, Steven L. Suib

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Abstract

The development of highly active perovskite-based catalysts for the oxidation of volatile organic chemicals (VOCs) has drawn a great deal of attention. A-site defect regulation is found to be effective to improve the catalytic performance, but the relationship between structure variation and catalytic activity has not been clearly unveiled. Herein, this issue was interpreted by the variation of physicochemical properties and electronic structure (O p-band center). An in situ one-step calcination method with NH₄HCO₃ addition was adopted to prepare a series of A-site-deficient LaCoO₃ perovskites (L_xCO), which were characterized by XRD, TEM, EELS, ESR, XPS, UPS, H₂-TPR, and O₂-TPD and catalytic test toward toluene oxidation. The catalytic activity displayed a volcano-type relationship with an addition amount of NH₄HCO₃. The electronic structure determined the reducibility and active oxygen content and accordingly affected the catalytic activity of L_xCO. The obtained results provide theoretical and technical support for the design of efficient VOC oxidation catalysts.

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a位缺陷对钙钛矿LaCoO3催化活性的影响：来自电子结构的见解

高活性钙钛矿基催化剂在挥发性有机化合物（VOCs）氧化中的应用已引起广泛关注。发现a位缺陷调节对提高催化性能是有效的，但结构变化与催化活性之间的关系尚未明确揭示。本文通过物理化学性质和电子结构（O - p波段中心）的变化来解释这一问题。采用添加NH4HCO3的原位一步煅烧法制备了一系列缺乏a位的LaCoO3钙钛矿（LxCO），采用XRD、TEM、EELS、ESR、XPS、UPS、H2-TPR、O2-TPD对其进行了表征，并进行了甲苯氧化催化试验。催化活性与NH4HCO3的添加量呈火山型关系。电子结构决定了LxCO的还原性和活性氧含量，从而影响了LxCO的催化活性。所得结果为设计高效的VOC氧化催化剂提供了理论和技术支持。

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来源期刊

ACS Catalysis CHEMISTRY, PHYSICAL-

CiteScore

20.80

自引率

6.20%

发文量

1253

审稿时长

1.5 months

期刊介绍： ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels. The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.