Microkinetic Modeling with Size-Dependent and Adsorbate-Adsorbate Interactions for the Direct Synthesis of H2O2 over Pd Nanoparticles
2023-11-17
发表期刊ACS CATALYSIS (IF:11.3[JCR-2023],12.6[5-Year])
ISSN2155-5435
EISSN2155-5435
卷号13期号:22页码:15054-15073
发表状态已发表
DOI10.1021/acscatal.3c03893
摘要

As a bottleneck in the direct synthesis of hydrogen peroxide, the development of an efficient palladium-based catalyst has garnered great attention. However, elusive active centers and reaction mechanism issues inhibit further optimization of its performance. In this work, advanced microkinetic modeling with the adsorbate-adsorbate interaction and nanoparticle size effect based on first-principles calculations is developed. A full mechanism uncovering the significance of adsorbate-adsorbate interaction is determined on Pd nanoparticles. We demonstrate unambiguously that Pd(100) with main coverage species of O2 and H is beneficial to H2O2 production, being consistent with experimental operando observation, while H2O forms on Pd(111) covered by O species and Pd(211) covered by O and OH species. Kinetic analyses further enable quantitative estimation of the influence of temperature, pressure, and particle size. Large-size Pd nanoparticles are found to achieve a high H2O2 reaction rate when the operating conditions are moderate temperature and higher oxygen partial pressure. We reveal that specific facets of the Pd nanoparticles are crucial factors for their selectivity and activity. Consistent with the experiment, the production of H2O2 is discovered to be more favorable on Pd nanoparticles containing Pd(100) facets. The ratio of H2/O2 induces substantial variations in the coverage of intermediates of O2 and H on Pd(100), resulting in a change in product selectivity. © 2023 The Authors. Published by American Chemical Society.

关键词Nanoparticles Oxidation Palladium Palladium compounds Particle size Particle size analysis Synthesis (chemical) Active center Adsorbate-adsorbate interaction DFT Direct synthesis Direct synthesis of hydrogen peroxide Microkinetic modeling Palladium based catalysts Pd nanoparticles Size dependent Sizes effect
收录类别EI
语种英语
出版者American Chemical Society
EI入藏号20234915144350
EI主题词Hydrogen peroxide
EI分类号547.1 Precious Metals ; 761 Nanotechnology ; 802.2 Chemical Reactions ; 804.2 Inorganic Compounds ; 933 Solid State Physics ; 951 Materials Science
原始文献类型Journal article (JA)
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文献类型期刊论文
条目标识符https://kms.shanghaitech.edu.cn/handle/2MSLDSTB/347894
专题物质科学与技术学院
生物医学工程学院_PI研究组_胡鹏组
通讯作者Yao, Zihao; Hu, P.; Wang, Jianguo
作者单位
1.Institute of Industrial Catalysis, College of Chemical Engineering, Zhejiang University of Technology, Hangzhou; 310032, China;
2.School of Chemistry and Chemical Engineering, The Queen’s University of Belfast, Belfast; BT9 5AG, United Kingdom;
3.School of Physical Science and Technology, ShanghaiTech University, Shanghai; 201210, China;
4.Institute of Science and Technology Austria, Klosterneuburg; 3400, Austria
通讯作者单位物质科学与技术学院
推荐引用方式
GB/T 7714
Zhao, Jinyan,Yao, Zihao,Bunting, Rhys J.,et al. Microkinetic Modeling with Size-Dependent and Adsorbate-Adsorbate Interactions for the Direct Synthesis of H2O2 over Pd Nanoparticles[J]. ACS CATALYSIS,2023,13(22):15054-15073.
APA Zhao, Jinyan,Yao, Zihao,Bunting, Rhys J.,Hu, P.,&Wang, Jianguo.(2023).Microkinetic Modeling with Size-Dependent and Adsorbate-Adsorbate Interactions for the Direct Synthesis of H2O2 over Pd Nanoparticles.ACS CATALYSIS,13(22),15054-15073.
MLA Zhao, Jinyan,et al."Microkinetic Modeling with Size-Dependent and Adsorbate-Adsorbate Interactions for the Direct Synthesis of H2O2 over Pd Nanoparticles".ACS CATALYSIS 13.22(2023):15054-15073.
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