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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]) |
ISSN | 2155-5435 |
EISSN | 2155-5435 |
卷号 | 13期号:22页码:15054-15073 |
发表状态 | 已发表 |
DOI | 10.1021/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) |
引用统计 | 正在获取...
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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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