Microstructures and reaction kinetics of catalysts

DUAN Xuezhi; CHEN Wenyao; ZHOU Xinggui; YUAN Weikang

doi:10.11949/0438-1157.20190850

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Microstructures and reaction kinetics of catalysts

Reviews and monographs | 更新时间：2026-07-24

- Microstructures and reaction kinetics of catalysts
- CIESC Journal Vol. 70, Issue 10, Pages: 3645-3650(2019)
- 作者机构：
  
  华东理工大学化学工程联合国家重点实验室，上海 200237
- 作者简介：
- 基金信息：
- DOI：10.11949/0438-1157.20190850
  CLC： TQ 138.2
- Received：24 July 2019，
  
  Revised：2019-08-13，
  
  Online First：24 July 2026，
  
  Published：05 October 2019
- 稿件说明：
移动端阅览
段学志, 陈文尧, 周兴贵, 袁渭康. 催化剂微尺度结构与反应动力学[J]. 化工学报, 2019, 70(10): 3645-3650

DUAN Xuezhi, CHEN Wenyao, ZHOU Xinggui, YUAN Weikang. Microstructures and reaction kinetics of catalysts[J]. CIESC Journal, 2019, 70(10): 3645-3650
段学志, 陈文尧, 周兴贵, 袁渭康. 催化剂微尺度结构与反应动力学[J]. 化工学报, 2019, 70(10): 3645-3650 DOI： 10.11949/0438-1157.20190850.

DUAN Xuezhi, CHEN Wenyao, ZHOU Xinggui, YUAN Weikang. Microstructures and reaction kinetics of catalysts[J]. CIESC Journal, 2019, 70(10): 3645-3650 DOI： 10.11949/0438-1157.20190850.

摘要

传统催化反应动力学研究主要关注宏观变量与性质（如温度和浓度敏感性），能用于指导工业反应器的优化设计，但极少关注催化剂微尺度结构与性质的影响，因而不能用于指导催化剂的优化设计。重点介绍了近年来发展的催化反应速率解析的方法，归纳总结了基于动力学分析的催化剂活性位的辨认方法，探讨了易实验测量的活化熵作为催化剂活性描述符的可能性，并阐明了炭载体表面化学性质对负载金属电子结构和催化性能的调变规律，将动力学分析方法的应用从反应器设计拓展到催化剂设计。

Abstract

Traditional catalytic reaction kinetics studies focus on macroscopic variables and properties (such as temperature and concentration sensitivity) and can be used to guide the optimal design of industrial reactors

but pay little attention to the effects of catalyst microscale structures and properties. It cannot therefore be used to guide the optimal design of the catalyst. This review mainly discusses the development and application of multifaceted kinetics analysis method

which can discriminate the dominant active sites of supported metal catalysts

and the possibility to use the activation entropy (Δ

) as an experimentally measurable descriptor of catalytic reaction rate

which can be fine-tuned by tailoring the electronic properties of supported metal nanoparticles in terms of the surface chemistry and properties of carbon supports. It can extend the application of the kinetics analysis from the reactor design to the catalyst design.

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references

Chorkendorff I , Niemantsverdriet J W . Concepts of Modern Catalysis and Kinetics [M ] . 3rd ed . Hoboken: Wiley-VCH , 2017 .

Mizuno N , Misono M . Heterogeneous catalysis [J ] . Chemical Reviews , 1998 , 98 ( 1 ): 199 - 218 .

Bell A T . The impact of nanoscience on heterogeneous catalysis [J ] . Science , 2003 , 299 ( 5613 ): 1688 - 1691 .

Levenspiel O . Chemical reaction engineering [J ] . Industrial & Engineering Chemistry Research , 1999 , 38 ( 11 ): 4140 - 4143 .

Kreutzer M T , Kapteijn F , Moulijn J A , et al . Multiphase monolith reactors: chemical reaction engineering of segmented flow in microchannels [J ] . Chemical Engineering Science , 2005 , 60 ( 22 ): 5895 - 5916 .

Aris R . On stability criteria of chemical reaction engineering [J ] . Chemical Engineering Science , 1969 , 24 ( 1 ): 149 - 169 .

Lerou J J , Ng K M . Chemical reaction engineering: a multiscale approach to a multiobjective task [J ] . Chemical Engineering Science , 1996 , 51 ( 10 ): 1595 - 1614 .

Mao Y , Wang H F , Hu P . Theory and applications of surface micro-kinetics in the rational design of catalysts using density functional theory calculations [J ] . Wiley Interdisciplinary Reviews: Computational Molecular Science , 2017 , 7 ( 6 ): e1321 .

Motagamwala A H , Ball M R , Dumesic J A . Microkinetic analysis and scaling relations for catalyst design [J ] . Annual Review of Chemical and Biomolecular Engineering , 2018 , 9 : 413 - 450 .

Nørskov J K , Bligaard T , Rossmeisl J , et al . Towards the computational design of solid catalysts [J ] . Nature Chemistry , 2009 , 1 ( 1 ): 37 - 46 .

Chin Y H , Buda C , Neurock M , et al . Reactivity of chemisorbed oxygen atoms and their catalytic consequences during CH 4 -O 2 catalysis on supported Pt clusters [J ] . Journal of the American Chemical Society , 2011 , 133 ( 40 ): 15958 - 15978 .

Kulkarni A , Siahrostami S , Patel A , et al . Understanding catalytic activity trends in the oxygen reduction reaction [J ] . Chemical Reviews , 2018 , 118 ( 5 ): 2302 - 2312 .

Boudart M . From the century of the rate equation to the century of the rate constants: a revolution in catalytic kinetics and assisted catalyst design [J ] . Catalysis Letters , 2000 , 65 ( 1 / 2 / 3 ): 1 - 3 .

Chen W , Ji J , Feng X , et al . Mechanistic insight into size-dependent activity and durability in Pt/CNT catalyzed hydrolytic dehydrogenation of ammonia borane [J ] . Journal of the American Chemical Society , 2014 , 136 ( 48 ): 16736 - 16739 .

Lim B , Jiang M , Camargo P H , et al . Pd-Pt bimetallic nanodendrites with high activity for oxygen reduction [J ] . Science , 2009 , 324 ( 5932 ): 1302 - 1305 .

Wang C , Daimon H , Onodera T , et al . A general approach to the size-and shape-controlled synthesis of platinum nanoparticles and their catalytic reduction of oxygen [J ] . Angewandte Chemie International Edition , 2008 , 47 ( 19 ): 3588 - 3591 .

van Hardeveld R , Hartog F . The statistics of surface atoms and surface sites on metal crystals [J ] . Surface Science , 1969 , 15 ( 2 ): 189 - 230 .

Yan H , Lin Y , Wu H , et al . Bottom-up precise synthesis of stable platinum dimers on graphene [J ] . Nature Communications , 2017 , 8 ( 1 ): 1070 .

Chen W , Li D , Wang Z , et al . Reaction mechanism and kinetics for hydrolytic dehydrogenation of ammonia borane on a Pt/CNT catalyst [J ] . AIChE Journal , 2017 , 63 ( 1 ): 60 - 65 .

Fu W , Chen W , Qian G , et al . Kinetics-assisted discrimination of active sites in Ru catalyzed hydrolytic dehydrogenation of ammonia borane [J ] . Reaction Chemistry & Engineering , 2019 , 4 ( 2 ): 316 - 322 .

Feng X , Duan X , Qian G , et al . Insights into size-dependent activity and active sites of Au nanoparticles supported on TS-1 for propene epoxidation with H 2 and O 2 [J ] . Journal of Catalysis , 2014 , 317 : 99 - 104 .

Cao Y , Fu W , Sui Z , et al . Kinetics insights and active sites discrimination of Pd-catalyzed selective hydrogenation of acetylene [J ] . Industrial & Engineering Chemistry Research , 2019 , 58 ( 5 ): 1888 - 1895 .

Pan M J , Wang J N , Fu W Z , et al . Active sites of Pt/CNTs nanocatalysts for aerobic base-free oxidation of glycerol [J ] . Green Energy & Environment , https://doi.ogr/10.1016/j.gee. 2019.08.001 https://doi.ogr/10.1016/j.gee. 2019.08.001 .

Qu J , Cao Y , Duan X , et al . Eye-readable detection and oxidation of CO with Pt-based catalyst and binuclear rhodium complexes [J ] . Angewandte Chemie , 2019 , 58 ( 35 ): 12258 - 12263 .

Dong C , Lian C , Hu S , et al . Size-dependent activity and selectivity of carbon dioxide photocatalytic reduction over platinum nanoparticles [J ] . Nature Communications , 2018 , 9 ( 1 ): 1252 .

Wang Y , Tao Z , Wu B , et al . Shape-controlled synthesis of Pt particles and their catalytic performances in the n -hexadecane hydroconversion [J ] . Catalysis Today , 2016 , 259 : 331 - 339 .

Chen A , Chen P , Cao D , et al . Aqueous-phase reforming of the low-boiling fraction of bio-oil for hydrogen production: the size effect of Pt/Al 2 O 3 [J ] . International Journal of Hydrogen Energy , 2015 , 40 ( 43 ): 14798 - 14805 .

Chen W , Li D , Peng C , et al . Mechanistic and kinetic insights into the Pt-Ru synergy during hydrogen generation from ammonia borane over PtRu/CNT nanocatalysts [J ] . Journal of Catalysis , 2017 , 356 : 186 - 196 .

Zhu X , Guo Q , Sun Y , et al . Optimising surface d charge of AuPd nanoalloy catalysts for enhanced catalytic activity [J ] . Nature Communications , 2019 , 10 ( 1 ): 1428 .

Guo Z , Chen Y , Li L , et al . Carbon nanotube-supported Pt-based bimetallic catalysts prepared by a microwave-assisted polyol reduction method and their catalytic applications in the selective hydrogenation [J ] . Journal of Catalysis , 2010 , 276 ( 2 ): 314 - 326 .

Wang X , Li N , Webb J A , et al . Effect of surface oxygen containing groups on the catalytic activity of multi-walled carbon nanotube supported Pt catalyst [J ] . Applied Catalysis B: Environmental , 2010 , 101 ( 1 / 2 ): 21 - 30 .

Chen W , Ji J , Duan X , et al . Unique reactivity in Pt/CNT catalyzed hydrolytic dehydrogenation of ammonia borane [J ] . Chemical Communications , 2014 , 50 ( 17 ): 2142 - 2144 .

Han C , Duan X , Zhang M , et al . Role of electronic properties in partition of radical and nonradical processes of carbocatalysis toward peroxymonosulfate activation [J ] . Carbon , 2019 , 153 : 73 - 80 .

Chen W , Duan X , Qian G , et al . Carbon nanotubes as support in the platinum-catalyzed hydrolytic dehydrogenation of ammonia borane [J ] . ChemSusChem , 2015 , 8 ( 17 ): 2927 - 2931 .

Chen W , Wang Z , Duan X , et al . Structural and kinetic insights into Pt/CNT catalysts during hydrogen generation from ammonia borane [J ] . Chemical Engineering Science , 2018 , 192 : 1242 - 1251 .

Fu W , Han C , Li D , et al . Polyoxometalates-engineered hydrogen generation rate and durability of Pt/CNT catalysts from ammonia borane [J ] . Journal of Energy Chemistry , 2020 , 41 : 142 - 148 .

Zhang J , Chen W , Ge H , et al . Synergistic effects in atomic-layer-deposited PtCox/CNTs catalysts enhancing hydrolytic dehydrogenation of ammonia borane [J ] . Applied Catalysis B: Environmental , 2018 , 235 : 256 - 263 .

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