{"title":"含四个氢原子的碳氢化合物与缩合相的相互作用:H/D交换机制的分类及机制选择算法","authors":"Dmitriy M. Zakharov , Maxim V. Ananyev","doi":"10.1016/j.jcat.2025.116173","DOIUrl":null,"url":null,"abstract":"<div><div>The paper focuses on an analysis of the mechanisms of hydrogen interaction between gases containing 4 hydrogen atoms and a condensed phase in terms of H/D exchange. Based on the theory of five types of exchange, different cases of mechanisms are analysed according to the accepted values of probabilities of hydrogen isotope exchange between the gas and condensed phases. The analyses made it possible to classify the mechanisms into 3 groups: one-step, two-step, and multistep. Two-step and multistep groups contain two subgroups each. The paper shows that all groups of mechanisms are distinguishable experimentally. An algorithm for selecting the exchange mechanism is proposed. The implementation of the proposed algorithm is shown on a number of experimental data known in the literature. Hydrogen exchange mechanisms have been revised for the following systems: CH<sub>4</sub>-H<sub>2</sub>SO<sub>4</sub>, CH<sub>4</sub>-H<sub>2</sub>-Ni and CH<sub>4</sub>-H<sub>2</sub>-Pt-Rh.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"448 ","pages":"Article 116173"},"PeriodicalIF":6.5000,"publicationDate":"2025-04-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Interaction of hydrocarbons containing four hydrogen atoms with condensed phases: Classification of H/D exchange mechanisms and mechanism selection algorithm\",\"authors\":\"Dmitriy M. Zakharov , Maxim V. Ananyev\",\"doi\":\"10.1016/j.jcat.2025.116173\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>The paper focuses on an analysis of the mechanisms of hydrogen interaction between gases containing 4 hydrogen atoms and a condensed phase in terms of H/D exchange. Based on the theory of five types of exchange, different cases of mechanisms are analysed according to the accepted values of probabilities of hydrogen isotope exchange between the gas and condensed phases. The analyses made it possible to classify the mechanisms into 3 groups: one-step, two-step, and multistep. Two-step and multistep groups contain two subgroups each. The paper shows that all groups of mechanisms are distinguishable experimentally. An algorithm for selecting the exchange mechanism is proposed. The implementation of the proposed algorithm is shown on a number of experimental data known in the literature. Hydrogen exchange mechanisms have been revised for the following systems: CH<sub>4</sub>-H<sub>2</sub>SO<sub>4</sub>, CH<sub>4</sub>-H<sub>2</sub>-Ni and CH<sub>4</sub>-H<sub>2</sub>-Pt-Rh.</div></div>\",\"PeriodicalId\":346,\"journal\":{\"name\":\"Journal of Catalysis\",\"volume\":\"448 \",\"pages\":\"Article 116173\"},\"PeriodicalIF\":6.5000,\"publicationDate\":\"2025-04-28\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of Catalysis\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0021951725002386\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Catalysis","FirstCategoryId":"92","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0021951725002386","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Interaction of hydrocarbons containing four hydrogen atoms with condensed phases: Classification of H/D exchange mechanisms and mechanism selection algorithm
The paper focuses on an analysis of the mechanisms of hydrogen interaction between gases containing 4 hydrogen atoms and a condensed phase in terms of H/D exchange. Based on the theory of five types of exchange, different cases of mechanisms are analysed according to the accepted values of probabilities of hydrogen isotope exchange between the gas and condensed phases. The analyses made it possible to classify the mechanisms into 3 groups: one-step, two-step, and multistep. Two-step and multistep groups contain two subgroups each. The paper shows that all groups of mechanisms are distinguishable experimentally. An algorithm for selecting the exchange mechanism is proposed. The implementation of the proposed algorithm is shown on a number of experimental data known in the literature. Hydrogen exchange mechanisms have been revised for the following systems: CH4-H2SO4, CH4-H2-Ni and CH4-H2-Pt-Rh.
期刊介绍:
The Journal of Catalysis publishes scholarly articles on both heterogeneous and homogeneous catalysis, covering a wide range of chemical transformations. These include various types of catalysis, such as those mediated by photons, plasmons, and electrons. The focus of the studies is to understand the relationship between catalytic function and the underlying chemical properties of surfaces and metal complexes.
The articles in the journal offer innovative concepts and explore the synthesis and kinetics of inorganic solids and homogeneous complexes. Furthermore, they discuss spectroscopic techniques for characterizing catalysts, investigate the interaction of probes and reacting species with catalysts, and employ theoretical methods.
The research presented in the journal should have direct relevance to the field of catalytic processes, addressing either fundamental aspects or applications of catalysis.