{"title":"揭示克里基中间体 CH2OO 与二氧化硫反应的新途径。","authors":"Cangtao Yin, Gábor Czakó","doi":"10.1038/s42004-024-01237-9","DOIUrl":null,"url":null,"abstract":"Criegee intermediates play an important role in the tropospheric oxidation models through their reactions with atmospheric trace chemicals. We develop a global full-dimensional potential energy surface for the CH2OO + SO2 system and reveal how the reaction happens step by step by quasi-classical trajectory simulations. A new pathway forming the main products (CH2O + SO3) and a new product channel (CO2 + H2 + SO2) are predicted in our simulations. The new pathway appears at collision energies greater than 10 kcal/mol whose behavior demonstrates a typical barrier-controlled reaction. This threshold is also consistent with the ab initio transition state barrier height. For the minor products, a loose complex OCH2O ∙ ∙ ∙ SO2 is formed first, and then in most cases it soon turns into HCOOH + SO2, in a few cases it decomposes into CO2 + H2 + SO2 which is a new product channel, and rarely it remains as ∙OCH2O ∙ + SO2. Criegee intermediates such as CH2OO play an important role in tropospheric oxidation models through their reactions with atmospheric trace chemicals. Here, the authors develop a global full-dimensional potential energy surface for the CH2OO + SO2 system, reveal how the reaction happens step by step using quasi-classical trajectory simulations, to show a new direct stripping pathway forming the main products CH2O and SO3 and a new product channel.","PeriodicalId":10529,"journal":{"name":"Communications Chemistry","volume":null,"pages":null},"PeriodicalIF":5.9000,"publicationDate":"2024-07-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11246420/pdf/","citationCount":"0","resultStr":"{\"title\":\"Revealing new pathways for the reaction of Criegee intermediate CH2OO with SO2\",\"authors\":\"Cangtao Yin, Gábor Czakó\",\"doi\":\"10.1038/s42004-024-01237-9\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Criegee intermediates play an important role in the tropospheric oxidation models through their reactions with atmospheric trace chemicals. We develop a global full-dimensional potential energy surface for the CH2OO + SO2 system and reveal how the reaction happens step by step by quasi-classical trajectory simulations. A new pathway forming the main products (CH2O + SO3) and a new product channel (CO2 + H2 + SO2) are predicted in our simulations. The new pathway appears at collision energies greater than 10 kcal/mol whose behavior demonstrates a typical barrier-controlled reaction. This threshold is also consistent with the ab initio transition state barrier height. For the minor products, a loose complex OCH2O ∙ ∙ ∙ SO2 is formed first, and then in most cases it soon turns into HCOOH + SO2, in a few cases it decomposes into CO2 + H2 + SO2 which is a new product channel, and rarely it remains as ∙OCH2O ∙ + SO2. Criegee intermediates such as CH2OO play an important role in tropospheric oxidation models through their reactions with atmospheric trace chemicals. Here, the authors develop a global full-dimensional potential energy surface for the CH2OO + SO2 system, reveal how the reaction happens step by step using quasi-classical trajectory simulations, to show a new direct stripping pathway forming the main products CH2O and SO3 and a new product channel.\",\"PeriodicalId\":10529,\"journal\":{\"name\":\"Communications Chemistry\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":5.9000,\"publicationDate\":\"2024-07-13\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11246420/pdf/\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Communications Chemistry\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://www.nature.com/articles/s42004-024-01237-9\",\"RegionNum\":2,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Communications Chemistry","FirstCategoryId":"92","ListUrlMain":"https://www.nature.com/articles/s42004-024-01237-9","RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
Revealing new pathways for the reaction of Criegee intermediate CH2OO with SO2
Criegee intermediates play an important role in the tropospheric oxidation models through their reactions with atmospheric trace chemicals. We develop a global full-dimensional potential energy surface for the CH2OO + SO2 system and reveal how the reaction happens step by step by quasi-classical trajectory simulations. A new pathway forming the main products (CH2O + SO3) and a new product channel (CO2 + H2 + SO2) are predicted in our simulations. The new pathway appears at collision energies greater than 10 kcal/mol whose behavior demonstrates a typical barrier-controlled reaction. This threshold is also consistent with the ab initio transition state barrier height. For the minor products, a loose complex OCH2O ∙ ∙ ∙ SO2 is formed first, and then in most cases it soon turns into HCOOH + SO2, in a few cases it decomposes into CO2 + H2 + SO2 which is a new product channel, and rarely it remains as ∙OCH2O ∙ + SO2. Criegee intermediates such as CH2OO play an important role in tropospheric oxidation models through their reactions with atmospheric trace chemicals. Here, the authors develop a global full-dimensional potential energy surface for the CH2OO + SO2 system, reveal how the reaction happens step by step using quasi-classical trajectory simulations, to show a new direct stripping pathway forming the main products CH2O and SO3 and a new product channel.
期刊介绍:
Communications Chemistry is an open access journal from Nature Research publishing high-quality research, reviews and commentary in all areas of the chemical sciences. Research papers published by the journal represent significant advances bringing new chemical insight to a specialized area of research. We also aim to provide a community forum for issues of importance to all chemists, regardless of sub-discipline.