{"title":"可持续合成气转化过程中纳米催化剂中Mn价态的测定","authors":"Zhiping Li, Duohua Liao, Guo Tian*, Xiaoyu Fan, Xu Chai, Wenxi Chang, Yuan Gao, Bo Yuan, Zonglong Li, Fei Wei and Chenxi Zhang*, ","doi":"10.1021/jacs.5c06550","DOIUrl":null,"url":null,"abstract":"<p >Constructing structure–activity relationships (SAR) between nanocatalysts under reactive atmospheres makes them indispensable for chemical synthesis, energy transformation, and environmental remediation. However, this structure sensitivity remains ambiguous for metals/metal oxides due to dynamic changes in metal valences under a reductive atmosphere. Herein, this study delves into the complexities of Mn-based nanocatalysts, focusing on the impact of the Mn valence state in a test reaction converting sustainable syngas to aromatics-a process highly sensitive to the catalyst’s redox environment and active site characteristics. We conducted a thorough SAR analysis and discovered a direct correlation between the Sabatier effect, CO adsorption, and the space-time yields of aromatics. Notably, Mn in the +2-oxidation state emerged as the optimal valence for achieving the highest catalytic performance, with a maximum yield of 1.6 mmol·h<sup>–1</sup>·g<sub>cat</sub><sup>–1</sup>. Our findings provide critical insights into the role of the catalyst’s intrinsic properties in dictating the selectivity and efficiency of CO hydrogenation for the rational design of nanocatalysts that can sustainably transform small molecules into valuable chemicals and fuels.</p>","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":"147 36","pages":"32548–32559"},"PeriodicalIF":15.6000,"publicationDate":"2025-08-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Determination of Mn Valence States in Nanocatalysts During Sustainable Syngas Conversion\",\"authors\":\"Zhiping Li, Duohua Liao, Guo Tian*, Xiaoyu Fan, Xu Chai, Wenxi Chang, Yuan Gao, Bo Yuan, Zonglong Li, Fei Wei and Chenxi Zhang*, \",\"doi\":\"10.1021/jacs.5c06550\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >Constructing structure–activity relationships (SAR) between nanocatalysts under reactive atmospheres makes them indispensable for chemical synthesis, energy transformation, and environmental remediation. However, this structure sensitivity remains ambiguous for metals/metal oxides due to dynamic changes in metal valences under a reductive atmosphere. Herein, this study delves into the complexities of Mn-based nanocatalysts, focusing on the impact of the Mn valence state in a test reaction converting sustainable syngas to aromatics-a process highly sensitive to the catalyst’s redox environment and active site characteristics. We conducted a thorough SAR analysis and discovered a direct correlation between the Sabatier effect, CO adsorption, and the space-time yields of aromatics. Notably, Mn in the +2-oxidation state emerged as the optimal valence for achieving the highest catalytic performance, with a maximum yield of 1.6 mmol·h<sup>–1</sup>·g<sub>cat</sub><sup>–1</sup>. Our findings provide critical insights into the role of the catalyst’s intrinsic properties in dictating the selectivity and efficiency of CO hydrogenation for the rational design of nanocatalysts that can sustainably transform small molecules into valuable chemicals and fuels.</p>\",\"PeriodicalId\":49,\"journal\":{\"name\":\"Journal of the American Chemical Society\",\"volume\":\"147 36\",\"pages\":\"32548–32559\"},\"PeriodicalIF\":15.6000,\"publicationDate\":\"2025-08-02\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of the American Chemical Society\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://pubs.acs.org/doi/10.1021/jacs.5c06550\",\"RegionNum\":1,\"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":"Journal of the American Chemical Society","FirstCategoryId":"92","ListUrlMain":"https://pubs.acs.org/doi/10.1021/jacs.5c06550","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
Determination of Mn Valence States in Nanocatalysts During Sustainable Syngas Conversion
Constructing structure–activity relationships (SAR) between nanocatalysts under reactive atmospheres makes them indispensable for chemical synthesis, energy transformation, and environmental remediation. However, this structure sensitivity remains ambiguous for metals/metal oxides due to dynamic changes in metal valences under a reductive atmosphere. Herein, this study delves into the complexities of Mn-based nanocatalysts, focusing on the impact of the Mn valence state in a test reaction converting sustainable syngas to aromatics-a process highly sensitive to the catalyst’s redox environment and active site characteristics. We conducted a thorough SAR analysis and discovered a direct correlation between the Sabatier effect, CO adsorption, and the space-time yields of aromatics. Notably, Mn in the +2-oxidation state emerged as the optimal valence for achieving the highest catalytic performance, with a maximum yield of 1.6 mmol·h–1·gcat–1. Our findings provide critical insights into the role of the catalyst’s intrinsic properties in dictating the selectivity and efficiency of CO hydrogenation for the rational design of nanocatalysts that can sustainably transform small molecules into valuable chemicals and fuels.
期刊介绍:
The flagship journal of the American Chemical Society, known as the Journal of the American Chemical Society (JACS), has been a prestigious publication since its establishment in 1879. It holds a preeminent position in the field of chemistry and related interdisciplinary sciences. JACS is committed to disseminating cutting-edge research papers, covering a wide range of topics, and encompasses approximately 19,000 pages of Articles, Communications, and Perspectives annually. With a weekly publication frequency, JACS plays a vital role in advancing the field of chemistry by providing essential research.