Shaoxiong Liu, Yu Wang, Kyein Far Lyu, Xiaocheng Lan, Tiefeng Wang
{"title":"A one-pot strategy for anchoring single Pt atoms in MOFs with diverse coordination environments","authors":"Shaoxiong Liu, Yu Wang, Kyein Far Lyu, Xiaocheng Lan, Tiefeng Wang","doi":"10.1038/s44160-024-00585-7","DOIUrl":null,"url":null,"abstract":"It is challenging to precisely control and identify the coordination environment of single-atom active sites due to non-uniform substrate surfaces. This complicates the task of bridging experimental and theoretical investigations. Here, using a one-pot method, we immobilized single Pt(0) atoms within various terephthalic acid-based metal–organic frameworks, thereby constructing well-defined active sites with varied organic coordination environments. In the isoreticular metal–organic framework UiO-6–X (–X = –H, –NH2, –Br and –I), influenced by the functional groups, the resulting Pt1 sites exhibited distinct catalytic activities for hydrogenation and sintering resistance. Mechanistic studies reveal that this is related to alteration of the electronic state of Pt centres and the adsorption behaviour of intermediates on the Pt sites. Pt1@UiO-66–Br gave the highest activity and excellent thermal stability, with no metal agglomeration in H2 up to 300 °C. Our work introduces a strategy for the precise environmental modification of isolated metal atoms for better catalytic performance. Preventing the co-existence of single-atom active sites with differing coordination environments is challenging. Here the coordination environment of single Pt(0) atoms is precisely controlled within terephthalic acid-based metal–organic frameworks, resulting in distinct catalytic activities and sintering resistance.","PeriodicalId":74251,"journal":{"name":"Nature synthesis","volume":null,"pages":null},"PeriodicalIF":0.0000,"publicationDate":"2024-06-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Nature synthesis","FirstCategoryId":"1085","ListUrlMain":"https://www.nature.com/articles/s44160-024-00585-7","RegionNum":0,"RegionCategory":null,"ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"0","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 0
Abstract
It is challenging to precisely control and identify the coordination environment of single-atom active sites due to non-uniform substrate surfaces. This complicates the task of bridging experimental and theoretical investigations. Here, using a one-pot method, we immobilized single Pt(0) atoms within various terephthalic acid-based metal–organic frameworks, thereby constructing well-defined active sites with varied organic coordination environments. In the isoreticular metal–organic framework UiO-6–X (–X = –H, –NH2, –Br and –I), influenced by the functional groups, the resulting Pt1 sites exhibited distinct catalytic activities for hydrogenation and sintering resistance. Mechanistic studies reveal that this is related to alteration of the electronic state of Pt centres and the adsorption behaviour of intermediates on the Pt sites. Pt1@UiO-66–Br gave the highest activity and excellent thermal stability, with no metal agglomeration in H2 up to 300 °C. Our work introduces a strategy for the precise environmental modification of isolated metal atoms for better catalytic performance. Preventing the co-existence of single-atom active sites with differing coordination environments is challenging. Here the coordination environment of single Pt(0) atoms is precisely controlled within terephthalic acid-based metal–organic frameworks, resulting in distinct catalytic activities and sintering resistance.