{"title":"甲醇和水低温制氢过程中的铂电子调控","authors":"Qiankang Liao, You Wang, Chen Chen, Sai Zhang","doi":"10.1021/acssuschemeng.4c07671","DOIUrl":null,"url":null,"abstract":"The aqueous-phase reforming of the methanol (APRM) reaction provides a potential approach for hydrogen (H<sub>2</sub>) storage and transportation. However, the limited capacity of Pt nanocatalysts for H<sub>2</sub>O activation leads to the drawback of requiring high reaction temperatures (>200 °C) to achieve efficient H<sub>2</sub> generation through the APRM reaction. Herein, the electronic density of Pt nanocatalysts has been regulated by the phase of the Al<sub>2</sub>O<sub>3</sub> supports. Mechanism analysis revealed that the α-Al<sub>2</sub>O<sub>3</sub> supports with larger lattice fringe spacing resulted in an enhanced electronic density of Pt nanocatalysts, thereby enabling the effective adsorption and activation of H<sub>2</sub>O. Consequently, the Pt/α-Al<sub>2</sub>O<sub>3</sub> catalysts exhibited a TOF value of 69.8 h<sup>–1</sup> at 30 °C for H<sub>2</sub> generation via APRM reaction. Notably, this H<sub>2</sub> generation rate even suppressed that achieved by previous state-of-the-art homogeneous catalysts. This finding presents a promising avenue toward flexible hydrogen utilization.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"26 1","pages":""},"PeriodicalIF":7.1000,"publicationDate":"2024-12-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Electronic Regulation of Pt for Low-Temperature Hydrogen Generation from Methanol and Water\",\"authors\":\"Qiankang Liao, You Wang, Chen Chen, Sai Zhang\",\"doi\":\"10.1021/acssuschemeng.4c07671\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"The aqueous-phase reforming of the methanol (APRM) reaction provides a potential approach for hydrogen (H<sub>2</sub>) storage and transportation. However, the limited capacity of Pt nanocatalysts for H<sub>2</sub>O activation leads to the drawback of requiring high reaction temperatures (>200 °C) to achieve efficient H<sub>2</sub> generation through the APRM reaction. Herein, the electronic density of Pt nanocatalysts has been regulated by the phase of the Al<sub>2</sub>O<sub>3</sub> supports. Mechanism analysis revealed that the α-Al<sub>2</sub>O<sub>3</sub> supports with larger lattice fringe spacing resulted in an enhanced electronic density of Pt nanocatalysts, thereby enabling the effective adsorption and activation of H<sub>2</sub>O. Consequently, the Pt/α-Al<sub>2</sub>O<sub>3</sub> catalysts exhibited a TOF value of 69.8 h<sup>–1</sup> at 30 °C for H<sub>2</sub> generation via APRM reaction. Notably, this H<sub>2</sub> generation rate even suppressed that achieved by previous state-of-the-art homogeneous catalysts. This finding presents a promising avenue toward flexible hydrogen utilization.\",\"PeriodicalId\":25,\"journal\":{\"name\":\"ACS Sustainable Chemistry & Engineering\",\"volume\":\"26 1\",\"pages\":\"\"},\"PeriodicalIF\":7.1000,\"publicationDate\":\"2024-12-16\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"ACS Sustainable Chemistry & Engineering\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://doi.org/10.1021/acssuschemeng.4c07671\",\"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":"ACS Sustainable Chemistry & Engineering","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1021/acssuschemeng.4c07671","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
Electronic Regulation of Pt for Low-Temperature Hydrogen Generation from Methanol and Water
The aqueous-phase reforming of the methanol (APRM) reaction provides a potential approach for hydrogen (H2) storage and transportation. However, the limited capacity of Pt nanocatalysts for H2O activation leads to the drawback of requiring high reaction temperatures (>200 °C) to achieve efficient H2 generation through the APRM reaction. Herein, the electronic density of Pt nanocatalysts has been regulated by the phase of the Al2O3 supports. Mechanism analysis revealed that the α-Al2O3 supports with larger lattice fringe spacing resulted in an enhanced electronic density of Pt nanocatalysts, thereby enabling the effective adsorption and activation of H2O. Consequently, the Pt/α-Al2O3 catalysts exhibited a TOF value of 69.8 h–1 at 30 °C for H2 generation via APRM reaction. Notably, this H2 generation rate even suppressed that achieved by previous state-of-the-art homogeneous catalysts. This finding presents a promising avenue toward flexible hydrogen utilization.
期刊介绍:
ACS Sustainable Chemistry & Engineering is a prestigious weekly peer-reviewed scientific journal published by the American Chemical Society. Dedicated to advancing the principles of green chemistry and green engineering, it covers a wide array of research topics including green chemistry, green engineering, biomass, alternative energy, and life cycle assessment.
The journal welcomes submissions in various formats, including Letters, Articles, Features, and Perspectives (Reviews), that address the challenges of sustainability in the chemical enterprise and contribute to the advancement of sustainable practices. Join us in shaping the future of sustainable chemistry and engineering.