{"title":"2D Pt Metals at Rectifying Interface with Pronounced Negative Charge Density for Electrocatalytic Reduction Reactions","authors":"Peng Gao, Zhouhong Ren, Qi-Yuan Li, Shi-Nan Zhang, Qian-Yu Liu, Jing-Wen Li, Wei-Yao Hu, Panzhe Qiao, Dong Xu, Si-Yuan Xia, Xi Liu*, Jie-Sheng Chen and Xin-Hao Li*, ","doi":"10.1021/acs.chemmater.4c01226","DOIUrl":null,"url":null,"abstract":"<p >Noble metals often exhibit excellent catalytic activity when downsized into two-dimensional (2D) metals owing to their high atomic utilization and unique electronic properties. However, the controllable formation of 2D metals/support composites with clean interfaces/surfaces for practical applications still remains a synthetic bottleneck, with rather limited cases of 2D metals prepared through metal–support bonds. Herein, we developed a built-in electronic interface-guided method for in situ reduction of preadsorbed Pt atoms into 2D Pt metals along the surface of 2D nitrogen-doped carbon (NC) support through the electronic interaction at nonbonded metal–support interface. The interfacial electron exchange, driven by the difference in work functions between 2D Pt metals and NC support, enables the controllable synthesis of 2D Pt-based Schottky heterojunctions with clean interfaces/surfaces and a mean Pt thickness of 1.3 nm. Both experimental and theoretical results confirm the enhanced electron exchange at the interface between 2D Pt and the 2D NC support, resulting in a doubled electron density for 2D Pt. Consequently, the electron-rich 2D Pt metals exhibit remarkable mass activity of 67.3 A mg<sub>Pt</sub><sup>–1</sup> for the hydrogen evolution reaction (HER) and a turnover frequency (TOF) value of 117 h<sup>–1</sup> in the electrocatalytic hydrogenation of phenol, notably outperforming those of the commercial Pt/C catalyst by a factor of 16.8 and 4.0, respectively. Our efficient built-in electronic interface-guided method not only facilitates the synthesis of novel 2D metal/2D support Schottky heterojunctions but also lays the groundwork for designing more powerful electronic interface catalysts with enhanced and diversified functionalities.</p>","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":null,"pages":null},"PeriodicalIF":7.2000,"publicationDate":"2024-06-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Chemistry of Materials","FirstCategoryId":"88","ListUrlMain":"https://pubs.acs.org/doi/10.1021/acs.chemmater.4c01226","RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
引用次数: 0
Abstract
Noble metals often exhibit excellent catalytic activity when downsized into two-dimensional (2D) metals owing to their high atomic utilization and unique electronic properties. However, the controllable formation of 2D metals/support composites with clean interfaces/surfaces for practical applications still remains a synthetic bottleneck, with rather limited cases of 2D metals prepared through metal–support bonds. Herein, we developed a built-in electronic interface-guided method for in situ reduction of preadsorbed Pt atoms into 2D Pt metals along the surface of 2D nitrogen-doped carbon (NC) support through the electronic interaction at nonbonded metal–support interface. The interfacial electron exchange, driven by the difference in work functions between 2D Pt metals and NC support, enables the controllable synthesis of 2D Pt-based Schottky heterojunctions with clean interfaces/surfaces and a mean Pt thickness of 1.3 nm. Both experimental and theoretical results confirm the enhanced electron exchange at the interface between 2D Pt and the 2D NC support, resulting in a doubled electron density for 2D Pt. Consequently, the electron-rich 2D Pt metals exhibit remarkable mass activity of 67.3 A mgPt–1 for the hydrogen evolution reaction (HER) and a turnover frequency (TOF) value of 117 h–1 in the electrocatalytic hydrogenation of phenol, notably outperforming those of the commercial Pt/C catalyst by a factor of 16.8 and 4.0, respectively. Our efficient built-in electronic interface-guided method not only facilitates the synthesis of novel 2D metal/2D support Schottky heterojunctions but also lays the groundwork for designing more powerful electronic interface catalysts with enhanced and diversified functionalities.
期刊介绍:
The journal Chemistry of Materials focuses on publishing original research at the intersection of materials science and chemistry. The studies published in the journal involve chemistry as a prominent component and explore topics such as the design, synthesis, characterization, processing, understanding, and application of functional or potentially functional materials. The journal covers various areas of interest, including inorganic and organic solid-state chemistry, nanomaterials, biomaterials, thin films and polymers, and composite/hybrid materials. The journal particularly seeks papers that highlight the creation or development of innovative materials with novel optical, electrical, magnetic, catalytic, or mechanical properties. It is essential that manuscripts on these topics have a primary focus on the chemistry of materials and represent a significant advancement compared to prior research. Before external reviews are sought, submitted manuscripts undergo a review process by a minimum of two editors to ensure their appropriateness for the journal and the presence of sufficient evidence of a significant advance that will be of broad interest to the materials chemistry community.