Zhihong Huang, Tao Cheng, Aamir Hassan Shah, Guangyan Zhong, Chengzhang Wan, Peiqi Wang, Mengning Ding, Jin Huang, Zhong Wan, Sibo Wang, Jin Cai, Bosi Peng, Haotian Liu, Yu Huang, William A. Goddard III, Xiangfeng Duan
{"title":"Edge sites dominate the hydrogen evolution reaction on platinum nanocatalysts","authors":"Zhihong Huang, Tao Cheng, Aamir Hassan Shah, Guangyan Zhong, Chengzhang Wan, Peiqi Wang, Mengning Ding, Jin Huang, Zhong Wan, Sibo Wang, Jin Cai, Bosi Peng, Haotian Liu, Yu Huang, William A. Goddard III, Xiangfeng Duan","doi":"10.1038/s41929-024-01156-x","DOIUrl":null,"url":null,"abstract":"Platinum nanocatalysts facilitate the hydrogen evolution reaction (HER) for renewable chemical fuel generation. These nanostructures encompass diverse surface sites, including (111) and (100) facets and edge sites between them. Identifying the exact active sites is essential for optimal catalyst design, but remains challenging. Here, combining electrical transport spectroscopy (ETS) with reactive force field (ReaxFF) calculations, we profile hydrogen adsorption on platinum nanowires and reveal two distinct peaks: one at 0.20 VRHE for (111) and (100) facets and one at 0.038 VRHE for edge sites. Concurrent ETS and cyclic voltammetry show that edge site adsorption coincides with the onset of the HER, indicating the critical role of edge sites. ReaxFF molecular dynamics calculations confirm lower activation barriers for the HER at edge sites, with two to four orders of magnitude higher turnover frequencies. ETS in alkaline media reveals substantially suppressed hydrogen adsorption on edge sites, contributing to the more sluggish HER kinetics. These findings resolve the elusive role of different sites on platinum surfaces, offering critical insights for HER catalyst design. Pt is the most active catalyst for the hydrogen evolution reaction in acidic media, but the precise nature of its active sites remains elusive. Now electrical transport spectroscopy and molecular dynamics are combined to map the hydrogen adsorption sites on Pt nanowires and reveal the much higher activity of (111)/(100) edge sites.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"7 6","pages":"678-688"},"PeriodicalIF":42.8000,"publicationDate":"2024-05-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Nature Catalysis","FirstCategoryId":"92","ListUrlMain":"https://www.nature.com/articles/s41929-024-01156-x","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
引用次数: 0
Abstract
Platinum nanocatalysts facilitate the hydrogen evolution reaction (HER) for renewable chemical fuel generation. These nanostructures encompass diverse surface sites, including (111) and (100) facets and edge sites between them. Identifying the exact active sites is essential for optimal catalyst design, but remains challenging. Here, combining electrical transport spectroscopy (ETS) with reactive force field (ReaxFF) calculations, we profile hydrogen adsorption on platinum nanowires and reveal two distinct peaks: one at 0.20 VRHE for (111) and (100) facets and one at 0.038 VRHE for edge sites. Concurrent ETS and cyclic voltammetry show that edge site adsorption coincides with the onset of the HER, indicating the critical role of edge sites. ReaxFF molecular dynamics calculations confirm lower activation barriers for the HER at edge sites, with two to four orders of magnitude higher turnover frequencies. ETS in alkaline media reveals substantially suppressed hydrogen adsorption on edge sites, contributing to the more sluggish HER kinetics. These findings resolve the elusive role of different sites on platinum surfaces, offering critical insights for HER catalyst design. Pt is the most active catalyst for the hydrogen evolution reaction in acidic media, but the precise nature of its active sites remains elusive. Now electrical transport spectroscopy and molecular dynamics are combined to map the hydrogen adsorption sites on Pt nanowires and reveal the much higher activity of (111)/(100) edge sites.
期刊介绍:
Nature Catalysis serves as a platform for researchers across chemistry and related fields, focusing on homogeneous catalysis, heterogeneous catalysis, and biocatalysts, encompassing both fundamental and applied studies. With a particular emphasis on advancing sustainable industries and processes, the journal provides comprehensive coverage of catalysis research, appealing to scientists, engineers, and researchers in academia and industry.
Maintaining the high standards of the Nature brand, Nature Catalysis boasts a dedicated team of professional editors, rigorous peer-review processes, and swift publication times, ensuring editorial independence and quality. The journal publishes work spanning heterogeneous catalysis, homogeneous catalysis, and biocatalysis, covering areas such as catalytic synthesis, mechanisms, characterization, computational studies, nanoparticle catalysis, electrocatalysis, photocatalysis, environmental catalysis, asymmetric catalysis, and various forms of organocatalysis.