Constructing Heterojunction Photocatalyst Systems with Spatial Distribution of Au Single Atoms for CO2 Reduction

IF 8.3 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY ACS Applied Materials & Interfaces Pub Date : 2024-12-21 DOI:10.1021/acsami.4c17745
Xiaoguang Wang, Lihui Liu, Huiming Cao, Shihao Gong, Honghui Pan, Xiaowen Liu, Pu Wang, Yanrong Zhang
{"title":"Constructing Heterojunction Photocatalyst Systems with Spatial Distribution of Au Single Atoms for CO2 Reduction","authors":"Xiaoguang Wang, Lihui Liu, Huiming Cao, Shihao Gong, Honghui Pan, Xiaowen Liu, Pu Wang, Yanrong Zhang","doi":"10.1021/acsami.4c17745","DOIUrl":null,"url":null,"abstract":"In single-atomic photocatalyst systems, the spatial distribution of single atoms on heterojunctions and its impact on photocatalytic processes, particularly on carrier dynamics and the CO<sub>2</sub> reduction process involving multielectron reactions, remains underexplored. To address this gap, a WO<sub>3</sub>/TiO<sub>2</sub> nanotube heterojunction with a spatially selective distribution of Au single atoms was developed using an oxygen vacancy anchoring strategy for CO<sub>2</sub> photoreduction. By anchoring Au atoms onto the WO<sub>3</sub> or TiO<sub>2</sub> components, a substantial number of active sites are generated and the electron transfer pathways from the heterojunction toward Au sites are formed, thereby enhancing carrier separation and concentration. As a result, the total yield of CO<sub>2</sub> reduction products increases by 6.3 times and 3.9 times, respectively. More importantly, due to significant differences in adsorption properties, energy band structures, and reaction energy barrier, as well as a 2-fold difference in carrier lifetime, the selective distribution of Au single-atom sites results in completely different CO<sub>2</sub> photoreduction products: when Au atoms are anchored on WO<sub>3</sub> and TiO<sub>2</sub> components, the product selectivity is 67.6% CH<sub>4</sub> and 82.9% CO, respectively. This study clarifies the vital role of the spatial distribution of single atoms on the selectivity of electron-demanding products.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"13 1","pages":""},"PeriodicalIF":8.3000,"publicationDate":"2024-12-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"ACS Applied Materials & Interfaces","FirstCategoryId":"88","ListUrlMain":"https://doi.org/10.1021/acsami.4c17745","RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"MATERIALS SCIENCE, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 0

Abstract

In single-atomic photocatalyst systems, the spatial distribution of single atoms on heterojunctions and its impact on photocatalytic processes, particularly on carrier dynamics and the CO2 reduction process involving multielectron reactions, remains underexplored. To address this gap, a WO3/TiO2 nanotube heterojunction with a spatially selective distribution of Au single atoms was developed using an oxygen vacancy anchoring strategy for CO2 photoreduction. By anchoring Au atoms onto the WO3 or TiO2 components, a substantial number of active sites are generated and the electron transfer pathways from the heterojunction toward Au sites are formed, thereby enhancing carrier separation and concentration. As a result, the total yield of CO2 reduction products increases by 6.3 times and 3.9 times, respectively. More importantly, due to significant differences in adsorption properties, energy band structures, and reaction energy barrier, as well as a 2-fold difference in carrier lifetime, the selective distribution of Au single-atom sites results in completely different CO2 photoreduction products: when Au atoms are anchored on WO3 and TiO2 components, the product selectivity is 67.6% CH4 and 82.9% CO, respectively. This study clarifies the vital role of the spatial distribution of single atoms on the selectivity of electron-demanding products.

Abstract Image

查看原文
分享 分享
微信好友 朋友圈 QQ好友 复制链接
本刊更多论文
构建具有空间分布Au单原子的异结光催化剂体系用于CO2还原
在单原子光催化体系中,单原子在异质结上的空间分布及其对光催化过程的影响,特别是对载流子动力学和涉及多电子反应的CO2还原过程的影响,仍有待进一步研究。为了解决这一问题,利用氧空位锚定策略开发了具有空间选择性Au单原子分布的WO3/TiO2纳米管异质结,用于CO2光还原。通过将Au原子锚定在WO3或TiO2组分上,产生了大量的活性位点,形成了从异质结向Au位点的电子转移途径,从而增强了载流子的分离和浓度。因此,CO2还原产物的总产率分别提高了6.3倍和3.9倍。更重要的是,由于吸附性质、能带结构和反应能垒的显著差异,以及载子寿命的2倍差异,Au单原子位的选择性分布导致CO2光还原产物完全不同:当Au原子锚定在WO3和TiO2组分上时,产物选择性分别为67.6% CH4和82.9% CO。本研究阐明了单原子的空间分布对需要电子的产物的选择性的重要作用。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
求助全文
约1分钟内获得全文 去求助
来源期刊
ACS Applied Materials & Interfaces
ACS Applied Materials & Interfaces 工程技术-材料科学:综合
CiteScore
16.00
自引率
6.30%
发文量
4978
审稿时长
1.8 months
期刊介绍: ACS Applied Materials & Interfaces is a leading interdisciplinary journal that brings together chemists, engineers, physicists, and biologists to explore the development and utilization of newly-discovered materials and interfacial processes for specific applications. Our journal has experienced remarkable growth since its establishment in 2009, both in terms of the number of articles published and the impact of the research showcased. We are proud to foster a truly global community, with the majority of published articles originating from outside the United States, reflecting the rapid growth of applied research worldwide.
期刊最新文献
Clinically Oriented Oral Environment-Triggered Underwater Adhesives for Root Caries Treatment through Dentinal Tubule Occlusion and Remineralization Hot Electron Photoemission from Tunable Electron Affinity Semiconductor Cathodes Ferroelectric Tunable Nonvolatile Polarization Detection Based on 2H α-In2Se3 Fluoride Ion Passivation of CsPbBr3 Nanocrystals at Room Temperature for Highly Efficient and Stable White Light-Emitting Diodes Butylammonium-Based Chiral 2D Perovskite Single Crystals for Efficient UV Circularly Polarized Light Differentiation and High-Performance X-ray Detection
×
引用
GB/T 7714-2015
复制
MLA
复制
APA
复制
导出至
BibTeX EndNote RefMan NoteFirst NoteExpress
×
×
提示
您的信息不完整,为了账户安全,请先补充。
现在去补充
×
提示
您因"违规操作"
具体请查看互助需知
我知道了
×
提示
现在去查看 取消
×
提示
确定
0
微信
客服QQ
Book学术公众号 扫码关注我们
反馈
×
意见反馈
请填写您的意见或建议
请填写您的手机或邮箱
已复制链接
已复制链接
快去分享给好友吧!
我知道了
×
扫码分享
扫码分享
Book学术官方微信
Book学术文献互助
Book学术文献互助群
群 号:481959085
Book学术
文献互助 智能选刊 最新文献 互助须知 联系我们:info@booksci.cn
Book学术提供免费学术资源搜索服务,方便国内外学者检索中英文文献。致力于提供最便捷和优质的服务体验。
Copyright © 2023 Book学术 All rights reserved.
ghs 京公网安备 11010802042870号 京ICP备2023020795号-1