Single-molecule quantification of photoredox activities and dynamics at the nanoscale on multi-faceted 2D materials†

IF 10.7 2区 材料科学 Q1 CHEMISTRY, PHYSICAL
Shuyang Wu, Jinn-Kye Lee, Mingyu Ma, Jia Xin Chan and Zhengyang Zhang
{"title":"Single-molecule quantification of photoredox activities and dynamics at the nanoscale on multi-faceted 2D materials†","authors":"Shuyang Wu, Jinn-Kye Lee, Mingyu Ma, Jia Xin Chan and Zhengyang Zhang","doi":"10.1039/D4TA07149B","DOIUrl":null,"url":null,"abstract":"<p >Two-dimensional bismuth oxybromide (BiOBr) with multiple facets has been widely used in photocatalytic pollutant degradation and clean energy production. Herein, we used <em>in situ</em> single-molecule fluorescence microscopy to quantify structure-specific photoredox activities of facet-dependent BiOBr. The nanometric-mapping of photoredox reactions (resolution: 20 nm) clearly unveils the catalytic heterogeneity on {001} facet-dominant and {010} facet-dominant BiOBr, respectively (BiOBr-001 and BiOBr-010). The corners of BiOBr nanoplates exhibit the highest photoredox activities, followed by edges and basal planes, which are attributed to the unsaturated coordination sites in corners and edges. BiOBr-001 corners show the photoreduction and photo-oxidation activities of 108.0 ± 11.5 and 654.5 ± 83.2 s<small><sup>−1</sup></small> μm<small><sup>−2</sup></small>, respectively, which are 1.2 and 3.4 times those of BiOBr-010 corners. Other structures of BiOBr-001 also exhibit superior reactivity to BiOBr-010. Such phenomena are ascribed to shorter charge transfer distance and the existence of high-index facets in BiOBr-001. Bulk activity evaluation further supports the single-molecule analysis. The investigation of temporal activity fluctuation reveals surface restructuring probably accounts for the activity enhancement at the nanoscale under practical reaction conditions. Hence, our study correlates the catalyst structure and reaction dynamics at nanometer resolution, which guides the performance improvement at both single-molecule and ensemble levels.</p>","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":" 5","pages":" 3825-3833"},"PeriodicalIF":10.7000,"publicationDate":"2025-01-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Materials Chemistry A","FirstCategoryId":"88","ListUrlMain":"https://pubs.rsc.org/en/content/articlelanding/2025/ta/d4ta07149b","RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
引用次数: 0

Abstract

Two-dimensional bismuth oxybromide (BiOBr) with multiple facets has been widely used in photocatalytic pollutant degradation and clean energy production. Herein, we used in situ single-molecule fluorescence microscopy to quantify structure-specific photoredox activities of facet-dependent BiOBr. The nanometric-mapping of photoredox reactions (resolution: 20 nm) clearly unveils the catalytic heterogeneity on {001} facet-dominant and {010} facet-dominant BiOBr, respectively (BiOBr-001 and BiOBr-010). The corners of BiOBr nanoplates exhibit the highest photoredox activities, followed by edges and basal planes, which are attributed to the unsaturated coordination sites in corners and edges. BiOBr-001 corners show the photoreduction and photo-oxidation activities of 108.0 ± 11.5 and 654.5 ± 83.2 s−1 μm−2, respectively, which are 1.2 and 3.4 times those of BiOBr-010 corners. Other structures of BiOBr-001 also exhibit superior reactivity to BiOBr-010. Such phenomena are ascribed to shorter charge transfer distance and the existence of high-index facets in BiOBr-001. Bulk activity evaluation further supports the single-molecule analysis. The investigation of temporal activity fluctuation reveals surface restructuring probably accounts for the activity enhancement at the nanoscale under practical reaction conditions. Hence, our study correlates the catalyst structure and reaction dynamics at nanometer resolution, which guides the performance improvement at both single-molecule and ensemble levels.

Abstract Image

Abstract Image

纳米尺度上多面二维材料的光氧化还原活性和动力学的单分子定量
具有多面性的二维氧化溴化铋(BiOBr)在光催化污染物降解和清洁能源生产中有着广泛的应用。在这里,我们使用原位单分子荧光显微镜来量化面依赖性BiOBr的结构特异性光氧化还原活性。光氧化还原反应的纳米图谱(分辨率:20 nm)清楚地揭示了{001}面显性和{010}面显性BiOBr (BiOBr-001和BiOBr-010)的催化非均质性。BiOBr纳米片的光氧化还原活性最高,其次是边缘和基面,这与角和边缘的不饱和配位有关。BiOBr-001的光还原活性和光氧化活性分别为108.0±11.5和654.5±83.2 s−1 μm−2,是BiOBr-010的1.2倍和3.4倍。BiOBr-001的其他结构也对BiOBr-010表现出优异的反应性。这种现象归因于BiOBr-001中较短的电荷转移距离和高折射率面的存在。散装活性评价进一步支持单分子分析。对时间活性波动的研究表明,在实际反应条件下,表面重组可能是纳米尺度上活性增强的原因。因此,我们的研究将催化剂结构和反应动力学在纳米分辨率上联系起来,这将指导单分子和系综水平上的性能改进。
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 求助全文
来源期刊
Journal of Materials Chemistry A
Journal of Materials Chemistry A CHEMISTRY, PHYSICAL-ENERGY & FUELS
CiteScore
19.50
自引率
5.00%
发文量
1892
审稿时长
1.5 months
期刊介绍: The Journal of Materials Chemistry A, B & C covers a wide range of high-quality studies in the field of materials chemistry, with each section focusing on specific applications of the materials studied. Journal of Materials Chemistry A emphasizes applications in energy and sustainability, including topics such as artificial photosynthesis, batteries, and fuel cells. Journal of Materials Chemistry B focuses on applications in biology and medicine, while Journal of Materials Chemistry C covers applications in optical, magnetic, and electronic devices. Example topic areas within the scope of Journal of Materials Chemistry A include catalysis, green/sustainable materials, sensors, and water treatment, among others.
×
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
确定
请完成安全验证×
copy
已复制链接
快去分享给好友吧!
我知道了
右上角分享
点击右上角分享
0
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 布克学术 All rights reserved.
京ICP备2023020795号-1
ghs 京公网安备 11010802042870号
Book学术文献互助
Book学术文献互助群
群 号:481959085
Book学术官方微信