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二维纳米片上特定位置光氧化还原活性的纳米尺度映射与原位定量分析。

Nanometric-Mapping and In Situ Quantification of Site-specific Photoredox Activities on 2D Nanoplates.

作者信息

Wu Shuyang, Lee Jinn-Kye, Zhang Zhengyang

机构信息

School of Chemistry, Chemical Engineering and Biotechnology, Nanyang Technological University, 21 Nanyang Link, Singapore, 637371, Singapore.

出版信息

Small. 2024 Nov;20(45):e2401120. doi: 10.1002/smll.202401120. Epub 2024 Jul 19.

DOI:10.1002/smll.202401120
PMID:39031107
Abstract

Defective layered bismuth oxychloride (BiOCl) exhibits excellent photocatalytic activities in water purification and environmental remediation. Herein, in situ single-molecule fluorescence microscopy is used to spatially resolve the photocatalytic heterogeneity and quantify the photoredox activities on individual structural features of BiOCl. The BiOCl nanoplates with respective dominant {001} and {010} facets (BOC-001 and BOC-010) are fabricated through tuning the pH of the solution. The corner position of BOC-001 exhibits the highest photo-oxidation turnover rate of 262.7 ± 30.8 s µm, which is 2.1 and 65.7 times of those of edges and basal planes, respectively. A similar trend is also observed on BOC-010, which can be explained by the heterogeneous distribution of defects at each structure. Besides, BOC-001 shows a higher photoredox activity than BOC-010 at corners and edges. This can be attributed to the superior charge separation ability, active high-index facets of BOC-001, and its co-exposure of anisotropic facets steering the charge flow. Therefore, this work provides an effective strategy to understand the facet-dependent properties of single-crystalline materials at nanometer resolution. The quantification of site-specific photoredox activities on BiOCl nanoplates sheds more light on the design and optimization of 2D materials at the single-molecule level.

摘要

缺陷层状氯氧化铋(BiOCl)在水净化和环境修复中表现出优异的光催化活性。在此,利用原位单分子荧光显微镜在空间上解析光催化异质性,并量化BiOCl单个结构特征上的光氧化还原活性。通过调节溶液的pH值制备了分别具有主导{001}和{010}晶面的BiOCl纳米片(BOC - 001和BOC - 010)。BOC - 001的角位置表现出最高的光氧化周转速率,为262.7±30.8 s µm,分别是边缘和基面的2.1倍和65.7倍。在BOC - 010上也观察到类似趋势,这可以用每个结构处缺陷的不均匀分布来解释。此外,BOC - 001在角和边缘处显示出比BOC - 010更高的光氧化还原活性。这可归因于BOC - 001卓越的电荷分离能力、活性高指数晶面以及其各向异性晶面的共同暴露引导电荷流动。因此,这项工作提供了一种有效的策略,以纳米分辨率理解单晶材料的晶面依赖性性质。对BiOCl纳米片上特定位置光氧化还原活性的量化为二维材料在单分子水平上的设计和优化提供了更多见解。

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