Strain engineering in two-dimensional nanomaterials holds significant potential for modulating the lattice and band structure, particularly through localized strain, which enables modulation at specific regions. Despite the remarkable effects of local strain, the relationships among local strain, spatial correlation of photogenerated charge carriers, and photocatalytic performance remain elusive. The current study coupled single-molecule localization microscopy with coordinate-based colocalization (CBC) analysis to explain these relationships. The methodology involved mapping the spatial distributions of photoinduced oxidation and reduction reaction sites across graphitic carbon nitride (g-C₃N₄) nanosheets, quantifying and spatially resolving their spatial correlation, and also evaluating their photocatalytic activity. The study examined 65 individual g-C₃N₄ nanosheets, revealing interparticle and intraparticle heterogeneity, which was classified based on their CBC score distributions. Among the 65 g-C₃N₄ nanosheets, type A nanosheets predominated (45 out of 65) and demonstrated both correlated and noncorrelated subregions along some wrinkles. In contrast, type B nanosheets (20 out of 65) were primarily characterized by noncorrelated subregions with minimal correlated localizations. The coexistence of both noncorrelated and correlated subregions inferred the structure of the wrinkles as folding wrinkles, which have larger tensile-strained areas than rippling wrinkles. Folding wrinkles promote colocalization through the formation of type I band alignment at tensile-strained subregions. This band alignment also enhances photocatalytic activity through a funneling effect and improved light absorption, leading to higher specific activity in correlated subregions compared to noncorrelated ones. The role of strain-induced band alignment in modulating the spatial correlation of the photoredox reaction and the photocatalytic performance at the subregion level is highlighted.

中文翻译：

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应变对石墨态氮化碳光催化反应的影响：来自单分子定位显微镜的见解


二维纳米材料中的应变工程在调制晶格和能带结构方面具有重要潜力，特别是通过局部应变，从而可以在特定区域进行调制。尽管局部应变的影响显著，但局部应变、光生载流子的空间相关性和光催化性能之间的关系仍然难以捉摸。目前的研究将单分子定位显微镜与基于坐标的共定位 （CBC） 分析相结合，以解释这些关系。该方法涉及绘制石墨氮化碳 （g-C₃N₄） 纳米片上光诱导氧化和还原反应位点的空间分布，量化和空间解析它们的空间相关性，并评估它们的光催化活性。该研究检查了 65 个单独的 g-C₃N₄ 纳米片，揭示了颗粒间和颗粒内异质性，这是根据它们的 CBC 分数分布进行分类的。在 65 g-C₃N₄ 纳米片中，A 型纳米片占主导地位（65 片中的 45 片），并且沿一些皱纹表现出相关和非相关子区域。相比之下，B 型纳米片 （65 片中的 20 片） 主要以非相关亚区和最小相关定位为特征。不相关和相关子区域的共存推断皱纹的结构为折叠皱纹，其拉伸应变区域比波纹皱纹大。折叠皱纹通过在拉伸应变亚区域形成 I 型带对齐来促进共定位。 这种带对齐还通过漏斗效应和改善光吸收增强了光催化活性，导致与非相关亚区相比，相关亚区的比活性更高。强调了应变诱导的能带对齐在调节光氧化还原反应的空间相关性和亚区域水平的光催化性能中的作用。