Tuning Dynamic Structural Evolution of Bi24O31Cl10 for Enhancing Piezo-Photocatalytic Nitrogen Oxidation to Nitrate

IF 9.6 1区材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Nano Letters Pub Date : 2024-06-17 DOI:10.1021/acs.nanolett.4c01697

Yi Wang, Haiyan Peng, Meiyang Song, Henghui Song, Yuhui Liu, Peng Chen* and Shuang-Feng Yin*,

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Abstract

Direct nitrogen oxidation into nitrate under ambient conditions presents a promising strategy for harsh and multistep industrial processes. However, the dynamic structural evolution of active sites in surface reactions constitutes a highly intricate endeavor and remains in its nascent stage. Here, we constructed a Bi₂₄O₃₁Cl₁₀ material with moiré superlattice structure (BCMS) for direct piezo-photocatalytic oxidation of nitrogen into nitrate. Excitingly, BCMS achieved excellent nitric acid production (15.44 mg g^–1 h^–1) under light and pressure conditions. Detailed experimental results show that the unique structure extracts the local strain tensor from the constricting Bi–Bi bond and Bi–O bond for internal structural reconstruction, which promotes the formation of electron and reactive molecule vortexes to facilitate charge transfer as well as N₂ and O₂ adsorption. Ultimately, these initiatives strengthen electron exchange between the superoxide radical and nitrogen as well as the binding strength of multiple intermediates, which swayingly adjusts the reaction path and energy barriers.

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调整 Bi24O31Cl10 的动态结构演化以增强压电光催化氮氧化为硝酸盐的能力

在环境条件下直接将氮氧化成硝酸盐是一种很有前途的策略，适用于苛刻的多步骤工业流程。然而，表面反应中活性位点的动态结构演化是一项非常复杂的工作，目前仍处于起步阶段。在此，我们构建了一种具有摩尔超晶格结构的 Bi24O31Cl10 材料（BCMS），用于直接压电光催化将氮氧化成硝酸盐。令人兴奋的是，在光和压力条件下，BCMS 实现了优异的硝酸生产（15.44 mg g-1 h-1）。详细的实验结果表明，这种独特的结构可从收缩的 Bi-Bi 键和 Bi-O 键中提取局部应变张量，用于内部结构重建，从而促进电子和活性分子涡旋的形成，促进电荷转移以及 N2 和 O2 的吸附。最终，这些举措加强了超氧自由基与氮之间的电子交换以及多个中间产物的结合强度，从而对反应路径和能垒进行了摇摆式调整。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Nano Letters 工程技术-材料科学：综合

CiteScore

16.80

自引率

2.80%

发文量

1182

审稿时长

1.4 months

期刊介绍： Nano Letters serves as a dynamic platform for promptly disseminating original results in fundamental, applied, and emerging research across all facets of nanoscience and nanotechnology. A pivotal criterion for inclusion within Nano Letters is the convergence of at least two different areas or disciplines, ensuring a rich interdisciplinary scope. The journal is dedicated to fostering exploration in diverse areas, including: - Experimental and theoretical findings on physical, chemical, and biological phenomena at the nanoscale - Synthesis, characterization, and processing of organic, inorganic, polymer, and hybrid nanomaterials through physical, chemical, and biological methodologies - Modeling and simulation of synthetic, assembly, and interaction processes - Realization of integrated nanostructures and nano-engineered devices exhibiting advanced performance - Applications of nanoscale materials in living and environmental systems Nano Letters is committed to advancing and showcasing groundbreaking research that intersects various domains, fostering innovation and collaboration in the ever-evolving field of nanoscience and nanotechnology.