Engineering the Atomic Configurations of Surface-Active Sites for Retuning the Photoreduction CO2 Selectivity

IF 11.3 1区化学 Q1 CHEMISTRY, PHYSICAL

ACS Catalysis Pub Date : 2024-10-11 DOI:10.1021/acscatal.4c03304

Min Shen, Yan Ye, Mingyue Wang, Xiaocong Liang, Hao Tang, Yulan Wang, Chuchu Zhou, Shilan Zhang, Sikang Xue, Can Yang, Wandong Xing, Zhiyang Yu

引用次数: 0

Abstract

The photoreduction of the CO₂ reaction is a potential technique for converting solar energy to fuel at room temperature, which speeds up the recycling and conversion of carbon compounds. Based on a highly active photocatalyst, however, disentangling the chemical environments of surface structures on the selectivity of the product at the atomic scale is challenging. Herein, we have explored a sulfur-assisted heat treatment strategy to induce the reconstruction from surface-ordered line defects to polygonal tungsten line defects, changing the main product from CH₄ (8.2 μmol h^–1, 5 mg) to CO (13.0 μmol h^–1, 5 mg) without any additive sacrificial agents. The experimental results reveal that the active sites are the surface terminations of the hexagonal-tungsten line defect, where the in-plane-neighboring W atoms can break the C–O bonds inside the *COOH intermediates, thereby promoting the desorption of CO gas.

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改造表面活性位点的原子构型，重新调整光氧化 CO2 选择性

二氧化碳的光还原反应是一种在室温下将太阳能转化为燃料的潜在技术，可加快碳化合物的循环和转化。然而，基于高活性光催化剂，在原子尺度上厘清表面结构对产物选择性的化学环境具有挑战性。在此，我们探索了一种硫辅助热处理策略，以诱导表面有序线缺陷向多边形钨线缺陷的重构，在不添加任何牺牲剂的情况下，将主要产物从 CH4（8.2 μmol h-1，5 mg）转变为 CO（13.0 μmol h-1，5 mg）。实验结果表明，活性位点是六方钨线缺陷的表面终端，平面内相邻的 W 原子可以打断 *COOH 中间体内部的 C-O 键，从而促进 CO 气体的解吸。

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

ACS Catalysis CHEMISTRY, PHYSICAL-

CiteScore

20.80

自引率

6.20%

发文量

1253

审稿时长

1.5 months

期刊介绍： ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels. The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.