Enriching surface-ordered defects on WO 3 for photocatalytic CO 2 -to-CH 4 conversion by water

IF 9.4 1区综合性期刊 Q1 MULTIDISCIPLINARY SCIENCES

Proceedings of the National Academy of Sciences of the United States of America Pub Date : 2024-04-25 DOI:10.1073/pnas.2319751121

Sikang Xue, Changgeng Wei, Min Shen, Xiaocong Liang, Jiali Wang, Can Yang, Wandong Xing, Sibo Wang, Wei Lin, Zhiyang Yu, Yidong Hou, Jimmy C. Yu, Xinchen Wang

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Abstract

Defect engineering has been widely applied in semiconductors to improve photocatalytic properties by altering the surface structures. This study is about the transformation of inactive WO 3 nanosheets to a highly effective CO 2 -to-CH 4 conversion photocatalyst by introducing surface-ordered defects in abundance. The nonstoichiometric WO 3- x samples were examined by using aberration-corrected electron microscopy. Results unveil abundant surface-ordered terminations derived from the periodic {013} stacking faults with a defect density of 20.2%. The {002} surface-ordered line defects are the active sites for fixation CO 2 , transforming the inactive WO 3 nanosheets into a highly active catalyst (CH 4 : O 2 = 8.2: 16.7 μmol h −1 ). We believe that the formation of the W-O-C-W-O species is a critical step in the catalytic pathways. This work provides an atomic-level comprehension of the structural defects of catalysts for activating small molecules.

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丰富 WO 3 表面有序缺陷，实现光催化水将 CO 2 转化为 CH 4

缺陷工程已被广泛应用于半导体领域，通过改变表面结构来改善光催化性能。本研究通过大量引入表面有序缺陷，将无活性的 WO 3 纳米片转化为高效的 CO 2 转化为 CH 4 光催化剂。我们使用像差校正电子显微镜对非全度 WO 3- x 样品进行了研究。结果揭示了大量的表面有序端点，这些端点来自周期性的{013}堆叠断层，缺陷密度为 20.2%。{002}表面有序线缺陷是固定 CO 2 的活性位点，将无活性的 WO 3 纳米片转化为高活性催化剂（CH 4 : O 2 = 8.2 : 16.7 μmol h -1 ）。我们认为，W-O-C-W-O 物种的形成是催化途径中的关键一步。这项工作从原子水平上理解了活化小分子催化剂的结构缺陷。

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

Proceedings of the National Academy of Sciences of the United States of America 综合性期刊-综合性期刊

CiteScore

19.00

自引率

0.90%

发文量

3575

审稿时长

2.5 months

期刊介绍： The Proceedings of the National Academy of Sciences (PNAS), a peer-reviewed journal of the National Academy of Sciences (NAS), serves as an authoritative source for high-impact, original research across the biological, physical, and social sciences. With a global scope, the journal welcomes submissions from researchers worldwide, making it an inclusive platform for advancing scientific knowledge.