Enhancing the Photocatalytic Activity of CaTaO2N for Overall Water Splitting through Surface Nitride Ion Enrichment

IF 11.3 1区化学 Q1 CHEMISTRY, PHYSICAL

ACS Catalysis Pub Date : 2024-06-28 DOI:10.1021/acscatal.4c01590

Xuecheng Liu, Linjie Yan, Wenpeng Li, Kaihong Chen, Faze Wang, Jiadong Xiao, Takashi Hisatomi, Tsuyoshi Takata and Kazunari Domen*,

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Abstract

Perovskite-type CaTaO₂N has a band structure suitable for one-step-excitation overall photocatalytic water splitting under visible light. However, the poor electron–hole separation characteristics of this material limit its water splitting activity. In the present work, N-enriched CaTaO₂N was prepared by sequential nitridation in the presence and then the absence of a flux. The nitride-enriched CaTaO₂N was found to promote one-step-excitation overall water splitting efficiently and evolved H₂ and O₂ stoichiometrically under visible light with an apparent quantum efficiency of 0.45% at 420 nm. This is the highest value yet reported for a CaTaO₂N-based material applied to overall water splitting. The increased activity of this photocatalyst is attributed to the incorporation of nitride ions, which enhanced the separation of photogenerated electrons and holes. This study suggests a promising approach to boosting one-step-excitation overall photocatalytic water splitting, using nitride ion enrichment as a means of manipulating charge transfer behavior.

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通过表面氮离子富集提高 CaTaO2N 的光催化活性以实现整体水分离

透辉石型 CaTaO2N 具有适合在可见光下进行一步激发整体光催化水分离的能带结构。然而，这种材料较差的电子-空穴分离特性限制了其水分离活性。在本研究中，通过在有助焊剂和无助焊剂的条件下依次进行氮化，制备了富含氮的 CaTaO2N。研究发现，氮富集的 CaTaO2N 能有效地促进一步激发的整体水分裂，并在可见光下按化学计量进化出 H2 和 O2，在 420 纳米波长下的表观量子效率为 0.45%。这是迄今为止报道的基于 CaTaO2N 的材料用于整体水分离的最高值。这种光催化剂活性的提高归功于氮化物离子的加入，它增强了光生电子和空穴的分离。这项研究表明，利用氮化物离子富集作为操纵电荷转移行为的一种手段，是促进一步激发整体光催化水分离的一种很有前途的方法。

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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.