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W–N Bonds Precisely Boost Z-Scheme Interfacial Charge Transfer in g-C3N4/WO3 Heterojunctions for Enhanced Photocatalytic H2 Evolution
ACS Catalysis ( IF 11.3 ) Pub Date : 2022-08-02 , DOI: 10.1021/acscatal.2c02416
Rongchen Shen 1 , Lu Zhang 2 , Neng Li 3 , Zaizhu Lou 4 , Tianyi Ma 5 , Peng Zhang 6 , Youji Li 7 , Xin Li 1
Affiliation  

Exploring and achieving precise electron-transfer channels in the interface of Z-scheme heterojunctions are essential and have been considered as immense challenges. A strategy to precisely connect the valence band (VB) site of g-C3N4 (CN) with the conduction band (CB) site of WO3 through the tungsten–nitrogen (W–N) bond was developed to create a chemically bonded Z-scheme heterojunction photocatalyst. Because of this reason, the photogenerated electrons from the CB site of WO3 could be accurately and directly injected into the VB site of CN, following the direct Z-scheme charge separation pathways. The photocatalytic hydrogen production rate of optimal CNWB was 482 μmol h–1, 4.3 times higher than that of CN/WO3 without an N–W bond (CNWU). The CNWB also shows better photocatalytic hydrogen evolution activity than the previous CN/WO3 systems. Theoretical and experimental results further confirm that the newly formed N–W bonds become metallic, which could act as atomic-level interfacial channels to precisely accelerate Z-scheme interfacial electron transfer and shorten the electron-transfer distance, thus substantially boosting photocatalytic H2 generation. This work paves a way to design and synthesize the chemically bonded Z-scheme interface with atomic precision for interesting photocatalytic applications in the future.

中文翻译:

W-N 键精确地促进 g-C3N4/WO3 异质结中的 Z 型界面电荷转移以增强光催化产氢

在 Z 型异质结的界面中探索和实现精确的电子转移通道是必不可少的,并且被认为是巨大的挑战。开发了一种通过钨-氮 (W-N) 键将 gC 3 N 4 (CN) 的价带 (VB) 位点与 WO 3的导带 (CB) 位点精确连接的策略,以创建化学键合 Z -方案异质结光催化剂。由于这个原因,来自WO 3 CB 位点的光生电子可以按照直接Z 型电荷分离途径准确直接地注入CN 的VB 位点。最佳CNWB的光催化产氢率为482 μmol h -1, 比没有 N-W 键的 CN/WO 3 (CNWU)高 4.3 倍。CNWB 还显示出比以前的 CN/WO 3系统更好的光催化析氢活性。理论和实验结果进一步证实,新形成的N-W键变成金属键,可以作为原子级界面通道,精确加速Z型界面电子转移,缩短电子转移距离,从而显着促进光催化H 2生成. 这项工作为设计和合成具有原子精度的化学键合 Z 型界面铺平了道路,以用于未来有趣的光催化应用。
更新日期:2022-08-02
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