Zou Hai, Bao Yunfeng, Du Shiwen, Xin Xueshang, Qi Yu, Shao Guosheng, Zhang Fuxiang
State Key Laboratory of Catalysis, Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Zhongshan Road 457, Dalian, 116023, China.
Xin University of Chinese Academy of Sciences, Beijing, 100049, China.
Chem Asian J. 2023 May 2;18(9):e202300145. doi: 10.1002/asia.202300145. Epub 2023 Mar 24.
Nitrogen doping into oxide has been proved to be an effective strategy to extend visible-light utilization of oxides with layered or channeled structure, but it is shortage for the bulk oxides free of layered or channeled structure. Here, we report a novel nitrogen-doped bulk oxide (denoted as YTaO N ) with good visible light response. As benefited from the strong hybridization of N 2p and O 2p electronic state according to the density functional theory (DFT) calculations, the band gap (3.6 eV) of YTaO precursor was sharply narrowed to 2.4 eV on YTaO N due to the obvious uplift of the valence band maximum (VBM). After decorated with the platinum cocatalyst, the Pt/YTaO N was used as the H -evolving photocatalyst for assembly of Z-scheme overall water splitting system by coupling with the PtO /WO as the oxygen evolution photocatalyst and using the I /IO as the shuttle ions. This work enriches the material database of nitrogen-doped oxide with wide visible light absorption and shows its promising application in solar-to-chemical conversion.
已证明将氮掺杂到氧化物中是一种有效的策略，可扩展具有层状或通道结构的氧化物对可见光的利用，但对于没有层状或通道结构的块状氧化物来说却存在不足。在此，我们报道了一种具有良好可见光响应的新型氮掺杂块状氧化物（表示为YTaO₃N）。根据密度泛函理论（DFT）计算，得益于N 2p和O 2p电子态的强杂化作用，YTaO₃前驱体的带隙（3.6 eV）在YTaO₃N上因价带最大值（VBM）明显升高而急剧缩小至2.4 eV。在用铂助催化剂修饰后，Pt/YTaO₃N用作析氢光催化剂，通过与作为析氧光催化剂的PtO₂/WO₃耦合并使用I⁻/IO₃⁻作为穿梭离子，组装成Z型全分解水体系。这项工作丰富了具有宽可见光吸收的氮掺杂氧化物的材料数据库，并展示了其在太阳能到化学能转化方面的广阔应用前景。
