Xiao Jiadong, Nishimae Shinji, Vequizo Junie Jhon M, Nakabayashi Mamiko, Hisatomi Takashi, Li Huihui, Lin Lihua, Shibata Naoya, Yamakata Akira, Inoue Yasunobu, Domen Kazunari
Research Initiative for Supra-Materials, Interdisciplinary Cluster for Cutting Edge Research, Shinshu University, Nagano-shi, Nagano, 380-8553, Japan.
Japan Technological Research Association of Artificial Photosynthetic Chemical Process (ARPChem), 2-11-16 Yayoi, Bunkyo-ku, Tokyo, 113-8656, Japan.
Angew Chem Int Ed Engl. 2022 Apr 19;61(17):e202116573. doi: 10.1002/anie.202116573. Epub 2022 Feb 28.
Solar-powered one-step-excitation overall water splitting (OWS) using semiconducting materials is a simple means of achieving scalable and sustainable hydrogen production. While tantalum oxynitride (TaON) is one of the few photocatalysts capable of promoting OWS via single-step visible-light excitation, the efficiency of this process remains extremely poor. The present work employed 15 nm amorphous Ta O ⋅3.3 H O nanoparticles as a new precursor together with Zr doping and an optimized nitridation duration to synthesize a TaON-based photocatalyst with reduced particle sizes and low defect densities. Upon loading with Ru/Cr O /IrO cocatalysts, this material exhibited stoichiometric water splitting into hydrogen and oxygen, with an order of magnitude improvement in efficiency. Our findings demonstrate the importance of inventing/selecting the appropriate synthetic precursor and of defect control for fabricating active OWS photocatalysts.
使用半导体材料的太阳能一步激发全水分解(OWS)是实现可扩展和可持续制氢的一种简单方法。虽然氧氮化钽(TaON)是少数能够通过单步可见光激发促进全水分解的光催化剂之一,但该过程的效率仍然极低。本研究采用15纳米非晶态TaO·3.3H₂O纳米颗粒作为新的前驱体,结合锆掺杂和优化的氮化时间,合成了粒径减小且缺陷密度低的基于TaON的光催化剂。负载Ru/Cr₂O₃/IrO助催化剂后,该材料实现了化学计量比的水分解为氢气和氧气,效率提高了一个数量级。我们的研究结果表明,发明/选择合适的合成前驱体以及控制缺陷对于制备活性全水分解光催化剂至关重要。