Qi Yu, Chen Shanshan, Li Mingrun, Ding Qian, Li Zheng, Cui Junyan, Dong Beibei, Zhang Fuxiang, Li Can
State Key Laboratory of Catalysis , iChEM , Dalian Institute of Chemical Physics , Chinese Academy of Sciences , Dalian National Laboratory for Clean Energy , Dalian , 116023 , China . Email:
University of Chinese Academy of Sciences , Beijing 100049 , China.
Chem Sci. 2017 Jan 1;8(1):437-443. doi: 10.1039/c6sc02750d. Epub 2016 Aug 18.
TaN is one of the most promising photocatalyst candidates for solar water splitting, but it still remains challenging to achieve overall water splitting TaN-based photocatalysts regardless of whether it uses a one step or two step method. Here we will address the relatively poor photocatalytic proton reduction of TaN with an effort for the promotion of charge separation barium modification. One-pot nitridation of barium nitrate-impregnated TaO precursor was adopted here for the synthesis of TaN accompanied with the creation of a TaN/BaTaON heterostructure and surface passivation. Due to the synergetic effect of the improved interfacial charge separation and the decreased defect density, the photocatalytic H evolution rate of barium-modified TaN is effectively promoted. Encouraged by this, a visible-light-driven Z-scheme overall water splitting system was successfully constructed by using the barium-modified TaN as a H-evolving photocatalyst, together with a PtO /WO and IO/I pair as an O-evolving photocatalyst and a redox mediator, respectively.
氮化钽是太阳能光解水最具潜力的光催化剂候选材料之一，但无论采用一步法还是两步法，基于氮化钽的光催化剂实现全解水仍具有挑战性。在此，我们将通过钡改性促进电荷分离，解决氮化钽光催化质子还原能力相对较差的问题。采用一锅法对浸渍硝酸钡的TaO前驱体进行氮化，合成氮化钽，同时形成TaN/BaTaON异质结构并实现表面钝化。由于界面电荷分离改善和缺陷密度降低的协同效应，钡改性氮化钽的光催化析氢速率得到有效提高。受此鼓舞，以钡改性氮化钽作为析氢光催化剂，分别以PtO /WO和IO/I对作为析氧光催化剂和氧化还原介质，成功构建了可见光驱动的Z型全解水体系。
