Qiu Bocheng, Cai Lejuan, Zhang Ning, Tao Xiaoming, Chai Yang
Department of Applied Physics The Hong Kong Polytechnic University Hung Hom Kowloon Hong Kong 999077 P. R. China.
The Hong Kong Polytechnic University Shenzhen Research Institute Shenzhen 518057 P. R. China.
Adv Sci (Weinh). 2020 Jul 14;7(17):1903568. doi: 10.1002/advs.201903568. eCollection 2020 Sep.
Solar-driven overall water splitting based on metal sulfide semiconductor photocatalysts remains as a challenge owing to the strong charge recombination and deficient catalytic active sites. Additionally, significant inhibition of back reactions, especially the oxidation of sulfide ions during the photocatalytic water oxidation catalysis, is an arduous task that requires an efficient photogenerated hole transfer dynamics. Here, a ternary dumbbell-shaped catalyst based on RuO/CdS/MoS with spatially separated catalytic sites is developed to achieve simultaneous production of hydrogen and oxygen under simulated solar-light without any sacrificial agents. Particularly, MoS nanosheets anchored on the two ends of CdS nanowires are identified as a reduction cocatalyst to accelerate hydrogen evolution, while RuO nanoparticles as an oxidation cocatalyst are deposited onto the sidewalls of CdS nanowires to facilitate oxygen evolution kinetics. The density functional theory simulations and ultrafast spectroscopic results reveal that photogenerated electrons and holes directionally migrate to MoS and RuO catalytic sites, respectively, thus achieving efficient charge carrier separation. The design of ternary dumbbell structure guarantees metal sulfides against photocorrosion and thus extends their range in solar water splitting.
基于金属硫化物半导体光催化剂的太阳能驱动全水分解仍然是一项挑战,这是由于强烈的电荷复合以及缺乏催化活性位点。此外,有效抑制逆反应,尤其是光催化水氧化催化过程中硫离子的氧化,是一项艰巨的任务,需要高效的光生空穴转移动力学。在此,开发了一种基于RuO/CdS/MoS的具有空间分离催化位点的三元哑铃形催化剂,以在无任何牺牲剂的模拟太阳光下同时产生氢气和氧气。特别地,锚定在CdS纳米线两端的MoS纳米片被确定为还原助催化剂以加速析氢,而作为氧化助催化剂的RuO纳米颗粒沉积在CdS纳米线的侧壁上以促进析氧动力学。密度泛函理论模拟和超快光谱结果表明,光生电子和空穴分别定向迁移到MoS和RuO催化位点,从而实现了有效的电荷载流子分离。三元哑铃结构的设计保证了金属硫化物不会发生光腐蚀,从而扩大了它们在太阳能水分解中的应用范围。