Efficient design principle for interfacial charge separation in hydrogen-intercalated nonstoichiometric oxides

CORC > 生态环境研究中心 > 中国科学院生态环境研究中心 > 中国科学院饮用水科学与技术重点实验室

	Efficient design principle for interfacial charge separation in hydrogen-intercalated nonstoichiometric oxides
	Qu, Jiuhui; Liu, Huijuan; Tang, Junwang; Cao, Xingzhong; Zhang, Jing; Chen, Tao; Liu, Li-Min; Lan, Huachun; An, Xiaoqiang; Wen, Bo
刊名	NANO ENERGY
	2018-11-01
卷号	53 页码:887-897
关键词	Charge separation Oxygen vacancy Photoelectrochemical water splitting Photoanodes DFT calculations
ISSN号	2211-2855
文献子类	Article
英文摘要	Establishing effective strategies to boost the separation of interfacial charge carriers is necessary to address the limiting bottlenecks of photocatalysis. Although oxygen vacancy modulation has become the prevalent strategy to improve the photoactivity, controversy persists regarding the real role of these defects in charge separation. To exert the great potential of nonstoichiometric semiconductors, one needs not only to establish a full atomistic picture of oxygen vacancies, but also to deliberate their possible interactions with other interfacial structures (represented by the ubiquitous intercalated hydrogen). Herein, WO3 was used as a typical model to demonstrate the principle of hydrogen-intercalated nonstoichiometric oxides for photoelectrochemical water splitting. Both experimental characterizations and theoretical calculations evidenced the synergetic interactions between oxygen vacancies and intercalated hydrogen. The sequential formation of subsurface defect clusters and surface O-H bonds contributed significantly to the spatial separation of charge carriers and the impressive stability of nonstoichiometric photoanodes. Profiting from this principle, an unprecedented photocurrent of 2.94 mA cm(-2) at 1.23 V vs. RHE was achieved, apart from a 100 mV cathodic shift in the onset potential. Our principle is applicable to several semiconductors, e.g. TiO2 and Fe2O3. Thus, it opens up a promising avenue into designing high-performance nonstoichiometric nanoarchitectures for a wide range of applications. The termination-dependent surface reactivity also provides new opportunities of reactive species modulation for high-performance photocatalysis.
内容类型	期刊论文
源URL	[http://ir.rcees.ac.cn/handle/311016/41353]
专题	生态环境研究中心_中国科学院饮用水科学与技术重点实验室
推荐引用方式 GB/T 7714	Qu, Jiuhui,Liu, Huijuan,Tang, Junwang,et al. Efficient design principle for interfacial charge separation in hydrogen-intercalated nonstoichiometric oxides[J]. NANO ENERGY,2018,53:887-897.
APA	Qu, Jiuhui.,Liu, Huijuan.,Tang, Junwang.,Cao, Xingzhong.,Zhang, Jing.,...&Gu, Zhenao.(2018).Efficient design principle for interfacial charge separation in hydrogen-intercalated nonstoichiometric oxides.NANO ENERGY,53,887-897.
MLA	Qu, Jiuhui,et al."Efficient design principle for interfacial charge separation in hydrogen-intercalated nonstoichiometric oxides".NANO ENERGY 53(2018):887-897.