Efficient design principle for interfacial charge separation in hydrogen-intercalated nonstoichiometric oxides | |
Gu, Zhenao; Zhang, Jing; Cao, Xingzhong; Tang, Junwang; Liu, Huijuan; Qu, Jiuhui; Chen T(陈涛); Zhang J(张静); Cao XZ(曹兴忠); Zhang, Le | |
刊名 | NANO ENERGY |
2018 | |
卷号 | 53页码:887-897 |
关键词 | Charge separation Oxygen vacancy Photoelectrochemical water splitting Photoanodes DFT calculations |
ISSN号 | 2211-2855 |
DOI | 10.1016/j.nanoen.2018.09.019 |
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. |
电子版国际标准刊号 | 2211-3282 |
WOS关键词 | GENERALIZED GRADIENT APPROXIMATION ; TOTAL-ENERGY CALCULATIONS ; WAVE BASIS-SET ; OXYGEN VACANCIES ; TIO2 NANOPARTICLES ; VANADIUM DIOXIDE ; NANOCRYSTALS ; DYNAMICS ; SURFACES ; PHOTOANODES |
WOS研究方向 | Astronomy & Astrophysics ; Physics |
语种 | 英语 |
WOS记录号 | WOS:000448994600097 |
内容类型 | 期刊论文 |
源URL | [http://ir.ihep.ac.cn/handle/311005/286610] |
专题 | 高能物理研究所_多学科研究中心 |
作者单位 | 中国科学院高能物理研究所 |
推荐引用方式 GB/T 7714 | Gu, Zhenao,Zhang, Jing,Cao, Xingzhong,et al. Efficient design principle for interfacial charge separation in hydrogen-intercalated nonstoichiometric oxides[J]. NANO ENERGY,2018,53:887-897. |
APA | Gu, Zhenao.,Zhang, Jing.,Cao, Xingzhong.,Tang, Junwang.,Liu, Huijuan.,...&Chen, Tao.(2018).Efficient design principle for interfacial charge separation in hydrogen-intercalated nonstoichiometric oxides.NANO ENERGY,53,887-897. |
MLA | Gu, Zhenao,et al."Efficient design principle for interfacial charge separation in hydrogen-intercalated nonstoichiometric oxides".NANO ENERGY 53(2018):887-897. |
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