Gu, Z;
Zhang, L;
Wen, B;
An, X;
Lan, H;
Liu, L-M;
Chen, T;
... Qu, J; + view all
(2018)
Efficient design principle for interfacial charge separation in hydrogen-intercalated nonstoichiometric oxides.
Nano Energy
, 53
pp. 887-897.
10.1016/j.nanoen.2018.09.019.
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Abstract
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.
| Type: | Article |
|---|---|
| Title: | Efficient design principle for interfacial charge separation in hydrogen-intercalated nonstoichiometric oxides |
| Open access status: | An open access version is available from UCL Discovery |
| DOI: | 10.1016/j.nanoen.2018.09.019 |
| Publisher version: | https://doi.org/10.1016/j.nanoen.2018.09.019 |
| Language: | English |
| Additional information: | This version is the author accepted manuscript. For information on re-use, please refer to the publisher’s terms and conditions. |
| Keywords: | Science & Technology, Physical Sciences, Technology, Chemistry, Physical, Nanoscience & Nanotechnology, Materials Science, Multidisciplinary, Physics, Applied, Chemistry, Science & Technology - Other Topics, Materials Science, Physics, Charge separation, Oxygen vacancy, Photoelectrochemical water splitting, Photoanodes, DFT calculations, GENERALIZED GRADIENT APPROXIMATION, TOTAL-ENERGY CALCULATIONS, WAVE BASIS-SET, OXYGEN VACANCIES, TIO2 NANOPARTICLES, VANADIUM DIOXIDE, NANOCRYSTALS, DYNAMICS, SURFACES, PHOTOANODES |
| UCL classification: | UCL UCL > Provost and Vice Provost Offices > UCL BEAMS UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Engineering Science UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Engineering Science > Dept of Chemical Engineering |
| URI: | https://discovery.ucl.ac.uk/id/eprint/10085930 |
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