Enriched Surface Oxygen Vacancies of Photoanodes by Photoetching with Enhanced Charge Separation

Enriched Surface Oxygen Vacancies of Photoanodes by Photoetching with Enhanced Charge Separation
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DOI:
10.1002/anie.201913295
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发表时间:
2019-12-23
影响因子:
16.6
通讯作者:
Gong, Jinlong
Gong, Jinlong
中科院分区:
化学1区
文献类型:
--
作者:
Feng, Shijia;Wang, Tuo;Gong, Jinlong

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介绍了一种简单的光刻方法,该方法通过限制BiVO4光阳极表面的氧空位(O-VAc),通过10分钟的光刻来减轻体缺陷的负面影响。这一策略可以在BiVO4表面诱导丰富的O-VAc,从而避免形成过多的体缺陷。根据密度泛函理论(DFT)的计算结果,提出了BiVO4/电解液界面电荷分离增强的机理。优化后的富集面O-VAc的BiVO4在未掺杂的BiVO4光阳极中表现出最大的光电流。当负载FeOOH/NiOOH共催化剂时,光刻BiVO4光阳极在0.6V与可逆氢电极相比可获得相当大的水氧化光电流3.0 mA cm(-2)。这种BiVO4光阳极和硅光阴极在1个太阳光照度下实现了3.5%的无偏压光-氢转换效率。
A facile photoetching approach is described that alleviates the negative effects from bulk defects by confining the oxygen vacancy (O-vac) at the surface of BiVO4 photoanode, by 10-minute photoetching. This strategy could induce enriched O-vac at the surface of BiVO4, which avoids the formation of excessive bulk defects. A mechanism is proposed to explain the enhanced charge separation at the BiVO4 /electrolyte interface, which is supported by density functional theory (DFT) calculations. The optimized BiVO4 with enriched surface O-vac presents the highest photocurrent among undoped BiVO4 photoanodes. Upon loading FeOOH/NiOOH cocatalysts, photoetched BiVO4 photoanode reaches a considerable water oxidation photocurrent of 3.0 mA cm(-2) at 0.6 V vs. reversible hydrogen electrode. An unbiased solar-to-hydrogen conversion efficiency of 3.5 % is realized by this BiVO4 photoanode and a Si photocathode under 1 sun illumination.