Insight into the charge transfer in particulate Ta(3)N(5) photoanode with high photoelectrochemical performance.
Insight into the charge transfer in particulate Ta(3)N(5) photoanode with high photoelectrochemical performance.
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DOI：
10.1039/c6sc00245e
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发表时间：
2016-07-01
期刊：
影响因子：
8.4
通讯作者：
Li C
中科院分区：
文献类型：
--
作者：
Wang Z;Qi Y;Ding C;Fan D;Liu G;Zhao Y;Li C
电荷转移在微粒Ta 3 N5电极中具有重要的作用，是实现高效光电化学水氧化的基础。电荷分离是通过光电化学水裂解产生太阳能燃料的最关键因素之一，但它仍然没有得到很好的理解。这项工作揭示了光阳极中电荷转移对于实现高电荷分离效率的基本作用。具体而言，我们通过自下而上的方法制备了颗粒状Ta 3 N5光阳极。通过精细颈缩处理改善电荷分离，光电流增加了两个数量级。电荷分离效率（ηsep）通过将其分为电荷产生效率（Φgene）和传输效率（Φ transs）来分析。颈缩处理被发现大大提高电子转移。瞬态光电压（TPV）的测量的基础上的Duplex效应被用来确认颈缩处理的好处，在改善电荷传输。颈缩-Ta_3 N_5电极中的上级电子转移通过与铁/亚铁氰化物氧化还原对的容易的电子交换反应进一步证明。此外，磷酸钴被发现促进电荷分离和表面反应，导致在1.23 V时的光电流为6.1 mA cm-2（相对于RHE），这是颗粒光电阳极的最高响应。
Charge transfer has been demonstrated to have a fundamental role in particulate Ta3N5 electrode for achieving high efficient photoelectrochemical water oxidation. Charge separation is one of the most critical factors for generating solar fuels via photoelectrochemical water splitting, but it is still not well understood. This work reveals the fundamental role of charge transfer in photoanodes for achieving high charge separation efficiency. Specifically, we fabricated a particulate Ta3N5 photoanode by a bottom-up method. By improving the charge separation with refined necking treatment, the photocurrent is increased by two orders of magnitude. The charge separation efficiency (ηsep) is analyzed by dividing it into charge generation efficiency (Φgene) and transportation efficiency (Φtrans). Necking treatment is found to substantially improve the electron transfer. Transient photovoltage (TPV) measurements based on the Dember effect is used to confirm the benefit of necking treatment in improving the charge transportation. The superior electron transfer in the necked-Ta3N5 electrode is further evidenced by the facile electron exchange reaction with the ferri/ferrocyanide redox couple. Moreover, cobalt phosphate is found to promote both charge separation and surface reaction, resulting in a photocurrent of 6.1 mA cm–2 at 1.23 V vs. RHE, which is the highest response for a particulate photoanode.
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