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首页> 外文期刊>Applied Catalysis, B. Environmental: An International Journal Devoted to Catalytic Science and Its Applications >Photoelectrochemical hydrogen production by water splitting over dual-functionally modified oxide: p-Type N-doped Ta2O5 photocathode active under visible light irradiation
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Photoelectrochemical hydrogen production by water splitting over dual-functionally modified oxide: p-Type N-doped Ta2O5 photocathode active under visible light irradiation

机译：通过双功能改性氧化物上的水分解产生光电化学制氢：可见光下活化的p型N掺杂Ta2O5光阴极

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摘要

Doping of nitrogen into tantalum pentoxide (Ta2O5) drastically modifies two semiconductor characteristics simultaneously; first is activation toward visible light region from 320 to 520 nm in wavelength and second is reversed polarity in photoresponse from n-type to p-type conduction. N-doped Ta2O5 (N-Ta2O5) was also found to possess highly negative energy position of conduction band minimum (-1.3 V vs NHE) compared to those of Ta2O5 and TaON (-0.3 V), which was originated from surface dipole effect as recently clarified by DFT calculation reported in a literature. Here, we exhibit the first demonstration of photoreaction over N-Ta2O5 in an aqueous solution. The surface of N-Ta2O5 was found to be almost inert for hydrogen production by water splitting. However, the hydrogen generation rate was highly enhanced by surface modification with Pt, Rh or Au, which was assessed by photocathodic current over N-Ta2O5 films under visible light irradiation (lambda >= 410 nm). Among them, loading with either Pt or Rh greatly enhanced the H-2 evolution rate in an aqueous solution by two orders of magnitude compared to that over unmodified N-Ta2O5 for both films and powders. These results imply that the dual functional modification by single doping of N has a potential to generate new photocathodes for water splitting reaction under visible light irradiation. (C) 2016 Elsevier B.V. All rights reserved.
机译：将氮掺杂到五氧化二钽（Ta2O5）中会同时极大地改变两个半导体特性。首先是朝波长为320至520 nm的可见光区域激活，其次是将光响应的极性从n型传导转换为p型。与Ta2O5和TaON（-0.3 V）相比，N掺杂的Ta2O5（N-Ta2O5）还具有最小的导带负能量位置（-1.3 V vs NHE），这是由于表面偶极效应引起的。最近通过文献报道的DFT计算进行了澄清。在这里，我们展示了在水溶液中通过N-Ta2O5进行光反应的第一个演示。发现N-Ta2O5的表面对于通过水分解产生的氢气几乎是惰性的。但是，通过用Pt，Rh或Au进行表面改性可以大大提高氢的产生速率，这是通过可见光照射下（λ> 410 nm）N-Ta2O5薄膜上的光阴极电流来评估的。其中，与未改性的N-Ta2O5相比，无论是薄膜还是粉末，Pt或Rh的负载都大大提高了水溶液中H-2的析出速率两个数量级。这些结果表明，通过单次掺杂N进行的双功能改性有可能在可见光照射下产生用于水分解反应的新光阴极。 （C）2016 Elsevier B.V.保留所有权利。

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