Engineering Cobalt Phosphide (CoP) Thin Film Catalysts for Enhanced Hydrogen Evolution Activity on Silicon Photocathodes

Engineering Cobalt Phosphide (CoP) Thin Film Catalysts for Enhanced Hydrogen Evolution Activity on Silicon Photocathodes
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DOI:
10.1002/aenm.201501758
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发表时间:
2016-02-18
影响因子:
27.8
通讯作者:
Jaramillo, Thomas F.
Jaramillo, Thomas F.
中科院分区:
材料科学1区
文献类型:
--
作者:
Hellstern, Thomas R.;Benck, Jesse D.;Jaramillo, Thomas F.

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过渡金属磷化物催化剂最近已成为贵金属的活性、地球丰富的替代物,用于酸中的析氢反应。高性能、可扩展的催化剂对于成功实施光电化学水裂解装置是必要的,光电化学水裂解装置具有以可持续的方式产生氢气的潜力。本文报道了一种制备过渡金属磷化物薄膜的一般合成路线,其用于制备具有高平均转换频率(TOFavg)的磷化钴(CoP)催化剂,在100和120 mV的过电位下,TOFavg分别为0.48 H-2 s(-1)和1.0 H-2 s(-1)。此外,它表明,CoP薄膜可以应用到硅光吸收剂,以产生迄今为止最活跃的不含贵金属的晶体硅光电阴极之一,在+0.345 V vs.可逆氢电极下实现-10 mA cm(-2)。这里提出的合成路线提供了一个平台,明确的电催化剂的基础研究和高性能光电极的制造。
Transition metal phosphide catalysts have recently emerged as active, earth abundant alternatives to precious metals for the hydrogen evolution reaction in acid. High performance, scalable catalysts are necessary for the successful implementation of photoelectrochemical water splitting devices, which have the potential to generate hydrogen in a sustainable manner. Herein, a general synthetic route is reported to produce transition metal phosphide thin films, which is used to fabricate cobalt phosphide (CoP) catalysts with high average turnover frequency (TOFavg), 0.48 H-2 s(-1) and 1.0 H-2 s(-1) at 100 and 120 mV overpotential, respectively. Furthermore, it is shown that CoP thin films can be applied to silicon photoabsorbers to generate one of the most active precious metal-free crystalline silicon photocathodes to date, achieving -10 mA cm(-2) at +0.345 V vs. reversible hydrogen electrode. The synthesis route presented here provides a platform for both fundamental studies of well-defined electrocatalysts and the fabrication of high-performance photoelectrodes.