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Revealing and Facilitating the Rate-Determining Step for Efficient Sunlight-Driven Photocatalysis
The Journal of Physical Chemistry Letters ( IF 4.8 ) Pub Date : 2021-08-05 , DOI: 10.1021/acs.jpclett.1c02101
Houkui Xiang 1, 2 , Zhijian Wang 1 , Jiazang Chen 1, 2
Affiliation  

Because of the complex composition of the apparent activation energy, the rate-determining step in a photocatalytic reaction like hydrogen evolution is still being explored even after sluggish oxygen evolution is replaced with efficient hole extraction. This issue severely limits the implementation of certain strategies like the synergistic thermal effect. Here, by developing a combined monitor method based on open-circuit potential decay, we demonstrate that semiconductor–cocatalyst interfacial electron transfer occurring on a decisecond to second time scale dominates photocatalytic hydrogen evolution. This time scale is approximately 6–12 orders of magnitude larger than the widely reported values of picoseconds to microseconds and is comparable to that predicted by Durrant et al. To improve photocatalytic hydrogen evolution, we manage to create more intermediate sites by electronically doping the semiconductor surface. This measure promotes semiconductor–cocatalyst interfacial electron transfer by charge recombination and makes the synergistic thermal effect very evident.

中文翻译:

揭示和促进高效阳光驱动光催化的速率决定步骤

由于表观活化能的复杂组成,即使在用有效的空穴提取代替缓慢的析氧之后,仍在探索光催化反应(如析氢)中的速率决定步骤。这个问题严重限制了某些策略的实施,如协同热效应。在这里,通过开发一种基于开路电位衰减的联合监测方法,我们证明了发生在分秒到秒时间尺度上的半导体-助催化剂界面电子转移主导了光催化析氢。这个时间尺度比广泛报道的皮秒到微秒的值大大约 6-12 个数量级,并且与 Durrant 等人预测的值相当。为了改善光催化析氢,我们设法通过对半导体表面进行电子掺杂来创建更多的中间位点。该措施通过电荷复合促进半导体-助催化剂界面电子转移,并使协同热效应非常明显。
更新日期:2021-08-19
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