期刊
NATURE REVIEWS CHEMISTRY
卷 6, 期 4, 页码 243-258出版社
NATURE PORTFOLIO
DOI: 10.1038/s41570-022-00366-w
关键词
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资金
- King Abdullah University of Science and Technology
- Swedish Research Council [VR-2015-03814]
- Swedish Research Council for Sustainable Development [2016-00908]
- Swedish Energy Agency [44648-1]
- Formas [2016-00908] Funding Source: Formas
In the photochemical production of hydrogen from water, the rate-determining step is the hole-mediated oxidation reaction. A mismatch between the internal quantum efficiency of photon-induced hole generation and the apparent quantum yield of hydrogen often leads to a poor solar-to-hydrogen efficiency. This article critically assesses the issue of wasted holes and their consequential chemical effects, and outlines various approaches to improve overall efficiency in solar fuel production.
In photochemical production of hydrogen from water, the hole-mediated oxidation reaction is the rate-determining step. A poor solar-to-hydrogen efficiency is usually related to a mismatch between the internal quantum efficiency of photon-induced hole generation and the apparent quantum yield of hydrogen. This waste of photogenerated holes is unwanted yet unavoidable. Although great progress has been made, we are still far away from the required level of dexterity to deal with the associated challenges of wasted holes and its consequential chemical effects that have placed one of the greatest bottlenecks in attaining high solar-to-hydrogen efficiency. A critical assessment of the hole and its related phenomena in solar hydrogen production would, therefore, pave the way moving forward. In this regard, we focus on the contextual and conceptual understanding of the dynamics and kinetics of photogenerated holes and its critical role in driving redox reactions, with the objective of guiding future research. The main reasons behind and consequences of unused holes are examined and different approaches to improve overall efficiency are outlined. We also highlight yet unsolved research questions related to holes in solar fuel production.
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