Theoretical efficiency limits of photoelectrochemical CO2 reduction: A route-dependent thermodynamic analysis.
Theoretical efficiency limits of photoelectrochemical CO2 reduction: A route-dependent thermodynamic analysis.
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DOI：
10.1002/cphc.201901041
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发表时间：
2019-12
期刊：
影响因子：
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通讯作者：
Evangelos Kalamaras;Huizhi Wang;M. Mercedes Maroto-Valer;J. Andresen;J. Xuan
中科院分区：
文献类型：
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作者：
Evangelos Kalamaras;Huizhi Wang;M. Mercedes Maroto-Valer;J. Andresen;J. Xuan
以水和二氧化碳为原料，通过光电化学（PEC）路线形成太阳能燃料引起了广泛关注。大多数 PEC CO2 减排研究都集中在新型光敏材料的开发上；然而，对于这一过程的关键限制因素仍然缺乏了解。在这项研究中，说明了单步多电子 CO2 还原为包括 HCOO-、CO、CH3OH 和 C2H5OH 在内的燃料的单结和双结光吸收材料的太阳能转化为燃料 (STF) 效率的理论极限。还需要强调的是，STF 效率取决于使用 CH3OH 作为模型燃料的两步 PEC CO2 还原过程的路线。最后，说明了双结光吸收电极、外部施加偏压和后续反应室等替代策略对 PEC CO2 还原最大理论效率的有益作用。
Solar fuel formation via photoelectrochemical (PEC) routes using water and CO2 as feedstock has attracted much attention. Most PEC CO2 reduction studies have been focused on the development of novel photoactive materials; however, there is still a lack of understanding of the key limiting factors of this process. In this study, the theoretical limits of Solar-to-Fuel (STF) efficiencies of single- and dual-junction photo-absorbing materials are illustrated for single-step multi-electron CO2 reduction into fuels including HCOO-, CO, CH3OH and C2H5OH. It is also highlighted that STF efficiency depends on the route of two-step PEC CO2 reduction process using CH3OH as a model fuel. Finally, it is illustrated the beneficial role of alternative strategies such as dual-junction photo-absorbing electrodes, externally applied bias and subsequent reactor chambers on the maximum theoretical efficiencies of PEC CO2 reduction.