Photo‐electrochemical production of solar fuels from carbon dioxide, water, and sunlight is an appealing approach. Nevertheless, it remains challenging to scale despite encouraging demonstrations at low power input. Higher current densities require notable voltage input as ohmic losses and activation overpotentials become more significant, resulting in lower solar‐to‐CO conversion efficiencies. A concentrated photovoltaic cell is integrated into a custom‐made heat managed photo‐electrochemical device. The heat is transferred from the photovoltaic module to the zero‐gap electrolyzer cell by the stream of anodic reactant and produce synergetic effects on both sides. With solar concentrations up to 450 suns (i.e., 450 kW m−2) applied for the first time to photo‐electrochemical reduction of CO2, a partial current for CO production of 4 A is achieved. At optimal conditions, the solar‐to‐CO conversion efficiency reaches 17% while maintaining a current density of 150 mA cm−2 in the electrolyzer and a CO selectivity above 90%, representing an overall 19% solar‐to‐fuel conversion efficiency. This study represents a first demonstration of photo‐electrochemical CO2 reduction under highly concentrated light, paving the way for resource efficient solar fuel production at high power input.

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Achieving high current densities while maintaining a high energy conversion efficiency is one of the main challenges for enhancing the economic competitiveness of solar fuel producing photo-electrochemical devices [1]. I will discuss two device implementations utilizing concentrated irradiation to achieve high current density operation. The water-splitting device is utilizing thermal integration to sustain high performance while dealing with high current density and the corresponding overpotentials [2]. I will quantify the theoretical increase in the maximum efficiencies at given current densities of photoelectrochemical devices resulting from thermal synergies. I will then discuss device implementation of such an approach and show how more realistic device models (multi-dimensional, multi-scale, multi-physics) can be used to support the device implementation and its operational understanding [3]. I will then show how the design principles developed for water splitting can be translated to CO2 reduction devices and discuss a corresponding device implementation. [1] M. Dumortier, S. Tembhurne, S. Haussener, Energy Environmental Science, 8: 3614-3628, 2015. [2] S. Tembhurne, F. Nandjou, S. Haussener, Nature Energy, 4: 399-407, 2019. [3] S. Tembhurne, S. Haussener, Journal of The Electrochemical Society, 163: H1008-H1018, 2016.