Department of Electrical and Computer Engineering National University of Singapore, 4 Engineering Drive 3, Singapore, 117583, Singapore.
Institute of Materials Research and Engineering, A*STAR (Agency for Science, Technology and Research), 2 Fusionopolis Way, Innovis, Singapore, 138634, Singapore.
Adv Mater. 2019 Sep;31(37):e1903605. doi: 10.1002/adma.201903605. Epub 2019 Jul 31.
Converting and storing intermittent solar energy into stable chemical fuels of high efficiency depend crucially on harvesting excess energy beyond the conventional ultraviolet light spectrum. The means of applying highly efficient solar-thermal conversion on practical electricity-driven water splitting could be a significant stride toward this goal, while some bottlenecks remain unresolved. Herein, photothermic electrocatalytic oxygen and hydrogen evolution reactions are proposed, which bestow a distinctive exothermic activation and electrochemical reactivity in a reconstructed electrolyzer system, and which are poised for efficient renewable energy production. Attributed to the synergistic in situ coupling of the N-doped carbon, metallic alloy and oxides, in view of their broadband light absorption, high electrochemical surface area, and efficient charge transfer attributes, the hybrid photothermal electrocatalytic electrode simultaneously satisfies efficient photon-to-heat conversion and augmented electrochemical catalytic activity. Finally, a system level design of an appropriate photothermally mediated electrolytic cell with close-proximity light-illumination window along with a low-thermal-emittance electrolyte separator that preserve an overall large localized thermal gradient and efficient mass transport is devised. Such a photothermally mediated electrocatalytic system presented here may open up new avenues for the development of solar-thermal energy utilization in other forms.
将间歇性太阳能转化和储存为高效稳定的化学燃料，关键取决于如何在传统紫外线光谱之外捕获多余的能量。在实际的电力驱动水分解中应用高效太阳能热转化的方法可能是实现这一目标的重要一步，但仍存在一些尚未解决的瓶颈。在此，提出了光热电催化氧气和氢气的析出反应，在重构的电解槽系统中赋予了独特的放热激活和电化学反应性，为高效可再生能源的生产提供了可能。由于氮掺杂碳、金属合金和氧化物的协同原位耦合，它们具有宽频光吸收、高电化学表面积和高效电荷转移特性，混合光热电化学催化电极同时满足高效的光子-热转换和增强的电化学催化活性。最后，设计了一个具有适当的光热介导电解槽的系统级设计，该电解槽具有靠近光照明窗口的位置以及低热发射率的电解质分离器，以保持整体较大的局部热梯度和有效的质量传递。这里提出的光热介导电催化系统可能为开发其他形式的太阳能热能利用开辟新途径。
