(Invited) Electrocatalysts and Processes for Carbon Dioxide Reduction

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Efficient and robust electrocatalytic processes that convert climate-damaging carbon dioxide into useful fuels and chemicals are essential to decarbonize our economy. The accelerated discovery of effective catalysts critically depends on rational materials design, predicated on mechanistic and structural understanding of catalysts, electrode–electrolyte interfaces, and mass transport and catalytic processes. New synthetic methods are needed that enable the preparation of tailored multimetallic nanomaterials with precisely controlled properties, for which pulsed laser in liquids synthesis is an ideal tool. Laser-made catalysts are intrinsically more active than analogs made by conventional equilibrium methods.[1] For electrolyzer devices, nanoparticulate catalysts must be immobilized on inert, high surface area carbon substrates for electrocatalysis in aqueous electrolytes. We solved this challenge by preparing carbon fiber paper with intact mesostructures and long-lasting hydrophilicity by a green chemistry process.[2] We developed novel copper-free trimetallic electrocatalysts for aqueous carbon dioxide reduction [3] that produced C–C-coupled products. Systematic variation of metal ratios revealed trends in product distributions. We also assessed gold nanoparticle–hydrophilic carbon fiber paper assemblies with ionomer overlayers for clean syngas generation. Our laser-made catalysts together with the newly developed ability to use them on high surface area electrode supports provide the foundation towards the realization of viable successor technologies.