Integrated design for electrocatalytic carbon dioxide reduction

Electrocatalytic carbon dioxide reduction reaction (CO2RR) to produce valuable fuels and chemicals with renewable energy inputs is an attractive route to convert intermittent green energy sources (e.g., solar and wind) to chemical energy, alleviate our dependence on fossil fuels, and simultaneously reduce net carbon dioxide emission. However, the generation of reduced multi-carbon products with high energy density and wide applicability from CO2RR, such as oxygenates and hydrocarbons, suffers from high overpotential, slow reaction rate, and low selectivity due to the intrinsicmulti-electron transfer nature. Moreover, the involved anodic oxygen evolution reaction (OER) also requires large overpotential and its product O2 bears limited economic value. The potentially generated reactive oxygen species (ROS) during OER may also degrade the membrane of a CO2 reduction electrolyzer. Herein, we review the recent progress in novel integrated strategies to address the aforementioned challenges in electrocatalytic CO2RR. These innovative strategies include (1) concurrent CO2 electroreduction via co-feeding additional chemicals besides CO2 gas, (2) tandem CO2 electroreduction utilizing other catalysts for converting the in-situ formed products from CO2RR to more valuable chemicals, and (3) hybrid CO2 electroreduction through integrating thermodynamically more favourable organic upgrading reactions to replace anodic OER. We specifically highlight these novel integrated electrolyzer designs instead of focusing on nanostructured engineering of various electrocatalysts, in the hope of inspiring others to approach CO2 electroreduction from a wholistic perspective. The current challenges and future opportunities of electrocatalytic CO2 reduction will also be discussed at the end.