Fundamental Insights for Practical Electrocatalytic CO2 Reduction.

Abstract

ConspectusGlobal energy's continuous reliance on fossil fuels has driven unprecedented CO2 emission growth, intensifying climate volatility through heightened frequency and severity of extreme weather events. These crises underscore the critical need for accelerating innovation in sustainable energy technologies capable of reconciling two urgent imperatives: ensuring reliable energy access while delivering measurable progress toward global decarbonization commitments. Electrocatalytic CO2 reduction reaction (CO2RR) technology implementation could not only help to reduce CO2 concentrations in the atmosphere but also provide new possibilities for renewable energy storage, thus playing a crucial role in driving the energy transition and achieving carbon neutrality. To advance the industrialization of this technology, multiple global companies (Sunfire, Germany; Dioxide Materials, USA; Carbon Energy Technology, China, etc.) have initiated pilot-scale research. However, progress has been slow due to challenges related to catalyst, electrode, and electrolyzer design. Through integrated optimizations spanning catalyst structural engineering, electrode configuration fabrication, and electrolyzer system design, we have demonstrated progressive milestones in the technology of CO2RR.This Account systematically presents our research group's groundbreaking contributions to practical CO2RR, spanning catalyst design, electrode architecture fabrication, and advanced electrolyzer development. Based on the current research foundation in our group, we contend that for the industrial-scale development of CO2 reduction reactions, greater emphasis should be placed on catalyst stability rather than solely on catalytic activity. To improve the stability of catalytic systems, several strategies can be implemented, including enhancing electron transfer rate and strengthening interatomic bonds to mitigate catalyst degradation during operation. We have also proposed a strategy for customizing highly efficient catalysts by simulating the degradation path of the catalyst. In addition, we also advocate heightened attention to electrode fabrication processes, encompassing structural design and paired electrolysis configurations, as these factors critically influence the overall system's conversion efficiency, stability and ultimately the economic viability of industrial applications. Additionally, we highlight our progress in electrolyzer research, particularly demonstrating the advantages and potential of the proton exchange membrane (PEM) electrolyzer in CO2 reduction systems. Given their ability to concurrently address challenges such as high CO2 loss rates and the carbonate deposition problem, we propose that this direction needs superior development to advance CO2RR industrialization. Finally, we summarize this Account and propose future research directions, focusing on scalable production of catalysts, CO2 capture technologies, direct flue gas electrolysis, system integration, and economic and environmental assessments. This systematic progress bridges gaps between fundamental electrocatalysis and practical implementation, charting a viable pathway toward carbon-negative chemical manufacturing.