Congratulations to Rileigh and Kelsey for publishing their review/perspective paper in Joule (https://doi.org/10.1016/j.joule.2021.05.014).
Given the recent surge of interest in electrochemical CO2 reduction and in particular, recent discoveries of the curious effects of using pulsed potentials, we felt that this is a perfect time to write a review and perspective paper to share recent advances and hopefully inspire other researchers to pursue these exciting opportunities . To put the compelling prospects of pulsed methods in broader context, we provide a brief review of fundamental considerations in electrochemical CO2reduction as a segue to our forward-looking perspective on exciting emerging opportunities in this field.
Amidst growing concerns about increasing atmospheric CO2levels, electrochemical CO2reduction has emerged as a promising approach to valorize CO2under commercially relevant conditions. Intensive recent experimental and computational research efforts have significantly advanced our understanding of the role of the electrode, electrolyte, and electrolyzer design. Among this flurry of research activity, the application of pulsed potentials has led to several discoveries, primarily that the pulse profile presents a new, yet unexplored, ‘knob’ to control product selectivity. The ostensibly simple process of switching the potential on (or off) influencesthe choreography and complex interrelation of underlying physicochemical processes including hydrodynamics, ad-and desorption, and changes in the electrode structure and composition. The leitmotif of this perspective is that amidst this complexity resides a compelling opportunity for both scientific and technological advances in electrosynthetic processes beyond CO2reduction. We have organized the perspective as follows: we first discuss critical general electrochemical considerations and then review recent achievements with regards to pulsed electrochemical CO2reduction before diving into specific aspects of physical processes and the reaction mechanism. We provide an outlook to both future scientific challenges and potential technological applications
