Killing Two Birds with One Stone: Upgrading Organic Compounds via Electrooxidation in Electricity-Input Mode and Electricity-Output Mode

The electrochemically oxidative upgrading reaction (OUR) of organic compounds has gained enormous interest over the past few years, owing to the advantages of fast reaction kinetics, high conversion efficiency and selectivity, etc., and it exhibits great potential in becoming a key element in coupling with electricity, synthesis, energy storage and transformation. On the one hand, the kinetically more favored OUR for value-added chemical generation can potentially substitute an oxygen evolution reaction (OER) and integrate with an efficient hydrogen evolution reaction (HER) or CO(2) electroreduction reaction (CO(2)RR) in an electricity-input mode. On the other hand, an OUR-based cell or battery (e.g., fuel cell or Zinc–air battery) enables the cogeneration of value-added chemicals and electricity in the electricity-output mode. For both situations, multiple benefits are to be obtained. Although the OUR of organic compounds is an old and rich discipline currently enjoying a revival, unfortunately, this fascinating strategy and its integration with the HER or CO(2)RR, and/or with electricity generation, are still in the laboratory stage. In this minireview, we summarize and highlight the latest progress and milestones of the OUR for the high-value-added chemical production and cogeneration of hydrogen, CO(2) conversion in an electrolyzer and/or electricity in a primary cell. We also emphasize catalyst design, mechanism identification and system configuration. Moreover, perspectives on OUR coupling with the HER or CO(2)RR in an electrolyzer in the electricity-input mode, and/or the cogeneration of electricity in a primary cell in the electricity-output mode, are offered for the future development of this fascinating technology.