Metal single-site catalyst design for electrocatalytic production of hydrogen peroxide at industrial-relevant currents

• Published in: Nature communications Vol. 14; no. 1; p. 172
• Main Authors: Cao, Peike, Quan, Xie, Nie, Xiaowa, Zhao, Kun, Liu, Yanming, Chen, Shuo, Yu, Hongtao, Chen, Jingguang G.
• Format: Journal Article
• Language: English
• Published: London Nature Publishing Group UK 12.01.2023; Nature Publishing Group; Nature Portfolio
• Subjects: 119/118; 140/133; 140/146; 147/135; 147/143; 639/638/77/886; 704/172/169/896; Anthraquinone; Anthraquinones; Catalysts; Chemical reduction; Chemical synthesis; Cobalt; Electrocatalysts; Electrolytes; Energy; Humanities and Social Sciences; Hydrogen peroxide; Hydrogen production; multidisciplinary; Oxygen; Oxygen reduction reactions; Science; Science (multidisciplinary); Transition metals
• ISSN: 2041-1723; 2041-1723
• DOI: 10.1038/s41467-023-35839-z

Direct hydrogen peroxide (H 2 O 2 ) electrosynthesis via the two-electron oxygen reduction reaction is a sustainable alternative to the traditional energy-intensive anthraquinone technology. However, high-performance and scalable electrocatalysts with industrial-relevant production rates remain to be challenging, partially due to insufficient atomic level understanding in catalyst design. Here we utilize theoretical approaches to identify transition-metal single-site catalysts for two-electron oxygen reduction using the *OOH binding energy as a descriptor. The theoretical predictions are then used as guidance to synthesize the desired cobalt single-site catalyst with a O-modified Co-(pyrrolic N) 4 configuration that can achieve industrial-relevant current densities up to 300 mA cm − 2 with 96–100% Faradaic efficiencies for H 2 O 2 production at a record rate of 11,527 mmol h − 1  g cat − 1 . Here, we show the feasibility and versatility of metal single-site catalyst design using various commercial carbon and cobalt phthalocyanine as starting materials and the high applicability for H 2 O 2 electrosynthesis in acidic, neutral and alkaline electrolytes. Direct hydrogen peroxide electrosynthesis offers a sustainable alternative to the traditional energy-intensive anthraquinone technology. Here, the authors report a scalable cobalt single-site catalyst for hydrogen peroxide synthesis at industrial-relevant currents in acidic, neutral or alkaline electrolyte.