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

Cao, Peike; Quan, Xie; Nie, Xiaowa; Zhao, Kun; Liu, Yanming; Chen, Shuo; Yu, Hongtao; Chen, Jingguang G · Nat Commun · 2023

basic_science · Level V

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Abstract

Direct hydrogen peroxide (H2O2) 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 H2O2 production at a record rate of 11,527 mmol h-1 gcat-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 H2O2 electrosynthesis in acidic, neutral and alkaline electrolytes.