Theory-guided design of hydrogen-bonded cobaltoporphyrin frameworks for highly selective electrochemical H2O2 production in acid

Xuan Zhao, Qi Yin, Xinnan Mao, Chen Cheng, Liang Zhang, Lu Wang (), Tian-Fu Liu (), Youyong Li and Yanguang Li ()
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Xuan Zhao: Soochow University
Qi Yin: Chinese Academy of Sciences
Xinnan Mao: Soochow University
Chen Cheng: Soochow University
Liang Zhang: Soochow University
Lu Wang: Soochow University
Tian-Fu Liu: Chinese Academy of Sciences
Youyong Li: Soochow University
Yanguang Li: Soochow University

Nature Communications, 2022, vol. 13, issue 1, 1-8

Abstract: Abstract The pursuit of selective two-electron oxygen reduction reaction to H2O2 in acids is demanding and largely hampered by the lack of efficient non-precious-metal-based electrocatalysts. Metal macrocycles hold promise, but have been relatively underexplored. Efforts are called for to promote their inherent catalytic activities and/or increase the surface exposure of active sites. In this contribution, we perform the high-throughput computational screening of thirty-two different metalloporphyrins by comparing their adsorption free energies towards key reaction intermediates. Cobalt porphyrin is revealed to be the optimal candidate with a theoretical overpotential as small as 40 mV. Guided by the computational predictions, we prepare hydrogen-bonded cobaltoporphyrin frameworks in order to promote the solution accessibility of catalytically active sites for H2O2 production in acids. The product features an onset potential at ~0.68 V, H2O2 selectivity of >90%, turnover frequency of 10.9 s−1 at 0.55 V and stability of ~30 h, the combination of which clearly renders it stand out from existing competitors for this challenging reaction.

Date: 2022
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DOI: 10.1038/s41467-022-30523-0

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