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Supramolecular tuning of supported metal phthalocyanine catalysts for hydrogen peroxide electrosynthesis

Cited 36 time in Web of Science Cited 36 time in Scopus
Authors

Lee, Byoung-Hoon; Shin, Heejong; Rasouli, Armin Sedighian; Choubisa, Hitarth; Ou, Pengfei; Dorakhan, Roham; Grigioni, Ivan; Lee, Geonhui; Shirzadi, Erfan; Miao, Rui Kai; Wicks, Joshua; Park, Sungjin; Lee, Hyeon Seok; Zhang, Jinqiang; Chen, Yuanjun; Chen, Zhu; Sinton, David; Hyeon, Taeghwan; Sung, Yung-Eun; Sargent, Edward H.

Issue Date
2023-03
Publisher
NATURE PUBLISHING GROUP
Citation
Nature Catalysis, Vol.6 No.3, pp.234-243
Abstract
Two-electron oxygen reduction offers a route to H2O2 that is potentially cost-effective and less energy-intensive than the industrial anthraquinone process. However, the catalytic performance of the highest performing prior heterogeneous electrocatalysts to H2O2 has lain well below the >300 mA cm−2 needed for capital efficiency. Herein, guided by computation, we present a supramolecular approach that utilizes oxygen functional groups in a carbon nanotube substrate that—when coupled with a cobalt phthalocyanine catalyst—improve cobalt phthalocyanine adsorption, preventing agglomeration; and that further generate an electron-deficient Co centre whose interaction with the key H2O2 intermediate is tuned towards optimality. The catalysts exhibit an overpotential of 280 mV at 300 mA cm−2 with turnover frequencies over 50 s−1 in a neutral medium, an order of magnitude higher activity compared with the highest performing prior H2O2 electrocatalysts. This performance is sustained for over 100 h of operation. [Figure not available: see fulltext.].
ISSN
2520-1158
URI
https://hdl.handle.net/10371/192249
DOI
https://doi.org/10.1038/s41929-023-00924-5
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