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.

Supramolecular tuning of supported metal phthalocyanine catalysts for hydrogen peroxide electrosynthesis / B. Lee, H. Shin, A. Rasouli, H. Choubisa, P. Ou, R. Dorakhan, I. Grigioni, G. Lee, E. Shirzadi, R. Miao, J. Wicks, S. Park, H. Lee, J. Zhang, Y. Chen, Z. Chen, D. Sinton, T. Hyeon, Y. Sung, E. Sargent. - In: NATURE CATALYSIS. - ISSN 2520-1158. - 6:3(2023 Mar 13), pp. 234-243. [10.1038/s41929-023-00924-5]

Supramolecular tuning of supported metal phthalocyanine catalysts for hydrogen peroxide electrosynthesis

I. Grigioni;
2023

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.
Settore CHIM/02 - Chimica Fisica
Settore ING-IND/23 - Chimica Fisica Applicata
Settore CHIM/04 - Chimica Industriale
13-mar-2023
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Utilizza questo identificativo per citare o creare un link a questo documento: https://hdl.handle.net/2434/972948
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