Supramolecular tuning of supported metal phthalocyanine catalysts for hydrogen peroxide electrosynthesis

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

doi:10.1038/s41929-023-00924-5

Supramolecular tuning of supported metal phthalocyanine catalysts for hydrogen peroxide electrosynthesis

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

^*Corresponding author for this work

Chemistry

Research output: Contribution to journal › Article › peer-review

139 Scopus citations

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.].

Original language	English (US)
Pages (from-to)	234-243
Number of pages	10
Journal	Nature Catalysis
Volume	6
Issue number	3
DOIs	https://doi.org/10.1038/s41929-023-00924-5
State	Published - Mar 2023

Funding

This work was supported by the Natural Gas Innovation Fund, the Natural Sciences and Engineering Research Council of Canada, the Natural Resources Canada Clean Growth Program, and the Ontario Research Fund—Research Excellence programme. All DFT computations were performed on the Niagara supercomputer at the SciNet HPC Consortium. SciNet is funded by the Canada Foundation for Innovation, the Government of Ontario, the Ontario Research Fund Research Excellence Program, and the University of Toronto. This work was also supported by the Research Center Program of the IBS (IBS-R006-A2, Y.-E.S; IBS-R006-D1, T.H) in Korea.

ASJC Scopus subject areas

Catalysis
Bioengineering
Biochemistry
Process Chemistry and Technology

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Cite this

Lee, B. H., Shin, H., Rasouli, A. S., Choubisa, H., Ou, P., Dorakhan, R., Grigioni, I., Lee, G., Shirzadi, E., Miao, R. K., Wicks, J., Park, S., Lee, H. S., Zhang, J., Chen, Y., Chen, Z., Sinton, D., Hyeon, T., Sung, Y. E., & Sargent, E. H. (2023). Supramolecular tuning of supported metal phthalocyanine catalysts for hydrogen peroxide electrosynthesis. Nature Catalysis, 6(3), 234-243. https://doi.org/10.1038/s41929-023-00924-5

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title = "Supramolecular tuning of supported metal phthalocyanine catalysts for hydrogen peroxide electrosynthesis",

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.].",

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

note = "Publisher Copyright: {\textcopyright} 2023, The Author(s), under exclusive licence to Springer Nature Limited.",

year = "2023",

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Lee, BH, Shin, H, Rasouli, AS, Choubisa, H, Ou, P, Dorakhan, R, Grigioni, I, Lee, G, Shirzadi, E, Miao, RK, Wicks, J, Park, S, Lee, HS, Zhang, J, Chen, Y, Chen, Z, Sinton, D, Hyeon, T, Sung, YE & Sargent, EH 2023, 'Supramolecular tuning of supported metal phthalocyanine catalysts for hydrogen peroxide electrosynthesis', Nature Catalysis, vol. 6, no. 3, pp. 234-243. https://doi.org/10.1038/s41929-023-00924-5

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AU - Ou, Pengfei

AU - Dorakhan, Roham

AU - Grigioni, Ivan

AU - Lee, Geonhui

AU - Shirzadi, Erfan

AU - Miao, Rui Kai

AU - Wicks, Joshua

AU - Park, Sungjin

AU - Lee, Hyeon Seok

AU - Zhang, Jinqiang

AU - Chen, Yuanjun

AU - Chen, Zhu

AU - Sinton, David

AU - Hyeon, Taeghwan

AU - Sung, Yung Eun

AU - Sargent, Edward H.

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N2 - 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.].

AB - 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.].

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Supramolecular tuning of supported metal phthalocyanine catalysts for hydrogen peroxide electrosynthesis

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