Supramolecular tuning of supported metal phthalocyanine catalysts for hydrogen peroxide electrosynthesis

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

Supramolecular tuning of supported metal phthalocyanine catalysts for hydrogen peroxide electrosynthesis

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

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Publisher:: NATURE PORTFOLIO
Publication Type:: Journal Article
Citation:: Nature Catalysis, 2023, 6, (3), pp. 234-243
Issue Date:: 2023-03-01

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Field	Value	Language
dc.contributor.author	Lee, BH
dc.contributor.author	Shin, H
dc.contributor.author	Rasouli, AS
dc.contributor.author	Choubisa, H
dc.contributor.author	Ou, P
dc.contributor.author	Dorakhan, R
dc.contributor.author	Grigioni, I
dc.contributor.author	Lee, G
dc.contributor.author	Shirzadi, E
dc.contributor.author	Miao, RK
dc.contributor.author	Wicks, J
dc.contributor.author	Park, S
dc.contributor.author	Lee, HS
dc.contributor.author	Zhang, J https://orcid.org/0000-0001-5476-0134
dc.contributor.author	Chen, Y
dc.contributor.author	Chen, Z
dc.contributor.author	Sinton, D
dc.contributor.author	Hyeon, T
dc.contributor.author	Sung, YE
dc.contributor.author	Sargent, EH
dc.date.accessioned	2024-03-10T23:49:51Z
dc.date.available	2024-03-10T23:49:51Z
dc.date.issued	2023-03-01
dc.identifier.citation	Nature Catalysis, 2023, 6, (3), pp. 234-243
dc.identifier.issn	2520-1158
dc.identifier.issn	2520-1158
dc.identifier.uri	http://hdl.handle.net/10453/176424
dc.description.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.].
dc.language	English
dc.publisher	NATURE PORTFOLIO
dc.relation.ispartof	Nature Catalysis
dc.relation.isbasedon	10.1038/s41929-023-00924-5
dc.rights	info:eu-repo/semantics/closedAccess
dc.subject.classification	3402 Inorganic chemistry
dc.subject.classification	3406 Physical chemistry
dc.subject.classification	4004 Chemical engineering
dc.title	Supramolecular tuning of supported metal phthalocyanine catalysts for hydrogen peroxide electrosynthesis
dc.type	Journal Article
utslib.citation.volume	6
pubs.organisational-group	University of Technology Sydney
pubs.organisational-group	University of Technology Sydney/Faculty of Science
pubs.organisational-group	University of Technology Sydney/Faculty of Science/School of Mathematical and Physical Sciences
utslib.copyright.status	closed_access	*
dc.date.updated	2024-03-10T23:49:48Z
pubs.issue	3
pubs.publication-status	Published
pubs.volume	6
utslib.citation.issue	3

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.].

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http://hdl.handle.net/10453/176424