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

Research output: Contribution to journalArticlepeer-review

67 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 languageEnglish (US)
Pages (from-to)234-243
Number of pages10
JournalNature Catalysis
Volume6
Issue number3
DOIs
StatePublished - Mar 2023

ASJC Scopus subject areas

  • Catalysis
  • Bioengineering
  • Biochemistry
  • Process Chemistry and Technology

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