Combination of Highly Efficient Electrocatalytic Water Oxidation with Selective Oxygenation of Organic Substrates using Manganese Borophosphates

Prashanth W. Menezes, Carsten Walter, Biswarup Chakraborty, Jan Niklas Hausmann, Ivelina Zaharieva, Achidi Frick, Elizabeth von Hauff, Holger Dau, Matthias Driess

Research output: Contribution to journalArticlepeer-review

46 Scopus citations

Abstract

One of the key catalytic reactions for life on earth, the oxidation of water to molecular oxygen, occurs in the oxygen-evolving complex of the photosystem II (PSII) mediated by a manganese-containing cluster. Considerable efforts in this research area embrace the development of efficient artificial manganese-based catalysts for the oxygen evolution reaction (OER). Using artificial OER catalysts for selective oxygenation of organic substrates to produce value-added chemicals is a worthwhile objective. However, unsatisfying catalytic performance and poor stability have been a fundamental bottleneck in the field of artificial PSII analogs. Herein, for the first time, a manganese-based anode material is developed and paired up for combining electrocatalytic water oxidation and selective oxygenations of organics delivering the highest efficiency reported to date. This can be achieved by employing helical manganese borophosphates, representing a new class of materials. The uniquely high catalytic activity and durability (over 5 months) of the latter precursors in alkaline media are attributed to its unexpected surface transformation into an amorphous MnOx phase with a birnessite-like short-range order and surface-stabilized MnIII sites under extended electrical bias, as unequivocally demonstrated by a combination of in situ Raman and quasi in situ X-ray absorption spectroscopy as well as ex situ methods.

Original languageEnglish
Article number2004098
JournalAdvanced Materials
Volume33
Issue number9
DOIs
StatePublished - 1 Mar 2021
Externally publishedYes

Keywords

  • active catalytic structures
  • electrocatalytic water oxidation
  • helical manganese borophosphates
  • selective oxygenation

ASJC Scopus subject areas

  • General Materials Science
  • Mechanics of Materials
  • Mechanical Engineering

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