4.8 Article

Molecularly Functionalized Electrodes for Efficient Electrochemical Water Remediation

Journal

CHEMSUSCHEM
Volume 14, Issue 16, Pages 3267-3276

Publisher

WILEY-V C H VERLAG GMBH
DOI: 10.1002/cssc.202100878

Keywords

catalyst immobilization; hydroxyl radicals; pollutant degradation; sustainable chemistry; water remediation

Funding

  1. Advanced Materials for Energy-Water Systems (AMEWS) Center, an Energy Frontier Research Center - U.S. Department of Energy, Office of Science, Basic Energy Sciences
  2. Photosynthetic Systems program of the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-06CH11357]

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The study found that surface functionalization of metal oxides with a Ru(II)poly(pyridyl) complex can create hybrid assemblies with optimized electrochemical performance for water remediation. This approach effectively suppresses the formation of hydroxyl radicals and inhibits the competing side reaction of water splitting.
The development and investigation of materials that leverage unique interfacial effects on electronic structure and redox chemistry are likely to play an outstanding role in advanced technologies for wastewater treatment. Here, the use of surface functionalization of metal oxides with a Ru(II)poly(pyridyl) complex was reported as a way to create hybrid assemblies with optimized electrochemical performance for water remediation, superior to those that could be achieved with the molecular catalyst or metal-oxide electrodes used individually. Mechanistic analysis demonstrated that the molecularly functionalized electrodes could suppress the formation of hydroxyl radicals (i. e., the dominant remediation pathway for bare metal-oxide electrodes), allowing the water remediation to proceed through the highly oxidizing Ru3+ ions in the surface-bound complexes. Furthermore, the underlying metal-oxide substrates played a crucial role in altering the electronic structure and electrochemical properties of the surface-bound catalyst, such that the competing side reaction (i. e., water splitting) was largely inhibited.

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