Molecularly Functionalized Electrodes for Efficient Electrochemical Water Remediation

Document Type

Article

Publication Date

8-23-2021

Abstract

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 RuIIpoly(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.

Identifier

85109788594 (Scopus)

Publication Title

Chemsuschem

External Full Text Location

https://doi.org/10.1002/cssc.202100878

e-ISSN

1864564X

ISSN

18645631

PubMed ID

34143541

First Page

3267

Last Page

3276

Issue

16

Volume

14

Grant

DE‐AC02‐06CH11357

Fund Ref

U.S. Department of Energy

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