Rational design of electrocatalytic interfaces: The multielectron reduction of nitrate in aqueous electrolytes

Youjiang Chen, Huanfeng Zhu, Michelle Rasmussen, Daniel Alberto Scherson

Research output: Contribution to journalArticlepeer-review

13 Citations (Scopus)

Abstract

An electrode incorporating two distinct heterogeneous electrocatalysts acting in series was specifically designed to promote the reduction of nitrate beyond the nitrite stage in weakly buffered aqueous solutions (pH = 3) containing Cd2+. This novel interface consists of Au nanoparticles, Au(np), on which underpotentially deposited Cd reduces nitrate predominantly to nitrite, dispersed on a hemin-modified glassy carbon (GC) surface, Hm|GC, where nitrite is further reduced to yield hydroxylamine as the only product detected using a rotating Au(ring)|Hm|Au(np)|GC (disk) electrode. Additional evidence in support of this series mechanism was obtained from numerical simulations in which the bifunctional electrode was regarded as a hexagonal, closed-packed array of coplanar concentric Cd|Au(np) disks and Hm|GC rings (with no insulating gap), using rate constants determined independently from rotating Au and Hm|GC disk electrodes in solutions containing either nitrate or nitrite, respectively.

Original languageEnglish
Pages (from-to)1907-1911
Number of pages5
JournalJournal of Physical Chemistry Letters
Volume1
Issue number13
DOIs
Publication statusPublished - 2010 Jul 1
Externally publishedYes

ASJC Scopus subject areas

  • Materials Science(all)
  • Physical and Theoretical Chemistry

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