Enhanced Electrocatalytic N2 Reduction via Partial Anion Substitution in Titanium Oxide–Carbon Composites

Qing Qin, Yun Zhao, Max Schmallegger, Tobias Heil, Johannes Schmidt, Ralf Walczak, Georg Gescheidt-Demner, Haijun Jiao, Martin Oschatz*

*Corresponding author for this work

Research output: Contribution to journalArticle

Abstract

The electrochemical conversion of N2 at ambient conditions using renewably generated electricity is an attractive approach for sustainable ammonia (NH3) production. Considering the chemical inertness of N2, rational design of efficient and stable catalysts is required. Therefore, in this work, it is demonstrated that a C-doped TiO2/C (C-TixOy/C) material derived from the metal–organic framework (MOF) MIL-125(Ti) can achieve a high Faradaic efficiency (FE) of 17.8 %, which even surpasses most of the established noble metal-based catalysts. On the basis of the experimental results and theoretical calculations, the remarkable properties of the catalysts can be attributed to the doping of carbon atoms into oxygen vacancies (OVs) and the formation of Ti−C bonds in C-TixOy. This binding motive is found to be energetically more favorable for N2 activation compared to the non-substituted OVs in TiO2. This work elucidates that electrochemical N2 reduction reaction (NRR) performance can be largely improved by creating catalytically active centers through rational substitution of anions into metal oxides.

Original languageEnglish
Pages (from-to)13101-13106
Number of pages6
JournalAngewandte Chemie - International Edition
Volume58
Issue number37
DOIs
Publication statusPublished - 9 Sep 2019

Keywords

  • ammonia synthesis
  • anion substitution
  • MOF-derived catalysts
  • N fixation
  • non-noble metal catalysts

ASJC Scopus subject areas

  • Catalysis
  • Chemistry(all)

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