TY  - JOUR
A1  - Qin, Qing
A1  - Zhao, Yun
A1  - Schmallegger, Max
A1  - Heil, Tobias
A1  - Schmidt, Johannes
A1  - Walczak, Ralf
A1  - Gescheidt-Demner, Georg
A1  - Jiao, Haijun
A1  - Oschatz, Martin
T1  - Enhanced Electrocatalytic N-2 Reduction via Partial Anion Substitution in Titanium Oxide-Carbon Composites
JF  - Angewandte Chemie : a journal of the Gesellschaft Deutscher Chemiker ; International edition
N2  - The electrochemical conversion of N-2 at ambient conditions using renewably generated electricity is an attractive approach for sustainable ammonia (NH3) production. Considering the chemical inertness of N-2, 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 N-2 activation compared to the non-substituted OVs in TiO2. This work elucidates that electrochemical N-2 reduction reaction (NRR) performance can be largely improved by creating catalytically active centers through rational substitution of anions into metal oxides.
KW  - ammonia synthesis
KW  - anion substitution
KW  - MOF-derived catalysts
KW  - N-2 fixation
KW  - non-noble metal catalysts
Y1  - 2019
U6  - https://doi.org/10.1002/anie.201906056
SN  - 1433-7851
SN  - 1521-3773
VL  - 58
IS  - 37
SP  - 13101
EP  - 13106
PB  - Wiley-VCH
CY  - Weinheim
ER  -