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  - 
TY  - JOUR
A1  - Herzschuh, Ulrike
A1  - Cao, Xianyong
A1  - Laepple, Thomas
A1  - Dallmeyer, Anne
A1  - Telford, Richard J.
A1  - Ni, Jian
A1  - Chen, Fahu
A1  - Kong, Zhaochen
A1  - Liu, Guangxiu
A1  - Liu, Kam-Biu
A1  - Liu, Xingqi
A1  - Stebich, Martina
A1  - Tang, Lingyu
A1  - Tian, Fang
A1  - Wang, Yongbo
A1  - Wischnewski, Juliane
A1  - Xu, Qinghai
A1  - Yan, Shun
A1  - Yang, Zhenjing
A1  - Yu, Ge
A1  - Zhang, Yun
A1  - Zhao, Yan
A1  - Zheng, Zhuo
T1  - Position and orientation of the westerly jet determined Holocene rainfall patterns in China
JF  - Nature Communications
N2  - Proxy-based reconstructions and modeling of Holocene spatiotemporal precipitation patterns for China and Mongolia have hitherto yielded contradictory results indicating that the basic mechanisms behind the East Asian Summer Monsoon and its interaction with the westerly jet stream remain poorly understood. We present quantitative reconstructions of Holocene precipitation derived from 101 fossil pollen records and analyse them with the help of a minimal empirical model. We show that the westerly jet-stream axis shifted gradually southward and became less tilted since the middle Holocene. This was tracked by the summer monsoon rain band resulting in an early-Holocene precipitation maximum over most of western China, a mid-Holocene maximum in north-central and northeastern China, and a late-Holocene maximum in southeastern China. Our results suggest that a correct simulation of the orientation and position of the westerly jet stream is crucial to the reliable prediction of precipitation patterns in China and Mongolia.
Y1  - 2019
U6  - https://doi.org/10.1038/s41467-019-09866-8
SN  - 2041-1723
VL  - 10
PB  - Nature Publ. Group
CY  - London
ER  -