TY - JOUR
T1 - Coordination tunes selectivity
T2 - two‐electron oxygen reduction on high‐loading molybdenum single‐atom catalysts
AU - Tang, Cheng
AU - Jiao, Yan
AU - Shi, Bingyang
AU - Liu, Jia-Ning
AU - Xie, Zhenhua
AU - Chen, Xiao
AU - Zhang, Qiang
AU - Qiao, Shizhang
PY - 2020/6/2
Y1 - 2020/6/2
N2 - Single-atom catalysts (SACs) have great potential in electrocatalysis. Their performance can be rationally optimized by tailoring the metal atoms, adjacent coordinative dopants, and metal loading. However, doing so is still a great challenge because of the limited synthesis approach and insufficient understanding of the structure–property relationships. Herein, we report a new kind of Mo SAC with a unique O,S coordination and a high metal loading over 10 wt %. The isolation and local environment was identified by high-angle annular dark-field scanning transmission electron microscopy and extended X-ray absorption fine structure. The SACs catalyze the oxygen reduction reaction (ORR) via a 2 e− pathway with a high H2O2 selectivity of over 95 % in 0.10 m KOH. The critical role of the Mo single atoms and the coordination structure was revealed by both electrochemical tests and theoretical calculations.
AB - Single-atom catalysts (SACs) have great potential in electrocatalysis. Their performance can be rationally optimized by tailoring the metal atoms, adjacent coordinative dopants, and metal loading. However, doing so is still a great challenge because of the limited synthesis approach and insufficient understanding of the structure–property relationships. Herein, we report a new kind of Mo SAC with a unique O,S coordination and a high metal loading over 10 wt %. The isolation and local environment was identified by high-angle annular dark-field scanning transmission electron microscopy and extended X-ray absorption fine structure. The SACs catalyze the oxygen reduction reaction (ORR) via a 2 e− pathway with a high H2O2 selectivity of over 95 % in 0.10 m KOH. The critical role of the Mo single atoms and the coordination structure was revealed by both electrochemical tests and theoretical calculations.
KW - electrocatalysis
KW - molybdenum
KW - oxygen reduction reaction (ORR)
KW - selectivity
KW - single-atom catalyst
UR - http://www.scopus.com/inward/record.url?scp=85082939958&partnerID=8YFLogxK
UR - http://purl.org/au-research/grants/arc/DP160104866
UR - http://purl.org/au-research/grants/arc/LP160100927
UR - http://purl.org/au-research/grants/arc/DP190103472
UR - http://purl.org/au-research/grants/arc/FL170100154
U2 - 10.1002/anie.202003842
DO - 10.1002/anie.202003842
M3 - Article
C2 - 32196867
SN - 1433-7851
VL - 59
SP - 9171
EP - 9176
JO - Angewandte Chemie - International Edition
JF - Angewandte Chemie - International Edition
IS - 23
ER -