TY - JOUR
T1 - Single Atomic Cu-N2 Catalytic Sites for Highly Active and Selective Hydroxylation of Benzene to Phenol
AU - Zhang, Ting
AU - Nie, Xiaowa
AU - Yu, Weiwei
AU - Guo, Xinwen
AU - Song, Chunshan
AU - Si, Rui
AU - Liu, Yuefeng
AU - Zhao, Zhongkui
N1 - Publisher Copyright:
© 2019 The Author(s)
PY - 2019/12/20
Y1 - 2019/12/20
N2 - Searching for an efficient single-atom catalyst for benzene hydroxylation to phenol is of critical importance, but it still remains a challenge. Herein, a single-atom catalyst with unique Cu-N2 moieties (Cu1-N2/HCNS) was prepared and confirmed by HAADF-STEM and EXAFS. Turnover number (TON) over Cu1-N2/HCNS (6,935) is 3.4 times of Cu1-N3/HCNS (2,034) under the same reaction conditions, and both exhibit much higher phenol selectivity (close to 99%) and stability compared with Cu nanoparticles and nanoclusters. Experiments and DFT calculations reveal that atomically dispersed Cu species are active sites for benzene hydroxylation to phenol, and the Cu-N2 is more active than Cu-N3 owing to its much lower energy barrier concerning the activation of H2O2 led by its unique coordination state of local atomic structure. We envision that this work opens a new window for modulating coordination environments of single metallic atoms in catalysis design.
AB - Searching for an efficient single-atom catalyst for benzene hydroxylation to phenol is of critical importance, but it still remains a challenge. Herein, a single-atom catalyst with unique Cu-N2 moieties (Cu1-N2/HCNS) was prepared and confirmed by HAADF-STEM and EXAFS. Turnover number (TON) over Cu1-N2/HCNS (6,935) is 3.4 times of Cu1-N3/HCNS (2,034) under the same reaction conditions, and both exhibit much higher phenol selectivity (close to 99%) and stability compared with Cu nanoparticles and nanoclusters. Experiments and DFT calculations reveal that atomically dispersed Cu species are active sites for benzene hydroxylation to phenol, and the Cu-N2 is more active than Cu-N3 owing to its much lower energy barrier concerning the activation of H2O2 led by its unique coordination state of local atomic structure. We envision that this work opens a new window for modulating coordination environments of single metallic atoms in catalysis design.
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U2 - 10.1016/j.isci.2019.11.010
DO - 10.1016/j.isci.2019.11.010
M3 - Article
C2 - 31759238
AN - SCOPUS:85075177806
SN - 2589-0042
VL - 22
SP - 97
EP - 108
JO - iScience
JF - iScience
ER -