TY - JOUR
T1 - Design of Single-Atom Catalysts for Hg0Oxidation Using H2O2
AU - Yang, Weijie
AU - Chen, Xuelu
AU - Chen, Liugang
AU - Feng, Yajun
AU - Wu, Chongchong
AU - Ding, Xunlei
AU - Gao, Zhengyang
AU - Liu, Yanfeng
AU - Li, Hao
N1 - Funding Information:
This work was funded by the National Natural Science Foundation of China (Nos. 52006073, 52176104, and 92161115) and the Natural Science Foundation of Hebei (No. E2020502023). H.L. acknowledges the Center for Computational Materials Science, Institute for Materials Research, Tohoku University, for the use of MASAMUNE-IMR (Project No. 202208-SCKXX-0211) and the Institute for Solid State Physics (ISSP) at the University of Tokyo for the use of their supercomputers.
Publisher Copyright:
© 2022 American Chemical Society.
PY - 2022/12/22
Y1 - 2022/12/22
N2 - Hg0 removal is the most difficult part in mercury purification due to its insolubility in water and strong volatility. Catalytic oxidation is the main method for Hg0 removal. O2 and hydrogen halides (HCl and H2S) are common oxidants for catalytic Hg0 oxidation. However, previous studies showed that current catalytic oxidation routes have sluggish kinetics and may cause secondary pollution. Herein, we propose a new pathway for catalytic Hg0 oxidation on the surface of single-atom catalysts (SACs) using the green oxidant H2O2. Some potential catalysts were screened by analyzing the adsorption and activation mechanism of H2O2 on the surface of SACs. Spin-polarized density functional theory calculations with van der Waals corrections (DFT-D3) revealed that Zn1-N4-C has the lowest rate-determining step barrier (0.35 eV) among the analyzed systems. This study proposes a promising pathway for a kinetically facile catalytic Hg0 oxidation, providing a new option for effective Hg0 removal.
AB - Hg0 removal is the most difficult part in mercury purification due to its insolubility in water and strong volatility. Catalytic oxidation is the main method for Hg0 removal. O2 and hydrogen halides (HCl and H2S) are common oxidants for catalytic Hg0 oxidation. However, previous studies showed that current catalytic oxidation routes have sluggish kinetics and may cause secondary pollution. Herein, we propose a new pathway for catalytic Hg0 oxidation on the surface of single-atom catalysts (SACs) using the green oxidant H2O2. Some potential catalysts were screened by analyzing the adsorption and activation mechanism of H2O2 on the surface of SACs. Spin-polarized density functional theory calculations with van der Waals corrections (DFT-D3) revealed that Zn1-N4-C has the lowest rate-determining step barrier (0.35 eV) among the analyzed systems. This study proposes a promising pathway for a kinetically facile catalytic Hg0 oxidation, providing a new option for effective Hg0 removal.
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U2 - 10.1021/acs.jpcc.2c06266
DO - 10.1021/acs.jpcc.2c06266
M3 - Article
AN - SCOPUS:85144114944
SN - 1932-7447
VL - 126
SP - 21234
EP - 21242
JO - Journal of Physical Chemistry C
JF - Journal of Physical Chemistry C
IS - 50
ER -