TY - JOUR
T1 - Copper phosphosulfides as a highly active and stable photocatalyst for hydrogen evolution reaction
AU - Zhang, Xiandi
AU - Min, Kyung Ah
AU - Zheng, Weiran
AU - Hwang, Jeemin
AU - Han, Byungchan
AU - Lee, Lawrence Yoon Suk
N1 - Publisher Copyright:
© 2020 Elsevier B.V.
PY - 2020/9/15
Y1 - 2020/9/15
N2 - Transition-metal phosphosulfides (TMPSs) have recently shown outstanding electrocatalytic performances toward hydrogen evolution reaction (HER), superior to the sulfide and phosphide counterparts. However, there are only limited TMPSs available due to the synthetic challenge. Herein, we demonstrate a novel synthetic approach for copper phosphosulfide (CuPS) and the first application in photocatalytic HER. Based on the thermodynamic considerations of starting materials, two synthetic routes are designed to obtain two distinct crystal structures (CuS|P and Cu3P|S). Dramatically enhanced photocatalytic HER activities are achieved for both Cu3P|S (2,085 μmol g-1 h-1) and CuS|P (976 μmol g-1 h-1) without using co-catalysts. First-principles calculations unveil the underlying mechanism for the improved HER activity, in which the Gibbs free energy of hydrogen adsorption approaches close to 0 eV and the number of active sites considerably increases with the formation of CuPS structure. This work provides new insight and design principle on preparing TMPSs for high-performance energy conversion applications.
AB - Transition-metal phosphosulfides (TMPSs) have recently shown outstanding electrocatalytic performances toward hydrogen evolution reaction (HER), superior to the sulfide and phosphide counterparts. However, there are only limited TMPSs available due to the synthetic challenge. Herein, we demonstrate a novel synthetic approach for copper phosphosulfide (CuPS) and the first application in photocatalytic HER. Based on the thermodynamic considerations of starting materials, two synthetic routes are designed to obtain two distinct crystal structures (CuS|P and Cu3P|S). Dramatically enhanced photocatalytic HER activities are achieved for both Cu3P|S (2,085 μmol g-1 h-1) and CuS|P (976 μmol g-1 h-1) without using co-catalysts. First-principles calculations unveil the underlying mechanism for the improved HER activity, in which the Gibbs free energy of hydrogen adsorption approaches close to 0 eV and the number of active sites considerably increases with the formation of CuPS structure. This work provides new insight and design principle on preparing TMPSs for high-performance energy conversion applications.
KW - DFT calculations
KW - Hydrogen evolution reaction
KW - Photocatalysis
KW - Wet chemical approach
KW - copper phosphosulfide
UR - http://www.scopus.com/inward/record.url?scp=85084436690&partnerID=8YFLogxK
U2 - 10.1016/j.apcatb.2020.118927
DO - 10.1016/j.apcatb.2020.118927
M3 - 文章
AN - SCOPUS:85084436690
SN - 0926-3373
VL - 273
JO - Applied Catalysis B: Environmental
JF - Applied Catalysis B: Environmental
M1 - 118927
ER -