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Self‐Optimization of the Active Site of Molybdenum Disulfide by an Irreversible Phase Transition during Photocatalytic Hydrogen Evolution
Author(s) -
Wang Longlu,
Liu Xia,
Luo Jinming,
Duan Xidong,
Crittenden John,
Liu Chengbin,
Zhang Shuqu,
Pei Yong,
Zeng Yunxiong,
Duan Xiangfeng
Publication year - 2017
Publication title -
angewandte chemie
Language(s) - English
Resource type - Journals
eISSN - 1521-3757
pISSN - 0044-8249
DOI - 10.1002/ange.201703066
Subject(s) - catalysis , molybdenum disulfide , photocatalysis , exfoliation joint , active site , phase (matter) , materials science , hydrothermal circulation , transition metal , phase transition , chemical physics , chemical engineering , adsorption , molybdenum , hydrogen , nanotechnology , chemistry , photochemistry , inorganic chemistry , graphene , organic chemistry , physics , thermodynamics , engineering , metallurgy
The metallic 1T‐MoS 2 has attracted considerable attention as an effective catalyst for hydrogen evolution reactions (HERs). However, the fundamental mechanism about the catalytic activity of 1T‐MoS 2 and the associated phase evolution remain elusive and controversial. Herein, we prepared the most stable 1T‐MoS 2 by hydrothermal exfoliation of MoS 2 nanosheets vertically rooted into rigid one‐dimensional TiO 2 nanofibers. The 1T‐MoS 2 can keep highly stable over one year, presenting an ideal model system for investigating the HER catalytic activities as a function of the phase evolution. Both experimental studies and theoretical calculations suggest that 1T phase can be irreversibly transformed into a more active 1T′ phase as true active sites in photocatalytic HERs, resulting in a “catalytic site self‐optimization”. Hydrogen atom adsorption is the major driving force for this phase transition.

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