Premium
Fluorine‐Induced Surface Metallization for Ammonia Synthesis under Photoexcitation up to 1550 nm
Author(s) -
Fu Rong,
Wu Zewen,
Pan Ziye,
Gao Zhuoyang,
Li Zhen,
Kong Xianghua,
Li Lu
Publication year - 2021
Publication title -
angewandte chemie
Language(s) - English
Resource type - Journals
eISSN - 1521-3757
pISSN - 0044-8249
DOI - 10.1002/ange.202100572
Subject(s) - photoexcitation , work function , band bending , materials science , electron , metal , dissociation (chemistry) , photochemistry , irradiation , fluorine , photocatalysis , chemistry , chemical physics , atomic physics , optoelectronics , catalysis , excited state , biochemistry , physics , quantum mechanics , metallurgy , nuclear physics
The first observation of surface metallization of TiO 2− x induced by fluoride ions is presented. The emerging metallic states are contributed by the 3d orbital of surface Ti and the 2p orbital of surface bridging F, which are intrinsically originated from the strong electron repulsion between F − and adjacent Ti 3+ . The metalized TiO 2− x with reduced work function and downward band bending possesses high electron‐donating power to supported Ru species via atomic‐scale ohmic contacts, exhibiting unprecedented photocatalytic performances for ammonia synthesis across the entire solar spectrum region (200–1550 nm) at room temperature. Mechanism and kinetic analysis revealed that the loaded Ru could behave as efficient electron sinks to accumulate photogenerated electrons and that the metallic surface markedly enhanced the dissociation of H 2 and N 2 by the hot electrons generated by the visible or even infrared light irradiation.