期刊
ACS APPLIED MATERIALS & INTERFACES
卷 13, 期 31, 页码 37142-37151出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsami.1c09016
关键词
oxygen-containing single-atom catalyst; atomic-scale tailoring; structural evolution tracking; singlet oxygen generation; photocatalytic degradation
资金
- National Natural Science Foundation of China [51133006]
The study used amino-rich compounds to tailor metatungstate, fix W atoms, and obtain oxygen-containing W-SACs, revealing their structural evolution and potential for enhancing singlet oxygen generation. This research presents an efficient way to prepare high-efficiency SACs by atomic-scale tailoring and molecular-level structural evolution tracking.
The local coordination structure of metal atoms in single-atom catalysts (SACs) greatly influences their catalytic performance. And for most SACs, single metal atoms were anchored on carbon materials with N or C coordination. However, the rational design of oxygen-containing SACs and analyzing its structure-performance relationship remain challenging. Herein, we used amino-rich compounds to tailor the metatungstate and fix the W atoms and finally obtained the oxygen-containing W-SACs. The structural evolution of tungsten and its coordination atoms were tracked by electrospray ionization high-definition mass spectrometry. Furthermore, aberration-corrected transmission electron microscopy, X-ray absorption fine-structure spectroscopy, and first-principles calculation results revealed that different from the traditional SACs, the WO2N2 moiety (W coordinated with two O atoms and two N atoms) may be the favored structure for W species. This special structure promoted the energy transfer for enhancing singlet oxygen generation. This work presents an efficient way to prepare more highefficiency SACs by atomic-scale tailoring and structural evolution tracking at the molecular level.
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