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Thermolysis of Noble Metal Nanoparticles into Electron‐Rich Phosphorus‐Coordinated Noble Metal Single Atoms at Low Temperature
Author(s) -
Zhou Peng,
Li Ning,
Chao Yuguang,
Zhang Weiyu,
Lv Fan,
Wang Kai,
Yang Wenxiu,
Gao Peng,
Guo Shaojun
Publication year - 2019
Publication title -
angewandte chemie
Language(s) - English
Resource type - Journals
eISSN - 1521-3757
pISSN - 0044-8249
DOI - 10.1002/ange.201908351
Subject(s) - noble metal , metal , catalysis , nanoparticle , chemistry , photocatalysis , atom (system on chip) , materials science , inorganic chemistry , nanotechnology , organic chemistry , computer science , embedded system
Noble metal single atoms coordinated with highly electronegative atoms, especially N and O, often suffer from an electron‐deficient state or poor stability, greatly limiting their wide application in the field of catalysis. Herein we demonstrate a new PH 3 ‐promoted strategy for the effective transformation of noble metal nanoparticles (MNPs, M=Ru, Rh, Pd) at a low temperature (400 °C) into a class of thermally stabilized phosphorus‐coordinated metal single atoms (MPSAs) on g‐C 3 N 4 nanosheets via the strong Lewis acid–base interaction between PH 3 and the noble metal. Experimental work along with theoretical simulations confirm that the obtained Pd single atoms supported on g‐C 3 N 4 nanosheets exist in the form of PdP 2 with a novel electron‐rich feature, conceptionally different from the well‐known single atoms with an electron‐deficient state. As a result of this new electronic property, PdP 2 ‐loaded g‐C 3 N 4 nanosheets exhibit 4 times higher photocatalytic H 2 production activity than the state‐of‐art N‐coordinated PdSAs supported on g‐C 3 N 4 nanosheets. This enhanced photocatalytic activity of phosphorus‐coordinated metal single atoms with an electron‐rich state was quite general, and also observed for other active noble metal single atom catalysts, such as Ru and Rh.