Direct observation of noble metal nanoparticles transforming to thermally stable single atoms

Nature Nanotechnology
Shengjie WeiYadong Li

Abstract

Single noble metal atoms and ultrafine metal clusters catalysts tend to sinter into aggregated particles at elevated temperatures, driven by the decrease of metal surface free energy. Herein, we report an unexpected phenomenon that noble metal nanoparticles (Pd, Pt, Au-NPs) can be transformed to thermally stable single atoms (Pd, Pt, Au-SAs) above 900 °C in an inert atmosphere. The atomic dispersion of metal single atoms was confirmed by aberration-corrected scanning transmission electron microscopy and X-ray absorption fine structures. The dynamic process was recorded by in situ environmental transmission electron microscopy, which showed competing sintering and atomization processes during NP-to-SA conversion. Further, density functional theory calculations revealed that high-temperature NP-to-SA conversion was driven by the formation of the more thermodynamically stable Pd-N4 structure when mobile Pd atoms were captured on the defects of nitrogen-doped carbon. The thermally stable single atoms (Pd-SAs) exhibited even better activity and selectivity than nanoparticles (Pd-NPs) for semi-hydrogenation of acetylene.

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Citations

Apr 19, 2019·Chemphyschem : a European Journal of Chemical Physics and Physical Chemistry·Mario Pagliaro
Aug 8, 2019·Advanced Materials·Lei TangXinhe Bao
Oct 2, 2019·Chemical Society Reviews·Huilong FeiXiangfeng Duan
Feb 28, 2020·Nature Communications·Son HoangPu-Xian Gao
Sep 19, 2019·Angewandte Chemie·Xue Feng LuXiong Wen David Lou
Jun 20, 2020·Chemical Communications : Chem Comm·Chenliang YeYadong Li
Jul 10, 2020·Advanced Materials·Minhan LiJianping Yang
Jun 25, 2020·Chemistry : a European Journal·Dominik LungerichThomas Drewello
Jan 9, 2020·Angewandte Chemie·Yongpeng LeiYadong Li
Jun 19, 2019·Angewandte Chemie·Lei JiaoYuehe Lin
Aug 14, 2019·Nature Nanotechnology·Abhaya K Datye
Apr 2, 2020·Nature Nanotechnology·Yu XiongYadong Li
Jul 7, 2020·Chemical Communications : Chem Comm·Konglin WuChen Chen
Mar 3, 2019·Nature Communications·Kairui LiuZ Conrad Zhang
Jan 19, 2020·Nature Communications·Dongdong WangYanli Zhao
Apr 2, 2020·Nature Nanotechnology·Dohyung Kim, Matteo Cargnello
May 20, 2020·Research : a Science Partner Journal·Qingyuan BiFuqiang Huang
Jan 18, 2019·Nature Communications·Rui LangTao Zhang
Apr 24, 2019·Nature Materials·Leo DeRitaPhillip Christopher
Aug 31, 2020·Research : a Science Partner Journal·Junxing HanChunwen Sun
Feb 16, 2019·Physical Review Letters·Qiang Fu, Claudia Draxl

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Methods Mentioned

BETA
transmission electron microscopy
X-ray
chip

Software Mentioned

IFEFFIT
XANES
FEFF8

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