Atomic Imaging of Subsurface Interstitial Hydrogen and Insights into Surface Reactivity of Palladium Hydrides

Lin, Bingqing1; Wu, Xi1; Xie, Lin2; Kang, Yongqiang1; Du, Hongda1; Kang, Feiyu1; Li, Jia1; Gan, Lin1

2020-09-04

10.1002/anie.202006562

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION   影响因子和分区

1433-7851

1521-3773

Resolving interstitial hydrogen atoms at the surfaces and interfaces is crucial for understanding the mechanical and physicochemical properties of metal hydrides. Although palladium (Pd) hydrides hold important applications in hydrogen storage and electrocatalysis, the atomic position of interstitial hydrogen at Pd hydride near surfaces still remains undetermined. We report the first direct imaging of subsurface hydrogen atoms absorbed in Pd nanoparticles by using differentiated and integrated differential phase contrast within an aberration-corrected scanning transmission electron microscope. In contrast to the well-established octahedral interstitial sites for hydrogen in the bulk, subsurface hydrogen atoms are directly identified to occupy the tetrahedral interstices. DFT calculations show that the amount and the occupation type of subsurface hydrogen atoms play an indispensable role in fine-tuning the electronic structure and associated chemical reactivity of the Pd surface.

density functional calculations iDPC-STEM palladium hydrides subsurface hydrogen

SCI ; EI

英语

NI期刊

通讯

Natural Science Foundation of China (NSFC)[51622103][11874036] ; Guangdong Natural Science Foundation for Distinguished Young Scholars[2016A030306035] ; Basic Research Program of Shenzhen[JCYJ20170412171430026][JCYJ20190809145205497][JCYJ20170817161445322] ; Local Innovative and Research Team Project of Guangdong Pearl River Talents Program[2017BT01N111]

Chemistry

Chemistry, Multidisciplinary

WOS:000565713300001

WILEY-V C H VERLAG GMBH

20203609143284

Physicochemical properties ; Hydrogen storage ; Palladium compounds ; Transmission electron microscopy ; Electrocatalysis ; Atoms ; Electronic structure ; Hydrides

Gas Fuels:522 ; Physical Chemistry:801.4 ; Electrochemistry:801.4.1 ; Chemical Reactions:802.2 ; Inorganic Compounds:804.2 ; Probability Theory:922.1 ; Atomic and Molecular Physics:931.3 ; Quantum Theory; Quantum Mechanics:931.4

CHEMISTRY

Web of Science

1.Tsinghua Univ, Tsinghua Shenzhen Int Grad Sch, Shenzhen 518055, Peoples R China
2.Southern Univ Sci & Technol, Dept Phys, Shenzhen 518055, Peoples R China

Lin, Bingqing,Wu, Xi,Xie, Lin,et al. Atomic Imaging of Subsurface Interstitial Hydrogen and Insights into Surface Reactivity of Palladium Hydrides[J]. ANGEWANDTE CHEMIE-INTERNATIONAL EDITION,2020,59(46):20348-20352.

Lin, Bingqing.,Wu, Xi.,Xie, Lin.,Kang, Yongqiang.,Du, Hongda.,...&Gan, Lin.(2020).Atomic Imaging of Subsurface Interstitial Hydrogen and Insights into Surface Reactivity of Palladium Hydrides.ANGEWANDTE CHEMIE-INTERNATIONAL EDITION,59(46),20348-20352.

Lin, Bingqing,et al."Atomic Imaging of Subsurface Interstitial Hydrogen and Insights into Surface Reactivity of Palladium Hydrides".ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 59.46(2020):20348-20352.