Control of Local Electronic Structure of Pd Single Atom Catalyst by Adsorbate Induction.
Small
; 18(1): e2103852, 2022 Jan.
Article
de En
| MEDLINE
| ID: mdl-34766728
ABSTRACT
Aiming at regulating and controlling the localized electronic states while maintaining the metal atoms in the isolation form, an in situ adsorbate induced strategy is proposed at a programmed temperature to activate Zr-based metal-organic framework (MOF) supported single Pd atom catalyst. It is discovered that in situ treatment environments trigger the change of lattice parameters in MOF materials by reaction heat effect, observed by in situ X-ray diffraction, spherical aberration-corrected electron microscope, and X-ray adsorption fine structure (XAFS). The as-obtained electron-deficient Pd single atoms are critical to the high intrinsic activity (turnover frequency of 0.132 s-1 ) and selectivity of 93% with the long-term stability in the semihydrogenation of acetylene, which can be comparable to the state-of-the-art Pd catalysts. This superior catalytic behavior correlates with the reduced C2 H4 desorption energy and the activation barriers for the hydrogenation, confirmed by density functional theory calculation.
Texte intégral:
1
Collection:
01-internacional
Base de données:
MEDLINE
Langue:
En
Journal:
Small
Sujet du journal:
ENGENHARIA BIOMEDICA
Année:
2022
Type de document:
Article
Pays d'affiliation:
Chine
Pays de publication:
ALEMANHA
/
ALEMANIA
/
DE
/
DEUSTCHLAND
/
GERMANY