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Intercalating lithium into the lattice of silver nanoparticles boosts catalytic hydrogenation of carbon–oxygen bonds

DOI: 10.1039/D1SC01700D DOI Help

Authors: Xin-Ping Duan (University of Oxford; Xiamen University) , Tianyi Chen (Hong Kong Polytechnic University) , Tianxiang Chen (Hong Kong Polytechnic University) , Lele Huang (Xiamen University) , Li Ye (University of Oxford; Fudan University) , Benedict T. W. Lo (University of Oxford) , Youzhu Yuan (Xiamen University) , Shik Chi Edman Tsang (University of Oxford)
Co-authored by industrial partner: No

Type: Journal Paper
Journal: Chemical Science , VOL 8

State: Published (Approved)
Published: May 2021
Diamond Proposal Number(s): 20856

Open Access Open Access

Abstract: Coinage metal nanoparticles with high dispersion can serve as highly efficient heterogeneous catalysts. However, owing to their low melting point, poor thermal stability remains a major obstacle towards their application under reaction conditions. It is a common practice to use porous inorganic templates such as mesoporous silica SBA-15 to disperse Ag nanoparticles (NPs) against aggregation but their stability is far from satisfactory. Here, we show that the catalytic activity for hydrogenation of dimethyl oxalate (DMO) to methyl glycolate (MG) over Ag NPs dispersed on SBA-15 silica can be further promoted by incorporation of alkali metal ions at small loading, which follows the inverse order of their cationic size: Li+ > Na+ > K+ > Rb+. Among these, 5Ag1–Li0.05/SBA-15 can double the MG yield compared to pristine 5Ag/SBA-15 under identical conditions with superior thermal stability. Akin to the effect of an ionic surfactant on stabilization of a micro-emulsion, the cationic charge of an alkali metal ion can maintain dispersion and modulate the surface valence of Ag NPs. Interstitial Li in the octahedral holes of the face center packed Ag lattice is for the first time confirmed by X-ray pair distribution function and electron ptychography. It is believed that this interstitial-stabilization of coinage metal nanoparticles could be broadly applicable to multi-metallic nanomaterials for a broad range of C–O bond activating catalytic reactions of esters.

Subject Areas: Chemistry, Materials

Diamond Offline Facilities: Electron Physical Sciences Imaging Centre (ePSIC)
Instruments: B18-Core EXAFS , E01-JEM ARM 200CF

Added On: 09/06/2021 14:12

Documents:
d1sc01700d.pdf

Discipline Tags:

Physical Chemistry Catalysis Chemistry Materials Science Nanoscience/Nanotechnology

Technical Tags:

Microscopy Spectroscopy Electron Microscopy (EM) Transmission Electron Microscopy (TEM) X-ray Absorption Spectroscopy (XAS)