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Direct visualization of substitutional Li doping in supported Pt nanoparticles and their ultra-selective catalytic hydrogenation performance

DOI: 10.1002/chem.202101470 DOI Help

Authors: Tianyi Chen (University of Oxford) , Christopher Foo (University of Oxford) , Jianwei Zheng (University of Oxford) , Huihuang Fang (University of Oxford) , Peter Nellist (University of Oxford) , Edman Shik Chi Tsang (University of Oxford)
Co-authored by industrial partner: No

Type: Journal Paper
Journal: Chemistry – A European Journal

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

Abstract: It has only recently been established that doping light elements (lithium, boron, and carbon) into supported transition metals can fill interstitial sites, which can be observed by the expanded unit cell. As an example, interstitial lithium (intLi) can block H filling octahedral interstices of palladium metal lattice, which improves partial hydrogenation of alkynes to alkenes under hydrogen. In contrast, herein, we report intLi is not found in the case of Pt/C. Instead, we observe for the first time a direct ‘substitution’ of Pt with substitutional lithium (subLi) in alternating atomic columns using scanning transmission electron microscopy-annular dark field (STEM-ADF). This ordered substitutional doping results in a contraction of the unit cell as shown by high-quality synchrotron X-ray diffraction (SXRD). The electron donation of d-band of Pt without higher orbital hybridizations by subLi offers an alternative way for ultra-selectivity in catalytic hydrogenation of carbonyl compounds by suppressing the facile CO bond breakage that would form alcohols.

Journal Keywords: Bimetallic; Substitution; Ordered alloy; Nanoparticle; Hydrogenation

Diamond Keywords: Alloys

Subject Areas: Materials, Chemistry

Diamond Offline Facilities: Electron Physical Sciences Imaging Centre (ePSIC)
Instruments: B18-Core EXAFS , E01-JEM ARM 200CF , I11-High Resolution Powder Diffraction

Added On: 23/06/2021 09:50

Discipline Tags:

Physical Chemistry Catalysis Chemistry Materials Science Inorganic Chemistry Nanoscience/Nanotechnology Metallurgy

Technical Tags:

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