Journal of Materials Chemistry A p. 11282 - 11291 (2020)
Update date:2022-08-30
Topics:
García-Trenco, Andrés
Leung, Alice H. M.
Phanopoulos, Andreas
Pike, Sebastian D.
Regoutz, Anna
Schuster, Manfred E.
Shaffer, Milo S. P.
Williams, Charlotte K.
Doped-ZnO nanoparticles, capped with dioctylphosphinate ligands, are synthesised by the controlled hydrolysis of a mixture of organometallic precursors. Substitutional doping of the wurtzite ZnO nanoparticles with 5 mol% Mg(ii), Al(iii) and Cu(i) is achieved by the addition of sub-stoichiometric amounts of the appropriate dopant [(n-butyl)(sec-butyl)magnesium, triethylaluminium or mesitylcopper] to diethylzinc in the precursor mixture. After hydrolysis, the resulting colloidal nanoparticles (sizes of 2-3 nm) are characterised by powder X-ray crystallography, transmission electron microscopy, inductively-coupled plasma optical emission spectrometry and X-ray photoelectron spectroscopy. A solution of the doped-ZnO nanoparticles and colloidal Cu(0) nanoparticles [M:ZnO : Cu = 1 : 1] are applied as catalysts for the hydrogenation of CO2to methanol in a liquid-phase continuous flow stirred tank reactor [210 °C, 50 bar, CO2 : H2= 1 : 3, 150 mL min?1, mesitylene, 20 h]. All the catalyst systems display higher rates of methanol production and better stability than a benchmark heterogeneous catalyst, Cu-ZnO-Al2O3[480 μmol mmolmetal?1h?1], with approximately twice the activity for the Al(iii)-doped nanocatalyst. Despite outperforming the benchmark catalyst, Mg(ii) doping is detrimental towards methanol production in comparison to undoped ZnO. X-Ray photoelectron spectroscopy and transmission electron microscopy analysis of the most active post-catalysis samples implicate the migration of Al(iii) to the catalyst surface, and this surface enrichment is proposed to facilitate stabilisation of the catalytic ZnO/Cu interfaces.
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