Catalytic Activity Control via Crossover between Two Different Microstructures

Yuheng Zhou, Yihan Zhu, Zhi-Qiang Wang, Shihui Zou, Guicen Ma, Ming Xia, Xueqian Kong, Liping Xiao, Xue-Qing Gong, Jie Fan

Research output: Contribution to journalArticlepeer-review

19 Scopus citations

Abstract

Metal nanocatalysts hold great promise for a wide range of heterogeneous catalytic reactions, while the optimization strategy of catalytic activity is largely restricted by particle size or shape control. Here, we demonstrate that a reversible microstructural control through the crossover between multiply-twinned nanoparticle (MTP) and single crystal (SC) can be readily achieved by solvent post-treatment on gold nanoparticles (AuNPs). Polar solvents (e.g. water, methanol) direct the transformation from MTP to SC accompanied by the disappearance of twinning and stacking faults. A reverse transformation from SC to MTP is achieved in non-polar solvent (e.g. toluene) mixed with thiol ligands. The transformation between two different microstructures is directly observed by in-situ TEM and leads to a drastic modulation of catalytic activity towards the gas-phase selective oxidation of alcohols. There is a quasi-linear relationship between TOFs and MTP concentrations. Based on the combined experimental and theoretical investigations of alcohol chemisorption on these nanocatalysts, we propose that the exposure of {211}-like microfacets associated with twin boundaries and stack faults accounts for the strong chemisorption of alcohol molecules on MTP AuNPs and thus the exceptionally high catalytic activity.
Original languageEnglish (US)
Pages (from-to)13740-13748
Number of pages9
JournalJournal of the American Chemical Society
Volume139
Issue number39
DOIs
StatePublished - Sep 21 2017

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