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Intrinsic composition and electronic effects of multicomponent platinum nanocatalysts with high activity and selectivity for ethanol oxidation reaction

Abstract

The sluggish kinetics of ethanol oxidation reaction (EOR) challenges us to design and synthesize high-performance multicomponent nanocatalysts. Herein, we report the intrinsic composition and electronic effects for achieving the enhanced catalytic performances towards EOR by the combination of experiments and density functional theory (DFT) computations. Late 3d transition metals and main group (IIIA and IVA) metals were introduced to construct ternary Pt3RhM (M= Fe, Co, Ni, Cu; Ga, In, Sn, Pb) nanoalloys with a similar geometric structure (nearly spherical) and crystallize size (ca. 8.5 nm) by one-pot solvothermal method. The main group metals outperform the transition metals in the enhancement of the EOR activity and CO2 selectivity. Especially, Pt3RhSn/C exhibits 67- and 7-fold enhancements of the specific activity and mass activity at 0.45 V (vs RHE) for EOR in acidic condition, compared with the commercial Pt/C catalyst. The trends in catalytic activity were explained by DFT calculations which established a volcano-shaped relationship between the EOR activity and the sum of the oxygen and carbon binding energies (EO+EC). Among above catalysts, the state-of-the-art Pt3RhSn/C catalyst wins in an optimum EO+EC value with a moderate adsorption strength of stable intermediates. In addition, the CO2 selectivity is linearly correlated with the sum of oxygen and H2O binding energies (EO+EH2O), which matches well with the experimental results of typical catalysts. Therefore, the EO+EC and EO+EH2O were creatively served as the activity and selectivity descriptors to rationalize and predict these chemical trends presented in the experiments of nanoalloys catalyzed EOR. The revealed concept that the composition-performance relationship origins from the synergistic electronic effect of the nanoalloys, promises an alternative strategy for developing novel solid catalysts towards EOR.

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Publication details

The article was received on 11 Apr 2018, accepted on 15 May 2018 and first published on 16 May 2018


Article type: Paper
DOI: 10.1039/C8TA03320J
Citation: J. Mater. Chem. A, 2018, Accepted Manuscript
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    Intrinsic composition and electronic effects of multicomponent platinum nanocatalysts with high activity and selectivity for ethanol oxidation reaction

    L. Dai, X. Wang, S. Yang, T. Zhang, P. ren, J. Ye, B. Nan, X. Wen, Z. Zhou, R. Si, C. Yan and Y. Zhang, J. Mater. Chem. A, 2018, Accepted Manuscript , DOI: 10.1039/C8TA03320J

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