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

doi:10.1039/c8ta03320j

CORC > 上海应用物理研究所 > 中国科学院上海应用物理研究所 > 中科院上海应用物理研究所2011-2017年

	Intrinsic composition and electronic effects of multicomponent platinum nanocatalysts with high activity and selectivity for ethanol oxidation reaction
	Dai, LX ; Wang, XY ; Yang, SS ; Zhang, T ; Ren, PJ ; Ye, JY ; Nan, B ; Wen, XD ; Zhou, ZY ; Si, R
刊名	JOURNAL OF MATERIALS CHEMISTRY A
	2018
卷号	6 期号:24 页码:11270-11280
关键词	DENSITY-FUNCTIONAL THEORY TOTAL-ENERGY CALCULATIONS WAVE BASIS-SET FUEL-CELLS TRANSITION-METALS PLANE-WAVE OXIDIZING ETHANOL OXYGEN REDUCTION C-C ELECTROCATALYSTS
ISSN号	2050-7488
DOI	10.1039/c8ta03320j
文献子类	期刊论文
英文摘要	The sluggish kinetics of the ethanol oxidation reaction (EOR) challenges us to design and synthesize high-performance multicomponent nanocatalysts. Here, we report the intrinsic composition and electronic effects for achieving enhanced catalytic performance in the EOR by a 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 similar geometric structures (nearly spherical) and crystallite sizes (ca. 8.5 nm) by a one-pot solvothermal method. The main group metals outperformed the transition metals in the enhancement of EOR activity and CO2 selectivity. In particular, Pt3RhSn/C exhibited 67- and 7-fold increases in specific activity and mass activity, respectively, at 0.45 V (vs. RHE) in the EOR in acidic conditions in comparison with a 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 binding energies of oxygen and carbon (E-O + E-C). Among the above catalysts, the state-of-the-art Pt3RhSn/C catalyst performed best in terms of an optimum value of E-O + E-C with a moderate adsorption strength of stable intermediates. In addition, the CO2 selectivity was linearly correlated with the sum of the binding energies of oxygen and H2O (E-O + EH2O), which closely matched the experimental results for typical catalysts. Therefore, the values of E-O + E-C and E-O + EH2O served as descriptors of activity and selectivity, respectively, to rationalize and predict the chemical trends observed in experiments on the EOR catalyzed by nanoalloys. The concept that was revealed, namely, that the composition-performance relationship originates from the synergistic electronic effects of the nanoalloys, promises an alternative strategy for the development of novel solid catalysts for the EOR.
语种	英语
内容类型	期刊论文
源URL	[http://ir.sinap.ac.cn/handle/331007/31000]
专题	上海应用物理研究所_中科院上海应用物理研究所2011-2017年
作者单位	1.Xiamen Univ, Coll Chem & Chem Engn, Dept Chem, State Key Lab Phys Chem Solid Surfaces, Xiamen 361005, Peoples R China 2.Chinese Acad Sci, Shanghai Inst Appl Phys, Shanghai Synchrotron Radiat Facil, Shanghai 201204, Peoples R China 3.Chinese Acad Sci, Inst Coal Chem, State Key Lab Coal Convers, Taiyuan 030001, Shanxi, Peoples R China 4.Peking Univ, Coll Chem & Mol Engn, Beijing Natl Lab Mol Sci, Beijing 100871, Peoples R China 5.Synfuels China Co Ltd, Natl Energy Ctr Coal Clean Fuels, Beijing 101400, Peoples R China
推荐引用方式 GB/T 7714	Dai, LX,Wang, XY,Yang, SS,et al. Intrinsic composition and electronic effects of multicomponent platinum nanocatalysts with high activity and selectivity for ethanol oxidation reaction[J]. JOURNAL OF MATERIALS CHEMISTRY A,2018,6(24):11270-11280.
APA	Dai, LX.,Wang, XY.,Yang, SS.,Zhang, T.,Ren, PJ.,...&Zhang, YW.(2018).Intrinsic composition and electronic effects of multicomponent platinum nanocatalysts with high activity and selectivity for ethanol oxidation reaction.JOURNAL OF MATERIALS CHEMISTRY A,6(24),11270-11280.
MLA	Dai, LX,et al."Intrinsic composition and electronic effects of multicomponent platinum nanocatalysts with high activity and selectivity for ethanol oxidation reaction".JOURNAL OF MATERIALS CHEMISTRY A 6.24(2018):11270-11280.