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Shaping Single-Crystalline Trimetallic Pt-Pd-Rh Nanocrystals toward High-Efficiency C-C Splitting of Ethanol in Conversion to CO2
Zhu, W; Ke, J; Wang, SB; Ren, J; Wang, HH; Zhou, ZY; Si, R; Zhang, YW; Yan, CH
2015
Source PublicationACS CATALYSIS
Volume5Issue:3Pages:1995—2008
Subtype期刊文献
AbstractAtomic-scale construction and high-throughput screening of robust multicomponent nanocatalysts with tunable well-defined surface structures and associated active sites for the ethanol electro-oxidation reaction (EOR) in high activity and selectivity, referring to C-C bond cleavage and full oxidation of ethanol as a clean and sustainable energy source, has remained a great challenge. Herein, we demonstrate a powerful conceptual approach to design, synthesize, and optimize single crystalline Pt-Pd-Rh nanocrystals of altered shapes and compositions for enhanced EOR performance, based on combined density functional theory (DFT) calculations and experiment study. We prepared (111) terminated Pt-Pd-Rh nanotruncated-octahedrons (NTOs) and (100) terminated Pt-Pd-Rh nanocubes (NCs) with varied compositions by regulating the reduction tendency of metal precursors in a facile hydrothermal method. Aided by DFT calculations, PtPdRh NTOs, PtPdRh NTO, and 8.8 nm PtPdRh NCs-200 were screened to be the best performing catalysts with the highest EOR activity (five times as much as that of commercial Pt black) at 0.5 V vs NHE. Among these catalysts, PtPdRh NTOs exhibited the highest selectivity to CO2 at 0.5 V and the noteworthy capability to fully oxidize ethanol at extremely low potential (0.35 V); 8.8 nm PtPdRh NCs-200 possessed the best durability. Morphology and surface composition correlated to the synergistic effect of three metals were verified to affect the EOR performance of well shaped Pt-Pd-Rh nanocrystals. Combined with in situ FTIR, it was deduced that appropriate surface composition and exposed facets were the key factors to the promoted capability in the cleavage of C-C bond down to low potential. Through adjusting surface composition and morphology of Pt-Pd-Rh nanocrystals with homogeneous element distribution, enhanced EOR performance was achieved in light of DFT simulations of the two elementary reactions (i.e., breakdown of C-C bond and oxidation of COad). This work has offered an effective and useful strategy to promote the reactivity of multicomponent heterogeneous nanocatalysts with optimized compositions and surface structures for many industrial catalytic processes.
KeywordSulfuric-acid-solutions In-situ Ftir Transform Infrared-spectroscopy Core-shell Nanoparticles Fuel-cell Oxidizing Ethanol Anode Catalysts Online Dems Tin Oxide Oxidation
Indexed BySCI
Language英语
Document Type期刊论文
Identifierhttp://ir.sinap.ac.cn/handle/331007/24565
Collection中科院上海应用物理研究所2011-2020年
Recommended Citation
GB/T 7714
Zhu, W,Ke, J,Wang, SB,et al. Shaping Single-Crystalline Trimetallic Pt-Pd-Rh Nanocrystals toward High-Efficiency C-C Splitting of Ethanol in Conversion to CO2[J]. ACS CATALYSIS,2015,5(3):1995—2008.
APA Zhu, W.,Ke, J.,Wang, SB.,Ren, J.,Wang, HH.,...&Yan, CH.(2015).Shaping Single-Crystalline Trimetallic Pt-Pd-Rh Nanocrystals toward High-Efficiency C-C Splitting of Ethanol in Conversion to CO2.ACS CATALYSIS,5(3),1995—2008.
MLA Zhu, W,et al."Shaping Single-Crystalline Trimetallic Pt-Pd-Rh Nanocrystals toward High-Efficiency C-C Splitting of Ethanol in Conversion to CO2".ACS CATALYSIS 5.3(2015):1995—2008.
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