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首页> 外文期刊>ACS catalysis >Shaping Single-Crystalline Trimetallic Pt-Pd-Rh Nanocrystals toward High-Efficiency C-C Splitting of Ethanol in Conversion to CO2
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Shaping Single-Crystalline Trimetallic Pt-Pd-Rh Nanocrystals toward High-Efficiency C-C Splitting of Ethanol in Conversion to CO2

机译：将单晶三金属Pt-Pd-Rh纳米晶体成形为高效的C-C乙醇转化为CO2的乙醇裂解方法

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Atomic-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.
机译：原子级构建和高通量筛选具有可调的清晰定义的表面结构和相关活性位的强大的多组分纳米催化剂，用于乙醇电氧化反应（EOR），具有高活性和选择性，涉及CC键裂解和乙醇的完全氧化作为一种清洁，可持续的能源，仍然是一个巨大的挑战。在此，我们基于组合密度泛函理论（DFT）计算和实验研究，展示了一种强大的概念方法，可用于设计，合成和优化形状和成分改变的单晶Pt-Pd-Rh纳米晶体，以增强EOR性能。通过在方便的水热法中调节金属前体的还原趋势，我们制备了（111）端接的Pt-Pd-Rh纳米截短八面体（NTO）和（100）端接的Pt-Pd-Rh纳米立方（NCs）。在DFT计算的帮助下，在0.5 V vs. NHE的条件下，PtPdRh NTO，PtPdRh NTO和8.8 nm PtPdRh NCs-200被筛选为性能最佳的催化剂，具有最高的EOR活性（是市售Pt黑的五倍）。在这些催化剂中，PtPdRh NTO在0.5 V时表现出对CO2的最高选择性，并且在极低的电势（0.35 V）下具有将乙醇完全氧化的显着能力。 8.8 nm PtPdRh NCs-200具有最佳的耐久性。与三种金属的协同作用相关的形态和表面组成被证实会影响形状良好的Pt-Pd-Rh纳米晶体的EOR性能。结合原位FTIR，可以推断出适当的表面组成和裸露的小面是C-C键断裂至低电势时增强的能力的关键因素。通过调整具有均匀元素分布的Pt-Pd-Rh纳米晶体的表面组成和形态，根据两个基本反应的DFT模拟（即C-C键断裂和COad氧化）实现了增强的EOR性能。这项工作提供了有效和有用的策略，以促进具有优化的成分和表面结构的多组分非均相纳米催化剂的反应性，可用于许多工业催化过程。

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