Fast site-to-site electron transfer of high-entropy alloy nanocatalyst driving redox electrocatalysis.

Fast site-to-site electron transfer of high-entropy alloy nanocatalyst driving redox electrocatalysis.
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高熵合金纳米催化剂驱动氧化还原电催化的快速位点电子转移

DOI:
10.1038/s41467-020-19277-9
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发表时间:
2020-10-28
影响因子:
16.6
通讯作者:
Wang L
Wang L
中科院分区:
综合性期刊1区
文献类型:
--
作者:
Li H;Han Y;Zhao H;Qi W;Zhang D;Yu Y;Cai W;Li S;Lai J;Huang B;Wang L

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设计同时用于还原和氧化反应的高性能电催化剂面临着严峻的挑战。本文采用常压低温油相法制备了均匀、超小(~3.4 nm)的高熵合金Pt18Ni26Fe15Co14Cu27纳米粒子。Pt18Ni26Fe15Co14Cu27/C催化剂对析氢反应(HER)和甲醇氧化反应(MOR)表现出良好的电催化性能。该催化剂在电流密度为10 mA cm 2时表现出极小的过电位为11 mV,在碱性介质中具有良好的活性(10.96−A −1Ptat−0.07 V对可逆氢电极)和稳定性。此外,它也是迄今报道的在碱性溶液中用于MOR的高效催化剂(15.04 A mg−1pt)。周期性的密度泛函计算证实了HEA表面上HER和MOR的多活性中心是质子和中间体转化的关键因素。同时,HEA表面的构建为还原和氧化过程提供了快速的位置到位置的电子转移。
Designing electrocatalysts with high-performance for both reduction and oxidation reactions faces severe challenges. Here, the uniform and ultrasmall (~3.4 nm) high-entropy alloys (HEAs) Pt18Ni26Fe15Co14Cu27nanoparticles are synthesized by a simple low-temperature oil phase strategy at atmospheric pressure. The Pt18Ni26Fe15Co14Cu27/C catalyst exhibits excellent electrocatalytic performance for hydrogen evolution reaction (HER) and methanol oxidation reaction (MOR). The catalyst shows ultrasmall overpotential of 11 mV at the current density of 10 mA cm−2, excellent activity (10.96 A mg−1Ptat −0.07 V vs. reversible hydrogen electrode) and stability in the alkaline medium. Furthermore, it is also the efficient catalyst (15.04 A mg−1Pt) ever reported for MOR in alkaline solution. Periodic DFT calculations confirm the multi-active sites for both HER and MOR on the HEA surface as the key factor for both proton and intermediate transformation. Meanwhile, the construction of HEA surfaces supplies the fast site-to-site electron transfer for both reduction and oxidation processes.
DOI: 10.1038/ncomms14136
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影响因子: 16.6
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