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高度活性多金属钯纳米合金嵌入导电聚合物作为阳极催化剂用于乙醇的电氧化。

Highly Active Multimetallic Palladium Nanoalloys Embedded in Conducting Polymer as Anode Catalyst for Electrooxidation of Ethanol.

机构信息

Fuel Cell and Battery Division and ‡Materials Characterization Division, CSIR - Central Glass and Ceramic Research Institute , 196, Raja S. C. Mullick Road, Kolkata 700032, India.

出版信息

ACS Appl Mater Interfaces. 2017 Oct 4;9(39):33775-33790. doi: 10.1021/acsami.7b08327. Epub 2017 Sep 21.

DOI:10.1021/acsami.7b08327
PMID:28899089
Abstract

Fabrication of multimetallic nanocatalysts with controllable composition remains a challenge for the development of low-cost electrocatalysts, and incorporating metal-based catalysts into active carbon nanoarchitectures represents an emerging strategy to improve the catalytic performance of electrocatalysts. Herein, a facile method developed for Pd nanoparticle (NP)-based multimetallic alloys incorporated on polypyrrole (Ppy) nanofibers by in situ nucleation and growth of NPs using colloidal radiolytic technique is described. Electrochemical measurement suggests that the as-prepared catalysts demonstrate dramatically enhanced electrocatalytic activity for ethanol oxidation in alkaline medium. The ultrasmall PdPtAu/Ppy nanohybrids (∼8 nm) exhibit excellent electrocatalytic activity, which is ∼5.5 times higher than that of its monometallic counterparts (12 A/mg Pd, 5 times higher activity compared to that of Pd/C catalyst). Most importantly, the ternary nanocatalyst shows no obvious change in chemical structure and long-term stability, reflected in the 2% loss in forward current density during 1000 cycles. The superior catalytic activity and durability of the nanohybrids have been achieved due to the formation of Pt-Pd-Au heterojunctions with cooperative action of the three metals in the alloy composition, and the strong interactions between the Ppy nanofiber support with the metal NPs. The facile synthetic approach provides a new generation of polymer-supported metal alloy hybrid nanostructures as potential electrocatalysts with superior catalytic activity for fuel cell applications.

摘要

制备组成可控的多金属纳米催化剂仍然是开发低成本电催化剂的挑战,而将金属基催化剂纳入活性碳纳米结构代表了一种提高电催化剂催化性能的新兴策略。本文描述了一种通过胶体放射化学技术原位成核和生长 NPs 制备负载在聚吡咯(Ppy)纳米纤维上的 Pd 纳米颗粒(NP)基多金属合金的简便方法。电化学测量表明,所制备的催化剂在碱性介质中对乙醇氧化表现出显著增强的电催化活性。所制备的 ultrasmall PdPtAu/Ppy 纳米杂化物(∼8nm)具有优异的电催化活性,比其单金属对应物(12A/mgPd)高约 5.5 倍(比 Pd/C 催化剂高 5 倍)。最重要的是,三元纳米催化剂在 1000 次循环中,前向电流密度仅损失 2%,表明其化学结构没有明显变化,长期稳定性好。纳米杂化物具有优异的催化活性和耐久性,这是由于在合金组成中形成了 Pt-Pd-Au 异质结,三种金属具有协同作用,以及 Ppy 纳米纤维载体与金属 NPs 之间具有强相互作用。这种简便的合成方法提供了新一代聚合物负载金属合金混合纳米结构,作为具有优异催化活性的燃料电池应用的潜在电催化剂。

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