Sphere-like PdNi Alloy: Unveiling the Twin Functional Properties toward Oxygen Reduction and Temperature-Dependent Methanol Oxidation for Alkaline Direct Methanol Fuel Cells,ACS Sustainable Chemistry & Engineering

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Sphere-like PdNi Alloy: Unveiling the Twin Functional Properties toward Oxygen Reduction and Temperature-Dependent Methanol Oxidation for Alkaline Direct Methanol Fuel Cells
ACS Sustainable Chemistry & Engineering ( IF 7.1 ) Pub Date : 2023-03-27 , DOI: 10.1021/acssuschemeng.2c05220
Arunprasath Sathyaseelan ₁ , Vijayakumar Elumalai ₁ , Karthikeyan Krishnamoorthy _{1,

2} , Aparna Sajeev ₁ , Sang-Jae Kim _{1,

2,

3}

Affiliation

The development of high-performance bifunctional palladium-based (Pd) alloys for the oxygen reduction reaction (ORR) and methanol oxidation reaction (MOR) is a great challenge in direct methanol fuel cells. The incorporation of an oxophilic atom into the Pd atom is an effective strategy to enhance the electrocatalytic activity of the catalysts. Herein a sphere-like PdNi alloy (sPdNiA) was developed via a simple hydrazine-assisted reduction method to overcome the kinetic drawbacks of palladium and delivers superior ORR/MOR performance. The successful alloy formation, the induced strain effect in the electronic structure, and structural characteristics of the sPdNiA were confirmed through XRD, XPS, and HR-TEM studies. As a result, for ORR, the sPdNiA exhibits a positive halfwave potential (E_1/2) of ∼0.854 V (vs RHE) compared to the pure Pd (0.833 V vs RHE) nanoparticles. For MOR, the sPdNiA presents the low onset potential and high mass activity of 518 mA mg_Pd^–1 in 1.0 M KOH electrolyte. Furthermore, the temperature-dependent MOR and 3D Bode plot investigations reveal a five-fold higher mass activity at elevated temperature (60 °C) with a lower activation energy (E_a). For the first time, the direct methanol fuel cell is fabricated utilizing sPdNiA as a bifunctional electrode, exhibited a higher peak power density (P_max) of 34 mW cm^–2, whereas 22 mW cm^–2 was obtained for Pd Np-based fuel cells. Incorporating oxophilic atom (Ni) not only improves the performance of Pd but significantly reduces the cost of the catalyst material by lowering the Pd content.

中文翻译：

球状 PdNi 合金：揭示碱性直接甲醇燃料电池的氧还原和温度依赖性甲醇氧化的双重功能特性

开发用于氧还原反应（ORR）和甲醇氧化反应（MOR）的高性能双功能钯基（Pd）合金是直接甲醇燃料电池中的一个巨大挑战。将亲氧原子结合到Pd原子中是提高催化剂电催化活性的有效策略。在此，通过简单的肼辅助还原方法开发了一种球状 PdNi 合金 (sPdNiA)，以克服钯的动力学缺点并提供卓越的 ORR/MOR 性能。通过 XRD、XPS 和 HR-TEM 研究证实了成功的合金形成、电子结构中的诱导应变效应以及 sPdNiA 的结构特征。因此，对于 ORR，sPdNiA 表现出正半波电位 ( E _1/2) ~ 0.854 V (vs RHE) 与纯 Pd (0.833 V vs RHE) 纳米粒子相比。对于 MOR，sPdNiA在 1.0 M KOH 电解质中呈现出 518 mA mg _Pd^{–1的低起始电位和高质量活性。}此外，温度相关的 MOR 和 3D 波德图研究揭示了在高温 (60 °C) 下具有较低活化能 ( E _a ) 的五倍高质量活性。首次使用 sPdNiA 作为双功能电极制造直接甲醇燃料电池，表现出更高的峰值功率密度 ( P _max ) 34 mW cm ^–2，而 22 mW cm ^–2获得了基于 Pd Np 的燃料电池。掺入亲氧原子（Ni）不仅提高了Pd的性能，而且通过降低Pd含量显着降低了催化剂材料的成本。

更新日期：2023-03-27

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