Ga–Doped Pt–Ni Octahedral Nanoparticles as a Highly Active and Durable Electrocatalyst for Oxygen Reduction Reaction,Nano Letters

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Ga–Doped Pt–Ni Octahedral Nanoparticles as a Highly Active and Durable Electrocatalyst for Oxygen Reduction Reaction
Nano Letters ( IF 9.6 ) Pub Date : 2018-03-26 00:00:00 , DOI: 10.1021/acs.nanolett.8b00028
JeongHoon Lim ₁ , Hyeyoung Shin ₂ , MinJoong Kim ₁ , Hoin Lee ₁ , Kug-Seung Lee ₃ , YongKeun Kwon ₁ , DongHoon Song ₁ , SeKwon Oh ₁ , Hyungjun Kim _{4,

5} , EunAe Cho ₁

Affiliation

Bimetallic PtNi nanoparticles have been considered as a promising electrocatalyst for oxygen reduction reaction (ORR) in polymer electrolyte membrane fuel cells (PEMFCs) owing to their high catalytic activity. However, under typical fuel cell operating conditions, Ni atoms easily dissolve into the electrolyte, resulting in degradation of the catalyst and the membrane-electrode assembly (MEA). Here, we report gallium-doped PtNi octahedral nanoparticles on a carbon support (Ga–PtNi/C). The Ga–PtNi/C shows high ORR activity, marking an 11.7-fold improvement in the mass activity (1.24 A mg_Pt^–1) and a 17.3-fold improvement in the specific activity (2.53 mA cm^–2) compared to the commercial Pt/C (0.106 A mg_Pt^–1 and 0.146 mA cm^–2). Density functional theory calculations demonstrate that addition of Ga to octahedral PtNi can cause an increase in the oxygen intermediate binding energy, leading to the enhanced catalytic activity toward ORR. In a voltage-cycling test, the Ga–PtNi/C exhibits superior stability to PtNi/C and the commercial Pt/C, maintaining the initial Ni concentration and octahedral shape of the nanoparticles. Single cell using the Ga–PtNi/C exhibits higher initial performance and durability than those using the PtNi/C and the commercial Pt/C. The majority of the Ga–PtNi nanoparticles well maintain the octahedral shape without agglomeration after the single cell durability test (30,000 cycles). This work demonstrates that the octahedral Ga–PtNi/C can be utilized as a highly active and durable ORR catalyst in practical fuel cell applications.

中文翻译：

Ga掺杂的Pt-Ni八面体纳米粒子是一种高活性且持久的氧还原反应电催化剂

由于其高催化活性，双金属PtNi纳米颗粒已被认为是用于聚合物电解质膜燃料电池（PEMFC）中氧还原反应（ORR）的有前途的电催化剂。但是，在典型的燃料电池工作条件下，Ni原子容易溶解到电解质中，导致催化剂和膜电极组件（MEA）降解。在这里，我们报告了在碳载体（Ga-PtNi / C）上掺杂了镓的PtNi八面体纳米颗粒。Ga–PtNi / C具有较高的ORR活性，与市售品相比，质量活性（1.24 A mg _Pt^–1）提高了11.7倍，比活度（2.53 mA cm ^–2）提高了17.3倍。Pt / C（0.106 A mg _Pt^–1和0.146 mA cm^–2）。密度泛函理论计算表明，将Ga添加到八面体PtNi中可以导致氧中间键合能的增加，从而导致对ORR的催化活性增强。在电压循环测试中，Ga-PtNi / C表现出优于PtNi / C和市售Pt / C的稳定性，并保持了纳米粒子的初始Ni浓度和八面体形状。与使用PtNi / C和商用Pt / C的电池相比，使用Ga-PtNi / C的单电池具有更高的初始性能和耐久性。在单细胞耐久性试验（30,000次循环）后，大多数Ga-PtNi纳米颗粒都能很好地保持八面体形状而不会发生团聚。这项工作表明，八面体Ga-PtNi / C可以在实际的燃料电池应用中用作高活性和耐用的ORR催化剂。

更新日期：2018-03-26

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