Adding refractory 5d transition metal W into PtCo system: an advanced ternary alloy for efficient oxygen reduction reaction†,Journal of Materials Chemistry A

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Adding refractory 5d transition metal W into PtCo system: an advanced ternary alloy for efficient oxygen reduction reaction†
Journal of Materials Chemistry A ( IF 10.7 ) Pub Date : 2018-05-10 00:00:00 , DOI: 10.1039/c8ta00029h
Yijun Wu _{1,

2,

3,

4,

5} , Yige Zhao _{1,

2,

3,

4,

5} , Jingjun Liu _{1,

2,

3,

4,

5} , Feng Wang _{1,

2,

3,

4,

5}

Affiliation

Tungsten (W), as a refractory 5d transition high-valency metal with unique physical and chemical properties, can substantially improve Pt-based alloys, providing a superior electrocatalytic performance for the oxygen reduction reaction (ORR), which is considered a key cathode process in fuel cell automotives or portable devices. In this study, we developed a graphene-supported Pt–Co–W ternary alloy, by using a facile one-pot polyol co-reduction of the above three metals. In 0.1 M HClO₄ solution, the obtained Pt–Co–W ternary alloy exhibited a surprisingly high specific activity of 3.41 mA cm⁻², which is 4.3 times higher than that of the well-known Pt–Co binary alloy (0.80 mA cm⁻²) and 13 times more than that obtained by the state-of-the-art Pt/C (0.27 mA cm⁻²). The mass activity of the alloy was 2.25 A mg_Pt⁻¹, which is 4.2 times higher than that of the Pt–Co binary alloy (0.53 A mg_Pt⁻¹) and 12 times higher than that obtained by the state-of-the-art Pt/C (0.19 A mg_Pt⁻¹) at 0.9 V versus a reversible hydrogen electrode (RHE). The remarkably enhanced ORR activity could be attributed to the incorporation of a small amount of W into the Pt–Co alloy system at an atomic level. The added W atoms could not only strengthen the chemical adsorption of oxygen molecules but also significantly facilitate desorption of the oxygenated species on the active Pt sites in this ternary alloy, because W has a stronger electronegativity, higher unsaturated 5d orbitals, and higher valency coordinated with these oxygenated groups. Therefore, introducing cheap refractory transition metals, like W, into Pt-based binary alloys may open a door to fabricate efficient next-generation ternary catalysts for the ORR.

中文翻译：

在PtCo系统中添加难熔的5d过渡金属W：一种用于有效氧还原反应的高级三元合金†

钨（W）是具有独特物理和化学性质的难熔5d过渡高价金属，可以显着改善Pt基合金，为氧还原反应（ORR）提供卓越的电催化性能，这被认为是关键的阴极工艺在燃料电池汽车或便携式设备中。在这项研究中，我们使用上述三种金属的简便一锅多元醇共还原技术，开发了一种石墨烯负载的Pt-Co-W三元合金。在0.1 M HClO ₄溶液中，所得的Pt-Co-W三元合金具有出乎意料的高比活度，为3.41 mA cm ^-2，比著名的Pt-Co二元合金（0.80 mA cm）高4.3倍。^-2），是最新Pt / C（0.27 mA cm^-2）。合金的质量活度为2.25 A mg_Pt^-1，比Pt-Co二元合金的质量活度（0.53 A mg_Pt^-1）高4.2倍，比通过最新状态获得的质量活度高12倍。 -Pt / C（0.19 A mg_Pt^-1）在0.9 V与可逆氢电极（RHE）。ORR活性的显着提高可能归因于在原子级将少量W掺入Pt-Co合金体系中。添加的W原子不仅可以增强氧分子的化学吸附，而且可以显着促进该三元合金中活性Pt位点上的氧化物种的解吸，因为W具有较强的电负性，较高的不饱和5d轨道和较高的化合价，与这些含氧基团。因此，向Pt基二元合金中引入便宜的难熔过渡金属（如W）可能为制造ORR的下一代高效三元催化剂打开一扇门。

更新日期：2018-05-10

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