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Engineering stable electrocatalysts by synergistic stabilization between carbide cores and Pt shells.
Nature Materials ( IF 37.2 ) Pub Date : 2019-12-16 , DOI: 10.1038/s41563-019-0555-5
Daniel Göhl 1, 2 , Aaron Garg 3 , Paul Paciok 4 , Karl J J Mayrhofer 1, 5 , Marc Heggen 4 , Yang Shao-Horn 6 , Rafal E Dunin-Borkowski 4 , Yuriy Román-Leshkov 3 , Marc Ledendecker 1
Affiliation  

Core-shell particles with earth-abundant cores represent an effective design strategy for improving the performance of noble metal catalysts, while simultaneously reducing the content of expensive noble metals1-4. However, the structural and catalytic stabilities of these materials often suffer during the harsh conditions encountered in important reactions, such as the oxygen reduction reaction (ORR)3-5. Here, we demonstrate that atomically thin Pt shells stabilize titanium tungsten carbide cores, even at highly oxidizing potentials. In situ, time-resolved experiments showed how the Pt coating protects the normally labile core against oxidation and dissolution, and detailed microscopy studies revealed the dynamics of partially and fully coated core-shell nanoparticles during potential cycling. Particles with complete Pt coverage precisely maintained their core-shell structure and atomic composition during accelerated electrochemical ageing studies consisting of over 10,000 potential cycles. The exceptional durability of fully coated materials highlights the potential of core-shell architectures using earth-abundant transition metal carbide (TMC) and nitride (TMN) cores for future catalytic applications.

中文翻译:

通过碳化物核和Pt壳之间的协同稳定作用来设计稳定的电催化剂。

具有富含地球的核的核-壳颗粒代表了一种有效的设计策略,可提高贵金属催化剂的性能,同时减少昂贵的贵金属1-4的含量。但是,这些材料的结构和催化稳定性通常在重要反应(例如氧还原反应(ORR)3-5)中遇到的苛刻条件下受到损害。在这里,我们证明了即使在高氧化电位下,原子上薄的Pt壳也能稳定碳化钨钛芯。在时间上进行时间分辨的实验表明,Pt涂层如何保护通常不稳定的核免受氧化和溶解,详细的显微镜研究表明,在潜在的循环过程中,部分和完全涂覆的核-壳纳米粒子具有动力学特性。在由超过10,000个潜在循环组成的加速电化学老化研究过程中,具有完整Pt覆盖的颗粒可以精确地保持其核-壳结构和原子组成。全涂层材料的出色耐用性凸显了将核土壳结构用于未来催化应用的潜力,该结构使用了富含地球的过渡金属碳化物(TMC)和氮化物(TMN)核。
更新日期:2019-12-17
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