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Size and Composition Dependence of Oxygen Reduction Reaction Catalytic Activities of Mo-Doped PtNi/C Octahedral Nanocrystals
ACS Catalysis ( IF 11.3 ) Pub Date : 2021-08-31 , DOI: 10.1021/acscatal.1c01761 Shlomi Polani 1 , Katherine E. MacArthur 2 , Malte Klingenhof 1 , Xingli Wang 1 , Paul Paciok 2 , Lujin Pan 1 , Quanchen Feng 1 , Attila Kormányos 3 , Serhiy Cherevko 3 , Marc Heggen 2 , Peter Strasser 1
ACS Catalysis ( IF 11.3 ) Pub Date : 2021-08-31 , DOI: 10.1021/acscatal.1c01761 Shlomi Polani 1 , Katherine E. MacArthur 2 , Malte Klingenhof 1 , Xingli Wang 1 , Paul Paciok 2 , Lujin Pan 1 , Quanchen Feng 1 , Attila Kormányos 3 , Serhiy Cherevko 3 , Marc Heggen 2 , Peter Strasser 1
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A variety of synthesis protocols for octahedral PtNi nanocatalysts have led to remarkable improvements in platinum mass and specific activities for the oxygen reduction reaction. Nevertheless, the values achieved are still only one tenth of the activity measured from Pt3Ni single-crystal (111) surfaces. These particles lose activity during potential cycling, primarily because of Ni leaching and subsequent loss of shape. Here, we present the syntheses and high catalytic oxygen reduction reaction activities of molybdenum-doped PtNi octahedral catalysts with different sizes (6–14 nm) and compositions. We show that the Mo-doped, Ni-rich, PtNi octahedral catalysts exhibit enhanced stability over their undoped counterpart. Scanning transmission electron microscopy with energy-dispersive X-ray analysis reveals the particular elemental distribution for the size and composition of the different catalysts. By combining high-resolution compositional analysis with electrochemical measurements and online inductively coupled plasma mass spectrometry, it was possible to correlate the size, morphology, and composition with the oxygen reduction reaction activities before and after accelerated stress tests. The octahedral catalysts show high electrochemical surface areas and increasing specific activity with increasing surface area of the (111) facets and Ni content, leading to high mass activities. These results demonstrate the advantages of increasing the (111) surface area and Ni content of PtNi nano-octahedral catalysts to improve the performance and stability for the oxygen reduction reaction.
中文翻译：
Mo掺杂PtNi/C八面体纳米晶氧还原反应催化活性的尺寸和组成依赖性
八面体 PtNi 纳米催化剂的各种合成方案显着提高了铂质量和氧还原反应的比活性。尽管如此，所获得的值仍仅为从 Pt 3测量的活性的十分之一Ni单晶（111）表面。这些颗粒在潜在循环过程中失去活性，主要是因为镍浸出和随后的形状损失。在这里，我们展示了不同尺寸（6-14 nm）和组成的钼掺杂 PtNi 八面体催化剂的合成和高催化氧还原反应活性。我们表明，与未掺杂的对应物相比，Mo 掺杂、富 Ni、PtNi 八面体催化剂表现出更高的稳定性。具有能量色散 X 射线分析的扫描透射电子显微镜揭示了不同催化剂的尺寸和组成的特定元素分布。通过将高分辨率成分分析与电化学测量和在线电感耦合等离子体质谱相结合，可以将尺寸、形态、与加速应力试验前后氧还原反应活性的组成。八面体催化剂显示出高电化学表面积和随着（111）面的表面积和Ni含量的增加而增加的比活性，从而导致高质量的活性。这些结果证明了增加 PtNi 纳米八面体催化剂的 (111) 表面积和 Ni 含量以提高氧还原反应的性能和稳定性的优势。
更新日期：2021-09-17
中文翻译：
Mo掺杂PtNi/C八面体纳米晶氧还原反应催化活性的尺寸和组成依赖性
八面体 PtNi 纳米催化剂的各种合成方案显着提高了铂质量和氧还原反应的比活性。尽管如此，所获得的值仍仅为从 Pt 3测量的活性的十分之一Ni单晶（111）表面。这些颗粒在潜在循环过程中失去活性，主要是因为镍浸出和随后的形状损失。在这里，我们展示了不同尺寸（6-14 nm）和组成的钼掺杂 PtNi 八面体催化剂的合成和高催化氧还原反应活性。我们表明，与未掺杂的对应物相比，Mo 掺杂、富 Ni、PtNi 八面体催化剂表现出更高的稳定性。具有能量色散 X 射线分析的扫描透射电子显微镜揭示了不同催化剂的尺寸和组成的特定元素分布。通过将高分辨率成分分析与电化学测量和在线电感耦合等离子体质谱相结合，可以将尺寸、形态、与加速应力试验前后氧还原反应活性的组成。八面体催化剂显示出高电化学表面积和随着（111）面的表面积和Ni含量的增加而增加的比活性，从而导致高质量的活性。这些结果证明了增加 PtNi 纳米八面体催化剂的 (111) 表面积和 Ni 含量以提高氧还原反应的性能和稳定性的优势。
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