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Composition-Dependent Oxygen Reduction Reaction Activity of Pt-Surfaced PtNi Dodecahedral Nanoframes
ACS Applied Energy Materials ( IF 5.4 ) Pub Date : 2020-01-02 00:00:00 , DOI: 10.1021/acsaem.9b01930 Yongchen Wang 1 , Shutang Chen 1 , Xudong Wang 1 , Adam Rosen 2 , William Beatrez 2 , Lukasz Sztaberek 2, 3 , Haiyan Tan 4 , Liang Zhang 5 , Christopher Koenigsmann 2 , Jing Zhao 1, 4
ACS Applied Energy Materials ( IF 5.4 ) Pub Date : 2020-01-02 00:00:00 , DOI: 10.1021/acsaem.9b01930 Yongchen Wang 1 , Shutang Chen 1 , Xudong Wang 1 , Adam Rosen 2 , William Beatrez 2 , Lukasz Sztaberek 2, 3 , Haiyan Tan 4 , Liang Zhang 5 , Christopher Koenigsmann 2 , Jing Zhao 1, 4
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Pt-based bimetallic nanoframes have been demonstrated to have high activity for a number of electrocatalytic reactions. Their morphology, crystal facets, and compositions are important factors that regulate their catalytic activities. Herein, we synthesized a series of Pt-surfaced PtNi dodecahedral nanoframes with variable Pt/Ni ratios. The nanoframes were prepared by oxidative etching of presynthesized PtNi rhombic dodecahedron nanoparticles. The Pt ratio in the PtNi nanoframes have been tuned from 28% to 65% by changing the duration of oxidative etching. In terms of catalytic performance, the PtNi nanoframes display a volcano-type behavior in specific oxygen reduction reaction (ORR) activity as a function of Pt ratio with a maximum ORR specific activity of 1.9 mA cm–2 observed with 47% Pt. The mass activity of the particles ranges from 0.72 to 0.92 A mg–1, which significantly exceeds the mass activity of 0.19 A mg–1 measured for commercial Pt NP/C. Density functional theory calculations reveal that the Pt ratio underneath the Pt skin in the nanoframes affects the binding energy of oxygenate species and thus the ORR activity. The trend of OH binding energy versus PtNi composition from the computational results qualitatively agrees with the trend of ORR activity from the experiments.
中文翻译：
Pt表面PtNi十二面体纳米框架的成分依赖性氧还原反应活性
铂基双金属纳米框架已被证明对许多电催化反应具有高活性。它们的形态，晶面和组成是调节其催化活性的重要因素。本文中，我们合成了一系列具有可变Pt / Ni比的Pt表面PtNi十二面体纳米框架。通过对预先合成的PtNi菱形十二面体纳米粒子进行氧化蚀刻来制备纳米框架。通过更改氧化蚀刻的持续时间，PtNi纳米框架中的Pt比例已从28％调整为65％。在催化性能方面，PtNi纳米框架在比氧还原反应（ORR）活性方面表现出火山型行为，这是Pt比的函数，最大ORR比活性为1.9 mA cm –2用47％的Pt观察到。颗粒的质量活度在0.72至0.92 A mg –1的范围内，大大超过了商用Pt NP / C所测量的0.19 A mg –1的质量活度。密度泛函理论计算表明，纳米框架中Pt皮肤下方的Pt比会影响含氧物质的结合能，从而影响ORR活性。从计算结果来看，OH结合能与PtNi组成的趋势定性与实验中ORR活性的趋势一致。
更新日期：2020-01-02
中文翻译：
Pt表面PtNi十二面体纳米框架的成分依赖性氧还原反应活性
铂基双金属纳米框架已被证明对许多电催化反应具有高活性。它们的形态，晶面和组成是调节其催化活性的重要因素。本文中，我们合成了一系列具有可变Pt / Ni比的Pt表面PtNi十二面体纳米框架。通过对预先合成的PtNi菱形十二面体纳米粒子进行氧化蚀刻来制备纳米框架。通过更改氧化蚀刻的持续时间，PtNi纳米框架中的Pt比例已从28％调整为65％。在催化性能方面，PtNi纳米框架在比氧还原反应（ORR）活性方面表现出火山型行为，这是Pt比的函数，最大ORR比活性为1.9 mA cm –2用47％的Pt观察到。颗粒的质量活度在0.72至0.92 A mg –1的范围内，大大超过了商用Pt NP / C所测量的0.19 A mg –1的质量活度。密度泛函理论计算表明，纳米框架中Pt皮肤下方的Pt比会影响含氧物质的结合能，从而影响ORR活性。从计算结果来看，OH结合能与PtNi组成的趋势定性与实验中ORR活性的趋势一致。
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