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Behavior of gold-enhanced electrocatalytic performance of NiPtAu hollow nanocrystals for alkaline methanol oxidation

Au增强NiPtAu中空纳米晶体电催化碱性甲醇氧化性能的行为研究

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Abstract

The Pt-based catalyst tends to be poisoned by carbon monoxide (CO)-like intermediates produced in fuel cell reactions, which seriously deteriorates its catalytic performance. Herein, noble metal Au with the capacity of resistance to CO-like intermediates poisoning was employed to construct multi-element Pt-based catalysts. Two trimetallic NiPtAu hollow nanocrystals (HNCs) with different surface Au contents were synthesized to explore the role of Au in electrocatalysis for alkaline methanol oxidation reaction (MOR). The trimetallic NiPtAu-SRAu HNCs catalyst with the relative rich Au content (15.17 at%) on surface exhibits a much lower CO oxidation peak potential than the other HNCs counterpart and 20 wt% Pt/C, which indicates the more exceptional CO-resisting performance. Besides, the MOR specific activity of NiPtAu-SRAu HNCs (31.52 mA cm−2) is 7 times higher than that of 20wt% Pt/C (4.50 mA cm−2). This enhancement in catalytic activity as well as anti-CO poisoning capability for NiPtAu-SRAu HNCs can be mainly ascribed to the weakened CO adsorption due to the exposure of Au atoms on NiPt surface evidenced by the experimental data and density functional theory calculations. This study not only investigates the role of Au in MOR catalysis but also could be helpful for designing and optimizing the electrocatalysts for high-active and robust fuel cell applications.

摘要

甲醇氧化反应中产生的CO等中间体是导致Pt基催化剂中毒 而丧失催化活性的重要原因. 针对该问题, 本文利用具有较强抗CO中毒能力的贵金属Au构建多元Pt基催化剂. 采用置换法合成了两种表面Au元素含量不同的NiPtAu中空纳米晶体(HNCs), 分析了其电催化性能及抗CO毒化性能, 并探讨了Au在电催化碱性甲醇氧化反应中的作用. 研究结果表明, 相比于其他样品, 表面Au含量相对较高的NiPtAu-SRAu HNCs (15.17 at%)展现出更优异的电催化性能 以及抗CO毒化性能. NiPt表面暴露的Au能削弱催化剂表面对CO的吸附, 有利于提高电催化甲醇氧化的性能和抗CO中毒能力. 这一研究结果不仅有助于深化认识Au在电催化甲醇氧化反应中的作用机理, 同时也为燃料电池用新型高性能电催化剂的结构设计和优化提供了参考.

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Acknowledgements

This study was supported by the National Natural Science Foundation of China (91963113, 51701139, 51671143 and U1601216), and we are especially grateful for the support from the National Supercomputer Center in Lvliang, China. The calculations in this work were carried out using the supercomputer system, TianHe-2.

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Authors and Affiliations

  1. School of Materials Science and Engineering, Key Laboratory of Advanced Ceramics and Machining Technology of Ministry of Education, Tianjin Key Laboratory of Composite and Functional Materials, Tianjin University, Tianjin, 300372, China

    Chang Liu  (刘畅), Zelin Chen  (陈泽霖), Jinfeng Zhang  (张金凤), Yunwei Liu  (刘赟威), Yanan Chen  (邓意达), Yida Deng  (陈亚楠) & Wenbin Hu  (胡文彬)

  2. School of Materials Science and Engineering, Jiangsu University, Zhenjiang, 212013, China

    Dewei Rao  (饶德伟)

  3. Joint School of National University of Singapore and Tianjin University, International Campus of Tianjin University, Fuzhou, 350207, China

    Wenbin Hu  (胡文彬)

Authors
  1. Chang Liu  (刘畅)
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  2. Zelin Chen  (陈泽霖)
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  3. Dewei Rao  (饶德伟)
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  6. Yanan Chen  (邓意达)
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  7. Yida Deng  (陈亚楠)
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  8. Wenbin Hu  (胡文彬)
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Contributions

Author contributions Chen Y and Deng Y guided the whole project. Liu C designed and performed the experiments. Rao D performed the DFT calculations. All authors contributed to analyses and discussion of the results.

Corresponding authors

Correspondence to Yanan Chen  (邓意达) or Yida Deng  (陈亚楠).

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Conflict of interest The authors declare no conflict of interest.

Additional information

Chang Liu is a PhD candidate at the School of Materials Science and Engineering, Tianjin University. Her research interests focus on the design and synthesis of nanocatalysts for electrocatalytic application in fuel cells.

Yida Deng is a professor at the School of Materials Science and Engineering, Tianjin University. He received his PhD degree from Shanghai Jiao Tong University in 2006. His research interests include metal and metal oxide nanostructures for electrochemical and energy applications.

Yanan Chen is a professor at the School of Materials Science and Engineering, Tianjin University. He received his joint PhD degree from the University of Science and Technology Beijing/University of Maryland in 2017. He was an advanced innovative fellow at Tsinghua University before joining in Tianjin University. His research mainly focuses on nanomaterials, devices, and systems for advanced energy storage and conversion, including nanomaterials synthesis & nanomanufacturing, emerging energy storage Li-ion and beyond, catalysis, and Cryo-EM.

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Liu, C., Chen, Z., Rao, D. et al. Behavior of gold-enhanced electrocatalytic performance of NiPtAu hollow nanocrystals for alkaline methanol oxidation. Sci. China Mater. 64, 611–620 (2021). https://doi.org/10.1007/s40843-020-1460-y

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