高质量和深度凹陷的PtPdNi纳米立方体作为高效氧还原反应的催化剂

doi:10.1016/S1872-2067(20)63703-2

催化学报 ›› 2021, Vol. 42 ›› Issue (5): 772-780.DOI: 10.1016/S1872-2067(20)63703-2

高质量和深度凹陷的PtPdNi纳米立方体作为高效氧还原反应的催化剂

李彦杰, 吴日枫, 刘洋, 文颖, 沈培康^*()

广西大学可再生能源材料协同创新中心, 广西电化学能源材料重点实验室, 物理科学与工程中心, 广西南宁530004

收稿日期:2020-04-18 接受日期:2020-04-18 出版日期:2021-05-18 发布日期:2021-01-29
通讯作者: 沈培康
基金资助:
国家自然科学基金-福建联合基金(U1705252);广西重点基金(AA17204083);广西重点基金(AB16380030);广东自然科学基金(2015A030312007)

High-quality and deeply excavated PtPdNi nanocubes as efficient catalysts toward oxygen reduction reaction

Yanjie Li, Rifeng Wu, Yang Liu, Ying Wen, Pei Kang Shen^*()

Collaborative Innovation Center of Sustainable Energy Materials, Guangxi Key Laboratory of Electrochemical Energy Materials, State Key Laboratory of Processing for Non-ferrous Metal and Featured Materials, Guangxi University, Nanning 530004, Guangxi, China

Received:2020-04-18 Accepted:2020-04-18 Online:2021-05-18 Published:2021-01-29
Contact: Pei Kang Shen
About author:^* Tel: +86-771-3237990; E-mail: pkshen@gxu.edu.cn
Supported by:
link project of the National Natural Science Foundation of China and Fujian Province(U1705252);Guangxi Science and Technology Project(AA17204083);Guangxi Science and Technology Project(AB16380030);Natural Science Foundation of Guangdong Province(2015A030312007)

摘要/Abstract

摘要：

聚合物电解质燃料电池阴极上的氧还原反应需要使用铂基催化剂, 铂是地球上的贵金属之一. 采用将不同的金属优化到核心中等多种策略可提高铂基催化剂的活性, 从而降低铂的负载量. 通过致力于高催化活性Pt_2.7Pd_0.3Ni凹面立方结构与高指数晶面的复合, 表明凹面结构可以提供更多的活性位和高水平的催化活性, 如果与其他金属复合, 可以降低铂的比例, 提高其质量活性. 本文采用一锅法合成了PtPdNi凹立方体结构, 并发现DMF和油胺的比例是影响PtPdNi凹陷程度的主要因素. 通过对PtPdNi凹立方体的形态和组成进行详细表征, 研究了PtPdNi凹立方体的形成机理, 认为十六烷基三甲基溴化铵、油酸胺和二甲基甲酰胺的比例在PtPdNi凹立方体的合成中起着关键作用. 本文还对Pt_2.7Pd_0.3Ni凹立方结构形成的理论和条件进行了探讨, 并通过改变反应条件, 考察了其所表现出的差异. 电化学测试的氧还原性能结果表明, 凹面立方体形状的PtPdNi催化剂在0.9 V下的质量活性为1.28 mg_Pt^-1, 最高质量活性和比活性分别是市售铂炭的8.20倍和8.68倍. 铂钯镍三元纳米笼具有优异的结构稳定性, 经稳定性测试, 纳米结构没有明显的变化和性能退化. PtPdNi凹立方体对阴极具有很高的电催化活性和稳定性, 燃料电池的氧还原反应由于高凹度、高空间利用率和PtPdNi凹立方体丰富的高指数表面以及PtPdNi之间的协同效应, 为进一步控制铂基纳米催化剂的合成提供更多的思路和方法及未来工业应用的不同形态和结构.

关键词: 氧还原反应, 聚合物电解质燃料电池, 凹面立方结构, 电化学催化剂

Abstract:

The oxygen reduction reaction (ORR) on the cathode of a polymer electrolyte fuel cell requires the use of a catalyst based on Pt, one of the most expensive metals on the earth. A number of strategies, including optimization of a different metal into the core, have been investigated to enhance the activity of a Pt-based catalyst and thus reduce the loading of Pt. By dedicating to compounding high catalytic activity Pt_2.7Pd_0.3Ni concave cubic with high index crystal face, the paper shows that concave structures can offer more active site and high level of catalytic activity and if mixed with other metal, decrease the proportion of Pt and improve its mass activity. The paper also makes an exploration into the theory and conditions behind the formation of Pt_2.7Pd_0.3Ni concave cubic structure, and investigates the difference it demonstrates by modifying the reactive conditions. The results of the oxygen reduction performance of the electrochemical test are as follows: the concave cube-shaped Pt-Pd-Ni catalyst has a mass activity of 1.28 A mg_Pt^-1 at 0.9 V, its highest mass activity is 8.20 times that of commercial Pt/C, and its specific activity is 8.68 times of that commercial Pt/C. And the Pt-Pd-Ni ternary nanocage has excellent structural invariance. After the stability test, there is no obvious structural change and performance degradation in the nanostructure.

Key words: Oxygen reduction reaction, Polymer electrolyte fuel cells, Concave cubic structure, Electrochemical catalyst

李彦杰, 吴日枫, 刘洋, 文颖, 沈培康. 高质量和深度凹陷的PtPdNi纳米立方体作为高效氧还原反应的催化剂[J]. 催化学报, 2021, 42(5): 772-780.

Yanjie Li, Rifeng Wu, Yang Liu, Ying Wen, Pei Kang Shen. High-quality and deeply excavated PtPdNi nanocubes as efficient catalysts toward oxygen reduction reaction[J]. Chinese Journal of Catalysis, 2021, 42(5): 772-780.

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图/表 5

Fig. 1. TEM (a) and HAADF-STEM (b) images of Pt2.7Pd0.3Ni DENCs; (c1, c2, c3) TEM images and schematic models of individual Pt2.7Pd0.3Ni DENCs; (d) HRTEM image taken from the red region boxed in (c1); (e) Enlarged HRTEM image taken from the edge of an individual Pt2.7Pd0.3Ni DENC and illustration of the atomic arrangement; (f) Corresponding fast Fourier transform (FFT) pattern of the Pt2.7Pd0.3Ni DENC shown in (c1).

Fig. 2. (a) HAADF-STEM images and corresponding EDX mapping images of individual Pt-Pd-Ni DENC; (b) Line-scanning profiles for Pt, Pd and Ni recorded across the red line shown in the inset; EDX spectrum (c) and XRD patterns (d) of the Pt-Pd-Ni DENCs.

Fig. 3. TEM images of the gold products obtained after a reaction time of 5 min (a,a-1), 60 min (b,b-1), and TEM images of the Pt-Pd-Ni with different morphology controlled by tuning the feeding amounts of DMF and OAM (c,c-1) 1 mL DMF and 9 mL OAM resulting in the formation of Pt-Pd-Ni alloy hyperbranched nanostructures, (d,d-1) 3 mL DMF and 7 mL OAM resulting in the formation of concave cubic structure.

Fig. 4. (a) Cyclic voltammograms of Pt-Pd-Ni concaves, Pt-Ni concaves, Pt concaves and TKK-Pt/C catalyst recorded at 50 mV s-1; (b) ORR polarization curves of these catalysts recorded at 10 mV s-1; (c) Mass activities of different catalysts measured at 0.9 V versus RHE; (d) Specific activities of different catalysts measured at 0.9 V versus RHE.

Fig. 5. (a) CV curves for the Pt/C before and after 10,000 CV potential cycles; (b) ORR polarization curves of the Pt-Pd-Ni concaves and TKK-Pt/C catalyst before and after 10,000 potential cycles.

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高质量和深度凹陷的PtPdNi纳米立方体作为高效氧还原反应的催化剂

High-quality and deeply excavated PtPdNi nanocubes as efficient catalysts toward oxygen reduction reaction

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