具有经济性的碱性膜燃料电池氢气氧化反应催化剂

doi:10.3866/PKU.WHXB202009103

物理化学学报 >> 2021, Vol. 37 >> Issue (9): 2009103.doi: 10.3866/PKU.WHXB202009103

所属专题：燃料电池

具有经济性的碱性膜燃料电池氢气氧化反应催化剂

薛延荣¹, 王兴栋¹, 张向前¹, 方锦杰¹^,², 许志远¹^,², 张宇烽¹, 刘雪瑞¹^,², 刘梦园¹, 朱威¹, 庄仲滨¹^,²^,³^,*()

¹ 有机无机复合材料国家重点实验室，北京化工大学，北京 100029
² 北京软物质科学与工程高精尖创新中心，北京化工大学，北京 100029
³ 能源环境催化北京市重点实验室，北京化工大学，北京 100029

收稿日期:2020-09-30 录用日期:2020-11-02 发布日期:2020-11-12
通讯作者: 庄仲滨 E-mail:zhuangzb@mail.buct.edu.cn
作者简介:Zhongbin Zhuang, born in August 1983, received his Ph.D. degrees from Tsinghua University 2010. He joined Beijing University of Chemical Technology as a professor in 2015. His current research interests include electrocatalysts for fuel cell and electrolyzers, interfacial electrochemistry and methodology for nanocrystal synthesis
基金资助:
国家重点研发计划(2019YFA0210300);国家自然科学基金(21671014)

Cost-Effective Hydrogen Oxidation Reaction Catalysts for Hydroxide Exchange Membrane Fuel Cells

Yanrong Xue¹, Xingdong Wang¹, Xiangqian Zhang¹, Jinjie Fang¹^,², Zhiyuan Xu¹^,², Yufeng Zhang¹, Xuerui Liu¹^,², Mengyuan Liu¹, Wei Zhu¹, Zhongbin Zhuang¹^,²^,³^,*()

¹ State Key Lab of Organic-Inorganic Composites, Beijing University of Chemical Technology, Beijing 100029, China
² Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing 100029, China
³ Beijing Key Laboratory of Energy Environmental Catalysis, Beijing University of Chemical Technology, Beijing 100029, China

Received:2020-09-30 Accepted:2020-11-02 Published:2020-11-12
Contact: Zhongbin Zhuang E-mail:zhuangzb@mail.buct.edu.cn
About author:Zhongbin Zhuang, Email: zhuangzb@mail.buct.edu.cn. Tel.: +86-10-64434780
Supported by:
the National Key Research and Development Program of China(2019YFA0210300);the National Natural Science Foundation of China(21671014)

摘要/Abstract

摘要：

燃料电池是一种清洁高效的能量转换装置，可将储存在燃料中的化学能直接转化为电能。在过去的几十年中，燃料电池的开发取得了重大进展。聚合物电解质燃料电池，尤其是以质子交换膜燃料电池(PEMFC)为代表，可以实现高效率、高功率密度、快速启动，因而受到了广泛的关注。然而，PEMFC因使用昂贵的Pt基催化剂而导致成本较高，阻碍了其大规模的应用。近年来发展的碱性膜燃料电池(HEMFC)与PEMFC结构相似，但使用可传导氢氧根离子的聚合物电解质，并提供碱性工作环境。HEMFC由于具有使用非Pt电催化剂和较便宜双极板的可能性而备受关注。然而，HEMFC的一个巨大的挑战是阳极氢氧化反应(HOR)相对缓慢的动力学，这使得其需要较高载量的阳极催化剂才能实现较高的电池性能。因此，对于HEMFC而言，阳极催化剂的成本也很高，亟需开发在碱性条件下低成本、高活性和高稳定性的HOR催化剂。在本综述中，我们总结了HOR催化剂的最新研究进展，涉及文献中提出的各种HOR机理和催化剂，并分析了基于阳极催化剂成本的HEMFC性能。我们发现，最新报道的非Pt HOR催化剂可以降低阳极催化剂的成本，到达与PEMFC接近的成本水平。最后，我们对HOR的进一步研究进行了展望。

关键词: 碱性膜燃料电池, 氢气氧化反应, 电催化剂, 铂族金属, 成本

Abstract:

Fuel cells are clean, efficient energy conversion devices that produce electricity from chemical energy stored within fuels. The development of fuel cells has significantly progressed over the past decades. Specifically, polymer electrolyte fuel cells, which are representative of proton exchange membrane fuel cells (PEMFCs), exhibit high efficiency, high power density, and quick start-up times. However, the high cost of PEMFCs, partially from the Pt-based catalysts they employ, hinders their diverse applicability. Hydroxide exchange membrane fuel cells (HEMFCs), which are also known as alkaline polymer electrolyte fuel cells (APEFCs), alkaline anion-exchange membrane fuel cells (AAEMFCs), anion exchange membrane fuel cells (AEMFCs), or alkaline membrane fuel cells (AMFCs), have attracted much attention because of their capability to use non-Pt electrocatalysts and inexpensive bipolar plates. The HEMFCs are structurally similar to PEMFCs but they use a polymer electrolyte that conducts hydroxide ions, thus providing an alkaline environment. However, the relatively sluggish kinetics of the hydrogen oxidation reaction (HOR) inhibit the practical application of HEMFCs. The anode catalyst loading needed for HEMFCs to achieve high cell performance is larger than that required for other fuel cells, which substantially increases the cost of HEMFCs. Therefore, low-cost, highly active, and stable HOR catalysts in the alkaline condition are greatly desired. Here, we review the recent achievements in developing such HOR catalysts. First, plausible HOR mechanisms are explored and HOR activity descriptors are summarized. The HOR processes are mainly controlled by the binding energy between hydrogen and the catalysts, but they may also be influenced by OH adsorption, interfacial water adsorption, and the potential of zero (free) charge. Next, experimental methods used to elevate HOR activities are introduced, followed by HOR catalysts reported in the literature, including Pt-, Ir-, Pd-, Ru-, and Ni-based catalysts, among others. HEMFC performances when employing various anode catalysts are then summarized, where HOR catalysts with platinum-group metals exhibited the highest HEMFC performance. Although the Ni-based HOR catalyst activity was higher than those of other non-precious metal-based catalysts, they showed unsatisfactory performance in HEMFCs. We further analyzed HEMFC performances while considering anode catalyst cost, where we found that this cost can be reduced by using recently developed, non-Pt HOR catalysts, especially Ru-based catalysts. In fact, an HEMFC using a Ru-based HOR catalyst showed an anode catalyst cost-based performance similar to that of PEMFCs, making the HEMFC promising for use in practical applications. Finally, we proposed routes for developing future HOR catalysts for HEMFCs.

Key words: Hydroxide exchange membrane fuel cell, Hydrogen oxidation reaction, Electrocatalyst, Platinum-group metal, Cost

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薛延荣, 王兴栋, 张向前, 方锦杰, 许志远, 张宇烽, 刘雪瑞, 刘梦园, 朱威, 庄仲滨. 具有经济性的碱性膜燃料电池氢气氧化反应催化剂[J]. 物理化学学报, 2021, 37(9), 2009103. doi: 10.3866/PKU.WHXB202009103

Yanrong Xue, Xingdong Wang, Xiangqian Zhang, Jinjie Fang, Zhiyuan Xu, Yufeng Zhang, Xuerui Liu, Mengyuan Liu, Wei Zhu, Zhongbin Zhuang. Cost-Effective Hydrogen Oxidation Reaction Catalysts for Hydroxide Exchange Membrane Fuel Cells[J]. Acta Phys. -Chim. Sin. 2021, 37(9), 2009103. doi: 10.3866/PKU.WHXB202009103

链接本文: https://www.whxb.pku.edu.cn/CN/10.3866/PKU.WHXB202009103

https://www.whxb.pku.edu.cn/CN/Y2021/V37/I9/2009103

图/表 9

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Fig 6

The H2/O2 HEMFC performance by using NiCu/KB as anode catalyst (4 mg·cm-2) and Pd/C as cathode catalyst (0.2 mg·cm-2). The cell temperatures are 60, 70, 80 ℃, respectively 109. Modifying the Ni based catalysts by non-metallic elements, especially N, also shows the benefits. The modification can be done either on the support or Ni itself. Yan et al. 110 using nitrogen-doped carbon nanotubes (N-CNT) as the support and the mass activity and exchange current density of Ni/N-CNT increases by a factor of 33 and 21, respectively. The DFT calculations indicate that N-CNT stabilizes Ni nanoparticle and locally activated for the HOR because of nitrogen located at the edge of the nanoparticle tunes local adsorption sites by affecting the d-orbitals of Ni. Yang et al. 111 found that the HOR activity of Ni nanoparticles supported on N-doped carbon nanosheets exhibits a volcano dependence on the N-doping level, and the 8.7% (atomic fraction) N content of catalyst exhibits an optimal HOR activity. Directly doping N into Ni nanoparticles can also enhance its HOR activity. Sun et al. 112 reported a unique Ni3N/Ni electrocatalyst that exhibits exceptional HER/HOR activities in base, and the active sites are located at the interface between Ni3N and Ni. Hu et al. 113 using the ultraviolet photoemission spectroscopy (UPS) technique analyzed the downshift of the Ni d-band and interfacial charge transfer from Ni3N to the carbon which lead to the weak HBE in Ni3N/C. The HBE has the order of Ni > Ni3N > Ni3N/C, so the Ni3N/C has the highest HOR activity. In addition, the weak oxygen species adsorption energy of Ni3N/C is not conducive to the oxidation of Ni and therefore has a higher break-down potential. Furthermore, the doping with other non-metal elements than N has also been reported as efficient ways to improve the HOR activities of Ni. For example, Luo et al. 114 reported the HOR activity of Ni which supported on heteroatom (S, N, or B) doped carbon, and the trend following the sequence of Ni/S-C > Ni/N-C > Ni/B-C."

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具有经济性的碱性膜燃料电池氢气氧化反应催化剂

Cost-Effective Hydrogen Oxidation Reaction Catalysts for Hydroxide Exchange Membrane Fuel Cells

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