Binary oxide modified catalyst preparation and self-humidifying performance

doi:10.19799/j.cnki.2095-4239.2021.0386

Abstract

Abstract:

The Pt/C catalyst was modified by premodification and postmodification methods using tin-silicon binary oxide to prepare two composite catalysts. Furthermore, two composite catalysts were used on the anode to prepare a membrane electrode assembly (MEA). First, the influence of modification methods on the performance of MEA was investigated. The cell performance test of two MEAs demonstrated that the Pt/SnO₂-SiO₂/C composite catalyst prepared by the premodification method had better cell performance: the current density at 0.6 V is as high as 1100 mA/cm² under complete humidification at 50 ℃. At the same time, the MEA also exhibited excellent self-humidification performance and stability: the current density at 0.6 V is 930 mA/cm²at a 50 ℃ cell temperature and with no humidification (dry gas); after the 10 h stability test, the performance only decreased by 13%, while the performance of blank MEAs decreases by 63% within 2 h. Further comparisons of the MEA performance under different relative humidity conditions shows that the MEA exhibits excellent self-humidification performance under low relative humidity conditions. According to the experimental data, the self-humidification mechanism of a Pt/SnO₂-SiO₂/C composite catalyst is preliminarily speculated.

Key words: fuel cells, catalyst, composites, Sn/Si binary oxide, low humidity

CLC Number:

TM 911.4

Boya ZHANG, Bohong LIU, Yuanhang LI, Xin LIU, Qianfeng CHEN, Sanying HOU. Binary oxide modified catalyst preparation and self-humidifying performance[J]. Energy Storage Science and Technology, 2021, 10(6): 2013-2019.

Figures/Tables 9

Table 1

Fig. 1

Fig. 2

Fig. 3

Fig. 4

Fig. 5

Fig. 6

Fig. 7

Fig. 8

References 21

1	CANO Z P, BANHAM D, YE S Y, et al. Batteries and fuel cells for emerging electric vehicle markets[J]. Nature Energy, 2018, 3(4): 279-289.
2	GERBEC M, JOVAN V, PETROVČIČ J. Operational and safety analyses of a commercial PEMFC system[J]. International Journal of Hydrogen Energy, 2008, 33(15): 4147-4160.
3	TEIXEIRA F C, DE SÁ A I, TEIXEIRA A P S, et al. Nafion phosphonic acid composite membranes for proton exchange membranes fuel cells[J]. Applied Surface Science, 2019, 487: 889-897.
4	KETPANG K, LEE K, SHANMUGAM S. Facile synthesis of porous metal oxide nanotubes and modified nafion composite membranes for polymer electrolyte fuel cells operated under low relative humidity[J]. ACS Applied Materials & Interfaces, 2014, 6(19): 16734-16744.
5	SAKAMOTO M, NOHARA S, MIYATAKE K, et al. Effects of incorporation of SiO₂ nanoparticles into sulfonated polyimide electrolyte membranes on fuel cell performance under low humidity conditions[J]. Electrochimica Acta, 2014, 137: 213-218.
6	BAE I, OH K H, YUN S H, et al. Asymmetric silica composite polymer electrolyte membrane for water management of fuel cells[J]. Journal of Membrane Science, 2017, 542: 52-59.
7	KETPANG K, SHANMUGAM S, SUWANBOON C, et al. Efficient water management of composite membranes operated in polymer electrolyte membrane fuel cells under low relative humidity[J]. Journal of Membrane Science, 2015, 493: 285-298.
8	SHANMUGAM S, KETPANG K, AZIZ M A, et al. Composite polymer electrolyte membrane decorated with porous titanium oxide nanotubes for fuel cell operating under low relative humidity[J]. Electrochimica Acta, 2021, 384: doi: 10.1016/j.electacta.2021.138407
9	PATEL H A, MANSOR N, GADIPELLI S, et al. Superacidity in nafion/MOF hybrid membranes retains water at low humidity to enhance proton conduction for fuel cells[J]. ACS Applied Materials & Interfaces, 2016, 8(45): 30687-30691.
10	OH K, KWON O, SON B, et al. Nafion-sulfonated silica composite membrane for proton exchange membrane fuel cells under operating low humidity condition[J]. Journal of Membrane Science, 2019, 583: 103-109.
11	WATANABE M, UCHIDA H, EMORI M. Polymer electrolyte membranes incorporated with nanometer-size particles of Pt and/or metal-oxides: experimental analysis of the self-humidification and suppression of gas-crossover in fuel cells[J]. The Journal of Physical Chemistry B, 1998, 102(17): 3129-3137.
12	LIN C L, HSU S C, HO W Y. Addition of sulfonated silicon dioxide on an anode catalyst layer to improve the performance of a self-humidifying proton exchange membrane fuel cell[J]. Functional Materials Letters, 2016, 9(2): doi: 10.1142/S1793604716500259
13	JIENKULSAWAD P, CHEN Y S, ARPORNWICHANOP A. Modifying the catalyst layer using polyvinyl alcohol for the performance improvement of proton exchange membrane fuel cells under low humidity operations[J]. Polymers, 2020, 12(9): 1865.
14	LO A Y, HUANG C Y, SUNG L Y, et al. Electrophoretic deposited Pt/C/SiO₂ anode for self-humidifying and improved catalytic activity in PEMFC[J]. Electrochimica Acta, 2015, 180: 610-615.
15	GANESAN A, NARAYANASAMY M, SHUNMUGAVEL K. Self-humidifying manganese oxide-supported Pt electrocatalysts for highly-durable PEM fuel cells[J]. Electrochimica Acta, 2018, 285: 47-59.
16	SU H N, XU L M, ZHU H P, et al. Self-humidification of a PEM fuel cell using a novel Pt/SiO₂/C anode catalyst[J]. International Journal of Hydrogen Energy, 2010, 35(15): 7874-7880.
17	LO A Y, HUANG C Y, SUNG L Y, et al. Low humidifying proton exchange membrane fuel cells with enhanced power and Pt-C-h-SiO₂ anodes prepared by electrophoretic deposition[J]. ACS Sustainable Chemistry & Engineering, 2016, 4(3): 1303-1310.
18	JUNG C Y, YI J Y, YI S C. On the role of the silica-containing catalyst layer for proton exchange membrane fuel cells[J]. Energy, 2014, 68: 794-800.
19	HOU S Y, CHEN R, ZOU H B, et al. High-performance membrane electrode assembly with multi-functional Pt/SnO₂-SiO₂/C catalyst for proton exchange membrane fuel cell operated under low-humidity conditions[J]. International Journal of Hydrogen Energy, 2016, 41(21): 9197-9203.
20	LUO F, LIAO S J, DANG D, et al. Tin and silicon binary oxide on the carbon support of a Pt electrocatalyst with enhanced activity and durability[J]. ACS Catalysis, 2015, 5(4): 2242-2249.
21	LEIMIN X, SHIJUN L, LIJUN Y, et al. Investigation of a novel catalyst coated membrane method to prepare low-platinum-loading membrane electrode assemblies for PEMFCs[J]. Fuel Cells, 2009, 9(2): 101-105.

膜电极名称	阳极	阴极
MEA 0	Pt/C (40% Pt)	Pt/C (40% Pt)
MEA 1	Pt/SnO₂-SiO₂/C (20% Pt)	Pt/C (40% Pt)
MEA 2	Pt/C-SnO₂-SiO₂ (40% Pt)	Pt/C (40% Pt)
MEA 3	Pt/C (40% Pt)	Pt/SnO₂-SiO₂/C (20% Pt)

[1]	XIE Chenglu, HUANG Xiankun, KANG Lixia, LIU Yongzhong. Electrocatalytic performances of Ru nanoparticles supported on carbon nanotubes by colloidal solution for synthetic ammonia [J]. Energy Storage Science and Technology, 2022, 11(6): 1947-1956.
[2]	WANG Peican, WAN Lei, XU Ziang, XU Qin, PANG Maobin, CHEN Jinxun, WANG Baoguo. Interface engineering of self-supported electrode for electrochemical water splitting [J]. Energy Storage Science and Technology, 2022, 11(6): 1934-1946.
[3]	Jianxin CHEN, Nan SHENG, Chunyu ZHU, Zhonghao RAO. Study on nickel-based nanoparticles supported by biomass carbon for electrocatalytic hydrogen evolution [J]. Energy Storage Science and Technology, 2022, 11(5): 1350-1357.
[4]	Yezhou HU, Shuang WANG, Tao SHEN, Ye ZHU, Deli WANG. Recent progress in confined noble-metal electrocatalysts for oxygen reduction reaction [J]. Energy Storage Science and Technology, 2022, 11(4): 1264-1277.
[5]	Yunqi GUO, Nan SHENG, Chunyu ZHU, Zhonghao RAO. Preparation of Al₂O₃ fibers using a template method， and the investigation of the thermal properties of paraffin phase-change composite [J]. Energy Storage Science and Technology, 2022, 11(2): 511-520.
[6]	Linhui JIA, Zejia GAI, Moxi LI, Huagen LIANG. Research progress of MOFs and their derivatives as cathode catalysts for Li-O₂ batteries [J]. Energy Storage Science and Technology, 2022, 11(2): 503-510.
[7]	Linhan XIE, Wanzhong LI, Qianqian ZHANG, Gaoping CAO, Jingyi QIU, Hai MING, Wei FENG. Research advances in plant-power generation technology [J]. Energy Storage Science and Technology, 2022, 11(2): 442-466.
[8]	Yuexia LI, Quanbing LIU. Application of MXene-based nanomaterials in electrocatalysis for oxygen reduction reaction [J]. Energy Storage Science and Technology, 2021, 10(6): 1918-1930.
[9]	Feng HE, Jingjing ZHANG, Yijun CHEN, Jian ZHANG, Deli WANG. Recent progress on carbon-based catalysts for electrochemical synthesis of H₂O₂ via oxygen reduction reaction [J]. Energy Storage Science and Technology, 2021, 10(6): 1963-1976.
[10]	Shenzhi ZHANG, Likai WANG, Yinggang SUN, Heng LÜ, Ziyin YANG, Leilei LI, Zhongfang LI. Construction of two dimensional carbon-supported Au₄Pd₂ catalysts and their electrocatalytic performances [J]. Energy Storage Science and Technology, 2021, 10(6): 2028-2038.
[11]	Wenwu ZOU, Guoxing JIANG, Li DU. Recent advances in covalent organic frameworks （COFs） for electrocatalysis of oxygen electrodes [J]. Energy Storage Science and Technology, 2021, 10(6): 1891-1905.
[12]	Shishi ZHANG, Yanyang QIN, Yaqiong SU. Activity origin of single/double-atom catalyst for hydrogen evolution reaction [J]. Energy Storage Science and Technology, 2021, 10(6): 2008-2012.
[13]	Wenbing SONG, Yuanwei LU, Xiaotong CHEN, Cong HE, Zhansheng FAN, Yuting WU. The preparation and thermophysical properties of chloride/ceramic-shaped stabilized composite phase-change materials [J]. Energy Storage Science and Technology, 2021, 10(5): 1720-1728.
[14]	Zhong XU, Jing HOU, Jun LI, Enhui WU, Ping HUANG, Yalan TANG. Properties of different particle-sized activated carbon/myristic acid composite phase change material [J]. Energy Storage Science and Technology, 2021, 10(1): 177-189.
[15]	Chenlu YU, Xiaohua TIAN, han ZHENG, Zhejuan ZHANG, Zhuo SUN, Xianqing PIAO. Research progress in high stability of silicon/hard carbon anodes for LIBs [J]. Energy Storage Science and Technology, 2021, 10(1): 128-136.