光辅助直接甲醇燃料电池阳极催化剂的研究进展

doi:10.16085/j.issn.1000-6613.2023-2067

化工进展 ›› 2024, Vol. 43 ›› Issue (5): 2611-2628.DOI: 10.16085/j.issn.1000-6613.2023-2067

• 催化与材料技术 • 上一篇

光辅助直接甲醇燃料电池阳极催化剂的研究进展

方峣¹^,²^,³(), 刘雷², 高志华¹^,²^,³, 黄伟¹^,²^,³, 左志军¹^,²^,³()

^1.太原理工大学省部共建煤基能源清洁高效利用国家重点实验室，山西太原 030024
^2.太原理工大学化学工程与技术学院，山西太原 030024
^3.太原理工大学煤科学与技术教育部重点实验室，山西太原 030024

收稿日期:2023-11-28 修回日期:2024-03-11 出版日期:2024-05-15 发布日期:2024-06-15
通讯作者: 左志军
作者简介:方峣（1995—），男，博士研究生，研究方向为锂硫电池和燃料电池的理论研究。E-mail：932866749@qq.com。
基金资助:
国家自然科学基金(22078214);山西省科技创新人才团队专项资金(202204051001009);中央引导地方科技发展资金(YDZJSX2022A013)

Advances in anode catalysts for photo-assisted direct methanol fuel cells

FANG Yao¹^,²^,³(), LIU Lei², GAO Zhihua¹^,²^,³, HUANG Wei¹^,²^,³, ZUO Zhijun¹^,²^,³()

^1.State Key Laboratory of Clean and Efficient Coal Utilization, Taiyuan University of Technology, Taiyuan 030024, Shanxi, China
^2.College of Chemical Engineering and Technology, Taiyuan University of Technology, Taiyuan 030024, Shanxi, China
^3.Key Laboratory of Coal Science and Technology of Ministry of Education, Taiyuan University of Technology, Taiyuan 030024, Shanxi, China

Received:2023-11-28 Revised:2024-03-11 Online:2024-05-15 Published:2024-06-15
Contact: ZUO Zhijun

摘要/Abstract

摘要：

直接甲醇燃料电池（DMFCs）因其能够在较低工作温度下提供清洁、可持续能源方面的潜力而备受关注，但阳极缓慢的甲醇氧化反应（MOR）限制了其商业化应用。光辅助直接甲醇燃料电池（PMFCs）能利用光电耦合机制加速MOR过程，实现甲醇的化学能高效转化为电能，为开发高效、可持续的能源转换系统带来了巨大希望。本文首先简要回顾了PMFCs的背景、意义和在能源研究中的价值。从PMFCs的基本结构组成和酸碱介质下甲醇光电催化氧化的基本路径出发，总结了PMFCs阳极光电催化剂的研究进展。重点针对不同类型的PMFCs阳极光电催化剂，讨论光辅助下的MOR增强机制，如催化剂的尺寸效应、晶面效应、吸光性能、导电性以及表面等离激元共振（SPR）效应等方面的影响。PMFCs未来需要重点关注的研究方向是深入理解PMFCs的光电耦合机制和PMFCs阳极催化剂的构效关系，以及解决实际二电极系统下PMFCs光阳极的设计问题。

关键词: 光辅助直接甲醇燃料电池, 甲醇氧化, 光化学, 电化学, 催化剂

Abstract:

Direct methanol fuel cells (DMFCs) have gained attention because of their potential to provide clean, sustainable energy at lower temperatures. However, the slow methanol oxidation reaction (MOR) at anode has limited their commercial use. In contrast, photo-assisted direct methanol fuel cells (PMFCs) can accelerate the MOR process by a photoelectric coupling mechanism, which efficiently converts methanol’s chemical energy into electricity, and thus show great promise for developing efficient and sustainable energy conversion systems. This paper begins with a brief review of the background, significance, and value of PMFCs in energy research. It then summarizes the research progress of anode photocatalysts for PMFCs, starting from the basic structure and pathway of methanol photo electrocatalytic oxidation under an acid-base medium. According to different types of anodic photocatalysts for PMFCs, we discuss the mechanisms that may intensify the photo-assisted MOR, such as the catalyst size effect, crystal surface effect, light absorption property, electrical conductivity, and surface plasmon resonance (SPR). The future research direction for PMFCs should focus on understanding the mechanism of photoelectric coupling and the constitutive relationship of anodic catalysts in-depth. Additionally, it is crucial to address the design problems of the PMFCs photo-anode under the actual two-electrode system.

Key words: photo-assisted direct methanol fuel cells, methanol oxidation, photochemistry, electrochemistry, catalyst

中图分类号:

TM911.4

方峣, 刘雷, 高志华, 黄伟, 左志军. 光辅助直接甲醇燃料电池阳极催化剂的研究进展[J]. 化工进展, 2024, 43(5): 2611-2628.

FANG Yao, LIU Lei, GAO Zhihua, HUANG Wei, ZUO Zhijun. Advances in anode catalysts for photo-assisted direct methanol fuel cells[J]. Chemical Industry and Engineering Progress, 2024, 43(5): 2611-2628.

图/表 15

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催化剂	甲醇起始氧化电位	电流强度（暗态）	电流强度（光照）	增强因子	参考文献
Pt-TiO₂	—	—	—	1.48	[11]
Pt₃-CD₂/TiO₂	0.35V vs. Ag/AgCl	2.02mA/cm²	2.5mA/cm²	1.24	[12]
PtRu-TiO₂	0.38V vs. RHE	18.1mA	21.4mA	1.18	[13]
Pt(Cu)-TiO₂	-0.15V vs. SCE	—	—	1.66	[14]
G-TNRs	-0.4V vs. SCE	0.2μA/cm²	4.9μA/cm²	24.5	[15]
Pt-TNRs	-0.6V vs. Hg/HgO	1.86mA/mg_Pt	5.32mA/mg_Pt	2.86	[16]
Pt-TNTs	—	—	—	2.6	[17]
PtNi-TNTs	—	24.3mA/cm²	37.5mA/cm²	1.54	[18]
PtNi/C-TNTs	0.6V vs. Ag/AgCl	108mA/cm²	123mA/cm²	1.13	[19]
Pt-TNTs	0.4V vs. Ag/AgCl	357.4mA/mg_Pt	525mA/mg_Pt	1.47	[20]
Pt-TNTs/RGO	—	1.36mA/cm²	4.4mA/cm²	3.24	[21]
Pt-TiO₂/GNs	—	820mA/mg_Pt	1354mA/mg_Pt	1.65	[22]
Pt-RGO/TiO₂	—	363.9mA/mg_Pt	507.4mA/mg_Pt	1.39	[23]
Pt-TiO₂/G-PV	—	1214mA/mg_Pt	3293mA/mg_Pt	2.71	[24]
Pt-GNs/TiO₂	-0.373V vs. Hg/HgO	3368mA/mg_Pt	4715mA/mg_Pt	1.4	[25]
TiO₂-MWCNT	—	0.51mA/cm²	4.5mA/cm²	8.8	[26]
Pt-TiO₂@C	0.18V vs. RHE	1.15mA/cm²	2.86mA/cm²	2.5	[27]
Pt-TiO₂/SiO₂	-0.6V vs. SCE	0.3mA/cm²	0.95mA/cm²	3.17	[28]
Pt-MXene-TiO₂	0.33V vs. SCE	703.31mA/mg_Pt	2750.4mA/mg_Pt	3.9	[29]

催化剂	甲醇起始氧化电位	电流强度（暗态）	电流强度（光照）	增强因子	参考文献
Pt-TiO₂	—	—	—	1.48	[11]
Pt₃-CD₂/TiO₂	0.35V vs. Ag/AgCl	2.02mA/cm²	2.5mA/cm²	1.24	[12]
PtRu-TiO₂	0.38V vs. RHE	18.1mA	21.4mA	1.18	[13]
Pt(Cu)-TiO₂	-0.15V vs. SCE	—	—	1.66	[14]
G-TNRs	-0.4V vs. SCE	0.2μA/cm²	4.9μA/cm²	24.5	[15]
Pt-TNRs	-0.6V vs. Hg/HgO	1.86mA/mg_Pt	5.32mA/mg_Pt	2.86	[16]
Pt-TNTs	—	—	—	2.6	[17]
PtNi-TNTs	—	24.3mA/cm²	37.5mA/cm²	1.54	[18]
PtNi/C-TNTs	0.6V vs. Ag/AgCl	108mA/cm²	123mA/cm²	1.13	[19]
Pt-TNTs	0.4V vs. Ag/AgCl	357.4mA/mg_Pt	525mA/mg_Pt	1.47	[20]
Pt-TNTs/RGO	—	1.36mA/cm²	4.4mA/cm²	3.24	[21]
Pt-TiO₂/GNs	—	820mA/mg_Pt	1354mA/mg_Pt	1.65	[22]
Pt-RGO/TiO₂	—	363.9mA/mg_Pt	507.4mA/mg_Pt	1.39	[23]
Pt-TiO₂/G-PV	—	1214mA/mg_Pt	3293mA/mg_Pt	2.71	[24]
Pt-GNs/TiO₂	-0.373V vs. Hg/HgO	3368mA/mg_Pt	4715mA/mg_Pt	1.4	[25]
TiO₂-MWCNT	—	0.51mA/cm²	4.5mA/cm²	8.8	[26]
Pt-TiO₂@C	0.18V vs. RHE	1.15mA/cm²	2.86mA/cm²	2.5	[27]
Pt-TiO₂/SiO₂	-0.6V vs. SCE	0.3mA/cm²	0.95mA/cm²	3.17	[28]
Pt-MXene-TiO₂	0.33V vs. SCE	703.31mA/mg_Pt	2750.4mA/mg_Pt	3.9	[29]

催化剂	甲醇起始氧化电位	电流强度（暗态）	电流强度（光照）	增强因子	参考文献
Pt-ZnO@CC	—	2.58mA/cm²	3.86mA/cm²	1.5	[44]
Pt-ZnO/KB	—	432mA/mg_Pt	964mA/mg_Pt	2.23	[45]
Pt-ZnO	-0.796V vs. SCE	427.5mA/mg_Pt	547.96mA/mg_Pt	1.28	[46]
Pt(Pd)/ZnO/GNs	Pt 0.38V vs. Ag/AgCl	957.3mA/mg_Pt	1935.5mA/mg_Pt	2.02	[47]
	Pd -0.63V vs. Ag/AgCl	513.2mA/mg_Pt	818.3mA/mg_Pt	1.59

催化剂	甲醇起始氧化电位	电流强度（暗态）	电流强度（光照）	增强因子	参考文献
Pt-ZnO@CC	—	2.58mA/cm²	3.86mA/cm²	1.5	[44]
Pt-ZnO/KB	—	432mA/mg_Pt	964mA/mg_Pt	2.23	[45]
Pt-ZnO	-0.796V vs. SCE	427.5mA/mg_Pt	547.96mA/mg_Pt	1.28	[46]
Pt(Pd)/ZnO/GNs	Pt 0.38V vs. Ag/AgCl	957.3mA/mg_Pt	1935.5mA/mg_Pt	2.02	[47]
	Pd -0.63V vs. Ag/AgCl	513.2mA/mg_Pt	818.3mA/mg_Pt	1.59

催化剂	甲醇起始氧化电位	电流强度（暗态）	电流强度（光照）	增强因子	参考文献
Pt-WO₃/Gr	0.4V vs. SCE	—	—	1.2	[48]
Pt-2D Fe₂O₃	—	167.8mA/mg_Pt	太阳光 389.1mA/mg_Pt	2.32	[49]
			可见光 218.7mA/mg_Pt	1.30
Pt-Cu₂O/GNs	0.48V vs. Ag/AgCl	1321.9mA/mg_Pt	1800.6mA/mg_Pt	1.36	[50]
Pd-Cu₂O/GNs	-0.50V vs. Ag/AgCl	718mA/mg_Pt	899.5mA/mg_Pt	1.25
Pt/SnO₂/GNs	—	670.3mA/mg_Pt	1103mA/mg_Pt	1.64	[51]
PtPd/SnO₂/GNs	0.174V vs. Ag/AgCl	7718mA/mg_Pt	10029mA/mg_Pt	1.3	[52]
Pt-Bi₂WO₆/RGO	—	936mA/mg_Pt	1800mA/mg_Pt	1.92	[53]
CQDs-Pt@Bi₂WO₆/FTO	—	0.73mA/cm²	0.89mA/cm²	1.21	[54]
Pt-BiOBr (001)	—	251.1mA/mg_Pt	太阳光 1321.1mA/mg_Pt	5.2	[55]
			可见光 594.3mA/mg_Pt	2.4
Pt-g-C₃N₄	酸性：—	157.7mA/mg_Pt	520.4mA/mg_Pt	3.3	[56]
	碱性：-0.5V vs. SCE	49.89mA/mg_Pt	91.3mA/mg_Pt	1.83
Pt/N-g-C₃N₄/KB	—	1700mA/mg_Pt	2800mA/mg_Pt	1.63	[57]
Pt-Fe₂P	-0.6V vs. SCE	521.1mA/mg_Pt	2430mA/mg_Pt	4.7	[58]
Pt-CdS QDs	—	1.33mA/cm²	4.08mA/cm²	3.1	[59]

光辅助直接甲醇燃料电池阳极催化剂的研究进展

Advances in anode catalysts for photo-assisted direct methanol fuel cells

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催化剂	光源	电流强度（暗态）	电流强度（光照）	增强因子	参考文献
p-n异质结
Ni(OH)₂/TiO₂NTs	500W Xe lamp	23.8mA/cm²	28.3mA/cm²	1.2	[66]
Pt-CuI/TiO₂	500W Xe lamp	936mA/mg	3772mA/mg	4.0	[67]
Ⅱ型异质结
Pt-WO₃-TiO₂	8W UV light（λ=265nm）	0.35mA/cm²	2.2mA/cm²	6.3	[68]
Ni-TiO₂/PHI	365nm LED	—	11.0mA/cm²	—	[69]
Pt-CdS/MoS₂	150W Xe lamp（λ>400nm）	1.13mA/cm²	4.56mA/cm²	4.0	[70]
Pt/g-C₃N₄/CdS	150W Xe lamp（λ>420nm）	16.9mA/mg	127.7mA/mg	7.4	[71]
Pt-Bi₂WO₆/MoS₂	300W Xe lamp	1829mA/mg	2743mA/mg	1.5	[72]
Pt-Bi₂WO₆/Cu₂S	500W Xe lamp（λ>420nm）	1854.5mA/mg	5538mA/mg	3.0	[73]
Pt-BiOI/MoS₂	150W Xe lamp（λ>420nm）	222.3mA/mg	1007.2mA/mg	4.5	[74]
Pt-BiVO₄/Bi₂O₃	50W Xe lamp（λ>320nm）	281.4mA/mg	506.6mA/mg	1.8	[75]
CoS _x /NiS _x	50W Xe lamp	28.5A/g	30.4A/g	1.065	[76]
Z型异质结
Si NWs@ZnO	500W Xe lamp	67.0μA/cm²	100.5μA/cm²	1.5	[77]

催化剂	光源	电流强度（暗态）	电流强度（光照）	增强因子	参考文献
Au-CA	模拟太阳光100mW/cm²	115.86μA/μg	248.9μA/μg	2.2	[84]
Au NSs	300W Xe lamp	0.71mA/mg	1.65mA/mg	2.3	[85]
Au NMs		2.50mA/mg	7.98mA/mg	3.2
Au NRs		4.08mA/mg	12.50mA/mg	3.1
NPG	300W Xe lamp	—	531μA/cm²	＞2	[86]
Pt-Au NDs	300W Xe lamp（>420nm）	0.79mA/cm²	2.61mA/cm²	3.3	[87]
AgPt-tipped Au NSs	300W Xe lamp（>420nm）	2.74A/mg	4.0A/mg	1.5	[88]
PtNiCu alloy	300W Xe lamp（>420nm）	—	3.3A/mg_Pt	—	[89]
Pt-Ag/GNs	15W UV lamp	838.3mA/mg	1842.4mA/mg	2.2	[90]
Au-6T/SG/Cu	565nm LED	169.4μA/μg	288μA/μg	1.7	[91]
PtIn/3D-GNs	300W Xe lamp	612.3mA/mg	1570.7mA/mg	2.6	[92]
Au-DNFs/TiN	模拟太阳光150W（>400nm）	476.51μA/cm²	565.84μA/cm²	1.2	[93]
Au-DNFs/Si		423.48μA/cm²	514.93μA/cm²	1.2
Ag/TiO₂	模拟太阳光100mW/cm²	—	1mA/cm²	—	[94]
Pd/TiO₂	模拟太阳光100mW/cm²	可见光0.132mA/cm²	可见光0.353mA/cm²	2.7	[95]
		紫外光0.132mA/cm²	紫外光0.562mA/cm²	4.3
Au/TNT	Xe lamp 165mW/cm²	53.27mA/mg	189.51mA/mg	3.6	[96]
Pt/Ag_0.333V₂O₅-NR	Xe lamp	5.32mA/cm²	10.73mA/cm²	2.0	[97]

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