碳基催化剂催化有机液体氢载体脱氢研究进展

doi:10.1016/j.actphy.2024.100044

Abstract

Abstract:

Hydrogen energy is a widely available, flexible and efficient secondary energy source, and it is also an important energy medium. The development of low-cost, high-density hydrogen storage technology is a significant issue for the industrial application of hydrogen energy. Liquid organic hydrogen storage has attracted extensive attention due to advantages such as high mass hydrogen storage density, safe storage and transportation, as well as ease of long-distance transportation. However, compared with the relatively mature hydrogenation process, the dehydrogenation of liquid organic hydrogen carriers (LOHCs) still suffers from high reaction temperature and low efficiency. The key to solving these problems is the development of efficient dehydrogenation catalysts. In recent years, carbon-based catalysts have shown excellent reaction performance in the dehydrogenation of LOHCs due to their advantages of high dispersion of active components, tunable composition structure and surface physicochemical properties, and outstanding electrical and thermal conductivity, etc. In this review, we initially analyze the thermodynamics and kinetics of dehydrogenation, as well as the physicochemical properties of LOHCs, including cyclohexane, methylcyclohexane, decalin, and perhydro-N-ethylcarbazole. The special features of carbon supports are then outlined in terms of the activated carbon, carbon nanotubes, carbon fibers, and reduced graphene oxide. In addition, the structural characteristics, catalytic performance, structure-property relationship, and dehydrogenation mechanism of carbon-supported metal catalysts are summarized and analyzed. Based on this, we point out the main challenges of liquid organic hydrogen storage. Furthermore, future opportunities in this field are envisioned, with an emphasis on the modification and structuration of carbon support, the study of catalytic mechanisms and chemical process intensification.

Key words: Liquid organic hydrogen carrier, Catalytic dehydrogenation, Carbon-based catalyst, Structural design, Structure-property relationship

Xuejie Wang, Guoqing Cui, Congkai Wang, Yang Yang, Guiyuan Jiang, Chunming Xu. Research Progress on Carbon-based Catalysts for Catalytic Dehydrogenation of Liquid Organic Hydrogen Carriers[J]. Acta Phys. -Chim. Sin. 2025, 41(5), 100044. doi: 10.1016/j.actphy.2024.100044

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LOHCs	Mass hydrogen storage density (wt.%)	Melting point (℃)	Boiling point (℃)	Enthalpy of reaction (kJ∙mol_H2⁻¹)	Ref.
Cyclohexane	7.2	7	81	68.6	[24]
Methylcyclohexane	6.2	−127	101	68.3	[24]
Decalin	7.3	−30	187	66.4	[24]
Perhydro-dibenzyl toluene	6.2	−58	371	65.0	[24]
Perhydro-carbazole	6.7	58	264	51.1	[24]
Perhydro-N-ethylcarbazole	5.8	−85	281	50.6	[35]

LOHCs	Catalyst	Temperature/℃	Conversion/%	Hydrogen release	Ref.
H12-NEC	Pt/C	180	90.5 ^a	5.69 ^b	[64]
H12-NEC	Pt/TiO₂	180	63.9 ^a	5.62 ^b	[64]
H12-NEC	Pt/Al₂O₃	180	50.6 ^a	5.69 ^b	[64]
H12-NEC	Pt/SiO₂	180	17.2 ^a	3.29 ^b	[64]
Decalin	Pt/AC	300	83	880 ^c	[66]
Decalin	Pt/Al₂O₃	300	42	460 ^c	[66]
Methylcyclohexane	Pt/AC	300	88	1274 ^d	[68]
Methylcyclohexane	Pt/PTC-S	300	84.3	991.5 ^d	[69]
Methylcyclohexane	Pt/GAC-S	300	63	741.1 ^d	[70]
Methylcyclohexane	Pt/NPC-550-CEH	300	18	1086 ^d	[74]
Methylcyclohexane	Pt/NPC-550-IEH	300	66	3620 ^d	[74]

LOHCs	Catalyst	Temperature/℃	Hydrogen evolution rate ^a	Conversion/%	Ref.
Decalin	Pt/CNT-N	185	–	1.52	[83]
Decalin	Pt/CNT	185	–	0.62	[83]
Decalin Decalin Decalin	Pt/CNTs Pt/CB Pt/CNFs	196.6 194.1 167.5	320.5 251.1 102.1	– – –	[89] [89] [89]

LOHCs	Catalyst	Temperature (℃)	Conversion (%)	Hydrogen release (wt.%)	Ref.
H12-NEC	Pd/rGO	180	100	5.74	[106]
H12-NEC	Pd/Al₂O₃	180	100	4.64	[106]
H12-NEC	Pd_1.2Cu/rGO	180	100	5.79	[107]
H12-NEC	Pd_1.2Cu_0.5/rGO	180	100	5.50	[107]
H12-NEC	Pd_1.2Cu₂/rGO	180	100	4.82	[107]
H12-NEC	Pd{100}	180	100	5.73	[108]
H12-NEC	Pd{110}	180	100	4.71	[108]
H12-NEC	Pd{111}	180	100	3.24	[108]

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Research Progress on Carbon-based Catalysts for Catalytic Dehydrogenation of Liquid Organic Hydrogen Carriers

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