Advances in the studies of the supported ruthenium catalysts for CO2 methanation

doi:10.1016/S1872-2067(24)60090-2

Chinese Journal of Catalysis ›› 2024, Vol. 63: 1-15.DOI: 10.1016/S1872-2067(24)60090-2

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Advances in the studies of the supported ruthenium catalysts for CO₂ methanation

Chenyang Shen^a^,^b, Menghui Liu^a, Song He^c, Haibo Zhao^c^,^*(), Chang-jun Liu^a^,^*()

^aCollaborative Innovation Center of Chemical Science & Engineering, School of Chemical Engineering and Technology, Tianjin University, Tianjin, 300072, China
^bKey Laboratory of Mesoscopic Chemistry, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing 210023, Jiangsu, China
^cState Key Laboratory of Coal Combustion, School of Energy and Power Engineering, Huazhong University of Science and Technology, Wuhan, 430074, Hubei, China

Received:2024-05-06 Accepted:2024-06-22 Online:2024-08-18 Published:2024-08-19
Contact: *E-mail: cjL@tju.edu.cn (C.-J. Liu), hzhao@mail.hust.edu.cn (H. Zhao).
About author:Haibo Zhao is a professor in the School of Energy and Power Engineering at Huazhong University of Science and Technology. Prof. Haibo Zhao is also a Fellow of the Combustion Institute. His research interests include the low-carbon combustion and high-value utilization of fossil fuels, as well as the flame synthesis of functional nanoparticles. He has been supported by the National Science Fund for Distinguished Young Scholars of China, Alexander von Humboldt Foundation, etc. His research work won the Distinguished Paper Award in the 38th International Symposium on Combustion, and the Best Paper Award in the 3rd International Conference on Chemical Looping, etc. He served as an editorial board member or associate editor of Energy & Fuels, Engineering, and Energy Environmental Focus.
Chang-jun Liu is a professor in the School of Chemical Engineering and Technology at Tianjin University, a Chang Jiang Distinguished Professor and Fellow of the Royal Society of Chemistry. His research interests include CO₂ utilization, natural gas conversion, plasma nanoscience, and 3D printing. He has been in the list of highly cited Chinese authors (Chemical Engineering) by Elsevier since 2014. He served as the 2010 Program Chair of Fuel Chemistry Division of American Chemical Society and Chair of the 10th International Conference on CO₂ Utilization. He is in the editorial board of Applied Catalysis B and Chinese Journal of Catalysis. He is in the advisory board of Journal of Energy Chemistry, Greenhouse Gases: Science & Technology, Journal of CO₂ Utilization.
Supported by:
National Key Research and Development Program of China(2022YFA1504801);National Natural Science Foundation of China(22138009);Fundamental Research Funds for the Central Universities of China

Abstract

Abstract:

CO₂ methanation has a potential in the large-scale utilization of carbon dioxide. It has also been considered to be useful for the renewable energy storage. The commercial pipeline for natural gas transportation can be directly applied for the methane product of CO₂ methanation. The supported ruthenium (Ru) catalyst has been confirmed to be active and stable for CO₂ methanation with its high ability in the dissociation of hydrogen and the strong binding of carbon monoxide. CO₂ methanation over the supported Ru catalyst is structure sensitive. The size of the Ru catalyst and the support have significant effects on the activity and the mechanism. A significant challenge remained is the structural controllable preparation of the supported Ru catalyst toward a sufficiently high low-temperature activity. In this review, the recent progresses in the investigations of the supported Ru catalysts for CO₂ methanation are summarized. The challenges and the future developments are also discussed.

Key words: Ruthenium, Carbon dioxide, Methanation, Hydrogenation, Catalyst and metal-support interaction

Chenyang Shen, Menghui Liu, Song He, Haibo Zhao, Chang-jun Liu. Advances in the studies of the supported ruthenium catalysts for CO₂ methanation[J]. Chinese Journal of Catalysis, 2024, 63: 1-15.

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Figures/Tables 10

Fig. 1. The modified reaction network for CO2 hydrogenation.

Fig. 2. Thermodynamic analyses of CO2 methanation. (a) equilibrium CO2 conversion, CH4 and CO selectivity at 1 bar and 1/4 of CO2/H2; (b) the effect of the pressure on equilibrium CO2 conversion; (c) the effect of the pressure on CH4 selectivity; (d) the effect of CO2/H2 ratio on equilibrium CO2 conversion; (e) the effect of CO2/H2 ratio on CH4 selectivity. All thermodynamic analyses were conducted using the HSC Chemistry 9 software.

Fig. 3. (a-d) HAADF-STEM images and elemental mappings of Ru(SA)/CeO2 and Ru(NC)/CeO2. (e,f) HAADF-STEM and HR-TEM images of Ru(NP)/CeO2. Reprinted with permission from Ref. [54]. Copyright 2018, American Chemical Society. (g) Apparent activation energy as a function of ruthenium particle size for Ru/γ-Al2O3 catalysts. Reprinted with permission from Ref. [56]. Copyright 2019, Elsevier. (h) Configurations of CO2* and CO related species of Ru1/CeO2 and Ru4/CeO2 model catalysts. Reprinted with permission from Ref. [55]. Copyright 2021, American Chemical Society.

Intermediate	Ru₁/Ru(0001)	Ru₂/Ru(0001)	Ru₃/Ru(0001)	Ru₄/Ru(0001)
CO₂*	-0.45	-1.02	-1.26	-0.97
CO*	-1.67	-2.07	-2.03	-1.95
O*	-5.51	-6.36	-6.39	-6.03
H*	-2.62	-2.87	-2.87	-2.79
CH₄*	-0.31	-0.23	-0.14	-0.10
CH₃OH*	-0.96	-0.82	-0.79	-0.54
H₂O*	-0.87	-0.73	-0.59	-0.81
CO₂* configuration
CO* + O* configuration

Fig. 4. Overview of the size effect of the supported ruthenium catalysts.

Fig. 5. Schematic illustration of the generation process for oxygen vacancy, Ce3+, and surface hydroxyl in Ru/CeO2 catalyst in the reduction process. Reprinted with permission from Ref. [59]. Copyright 2016, American Chemical Society.

Fig. 6. (a) Overview of the promoted formate pathway via hydroxyl groups. (b) Comparison on the formation of HCOO* species with and without surface OH* on Ru/CeO2. Reprinted with permission from Ref. [77]. Copyright 2021, American Chemical Society. (c) Schematic representation of the generation of hydroxyl groups and carbonate species in CO2 activation during the methanation process. Reprinted with permission from Ref. [79]. Copyright 2016, American Chemical Society.

Fig. 7. CO2 conversion and selectivity of the supported Ru catalysts for CO2 hydrogenation. (a) Ru/a-TiO2; (b) a-TiO2; (c) Ru/CeO2; (d) Ru/SiO2; (e) Ru/r-TiO2, (f) Ru/MoO3. Reaction conditions: 1.0 MPa, CO2/H2/Ar = 24/73/3, 3000 mL gcat-1 h-1. Reprinted with permission from Ref. [76]. Copyright 2024, American Chemical Society.

Table 2 Overview of Ru-based CO2 methanation catalysts reported in literature.

Catalyst	H₂/CO₂ (v/v%)	T (°C)	CO₂ conversion (%)	CH₄ selectivity (%)	TOF (h^-1)	Ref.
Ru/TiO₂	4/1	150	0	0	0	[96]
Ru/TiO₂	4/1	200	15	68	290	[96]
Ru/TiO₂	4/1	250	40	78	770	[96]
Ru/TiO₂	4/1	300	70	85	1350	[96]
RuO₂/TiO₂	4/1	200	0	0	0	[96]
RuO₂/TiO₂	4/1	250	25	75	450	[96]
RuO₂/TiO₂	4/1	300	50	85	900	[96]
Ru/TiO₂	4/1	200	37	>99	216	[98]
Ru/γ-Al₂O₃	4/1	280	<1	>99	4720	[97]
Ru/Ce_0.9Cr_0.1O₂	4/1	225	5	>99	223.9	[77]
Ru/Ce_0.9Cr_0.1O₂	4/1	250	70	>99	540	[77]
Ru/TiO₂	3/1	200	1	>99	15	[88]
Ru/TiO₂	3/1	250	3	>99	45	[88]
Ru/TiO₂	3/1	300	8-21	>99	119-298	[88]
Ru/MnO_x	4/1	300	25	90	180	[95]
Ru/Al₂O₃	4/1	300	32	94	1296	[95]
Ru/CeO₂	4/1	300	83	99	540	[95]
Ru/ZnO	4/1	300	1	6	14.4	[95]
Ru/CeO₂	4/1	450	55	99	-	[61]
Ru/CeO₂	4/1	150	<10	99	2.2 ± 0.1	[60]
Ru/CeO₂	4/1	200	35	>99	-	[59]
Ru/CeO₂	4/1	250	92.7	>99	-	[59]
Ru/CeO₂	4/1	300	93	-	-	[59]
Ru/α-Al₂O₃	4/1	200	0	-	-	[59]
Ru/α-Al₂O₃	4/1	250	5	>99	2.5 ± 0.2	[59]
Ru/α-Al₂O₃	4/1	300	55	-	-	[59]
Ru/TiO₂	80.9/15.5	350	60	>99	83	[89]
0Al-Ru/SiC	4/1	300	19.1	-	756	[33]
10Al-Ru/SiC	4/1	300	17.8	-	1188	[33]
30Al-Ru/SiC	4/1	300	17	-	1368	[33]
70Al-Ru/SiC	4/1	300	16	-	1584	[33]
Ru@MIL-101	4/1	200	19	-	358 ± 46	[94]
Ru@MIL-101@Silica nanofibrous veil + brushing treatment	4/1	200	3.2	-	404 ± 6	[94]
	4/1	225	16	-	2064 ± 29	[94]
	4/1	250	26	-	3257 ± 19	[94]
	4/1	300	40	-	5134 ± 59	[94]

Fig. 8. Overview of the SMSI effect between ruthenium and various metal oxides.

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Advances in the studies of the supported ruthenium catalysts for CO₂ methanation

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