Artificial Carbon Sequestration Technology—Research Progress on the Catalysts for Thermal Catalytic Reduction of CO2

doi:10.19894/j.issn.1000-0518.210451

Chinese Journal of Applied Chemistry ›› 2022, Vol. 39 ›› Issue (4): 599-615.DOI: 10.19894/j.issn.1000-0518.210451

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Artificial Carbon Sequestration Technology—Research Progress on the Catalysts for Thermal Catalytic Reduction of CO₂

Xue-Ting WU, Yang YU(), Shu-Yan SONG(), Hong-Jie ZHANG

State Key Laboratory of Rare Earth Resources Utilization，Changchun Institute of Applied Chemistry，Chinese Academy of Sciences，Changchun 130022，China

Received:2021-09-05 Accepted:2021-11-25 Published:2022-04-01 Online:2022-04-19
Contact: Yang YU,Shu-Yan SONG
About author:songsy@ciac.ac.cn
Supported by:
the National Natural Science Foundation of China(21771173);the National Key R&D Program(2016YFA0203200)

Abstract

Abstract:

Selective hydrogenation has very important applications in the chemical industry such as synthesis of functional materials and purification of chemical products. In recent years， in order to reduce the impact of the greenhouse effect， the selective hydrogenation of CO₂ into other valuable chemicals has become a research hotspot. Among them， the thermal catalysis is widely used， easy to obtain a variety of target products and high yield of products. At present， the heterogeneous thermal catalytic hydrogenation of CO₂ to produce methane， methanol， light olefins and other high-value fuels and chemicals has made some progresses， but their development is still challenging. The preparation of high-efficiency catalysts is one of the keys. For a long time， researchers have been committed to solving the problem of catalyst activity and selectivity， and modifying the catalysts by doping with additives and adding functional carriers. In response to these problems， this article briefly introduces the background of the catalytic hydrogenation of CO₂ and reviews the catalysts used in the heterogeneous thermal catalytic hydrogenation of CO₂ into methane， methanol and light olefin products in recent five years. It is expected to provide a reference for the development of new catalysts in the heterogeneous catalytic hydrogenation of CO₂.

Key words: Catalytic hydrogenation of carbon dioxide, Thermal catalysis, Methane, Methanol, Light olefins

CLC Number:

O614

Xue-Ting WU, Yang YU, Shu-Yan SONG, Hong-Jie ZHANG. Artificial Carbon Sequestration Technology—Research Progress on the Catalysts for Thermal Catalytic Reduction of CO₂[J]. Chinese Journal of Applied Chemistry, 2022, 39(4): 599-615.

Figures/Tables 15

References 102

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	催化剂 Catalyst	n（H₂）∶n（CO₂）	温度 Temperature/℃	压力 Pressure/MPa	GHSV/ （mL·g^-1·h^-1）	CO₂转化率 Conversion/%	选择性 Selectivity/%	文献 Ref.
甲烷 Methane	20%Ni?TiO₂	4∶1	350	--	48 000	52	98	［17］
	Ni?5Mg/SBA?15?AE	4∶1	350	--	30 000	73	98	［18］
	Ni/Pr?Ce	4∶1	350	--	25 000	54.5	100	［19］
	NiO/Zn_0.3Zr_0.7	4∶1	500	--	24 000	79	94	［54］
	8%Ni@NaX	4∶1	380	0.1	15 000	92.70	≈99.9	［55］
	Ru_SA/TiO₂^*	4∶1	340	0.1	16 500	15.6	97.3	［43］
	0.89%Ru_SA/CeO₂	4∶1	260	0.1	4 800	28	100	［43］
甲醇 Methanol	ZrO₂/Cu?0.1	3∶1	220	3	48 000	<5	70	［20］
	Cu₁La_0.2/SBA?15	3∶1	240	3	12 000	5.7	81.2	［21］
	Pd?CZ?0.01	3∶1	150	4.5	10 800	30	65	［22］
	10Cu/CeO₂	3∶1	190	3	3 000	1.8	84	［56］
	1Pd?10Cu/CeO₂	3∶1	270	3	3 000	17.8	23.7	［56］
	Pd@Zn	3∶1	250	2	18 000	5	70.5	［57］
	In₂O₃/ZrO₂	4∶1	300	5	16 000	5.2	99.8	［58］
轻烯烃 Light olefin	35Fe?7Zr?1Ce?K	3∶1	320	2	6 000	57.3	55.6	［59］
	Fe?Co/K?Al₂O₃ （Fe/K=2.5）	3∶1	320	2	9 000	41.4	45	［60］
	C?Fe?Zn/K	3∶1	320	2	3 000	54.8	57.4	［61］
	Na?Fe₃O₄/HZSM?5	3∶1	320	1.1	3 600	22	46.6	［24］
	Fe/C+K（0.75）	3∶1	350	3	24 000	38.5	38.8	［25］
	In?Zr/SAPO?34	3∶1	400	3	9 000	30	84	［46］
	ZnZrO/SAPO	3∶1	380	2	3 600	12.6	80	［62］
	ZnGa₂O₄/SAPO?34	3∶1	370	3	5 400	13	86	［63］
	ZnAl₂O₄/SAPO?34	3∶1	370	3	5 400	15	87	［64］

	催化剂 Catalyst	n（H₂）∶n（CO₂）	温度 Temperature/℃	压力 Pressure/MPa	GHSV/ （mL·g^-1·h^-1）	CO₂转化率 Conversion/%	选择性 Selectivity/%	文献 Ref.
甲烷 Methane	20%Ni?TiO₂	4∶1	350	--	48 000	52	98	［17］
	Ni?5Mg/SBA?15?AE	4∶1	350	--	30 000	73	98	［18］
	Ni/Pr?Ce	4∶1	350	--	25 000	54.5	100	［19］
	NiO/Zn_0.3Zr_0.7	4∶1	500	--	24 000	79	94	［54］
	8%Ni@NaX	4∶1	380	0.1	15 000	92.70	≈99.9	［55］
	Ru_SA/TiO₂^*	4∶1	340	0.1	16 500	15.6	97.3	［43］
	0.89%Ru_SA/CeO₂	4∶1	260	0.1	4 800	28	100	［43］
甲醇 Methanol	ZrO₂/Cu?0.1	3∶1	220	3	48 000	<5	70	［20］
	Cu₁La_0.2/SBA?15	3∶1	240	3	12 000	5.7	81.2	［21］
	Pd?CZ?0.01	3∶1	150	4.5	10 800	30	65	［22］
	10Cu/CeO₂	3∶1	190	3	3 000	1.8	84	［56］
	1Pd?10Cu/CeO₂	3∶1	270	3	3 000	17.8	23.7	［56］
	Pd@Zn	3∶1	250	2	18 000	5	70.5	［57］
	In₂O₃/ZrO₂	4∶1	300	5	16 000	5.2	99.8	［58］
轻烯烃 Light olefin	35Fe?7Zr?1Ce?K	3∶1	320	2	6 000	57.3	55.6	［59］
	Fe?Co/K?Al₂O₃ （Fe/K=2.5）	3∶1	320	2	9 000	41.4	45	［60］
	C?Fe?Zn/K	3∶1	320	2	3 000	54.8	57.4	［61］
	Na?Fe₃O₄/HZSM?5	3∶1	320	1.1	3 600	22	46.6	［24］
	Fe/C+K（0.75）	3∶1	350	3	24 000	38.5	38.8	［25］
	In?Zr/SAPO?34	3∶1	400	3	9 000	30	84	［46］
	ZnZrO/SAPO	3∶1	380	2	3 600	12.6	80	［62］
	ZnGa₂O₄/SAPO?34	3∶1	370	3	5 400	13	86	［63］
	ZnAl₂O₄/SAPO?34	3∶1	370	3	5 400	15	87	［64］

催化剂 Catalyst	CO₂转化率 CO₂ conversion/%	CH₄产率 CH₄ yield/%	CH₄选择性 CH₄ selectivity/%
Ni/Ce	39.4	39.4	100
Ni/Sm?Ce	44.9	44.9	100
Ni/Pr?Ce	54.5	54.5	100
Ni/Mg?Ce	43.2	43.2	100

催化剂 Catalyst	CO₂转化率 CO₂ conversion/%	CH₄产率 CH₄ yield/%	CH₄选择性 CH₄ selectivity/%
Ni/Ce	39.4	39.4	100
Ni/Sm?Ce	44.9	44.9	100
Ni/Pr?Ce	54.5	54.5	100
Ni/Mg?Ce	43.2	43.2	100

催化剂 Catalyst	CO₂转化率 CO₂ conversion/%	CO选择性/% CO selectivity/%	CH₄选择性 CH₄ selectivity/%
Ni_SA/CNT_ox-400	5.4	93.7	6.3
Ni_SA?Na/CNT_ox-400	8.1	95.5	4.5
Ru_SA/CNT_ox-400	8.4	56.0	44.0
Ru_SA?Na/CNT_ox-400	20.2	79.5	20.5
Ni_SA/TiO₂^*	11.8	99.6	0.4
Ni/TiO₂	2.8	99.3	0.7
Ru_SA/TiO₂^*	15.6	2.7	97.3
Ru/TiO₂^*	11.5	3.6	96.4

Artificial Carbon Sequestration Technology—Research Progress on the Catalysts for Thermal Catalytic Reduction of CO₂

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催化剂 Catalyst	CO₂转化率 CO₂ conversion/%	C₂－C₄烯烃产率 C₂－C₄ olefin/%	烯烃/烷烃摩尔比 n（olefin）∶n（paraffin）
Fe/K?Al₂O₃	34.0	45.5	6.7∶1
Fe?Cu/K?Al₂O₃	36.0	42.2	5.4∶1
Fe?Zn/K?Al₂O₃	34.2	42.6	5.6∶1
Fe?Co/K?Al₂O₃	40.0	46.1	5.9∶1
Fe?Mn/K?Al₂O₃	29.4	48.7	7.4∶1
Fe?V/K?Al₂O₃	30.6	44.9	6.4∶1

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