铁基催化剂在COx加氢制高附加值烃反应中的应用

doi:10.1016/S1872-2067(21)63802-0

摘要/Abstract

摘要：

化石燃料的广泛使用导致大气中CO₂的排放量急剧增加, 进而引起全球变暖和海洋酸化等一系列问题. CO加氢(费托合成)反应是利用非石油来源的原料生产液体燃料和化学品的一种重要途径. 同时, 利用可再生的H₂将CO₂转化为高附加值的产品有利于减少对化石燃料的依赖, 减轻由于大气中CO₂浓度过高带来的负面影响. 开发新型、高效、稳定的催化剂是费托合成和CO₂加氢制高附加值烃的关键因素之一. Fe基、Co基和Ru基催化剂是费托合成中常用的催化剂. 而在CO₂加氢反应中, Co基和Ru基催化剂上主要发生甲烷化反应, 几乎没有长链烃生成. Fe基催化剂在费托合成和CO₂加氢反应中均表现出优异的催化生成长链烃性能. 同时, Fe储量丰富和价格便宜的特点也促进Fe基催化剂在两个反应中的广泛应用.
一般认为, 在Fe基催化剂上CO₂通过逆水煤气变换反应生成CO, CO通过费托合成反应继续加氢生成烃类. 因此, CO₂加氢反应和费托合成反应有相似之处, 同时也有较大的区别. 本文从活性相、助剂和载体的角度综述了各组分在Fe基催化剂催化CO/CO₂加氢反应中的作用, 总结了其中的区别与联系. 催化剂在反应中会发生复杂的相变过程, 形成多种铁物种; 其中, 碳化铁(χ-Fe₅C₂, ε-Fe₂C, Fe₇C₃和θ-Fe₃C)在费托合成反应中是C‒C偶联的活性相, 但对于θ-Fe₃C现还存在一些争议. 在CO₂加氢反应中Fe₃O₄催化逆水煤气变换反应, 碳化铁催化CO加氢反应. 金属助剂对CO/CO₂加氢反应的促进作用较为相似, 在两个反应中碱金属的促进作用最为明显. 费托合成反应对载体有较强的适应性, 而CO₂加氢反应对载体敏感性较强, Al₂O₃, ZrO₂和碳材料载体效果较好.
本文还总结了近些年来基于对活性相、助剂和载体的深入理解设计制备的一些新型催化剂及其在费托合成和CO₂加氢反应中的应用, 包括具有新颖结构的催化剂、金属-有机骨架衍生催化剂以及与沸石分子筛结合的双功能催化剂. 最后, 还分析了目前Fe基催化剂在费托合成和CO₂加氢反应应用中所面临的问题和挑战, 并对未来的发展趋势进行了展望.

关键词: Fe基催化剂, 费托合成, CO₂加氢, 助剂, 载体, 活性相

Abstract:

The widespread utilization of fossil fuels has caused an associated increase in CO₂ emissions over the past few decades, which has resulted in global warming and ocean acidification. CO hydrogenation (Fischer-Tropsch synthesis, FTS) is considered a significant route for the production of liquid fuels and chemicals from nonpetroleum sources to meet worldwide demand. Conversion of CO₂ with renewable H₂ into valuable hydrocarbons is beneficial for reducing dependence on fossil fuels and mitigating the negative effects of high CO₂ concentrations in the atmosphere. Iron-based catalysts exhibit superior catalytic performance in both FTS and CO₂ hydrogenation to value-added hydrocarbons. The abundance and low cost of iron-based catalysts also promote their wide application in CO_x hydrogenation. This paper provides a comprehensive overview of the significant developments in the application of iron-based catalysts in these two fields. The active phases, promoter effect, and support of iron-based catalysts are discussed in the present paper. Based on understanding of these three essential aspects, we also cover recent advances in the design and preparation of novel iron-based catalysts for FTS and CO₂ hydrogenation. Current challenges and future catalytic applications are also outlined.

Key words: Iron-based catalyst, Fischer-Tropsch synthesis, CO₂ hydrogenation, Promoter, Support, Active phase

刘军辉, 宋亚坤, 郭旭明, 宋春山, 郭新闻. 铁基催化剂在CO_x加氢制高附加值烃反应中的应用[J]. 催化学报, 2022, 43(3): 731-754.

Junhui Liu, Yakun Song, Xuming Guo, Chunshan Song, Xinwen Guo. Recent advances in application of iron-based catalysts for CO_x hydrogenation to value-added hydrocarbons[J]. Chinese Journal of Catalysis, 2022, 43(3): 731-754.

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Catalyst	H₂/CO	T (°C)	P (MPa)	GHSV (mL h^-1 g^-1)	CO conv. (%)	CO₂ sel. (%)	Product distribution (%)				Ref.
Catalyst	H₂/CO	T (°C)	P (MPa)	GHSV (mL h^-1 g^-1)	CO conv. (%)	CO₂ sel. (%)	CH₄	C₂‒C₄⁼	C₂‒C₄⁰	C₅₊	Ref.
FeSi	2	260	1.5	2000	53.0	32.4	24.9	0.46^a	0.46^a	23.7	[122]
LiFeSi	2	260	1.5	2000	36.1	25.4	17.5	0.59^a	0.59^a	31.3	[122]
NaFeSi	2	260	1.5	2000	50.1	32.0	16.9	0.63^a	0.63^a	35.4	[122]
KFeSi	2	260	1.5	2000	69.2	43.3	14.0	0.63^a	0.63^a	46.1	[122]
RbFeSi	2	260	1.5	2000	79.0	43.7	15.9	0.61^a	0.61^a	45.3	[122]
CsFeSi	2	260	1.5	2000	73.3	46.3	15.1	0.64^a	0.64^a	45.4	[122]
Fe/rGO	1	340	2.0	42000	342^b	49.7	42.3	33.2	23.4	1.1	[125]
FeK2/rGO	1	340	2.0	60000	545^b	49.0	22.0	63.7	6.4	7.9	[125]
FeMg/rGO	1	340	2.0	24000	247^b	40.7	35.6	33.0	26.9	4.5	[125]
FeMgK2/rGO	1	340	2.0	132000	1338^b	40.8	20.3	65.0	6.2	8.5	[125]
6 wt% Mn/Fe₃O₄	2	320	1.0	5^c	41.5	37.8	9.7	60.1	6.5	23.7	[70]
FeZn	65:24	350	2.0	3000	95.09	15.79	25.60	53.32	7.72	13.36	[146]
KFe/KIT-6(B5)	2	350	2.0	4000	70.8	—	16.0	6.7	8.4	68.9	[191]
Fe/CNF	1	340	2.0	—	29.8^b	—	13	52	12	18	[192]
Fe/α-Al₂O₃	1	340	2.0	—	13.5^b	—	11	53	6	21	[192]
Fe_xN-in-450(CNT)	1	300	0.5	15000	960.6^b	38.0	27.7	35.2	13.5	22.5	[193]
Fe/NG_-16.4	1	340	0.5	600	21.1	35.1	21.4	49.6	5.4	19.8	[194]
Fe/α-Al₂O₃-H-8S	1	350	0.1	9000	0.9	43	29	68	2	~1	[195]

Catalyst	H₂/CO	T (°C)	P (MPa)	GHSV (mL h^-1 g^-1)	CO conv. (%)	CO₂ sel. (%)	Product distribution (%)				Ref.
Catalyst	H₂/CO	T (°C)	P (MPa)	GHSV (mL h^-1 g^-1)	CO conv. (%)	CO₂ sel. (%)	CH₄	C₂‒C₄⁼	C₂‒C₄⁰	C₅₊	Ref.
FeSi	2	260	1.5	2000	53.0	32.4	24.9	0.46^a	0.46^a	23.7	[122]
LiFeSi	2	260	1.5	2000	36.1	25.4	17.5	0.59^a	0.59^a	31.3	[122]
NaFeSi	2	260	1.5	2000	50.1	32.0	16.9	0.63^a	0.63^a	35.4	[122]
KFeSi	2	260	1.5	2000	69.2	43.3	14.0	0.63^a	0.63^a	46.1	[122]
RbFeSi	2	260	1.5	2000	79.0	43.7	15.9	0.61^a	0.61^a	45.3	[122]
CsFeSi	2	260	1.5	2000	73.3	46.3	15.1	0.64^a	0.64^a	45.4	[122]
Fe/rGO	1	340	2.0	42000	342^b	49.7	42.3	33.2	23.4	1.1	[125]
FeK2/rGO	1	340	2.0	60000	545^b	49.0	22.0	63.7	6.4	7.9	[125]
FeMg/rGO	1	340	2.0	24000	247^b	40.7	35.6	33.0	26.9	4.5	[125]
FeMgK2/rGO	1	340	2.0	132000	1338^b	40.8	20.3	65.0	6.2	8.5	[125]
6 wt% Mn/Fe₃O₄	2	320	1.0	5^c	41.5	37.8	9.7	60.1	6.5	23.7	[70]
FeZn	65:24	350	2.0	3000	95.09	15.79	25.60	53.32	7.72	13.36	[146]
KFe/KIT-6(B5)	2	350	2.0	4000	70.8	—	16.0	6.7	8.4	68.9	[191]
Fe/CNF	1	340	2.0	—	29.8^b	—	13	52	12	18	[192]
Fe/α-Al₂O₃	1	340	2.0	—	13.5^b	—	11	53	6	21	[192]
Fe_xN-in-450(CNT)	1	300	0.5	15000	960.6^b	38.0	27.7	35.2	13.5	22.5	[193]
Fe/NG_-16.4	1	340	0.5	600	21.1	35.1	21.4	49.6	5.4	19.8	[194]
Fe/α-Al₂O₃-H-8S	1	350	0.1	9000	0.9	43	29	68	2	~1	[195]

Catalyst	H₂/CO₂	T (°C)	P (MPa)	GHSV (mL h^-1 g^-1)	CO₂ conv. (%)	Product sel. (%)					O/P	Ref.
Catalyst	H₂/CO₂	T (°C)	P (MPa)	GHSV (mL h^-1 g^-1)	CO₂ conv. (%)	CO	CH₄	C₂‒C₄⁼	C₂‒C₄⁰	C₅₊	O/P	Ref.
Fe/ZrO₂	3	340	2.0	1200	32	25	52.5	0.1	21.8	0.7	—	[155]
FeNa/ZrO₂	3	340	2.0	1200	39	21	12.4	28.9	5.2	12.5	—	[155]
FeCs/ZrO₂	3	340	2.0	1200	39	16	17.4	28.8	6.4	14.3	—	[155]
FeK/ZrO₂	3	340	2.0	1200	42	15	11.9	29.0	6.1	19.0	—	[155]
FeK/SiO₂	3	340	2.0	1200	7.1	92	5.8	1.5	0.7	0.1	—	[155]
FeK/Al₂O₃	3	340	2.0	1200	33	17	12.9	27.4	4.6	31.2	—	[155]
FeK/TiO₂	3	340	2.0	1200	21	55	8.4	16.3	2.7	10.6	—	[155]
FeK/Meso-C	3	340	2.0	1200	33	31	18.6	17.4	15.1	7.0	—	[155]
FeK/CNT	3	340	2.0	1200	35	12	19.2	27.4	4.6	31.2	—	[155]
Fe₃O₄	3	320	3.0	2000	29.3	16.6	50.3	0.1	30.4	2.6	0.0	[71]
FeNa(1.18)	3	320	3.0	2000	40.5	13.5	13.7	40.3	6.5	26.0	6.2	[71]
1Na/Fe	3	320	3.0	2040	36.8	10.1	7.0	23.4	2.1	56.9	11.0	[170]
5Mn-Na/Fe	3	320	3.0	2040	38.6	11.7	11.8	30.2	4.0	42.1	7.5	[170]
CuFeO₂-24	3	300	1.0	1800	16.7	31.4	1.6	22.4	22.4	44.5	7.7	[181]
ZnFe₂O₄	3	340	1.0	1800	34.0	11.7	8.6	28.1	28.1	51.6	11.3	[183]
Fe-Cu-K-La	3	300	1.1	3600	23.2	33	13	25	25	29	0.52	[179]
Fe-Co-K(0.1)/P25	3	300	1.1	3600	23.9	31	23	11	11	35	0.20	[180]
Fe-Cu-K(0.1)/P25	3	300	1.1	3600	19.9	49	12	8	8	31	0.38	[180]

Catalyst	H₂/CO₂	T (°C)	P (MPa)	GHSV (mL h^-1 g^-1)	CO₂ conv. (%)	Product sel. (%)					O/P	Ref.
Catalyst	H₂/CO₂	T (°C)	P (MPa)	GHSV (mL h^-1 g^-1)	CO₂ conv. (%)	CO	CH₄	C₂‒C₄⁼	C₂‒C₄⁰	C₅₊	O/P	Ref.
Fe/ZrO₂	3	340	2.0	1200	32	25	52.5	0.1	21.8	0.7	—	[155]
FeNa/ZrO₂	3	340	2.0	1200	39	21	12.4	28.9	5.2	12.5	—	[155]
FeCs/ZrO₂	3	340	2.0	1200	39	16	17.4	28.8	6.4	14.3	—	[155]
FeK/ZrO₂	3	340	2.0	1200	42	15	11.9	29.0	6.1	19.0	—	[155]
FeK/SiO₂	3	340	2.0	1200	7.1	92	5.8	1.5	0.7	0.1	—	[155]
FeK/Al₂O₃	3	340	2.0	1200	33	17	12.9	27.4	4.6	31.2	—	[155]
FeK/TiO₂	3	340	2.0	1200	21	55	8.4	16.3	2.7	10.6	—	[155]
FeK/Meso-C	3	340	2.0	1200	33	31	18.6	17.4	15.1	7.0	—	[155]
FeK/CNT	3	340	2.0	1200	35	12	19.2	27.4	4.6	31.2	—	[155]
Fe₃O₄	3	320	3.0	2000	29.3	16.6	50.3	0.1	30.4	2.6	0.0	[71]
FeNa(1.18)	3	320	3.0	2000	40.5	13.5	13.7	40.3	6.5	26.0	6.2	[71]
1Na/Fe	3	320	3.0	2040	36.8	10.1	7.0	23.4	2.1	56.9	11.0	[170]
5Mn-Na/Fe	3	320	3.0	2040	38.6	11.7	11.8	30.2	4.0	42.1	7.5	[170]
CuFeO₂-24	3	300	1.0	1800	16.7	31.4	1.6	22.4	22.4	44.5	7.7	[181]
ZnFe₂O₄	3	340	1.0	1800	34.0	11.7	8.6	28.1	28.1	51.6	11.3	[183]
Fe-Cu-K-La	3	300	1.1	3600	23.2	33	13	25	25	29	0.52	[179]
Fe-Co-K(0.1)/P25	3	300	1.1	3600	23.9	31	23	11	11	35	0.20	[180]
Fe-Cu-K(0.1)/P25	3	300	1.1	3600	19.9	49	12	8	8	31	0.38	[180]

Catalyst	H₂/CO	T (°C)	P (MPa)	GHSV (mL h^-1 g^-1)	CO conv. (%)	CO₂ sel. (%)	Product distribution (%)					Ref.
Catalyst	H₂/CO	T (°C)	P (MPa)	GHSV (mL h^-1 g^-1)	CO conv. (%)	CO₂ sel. (%)	CH₄		C₂‒C₄⁼	C₂‒C₄⁰	C₅₊
FeZr(0.3)	2	300	2.0	8000	82.1	41.2	4.6		5.3	4.5	85.6	[268]
Fe/PANI	1	350	2.0	9000	79	44	24		47	14	15	[269]
IO-CAT	1	275	1.5	2800^a	75.4	42.6	9.05		20.0	20.0	71	[271]
Fe@C-400	1	340	2.0	30000	74	47	28.3		30.2^b	26.4^b	—	[273]
Fe@C-500	1	340	2.0	30000	76	46	27.8		25.9^b	27.8^b	—	[273]
Fe@C-600	1	340	2.0	30000	74	46	25.9		24.1^b	31.5^b	—	[273]
Fe@C-900	1	340	2.0	30000	53	45	23.6		30.9^b	23.6^b	—	[273]
38Fe@C	1	340	1.5	3300^c	70	43	—		24.6	22.8	—	[274]
33Fe@C/Al	1	340	1.5	3300^c	68	43	—		28.1	22.8	—	[274]
Fe-MIL-88B-NH₂/C^d	1	300	2.0	36000	81.8	42.9	15.1		21.4	12.8	50.7	[275]
Fe-MIL-88B-NH₂/C^d	1	300	2.0	180000	27.8	25.5	18.7		17.5	9.4	54.4	[275]
R-Fe@HZSM-5	2	270	2.0	2240	93	12	7.5		21.5	21.5	71	[277]
Fe₃O₄@H-ZSM-5	1	270	2.0	960	87	—	16		36.2	36.2	47.8	[278]
FeCuK/ZSM-5	2	300	1.0	2000	81.1	35.6	19.6		30.3	12.3	37.8	[280]
FeCuK/Mordenite	2	300	1.0	2000	72.9	37.7	32.2		18.8	25.4	23.6	[280]
FeCuK/Beta-zeolite	2	300	1.0	2000	63.9	25.2	31.5		29.2	21.6	17.7	[280]
FeZnNa	8:3	340	2.0	10000	74.9	27.3	10.9		25.5	4.4	58.1(1.1)^e	[51]
FeZnNa@HZSM-5	8:3	340	2.0	10000	88.3	27.7	11.3		1.4	38.6	28.9(19.8)^e	[51]
FeZnNa@0.1-HZSM-5	8:3	340	2.0	10000	84.2	26.5	9.9		0.7	35.6	22.7(30.9)^e	[51]
FeZnNa@0.6-HZSM-5	8:3	340	2.0	10000	89.2	26.9	9.8		1.0	26.8	21.8(40.5)^e	[51]
FeZnNa@0.6-HZSM-5-a	8:3	340	2.0	10000	88.8	27.5	9.6		1.0	25.6	13.2(50.6)^e	[51]
FeMn	1	320	1.0	3600	58.7	42.4	19.6		26.9	11.1	42.4(0)^e	[284]
FeMn-HZSM-5 (particle mixing)	1	320	1.0	3600	49.4	39.8	19.9		0.3	41.5	9.6(28.7)^e	[284]
FeMn&HZSM-5 (layered, h = 3 cm)	1	320	1.0	3600	59.4	41.7	19.2		0.2	42.2	8.2(30.2)^e	[284]
FeMn-HZSM-5@Si-1	1	320	1.0	3600	60.0	42.7	22.5		1.0	31.5	11.4(33.6)^e	[284]
Fe/Ni-HZMS-5	2	330	4.0	1813	99.2	3.2	9.2	9.2		9.2	39.6(48.0)^e	[285]