分子筛结构设计及酸性调控在合成气催化转化中的应用研究进展

庹杰; 李石擎; 徐浩; 关业军; 吴鹏

doi:10.1016/S1872-5813(22)60035-5

分子筛结构设计及酸性调控在合成气催化转化中的应用研究进展

doi: 10.1016/S1872-5813(22)60035-5

庹杰^1,,
李石擎¹,
徐浩^{1, 2},
关业军^{1, 2, ,},
吴鹏^{1, 2, ,}

1.
华东师范大学化学与分子工程学院上海市绿色化学与化工过程绿色化重点实验室, 上海200062
2.
崇明生态研究院, 上海 202162

基金项目: 国家自然科学基金 (21872052, 21972044, 21773067)和科技部重点研发计划（2016YFA0202804）资助

详细信息

通讯作者:
Tel: 021-62232292, Fax: 021-62232292, E-mail: yjguan@chem.ecnu.edu.cn

pwu@chem.ecnu.edu.cn

中图分类号: O643.36; TQ519
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- 被引次数: 0
出版历程
- 收稿日期: 2022-04-30
- 修回日期: 2022-05-12
- 录用日期: 2022-05-19
- 网络出版日期: 2022-06-09
- 刊出日期: 2023-01-10

Research progress of structure design and acidity tuning of zeolites for the catalytic conversion of syngas

TUO Jie^1
,,
LI Shi-qing¹,
XU Hao^{1, 2},
GUAN Ye-jun^{1, 2
, ,},
WU Peng^{1, 2
, ,}

1.
Shanghai Key Laboratory of Green Chemistry and Chemical Processes, School of Chemistry and Molecular Engineering, East China Normal University, Shanghai 200062, China
2.
Institute of Eco-Chongming, Shanghai 202162, China

Funds: The project was supported by National Natural Science Foundation of China (21872052, 21972044, 21773067) and the Ministry of Science and Technology of the People’s Republic of China (2016YFA0202804).

摘要

摘要: 合成气催化转化是生物质或煤炭资源化清洁利用的重要路径，由此可获得烯烃和芳烃等多种高附加值碳氢化合物。分子筛由于具有独特的亚纳米孔道、可控活性位及分子择形性等优点，常被作为载体或直接作为活性组分用于催化合成气转化中C−C的形成和断裂等关键步骤。本综述总结了以分子筛负载金属、氧化物-分子筛(OX-ZEO)双功能以及核壳结构催化剂等直接催化转化合成气制备碳氢化合物的研究进展。重点介绍分子筛结构和酸性对反应路径和机理以及产物分布的影响，并展望分子筛催化合成气转化的未来发展方向。
- 分子筛 /
- 费托合成 /
- 双功能催化剂 /
- 合成气 /
- 反应机理 /
- 骨架结构 /
- 酸性
Abstract: The catalytic conversion of syngas to value-added hydrocarbons is an important strategy for the clean utilization of biomass and coal resources. Zeolites as supports and/or catalytic components are commonly used for C–C formation/cleavage in the syngas conversion, owing to their unique microporous structure, accurately tunable active sites, and molecular shape-selectivity. Herein, we have surveyed the research progress of direct conversion of syngas to hydrocarbons by using metal-loaded zeolites, bifunctional oxide-zeolite (OX-ZEO), and core-shell structured catalysts, focusing mainly on the influence of zeolite structure and acidity on the reaction mechanism as well as the product distribution for syngas conversion. In addition, an outlook is given on the perspective of zeolite synthesis and catalysis in the direct conversion of syngas.
- zeolite /
- Fischer-Tropsch synthesis /
- bifunctional catalysts /
- syngas /
- reaction mechanism /
- framework structure /
- acidity

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图 1 合成气转化制低烯烃和芳烃等烃类的典型途径

Figure 1 Typical routes for syngas conversion to lower olefins, aromatics and various hydrocarbons

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图 2 费托合成产物分布ASF模型^[2]

Figure 2 ASF model of Fischer-Tropsch synthesis^[2](with permission from RSC Publications)

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图 3 合成气通过Co/ASB直接合成异构烷烃的反应机理^[19]

Figure 3 Reaction mechanism of the direct synthesis of isoparaffins from syngas over Co/ASB^[19](with permission from ACS Publications)

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图 4 Co/Y_meso催化剂合成气转化催化性能^[28]

Figure 4 Catalytic performance of Co/Y_meso in the transformation of syngas^[28](a) FTS with conventional supports or Y_meso zeolites. Detailed product distribution over the Y_meso catalysts modified by different elements: (b) Co/Y_meso-Ce, (c) Co/Y_meso-La and (d) Co/Y_meso-K(with permission from Springer Nature)

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图 5 合成气转化OX-ZEO双功能催化剂

Figure 5 Syngas conversion with the OX-ZEO bifunctional catalyst systems

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图 6 分子筛骨架结构示意图

Figure 6 Framework structures of (a) Y, (b) MFI, and (c) CHA zeolites

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图 7 拓扑结构对双循环传播的影响^[64]

Figure 7 Impact of zeolite topology on the propagation of olefin- and aromatic-based cycles for the conversion of methanol to hydrocarbons (MTH) ((a), (b)): 8 MR zeolites, composed of large cavities with small window openings; ((c), (d)): 1D 10 MR zeolites; ((e), (f)): 3D 10 MR MFI zeolite; ((g), (h)): 1D 12 MR zeolite^[64](with permission from Springer Nature)

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图 8 ZnAlO_x/SAPO中SAPO分子筛的窗口尺寸对合成气转化反应的影响^[65]

Figure 8 Effect of window size of SAPO zeolites on the performance of related bifunctional ZnAlO_x /SAPO catalysts in the syngas conversion^[65](with permission from Elsevier)

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图 9 ZnAlO_x/SAPO 催化合成气转化反应中，SAPO分子筛(8 MR)笼的大小对反应的影响^[65]

Figure 9 Effect of cage size of SAPO zeolites with 8 MR windows on the performance of related bifunctional ZnAlO_x/SAPO catalysts in the syngas conversion^[65](with permission from Elsevier)

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图 10 MOR分子筛不同酸位对合成气、乙烯酮、甲醇转化反应的影响^[53]

Figure 10 Hydrocarbon distributions in the conversion of syngas, ketene and methanol over different sites of MOR zeolites at 648 K (a)−(c): 8 MR acid sites; (d)−(f): 12 MR acid sites; (g)−(i): both the 8 MR and 12 MR acid sites; ((a), (d), (g)): syngas over ZnCrO_x-MOR; ((b), (e), (h)); ketene conversion over MOR; ((c), (f), (i)): methanol conversion over MOR^[53](with permission from Wiley)

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图 11 ZnCrO_x-ZSM-5催化合成气制芳烃b/a取向长度比值对芳烃和C₆₊脂肪烃类分布的影响^[51]

Figure 11 Syngas to aromatics over ZnCrO_x-ZSM-5 Distributions of aromatics and C₆₊ aliphatics in C₆₊ hydrocarbons as a function of the length ratio of the b/a axes^[51](with permission from Elsevier)

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图 12 酸性对双循环传播过程的影响^[64]

Figure 12 Impact of acidity on the propagation of two cycles in MTH. dependence of selectivity to ${\rm{C}}_{3}^{{=}}$ (a) and aromatics (b) on the Si/Al ratio for the ZSM-5 zeolites summarized from literatures; the reaction process in the zeolite with low (c) and high (d) density of Brønsted acid site (BAS)^[64](with permission from Springer Nature)

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图 13 ZnCrO_x-SAPO-18双功能催化剂催化合成气转化的催化性能与硅铝比的关系^[44]

Figure 13 Performance of the bifunctional ZnCrO_x -SAPO-18 catalyst in syngas conversion as a function of the Si/Al ratio^[44] (a): CO conversion and selectivity; (b): ratio of C₃/C₂ and oleﬁns to paraffins (O/P) (with permission from American Chemical Society)

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图 14 B酸位点密度对双功能Zn-ZrO₂/SSZ-13催化剂催化行为的影响^[34]

Figure 14 Effect of density of Brønsted acid sites on the catalytic behaviors of the bifunctional Zn-ZrO₂/SSZ-13 catalyst in syngas conversion^[34](with permission from RSC Publications)

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图 15 Co/Al₂O₃/H-beta核壳催化剂^[87]

Figure 15 Core/shell catalyst of Co/Al₂O₃/H-beta^[87](with permission from Wiley Publications)

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图 16 Na-Zn-Fe₅C₂@ H-ZSM-5催化剂合成气制备芳烃的机理示意图^[93]

Figure 16 Proposed scheme for direct production of aromatics from syngas on Na-Zn-Fe₅C₂@ H-ZSM-5 catalyst^[93]

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表 1 FTS反应的代表性金属负载催化剂

Table 1 Representative metal loaded catalysts of FTS reaction

Catalyst	T/K	p/MPa	GHSV /(mL·g⁻¹·h⁻¹)	H₂/CO	CO conv. /%	CO₂ sel. /%	Main product /%	Ref.
mBulk Fe	613	2	1500	1	97	34	32^a (0.57^b)	[8]
Fe/α-Al₂O₃					80	40	53^a (8.48^b)
Fe/CNF					88	42	52^a (2.98^b)
Fe₃O₄	593	1.5	3000	2	97	44	35^a	[9]
Fe₃O₄@SiO₂	593	1.5	3000	2	34	23	30^a
Fe/PANI	623	1	9000	2	79	44	47^a	[11]
Co/SiO₂	503	2	2400	1	37	−	60^d (0.3^c)	[18]
Co/Al₂O₃					39	−	56^d (0.5^c)
Co/H-Y					36	−	72^d (3.2^c)
Co/H-meso-Y					40	−	79^d (2.7^c)
Co/SiO₂	513	1	2240	2	20	−	0.07^c	[19]
Co/Beta					30	−	2.43^c
Co/ASB					36	−	1.50^c
Ru/SiO₂	533	2	2400	1	32	−	25^e (0.42^c)	[16]
Ru/Al₂O₃					40	−	22^e (0.53^c)
Ru/TiO₂					20	−	26^e (1.1^c)
Ru/H-Mordenite					31	−	52^e (1.8^c)
Ru/H-Beta					24	−	58^e (3.3^c)
Ru/H-MCM-22					22	−	54^e (4.1^c)
Ru/H-ZSM-5					25	−	47^e (2.7^c)
Co/H-meso-ZSM-5-0.5_M	513	2	2400	2	42	−	70^e (2.3^b)	[20]
10%Fe/HZSM-5	593	2	4000	1	81	50	27 (60)	[21]
25%Fe/HZSM-5	593	2	4000	1	85	50	31 (70)
^a: Selectivity to ${\rm{C} }_{ {\rm{2-4} } }^{\rm{=} } $; ^b: FTY; ^c: Molar ratio of isoparaffins to n-paraffins; ^d: Selectivity to C₅₋₂₀; ^e: Selectivity to C₅₋₁₁; ^f: Aromatics selectivity in C₅₊ hydrocarbons

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表 2 合成气催化转化代表性OX-ZEO双功能催化剂

Table 2 Representative OX-ZEO bifunctional catalysts of syngas catalytic conversion

Zeolite topology	Zeolite	Oxide	T/K	p/MPa	GHSV/ (mL·g⁻¹·h⁻¹)	H₂/CO	CO conv. /%	CO₂ sel. /%	Main product /%		Ref.
Zeolite topology	Zeolite	Oxide	T/K	p/MPa	GHSV/ (mL·g⁻¹·h⁻¹)	H₂/CO	CO conv. /%	CO₂ sel. /%	${\boldsymbol{ {\rm{C} } } }_{2-4}^{\rm{=} }$	C₅₊	Ref.
CHA (3D, 8 MR)	SAPO-34	ZnCrO_x	673	3.5	4800	2.5	17	41	80	−	[34]
	SAPO-34	ZnO-ZrO₂	673	1	3600	2	7	43	69	2	[34]
	SAPO-34	ZnAlO_x	663	4	12000	1	7	33	78	4	[32]
	SAPO-34	MnO_x	673	2.5	4800	2.5	7	43	79	5	[38]
	SAPO-34	ZnCeZrO₄	573	1	5400	2	6	6	83	9	[40]
	SAPO-34	ZrCeZnO_x	673	1	3900	2	13	45	82	3	[35]
	SAPO-34	MnGaO_x	673	2.5	4875	2	14	45	88	2	[41]
	SAPO-34	ZnO	673	4	1600	2.5	32	42	77	5	[37]
	SAPO-34	Zr-In₂O₃	673	2.5	3600	1	28	40	74	2	[42]
	SSZ-13	Zn-ZrO₂	673	3	3000	2	29	42	77	3	[34]
	BAl-CHA	ZnAlO_x	623	1	2400	2	10	43	83	−	[43]
AEI (3D, 8 MR)	SAPO-18	ZnCrO_x	673	4	5000	2.5	36	41	82	−	[44]
AEI (3D, 8 MR)	AlPO-18	ZnCrO_x	663	4	3600	1	25	48	87	9	[45]
AEL (1D 10 MR)	SAPO-11	Zn₂Mn₁O_x	633	4	1000	1	20	−	−	77^a	[46]
TON (1D 10 MR)	ZSM-22	Zn₂Mn₁O_x	633	4	1000	1	19	−	−	64^a	[46]
MTW (1D 12 MR)	ZSM-12	Zn₂Mn₁O_x	633	4	1000	1	21	−		70^a	[46]
MFI (3D 10 MR)	ZSM-5	Zn₂Mn₁O_x	633	4	1000	1	23	−	−	67^a	[46]
	ZSM-5	CeZrO₂	653	2	600	1	8	32.9		83^b	[47]
	ZSM-5	Mo-ZrO₂	673	4	3000	2	22	−	−	76^b	[48]
	ZSM-5	MnO	623	2	333	2	21	−		83^b	[49]
	ZSM-5	ZnCrO_x	623	4	1500	1	16			74^b	[50]
	ZSM-5	ZnCrO_x	623	4	1500	1	18	49		69^b	[51]
	ZSM-5	1Zn-3Cr	668	2	4000	1	11	−	−	72^b	[52]
MEL (3D 10 MR)	ZSM-11	Zn₂Mn₁O_x	633	4	1000	1	23			64^a	[46]
MOR (3D, 8 MR &12 MR)	MOR	ZnCrO_x	633	2	1600	1	26	48	91	5	[53]
MOR (3D, 8 MR &12 MR)	MOR	ZnAl₂O₄	643	3	1500	1	10	44	77	6	[54]
^a: Selectivity of C_5–11 ^b: Aromatics

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分子筛结构设计及酸性调控在合成气催化转化中的应用研究进展

doi: 10.1016/S1872-5813(22)60035-5

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Research progress of structure design and acidity tuning of zeolites for the catalytic conversion of syngas

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分子筛结构设计及酸性调控在合成气催化转化中的应用研究进展

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Research progress of structure design and acidity tuning of zeolites for the catalytic conversion of syngas

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