CO/CO2加氢制芳烃的研究进展

doi:10.16085/j.issn.1000-6613.2020-0550

摘要/Abstract

摘要：

将CO/CO₂直接转化为芳烃是一种极具挑战性的非石油路线合成途径。本文主要对CO/CO₂通过不同反应途径制取芳烃过程中复合催化剂的开发和反应机理的研究进展进行了综述。阐述了利用反应耦合思想，构筑的复合催化剂在CO/CO₂的高效转化和产物调控等方面取得了突破性的进展。重点介绍了复合催化剂用于CO加氢制芳烃主要的两种反应途径，活性金属的类别、分子筛的结构与酸性和活性组分的组装方式与接触度对CO₂加氢制芳烃催化性能的影响。指出协同加氢与芳构化反应活性的匹配是影响催化剂性能的关键。提出开发高效稳定的催化剂用于提高CO/CO₂的转化率和芳烃产物的产率以及反应机理的探索仍然是未来研究的重点。

关键词: 一氧化碳, 二氧化碳, 加氢, 芳烃, 复合催化剂, 反应机理

Abstract:

The direct conversion of CO/CO₂ to aromatics is a very challenging non-petroleum pathway, which has important strategic significance. In this paper, the research progress of composite catalysts development and the reaction mechanism in producing aromatics by different reaction routes of CO/CO₂ were reviewed. Based on the reaction coupling theory, breakthroughs of the composite catalyst in CO/CO₂ conversion and product regulation have been made. Two main reaction pathways of CO hydrogenation to aromatics using composite catalysts, as well as the influences of active metals types, the structure and acidity of zeolites and the assembly mode and the contact degree of active components on the catalytic performance were emphatically introduced. The reactivity matching between the synergetic hydrogenation and the aromatization is the key factor affecting the performance of catalysts. The development of efficient and stable catalysts to improve the conversion rate of CO/CO₂ and the yield of aromatic products, and the exploration of the reaction mechanism remain the focus of future research.

Key words: carbon monoxide, carbon dioxide, hydrogenation, aromatics, composite catalyst, reaction mechanism

中图分类号:

TQ032.4

焦佳鹏, 田海锋, 何环环, 查飞, 郭效军, 唐小华. CO/CO₂加氢制芳烃的研究进展[J]. 化工进展, 2021, 40(1): 205-220.

Jiapeng JIAO, Haifeng TIAN, Huanhuan HE, Fei ZHA, Xiaojun GUO, Xiaohua TANG. Recent advanced of CO/CO₂ hydrogenation to aromatics[J]. Chemical Industry and Engineering Progress, 2021, 40(1): 205-220.

图/表 22

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催化剂	反应条件			CO转化率/%	芳烃选择性/%	参考文献
催化剂	温度/℃	压强/MPa	空速	CO转化率/%	芳烃选择性/%	参考文献
FeMn-HZSM-5	320	1.0	2220mL·g^-1·h^-1	81.9	32.8^①	[56]
FeK-HZSM-5	320	1.0	2220mL·g^-1·h^-1	94.7	53.8^①	[56]
Co/ZSM-5	280	2.1	1000h^-1	55.0	19.9^①	[59]
FeMnK/SiO₂-HZSM-5	320	2.0	4000h^-1	83.8	57.2^①	[65]
FeZrZn-Ni/ZSM-5	340	4.0	2000h^-1	93.6	36.6^①	[70]
K/FeZrZn-Ni/ZSM-5	340	4.0	2000h^-1	96.8	39.5^①	[70]
K-FeMnO/MoNi-ZSM-5	370	4.0	1395h^-1	98.2	75.9^①	[71]
Fe-Pd/HZSM?5	310	8.6	3000h^-1	75.7	32.0^②	[73]
FeZnNa@HZSM-5	340	2.0	—	88.8	50.6^①	[74]
FeMn-HZSM-5@Si	320	1.0	3600mL·g^-1·h^-1	60.0	33.6^①/93.0^②	[78]
Zn-ZrO₂/H-ZSM-5	400	3	—	21.0	81.0^①	[82]
Cr/Zn-Zn/Z5@S1	400	5	20.7g·h·mol^-1	55.0	62.0^①	[83]
ZnCrO_x-ZSM-5	350	4	1500mL·g^-1·h^-1	16.0	73.9^①	[84]
Mo/HZSM-5	380	6.9	3000h^-1	64.4	97.6^②	[86]
PdZnAl + HZSM-5	310	6.9	700h^-1	44.0	69.0^②	[87]
Mo-ZrO₂/H-ZSM-5	400	4	3000mL·g^-1·h^-1	22.0	76.0^①	[97]
CeZrO₂/HZSM-5	380	2	3500mL·g^-1·h^-1	8.1	83.1^①	[98]
Fe₂O₃-SiO₂/Nb-ZSM-5	330	4	1813h^-1	99.0	47.4^①	[99]
CuO-ZnO-Al₂O₃/Nb-Ni-ZSM-5	330	4	1813h^-1	95.0	46.5^①	[99]
Fe-CuO-ZnO-Al₂O₃/Nb-Ni-ZSM-5	330	4	1813h^-1	99.2	55.0^①	[99]
Zn-Cr/HZSM-5	395	2.0	4000h^-1	11.1	72.4^①	[100]
m-ZrO₂/HZSM-5	400	3.8	—	24.0	67.4^①	[101]
Mn-ZnO&H-ZSM-5	340	3.0	750mL·g^-1·h^-1	14.8	80.1^①	[102]

催化剂	反应条件			CO转化率/%	芳烃选择性/%	参考文献
催化剂	温度/℃	压强/MPa	空速	CO转化率/%	芳烃选择性/%	参考文献
FeMn-HZSM-5	320	1.0	2220mL·g^-1·h^-1	81.9	32.8^①	[56]
FeK-HZSM-5	320	1.0	2220mL·g^-1·h^-1	94.7	53.8^①	[56]
Co/ZSM-5	280	2.1	1000h^-1	55.0	19.9^①	[59]
FeMnK/SiO₂-HZSM-5	320	2.0	4000h^-1	83.8	57.2^①	[65]
FeZrZn-Ni/ZSM-5	340	4.0	2000h^-1	93.6	36.6^①	[70]
K/FeZrZn-Ni/ZSM-5	340	4.0	2000h^-1	96.8	39.5^①	[70]
K-FeMnO/MoNi-ZSM-5	370	4.0	1395h^-1	98.2	75.9^①	[71]
Fe-Pd/HZSM?5	310	8.6	3000h^-1	75.7	32.0^②	[73]
FeZnNa@HZSM-5	340	2.0	—	88.8	50.6^①	[74]
FeMn-HZSM-5@Si	320	1.0	3600mL·g^-1·h^-1	60.0	33.6^①/93.0^②	[78]
Zn-ZrO₂/H-ZSM-5	400	3	—	21.0	81.0^①	[82]
Cr/Zn-Zn/Z5@S1	400	5	20.7g·h·mol^-1	55.0	62.0^①	[83]
ZnCrO_x-ZSM-5	350	4	1500mL·g^-1·h^-1	16.0	73.9^①	[84]
Mo/HZSM-5	380	6.9	3000h^-1	64.4	97.6^②	[86]
PdZnAl + HZSM-5	310	6.9	700h^-1	44.0	69.0^②	[87]
Mo-ZrO₂/H-ZSM-5	400	4	3000mL·g^-1·h^-1	22.0	76.0^①	[97]
CeZrO₂/HZSM-5	380	2	3500mL·g^-1·h^-1	8.1	83.1^①	[98]
Fe₂O₃-SiO₂/Nb-ZSM-5	330	4	1813h^-1	99.0	47.4^①	[99]
CuO-ZnO-Al₂O₃/Nb-Ni-ZSM-5	330	4	1813h^-1	95.0	46.5^①	[99]
Fe-CuO-ZnO-Al₂O₃/Nb-Ni-ZSM-5	330	4	1813h^-1	99.2	55.0^①	[99]
Zn-Cr/HZSM-5	395	2.0	4000h^-1	11.1	72.4^①	[100]
m-ZrO₂/HZSM-5	400	3.8	—	24.0	67.4^①	[101]
Mn-ZnO&H-ZSM-5	340	3.0	750mL·g^-1·h^-1	14.8	80.1^①	[102]

催化剂	反应条件			CO₂转化率/%	芳烃选择性/%	参考文献
催化剂	温度/℃	压强/MPa	空速/mL·g^-1·h^-1	CO₂转化率/%	芳烃选择性/%	参考文献
ZnZrO/ZSM-5	320	4.0	1200	14.0	73.0^①	[39]
Na-Fe₃O₄/HZSM-5	320	3.0	4000	34.0	40.2^①	[109]
ZnAlO_x&H-ZSM-5	320	3.0	6000	9.1	73.9^①	[110]
ae-ZnO-ZrO₂/H-ZSM-5	340	4.0	7200	16.0	76.0^①	[111]
Cr₂O₃/H-ZSM-5	350	3.0	1200	34.5	75.9^①	[112]
Na-Fe@C/H-ZSM-5	320	3.0	9000	33.3	50.2^①	[114]
Na/Fe-HZSM-5	300	1.0	4800	21.8	54.7^①/91.5^②	[115]
Fe₂O₃@KO₂/ZSM-5	375	3.0	5000	47.4	23.4^①	[118]
FeK1.5/HSG\|HZSM-5	340	2.0	26000	35.0	68.0^①	[120]
ZnFeO_x-nNa/HZSM-5	320	3.0	4000	41.2	75.6^①	[121]
ZnCrOx-ZnZSM-5	320	5.0	2000	19.9	56.5^①/81.1^②	[123]
Cr₂O₃/Zn-ZSM-5@SiO₂	350	3.0	1200	22.1	70.1^①	[127]
Fe-Zn-Zr@HZSM-5	340	5.0	3000	23.5	92.2^②	[129]

催化剂	反应条件			CO₂转化率/%	芳烃选择性/%	参考文献
催化剂	温度/℃	压强/MPa	空速/mL·g^-1·h^-1	CO₂转化率/%	芳烃选择性/%	参考文献
ZnZrO/ZSM-5	320	4.0	1200	14.0	73.0^①	[39]
Na-Fe₃O₄/HZSM-5	320	3.0	4000	34.0	40.2^①	[109]
ZnAlO_x&H-ZSM-5	320	3.0	6000	9.1	73.9^①	[110]
ae-ZnO-ZrO₂/H-ZSM-5	340	4.0	7200	16.0	76.0^①	[111]
Cr₂O₃/H-ZSM-5	350	3.0	1200	34.5	75.9^①	[112]
Na-Fe@C/H-ZSM-5	320	3.0	9000	33.3	50.2^①	[114]
Na/Fe-HZSM-5	300	1.0	4800	21.8	54.7^①/91.5^②	[115]
Fe₂O₃@KO₂/ZSM-5	375	3.0	5000	47.4	23.4^①	[118]
FeK1.5/HSG\|HZSM-5	340	2.0	26000	35.0	68.0^①	[120]
ZnFeO_x-nNa/HZSM-5	320	3.0	4000	41.2	75.6^①	[121]
ZnCrOx-ZnZSM-5	320	5.0	2000	19.9	56.5^①/81.1^②	[123]
Cr₂O₃/Zn-ZSM-5@SiO₂	350	3.0	1200	22.1	70.1^①	[127]
Fe-Zn-Zr@HZSM-5	340	5.0	3000	23.5	92.2^②	[129]

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CO/CO₂加氢制芳烃的研究进展

Recent advanced of CO/CO₂ hydrogenation to aromatics

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