Recent advance in directing synthesis of aromatic hydrocarbon from syngas via oxygenated compound intermediates

doi:10.16085/j.issn.1000-6613.2020-2069

Abstract

Abstract:

Compared with the syngas to aromatics through methanol route, the one-step syngas to aromatics (namely STA) is a very promising non-petroleum base route, because of its advantages of low cost and short process. In this paper, the research progresses in the development of bi-functional catalyst for the one-step synthesis of aromatics were reviewed. Firstly, the process of one-step conversion of syngas to aromatic was introduced, with the focus on the preparing methods of various catalysts used. The impacts of the physical and chemical properties of metal oxide and zeolite on the catalytic behavior were summarized, including the composition of metal oxides, ratio of two metals, crystal morphology, crystal size, ratio of metal oxides to zeolite, and acidity and diffusivity of zeolite. Furthermore, it introduced the forms and formation mechanisms of different intermediates on bifunctional catalyst. Finally, this paper reviewed current issues and challenges on one-step conversion of syngas to aromatic, and pointed out that the development of high-performance catalyst is the main research direction in the future.

Key words: syngas, aromatic, bi-functional catalyst, catalysis, intermediate, mechanism

摘要：

相比于合成气（CO/H₂）经甲醇制芳烃的路线，合成气一步法制芳烃（STA）具有路线短、设备投资低等优势，是一条具有广阔应用前景的技术路线。本文首先简单陈述了合成气一步法制芳烃的基本过程，详细总结了合成气一步法制芳烃催化剂开发的进展。重点讨论了金属氧化物组成、双金属配比、晶型晶粒尺寸、氧化物与分子筛的配比以及分子筛的酸性、扩散性等物化性质对反应性能的影响规律。然后归纳了反应温度、反应压力、反应空速等反应工艺条件对反应性能的影响规律。接着总结了双功能催化剂上含氧中间体的形态及其形成机理，同时阐述了催化剂的失活研究以及抑制CO₂选择性的方法。最后分析了合成气一步法制芳烃存在的问题和面临的挑战，指出高性能催化剂的开发是今后的主要研究方向。

关键词: 合成气, 芳烃, 双功能催化剂, 催化（作用）, 反应中间体, 机理

CLC Number:

TQ241

SHANG Yunshan, WANG Qianjin, YANG Jiayi, YUAN Delin, ZHANG Fan, LIU Hua, XING Aihua, JI Shengfu. Recent advance in directing synthesis of aromatic hydrocarbon from syngas via oxygenated compound intermediates[J]. Chemical Industry and Engineering Progress, 2021, 40(10): 5535-5546.

尚蕴山, 王前进, 杨加义, 袁德林, 张凡, 刘华, 邢爱华, 季生福. 合成气经含氧化合物中间体一步法制芳烃研究进展[J]. 化工进展, 2021, 40(10): 5535-5546.

Figures/Tables 6

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氧化物	优点	缺点
CuO-ZnO-Al₂O₃	活性高，CO转化率高，经济实惠	无法高温长周期运行，高温不可逆失活
ZnCr₂O₄	活性适中，经济实惠	Cr有毒，Zn在反应过程逐渐脱除晶体结构，稳定性差
金属掺杂ZrO₂	热稳定好，潜在的再生性好	活性相对较低，价格昂贵，成本高
纳米ZnO	经济、环保	活性低

氧化物	优点	缺点
CuO-ZnO-Al₂O₃	活性高，CO转化率高，经济实惠	无法高温长周期运行，高温不可逆失活
ZnCr₂O₄	活性适中，经济实惠	Cr有毒，Zn在反应过程逐渐脱除晶体结构，稳定性差
金属掺杂ZrO₂	热稳定好，潜在的再生性好	活性相对较低，价格昂贵，成本高
纳米ZnO	经济、环保	活性低

催化剂组成	反应条件				转化率 /%	选择性/%	选择性（扣除CO₂）/%				中间体	参考文献
催化剂组成	H₂/CO比	压力 /MPa	温度 /K	空速 /mL·h^-1·g^-1	转化率 /%	CO₂	CH₄	C₂~C₄	C₅₊	芳烃	中间体	参考文献
ZnCr₂O₄&ZSM-5	1	8.3	700	1780	44.10	34.00	2.50	14.50	37.7	36.68	—^③	［2］
ZnCr₂O₄&ZSM-5	1	4	623	1500	16.00	48.00	1.70	15.10	2.7	73.90	乙烯酮	［4］
ZnCr₂O₄&Zn-Z5@S1	2.1	5	673	20.7	55.00	55.00	4.40	29.70		62.00	甲醇	［15］
ZnCr₂O₄&ZSM-5	1	2	668	4000	11.10	40.70	2.50	24.10		72.40	—	［14］
ZnCr₂O₄&Zn-ZSM-5	1	2	668	4000	13.20	40.00	2.10	24.40		73.50	—	［14］
ZrO₂&ZSM-5	1	3	673	500	26.20	12.50	24.50	38.20	37.4	53.00	—	［21］
Zn-ZrO₂&ZSM-5	2	3	673	500	21.00	2.00	<3.00	22.60	2.0	80.00	甲醇	［26］
CeZrO₂&HZSM-5	1	2	653	3500	8.10					83.10	甲醇、C₂₊醇、 C₆₊烯烃	［27］
CeZrO₂&HZSM-5	1	2	723	3500	22.40					56.30	甲醇、C₂₊醇、 C₆₊烯烃	［27］
Mo-ZrO₂&H-ZSM-5	2	4	673	3000	22.00	41.00	3.40	18.00	2.7	76.00	甲醇	［28］
ZrO₂&ZSM-5	1	6	623	3000	11.67	42.64	2.98	31.52	65.50	94.89^①	甲醇	［22］
ZrO₂&ZSM-5	1	6	673	1200	21.59	44.27	22.90	22.07	55.30	95.13^①	甲醇	［23］
ZnZrO₂@C&ZSM-5	2	3	633	3600	35.2		3.40			73.1	甲醇	［11］
ZnCr₂O₄&ZSM-5	1	2	668	4000	11.00	48.50	2.80	12.70		82.50	甲醇/乙烯酮	［13］
CAZ&ZSM-5	1	2	633	500	71.90					86.80^①	甲醇	［29］
CZA/Co-Nb&HZSM-5	2	4	603	1813	95.69	11.61			30.59	46.65	甲醇	［25］
CZA/Co-Nb&HZSM-5	2	4	623	1500	94.79	12.73			33.52	41.08
CZA&Nb-Ni-ZSM-5	2	4	603	1813	99.00					46.55
ZnO&ZSM-5	1	3	603	750	14.80					80.10	甲醇	［20］
MnCrO_x&ZSM-5-USY	1	4	703	1658	13.30	46.20	6.70	22.00		87.70^②	—	［29］

催化剂组成	反应条件				转化率 /%	选择性/%	选择性（扣除CO₂）/%				中间体	参考文献
催化剂组成	H₂/CO比	压力 /MPa	温度 /K	空速 /mL·h^-1·g^-1	转化率 /%	CO₂	CH₄	C₂~C₄	C₅₊	芳烃	中间体	参考文献
ZnCr₂O₄&ZSM-5	1	8.3	700	1780	44.10	34.00	2.50	14.50	37.7	36.68	—^③	［2］
ZnCr₂O₄&ZSM-5	1	4	623	1500	16.00	48.00	1.70	15.10	2.7	73.90	乙烯酮	［4］
ZnCr₂O₄&Zn-Z5@S1	2.1	5	673	20.7	55.00	55.00	4.40	29.70		62.00	甲醇	［15］
ZnCr₂O₄&ZSM-5	1	2	668	4000	11.10	40.70	2.50	24.10		72.40	—	［14］
ZnCr₂O₄&Zn-ZSM-5	1	2	668	4000	13.20	40.00	2.10	24.40		73.50	—	［14］
ZrO₂&ZSM-5	1	3	673	500	26.20	12.50	24.50	38.20	37.4	53.00	—	［21］
Zn-ZrO₂&ZSM-5	2	3	673	500	21.00	2.00	<3.00	22.60	2.0	80.00	甲醇	［26］
CeZrO₂&HZSM-5	1	2	653	3500	8.10					83.10	甲醇、C₂₊醇、 C₆₊烯烃	［27］
CeZrO₂&HZSM-5	1	2	723	3500	22.40					56.30	甲醇、C₂₊醇、 C₆₊烯烃	［27］
Mo-ZrO₂&H-ZSM-5	2	4	673	3000	22.00	41.00	3.40	18.00	2.7	76.00	甲醇	［28］
ZrO₂&ZSM-5	1	6	623	3000	11.67	42.64	2.98	31.52	65.50	94.89^①	甲醇	［22］
ZrO₂&ZSM-5	1	6	673	1200	21.59	44.27	22.90	22.07	55.30	95.13^①	甲醇	［23］
ZnZrO₂@C&ZSM-5	2	3	633	3600	35.2		3.40			73.1	甲醇	［11］
ZnCr₂O₄&ZSM-5	1	2	668	4000	11.00	48.50	2.80	12.70		82.50	甲醇/乙烯酮	［13］
CAZ&ZSM-5	1	2	633	500	71.90					86.80^①	甲醇	［29］
CZA/Co-Nb&HZSM-5	2	4	603	1813	95.69	11.61			30.59	46.65	甲醇	［25］
CZA/Co-Nb&HZSM-5	2	4	623	1500	94.79	12.73			33.52	41.08
CZA&Nb-Ni-ZSM-5	2	4	603	1813	99.00					46.55
ZnO&ZSM-5	1	3	603	750	14.80					80.10	甲醇	［20］
MnCrO_x&ZSM-5-USY	1	4	703	1658	13.30	46.20	6.70	22.00		87.70^②	—	［29］

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