Application of hydrocracking and hydroalkylation to enhance the value of C9 aromatics

doi:10.16085/j.issn.1000-6613.2020-1273

Abstract

Abstract:

In China, eight big refining and chemical bases have been built and in production in recent years, so the production of C₉ aromatics will increase significantly in the future. Large refineries need to focus on how to process C₉ aromatics efficiently. In this paper, C₉ aromatics from reformer are used to produce BTX and durene by hydrocracking ＆ hydroalkylation. The reaction conditions are mild and the products are of high economic value with high selectivity. Under the optimum reaction conditions, the average yield of oil is 86.94%, in which the average content of C₅ ~ C₉ fraction (rich in BTX ) is 80.93%, the average content of durene is 12.98%, and the average content of C $10 +$ fraction (excluding durene) is 6.09%. For the plant with an annual capacity of processing 90000 tons C₉ aromatics, an annual profit of 55.435 million yuan can be realized. The processing route proposed in this paper has high technical feasibility and economic feasibility, and is in line with the development trend of refining and chemical integration, therefore it is one of the preferred ways to process C₉ aromatics in the future.

Key words: C₉ aromatics, hydrocracking, hydroalkylation, durene, BTX

摘要：

随着国内八大炼化基地的逐步建成与投产，未来C₉混合芳烃的产量将大幅上涨，如何高效利用C₉混合芳烃将成为大型炼厂需要重点解决的问题。本文以重整装置副产的C₉混合芳烃为原料，经临氢裂解、临氢烷基化组合技术，生产高价值的苯/甲苯/二甲苯（BTX）和均四甲苯，反应条件缓和，目的产物选择性高。在最佳反应条件下，油相产物平均收率为86.94%，其中富含BTX的C₅~C₉馏分平均含量为80.93%，均四甲苯平均含量为12.98%，C₁₀⁺馏分（不含均四甲苯）平均含量为6.09%。对于C₉混合芳烃年处理量为9万吨的工业装置，通过本文提供的组合技术可实现年利润5543.5万元。本文提出的C₉混合芳烃的组合技术具有较高的技术可行性和经济可行性，符合炼化一体化的发展趋势，是未来炼厂解决C₉混合芳烃出路的首选途径之一。

关键词: C₉混合芳烃, 临氢裂解, 临氢烷基化, 均四甲苯, 苯/甲苯/二甲苯（BTX）

CLC Number:

TE624

ZANG Jiazhong, WANG Yinbin, HONG Luwei, YU Haibin, PENG Xiaowei, LI Chen, WANG Yang, GUO Chunlei. Application of hydrocracking and hydroalkylation to enhance the value of C₉ aromatics[J]. Chemical Industry and Engineering Progress, 2021, 40(5): 2593-2602.

臧甲忠, 王银斌, 洪鲁伟, 于海斌, 彭晓伟, 李晨, 汪洋, 郭春垒. 临氢裂解及烷基化组合技术应用于C₉混合芳烃的高值化[J]. 化工进展, 2021, 40(5): 2593-2602.

Figures/Tables 18

序号	名称	规格	厂家
1	硫酸铝	分析纯	天津市化学试剂批发公司
2	浓硫酸	纯度98%	天津市化学试剂批发公司
3	水玻璃	固含量26%	天津市化学试剂批发公司
4	正丁胺	分析纯	天津市化学试剂批发公司
5	CTAB	分析纯	天津市化学试剂批发公司
6	硫酸铵	分析纯	天津市化学试剂批发公司
7	六水硝酸镍	分析纯	天津市化学试剂批发公司
8	拟薄水铝石	工业品	山西铝业公司
9	ZSM-5分子筛	SiO₂/Al₂O₃=25	中海油天津化工研究设计院有限公司

样品	Al₂O₃/%	SiO₂/%	SiO₂/Al₂O₃	NiO/%
Z-1	5.22	94.53	30.8	—
Z-2	2.85	96.90	57.8	—
C-1	32.66	63.65	—	2.9
C-2	31.10	63.84	—	4.1

样品	S_BET/m²·g^-1	S_micro/m²·g^-1	S_ext/m²·g^-1	V_total/mL·g^-1	V_micro/mL·g^-1	D/nm
S-1	316.5	117.8	198.7	0.313	0.064	3.96
S-2	325.3	96.0	229.3	0.348	0.051	4.28
C-1	305.7	115.2	190.5	0.291	0.063	3.81
C-2	308.4	104.1	204.3	0.310	0.053	4.02

催化剂	酸量/mmol·g^-1	酸强度/℃
S-1	0.412	415.1
S-2	0.378	420.3
C-1	0.335	385.7
C-2	0.314	377.5

组分	质量分数/%
非芳	4.47
甲苯	1.10
二甲苯	8.20
三甲苯偏三甲苯	40.90 27.26
甲乙苯	28.27
丙苯	5.53
C $10 +$ 芳烃	11.53
合计/%	100

组分	质量分数/%
非芳	4.47
甲苯	1.10
二甲苯	8.20
三甲苯偏三甲苯	40.90 27.26
甲乙苯	28.27
丙苯	5.53
C $10 +$ 芳烃	11.53
合计/%	100

样品	油相收率/%	BTX质量分数/%	三甲苯质量分数/%	丙苯质量分数/%	甲乙苯质量分数/%	C $10 +$ 芳烃质量分数/%
原料	—	9.30	40.90	5.53	28.27	11.53
油相产物	91.37	50.43	33.38	0.06	4.83	6.96

样品	油相收率/%	BTX质量分数/%	三甲苯质量分数/%	丙苯质量分数/%	甲乙苯质量分数/%	C $10 +$ 芳烃质量分数/%
原料	—	9.30	40.90	5.53	28.27	11.53
油相产物	91.37	50.43	33.38	0.06	4.83	6.96

样品

气相收率

乙烷质量分数

组分	质量分数/%
苯	4.25
甲苯	21.40
二甲苯	23.67
均三甲苯	6.99
偏三甲苯	19.99
连三甲苯	6.30
均四甲苯	0.93
偏四甲苯	1.27
连四甲苯	0.33
合计/%	85.13

温度/℃	苯质量分数/%	甲苯质量分数/%	二甲苯质量分数/%	偏三甲苯质量分数/%	均四甲苯质量分数/%	均四甲苯选择性/%
350	3.04	13.07	21.38	23.31	9.40	68.9
370	2.34	10.28	18.69	21.95	13.22	85.0
390	2.38	10.33	20.41	22.13	13.55	82.3
410	2.63	11.70	20.63	22.50	11.74	75.7

压力

/MPa

乙烷质量分数

乙烯质量分数

丙烷质量分数

丙烯质量分数

压力/MPa	苯质量分数/%	甲苯质量分数/%	二甲苯质量分数/%	偏三甲苯质量分数/%	均四甲苯质量分数/%	均四甲苯选择性/%
2.0	2.32	10.20	19.26	21.65	12.98	84.9
3.0	2.34	10.28	18.69	21.95	13.22	85.0
4.0	2.46	10.61	19.21	21.90	13.34	84.8

空速/h^-1	苯质量分数/%	甲苯质量分数/%	二甲苯质量分数/%	偏三甲苯质量分数/%	均四甲苯质量分数/%	均四甲苯选择性/%
1.5	1.89	8.59	19.82	21.59	15.07	74.4
2.0	2.34	10.28	18.69	21.95	13.22	85.0
2.5	2.90	13.75	22.89	21.24	8.85	66.4

甲醇配比	苯质量分数/%	甲苯质量分数/%	二甲苯质量分数/%	偏三甲苯质量分数/%	均四甲苯质量分数/%	均四甲苯选择性/%	甲醇甲基利用率/%
1∶2	1.68	7.28	16.97	21.22	17.24	87.9	28.2
1∶3	2.34	10.28	18.69	21.95	13.22	85.0	30.6
1∶4	2.86	13.62	22.84	21.37	8.98	72.8	27.3

运行天数/天	油相产物收率/%	C₅~C₉馏分质量分数/%	均四甲苯质量分数/%	C $10 +$ 馏分质量分数/%	尾气中氢气体积分数/%
4	86.94	80.98	12.95	6.07	84.27
5	86.27	80.90	12.95	6.15	81.93
6	88.03	80.99	13.00	6.01	79.55
7	86.06	80.88	12.98	6.14	80.87
8	86.84	80.88	12.93	6.18	83.23
9	86.82	81.07	12.99	5.95	83.82
10	87.99	80.95	12.97	6.09	80.83
11	87.58	80.74	13.01	6.25	79.80
12	86.38	80.95	13.02	6.04	80.96
13	86.51	80.98	13.04	5.98	81.76
平均值	86.94	80.93	12.98	6.09	81.70

运行天数/天	油相产物收率/%	C₅~C₉馏分质量分数/%	均四甲苯质量分数/%	C $10 +$ 馏分质量分数/%	尾气中氢气体积分数/%
4	86.94	80.98	12.95	6.07	84.27
5	86.27	80.90	12.95	6.15	81.93
6	88.03	80.99	13.00	6.01	79.55
7	86.06	80.88	12.98	6.14	80.87
8	86.84	80.88	12.93	6.18	83.23
9	86.82	81.07	12.99	5.95	83.82
10	87.99	80.95	12.97	6.09	80.83
11	87.58	80.74	13.01	6.25	79.80
12	86.38	80.95	13.02	6.04	80.96
13	86.51	80.98	13.04	5.98	81.76
平均值	86.94	80.93	12.98	6.09	81.70

项目	物料名称	收率 /%	数量 /万吨·a^-1	单价 /元·t^-1	金额 /万元
消耗	C₉混合芳烃		9	-5000	-45000
	甲醇		3	-2300	-6900
	氢气		0.076	-15000	-1140
	加工费		12	-200	-2400
	催化剂		15	-200000	-300
产出	气相产物		1.426^①	2000	2852
	C₅~C₉混合芳烃	70.36	7.26	5800	40656
	均四甲苯	11.28	1.16	14000	16240
	C $10 +$ 重芳烃	5.29	0.54	3000	1620
	水		1.69	-50	-84.5
合计		86.93			5543.5

项目	物料名称	收率 /%	数量 /万吨·a^-1	单价 /元·t^-1	金额 /万元
消耗	C₉混合芳烃		9	-5000	-45000
	甲醇		3	-2300	-6900
	氢气		0.076	-15000	-1140
	加工费		12	-200	-2400
	催化剂		15	-200000	-300
产出	气相产物		1.426^①	2000	2852
	C₅~C₉混合芳烃	70.36	7.26	5800	40656
	均四甲苯	11.28	1.16	14000	16240
	C $10 +$ 重芳烃	5.29	0.54	3000	1620
	水		1.69	-50	-84.5
合计		86.93			5543.5

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Application of hydrocracking and hydroalkylation to enhance the value of C₉ aromatics

临氢裂解及烷基化组合技术应用于C₉混合芳烃的高值化

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