铜系材料的制备及其催化丁二酸二甲酯加氢的性能探究

doi:10.19964/j.issn.1006-4990.2022-0751

Abstract

Abstract:

At present，acetylene aldehyde method，maleic anhydride method，butadiene method and propylene oxide method are used in the industry to produce 1，4-butanediol（BDO）.However，due to the high energy consumption and pollution，the use of more green biological method to produce BDO gradually shows more advantages.At present，there are few researches on the hydrogenation of dimethyl succinic acid（DMS），which can be obtained from the esterification of succinic acid platform molecule，to BDO.Three inorganic materials of copper nitrate，zinc nitrate and aluminum nitrate，were selected to prepare the copper catalyst for the hydrogenation of dimethyl succinic acid（DMS） to 1，4-butanediol（BDO） by coprecipitate method.The products were characterized by XRF，BET，H₂-TPR，XRD and XPS.And the catalytic material properties were tested in order to obtain catalytic materials with good performance，providing ideas for subsequent research.The results showed that the catalytic material with copper mass fraction of 20% and zinc-aluminum molar ratio of 0.3 had good hydrogenation performance at 185 ℃，5 MPa，hydrogen-ester ratio of 150 and space velocity of 1 h^-1，with DMS conversion rate of 98.6% and BDO selectivity of 87.3%.And it had good stability after 1 000 h continuous operation which showed good industrial prospect.

Key words: dimethyl succinate, copper catalyst, hydrogenation, 1，4-butanediol

CLC Number:

O643.36

WANG Peng, ZHAO Shanshan, LU Yanfei, LI Shisong, WANG Chunlei, SHU Chang, ZHANG Dongsheng. Study on preparation of copper-based materials and its catalytic performance for hydrogenation of dimethyl succinate[J]. Inorganic Chemicals Industry, 2023, 55(10): 145-152.

Figures/Tables 13

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催化剂	理论值		实测值
催化剂	n（Zn）: n（Al）	w （CuO）/%	w （CuO）/%	w （Al₂O₃）/%	w （ZnO）/%
0.05CuZnAl	0.05:1	20.0	20.4	73.7	5.9
0.15CuZnAl	0.15:1	20.0	20.8	65.9	13.3
0.3CuZnAl	0.3:1	20.0	20.4	55.0	24.6
0.6CuZnAl	0.6:1	20.0	20.9	49.7	29.4

催化剂	比表面积/ （m²·g^-1）	孔容/ （cm³·g^-1）	孔径/ nm
0.05CuZnAl	40	0.35	5.1
0.15CuZnAl	44	0.34	5.0
0.3CuZnAl	50	0.32	5.5
0.6CuZnAl	47	0.30	5.2

催化剂	弱酸量（100~＜250 ℃）	中强酸量（250~400 ℃）	强酸量（>400 ℃）	总酸量
0.05CuZnAl	0.18（30.5%）	—	0.41（69.4%）	0.59
0.15CuZnAl	0.31（23.1%）	—	1.03（76.8%）	1.34
0.3CuZnAl	0.08（23.5%）	—	0.26（76.4%）	0.34
0.6CuZnAl	0.15（24.5%）	—	0.46（75.4%）	0.61

催化剂	DMS/DES/SA 转化率/%	BDO选择性/%	反应温度/℃	反应压力/MPa	反应时间/h
0.3CuZnAl	97.5（DMS）	87.2	185	5	1 000
n（Cu）/n（Zn）=1:1^［31］	99.0（DMS）	64.0	220	5	8
Cu/ZrO₂^［32］	100（DES）	10.0	220	7	—
CuO/ZnO^［33］	100（DES）	86.1	170	4	—
8%Cu-2%Pd/HPA^［34］	100（SA）	82.0	200	8	96
Re-Cu-MC^［35］	100（SA）	<41.9	200	8	20
0.3Re-0.3Ru/MC^［35］	100（SA）	71.2	200	8	7
ReRu/C^［36］	100（SA）	70.0	—	8	—
Re-Pd/SiO₂［n（Re）/ n（Pd）=8］^［37］	100（SA）	89.0	140	8	96

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Study on preparation of copper-based materials and its catalytic performance for hydrogenation of dimethyl succinate

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