Preparation of Pseudo-boehamite from Industrial Materials and Its Application in Selective Hydrogenation of Isophorone

doi:10.19894/j.issn.1000-0518.220089

Chinese Journal of Applied Chemistry ›› 2023, Vol. 40 ›› Issue (1): 79-90.DOI: 10.19894/j.issn.1000-0518.220089

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Preparation of Pseudo-boehamite from Industrial Materials and Its Application in Selective Hydrogenation of Isophorone

Jin LIN, Fang-Zhu WANG(), Ling-Ling LYU()

College of Chemistry and Chemical Engineering，China University of Petroleum （East China），Qingdao 266580，China

Received:2022-03-23 Accepted:2022-09-15 Published:2023-01-01 Online:2023-01-28
Contact: Fang-Zhu WANG,Ling-Ling LYU
About author:zkde2l@126.com
wangfangzhu@126.com；

Abstract

Abstract:

Pseudo-boehmite is prepared from industrial grade aluminum sulfate and sodium meta-aluminate coming from waste FCC catalysts. The effects of preparation technology， conditions and modification on crystal type， pore structure， surface acidity and morphology of pseudo-boehmites are investigated. The activity and selectivity of Pd/Al₂O₃ catalyst prepared by modified Al₂O₃ carrier and PdCl₂ and Pd（acac）₂ precursors for the selective hydrogenation of isoporone CC are studied. The pseudo-boehmite with specific surface area of 413 m²/g， pore volume of 0.84 cm³/g and pore size of 6.84 nm is obtained at the optimized preparation conditions. After the addition of ammonium carbonate and sodium silicate， the pore volume of pseudo-boehmite increases to 0.98 cm³/g and 1.53 cm³/g， and the average pore size increases to 7.70 nm and 12.34 nm， respectively. The Pd/Al₂O₃ catalyst that is prepared using Al₂O₃ obtained by ammonium carbonate modifier as the carrier and PdCl₂ as the precursor shows an activity of 98.69% for the selective hydrogenation of isophorone CC， more than 99% selectivity of 3，3，5-trimethyl-cycloheeanon （TMCH）， and high activity stability.

Key words: Pseudo-boehmite, Preparation, Modification, Isophorone, Selective hydrogenation

CLC Number:

O643.3

Jin LIN, Fang-Zhu WANG, Ling-Ling LYU. Preparation of Pseudo-boehamite from Industrial Materials and Its Application in Selective Hydrogenation of Isophorone[J]. Chinese Journal of Applied Chemistry, 2023, 40(1): 79-90.

Figures/Tables 17

References 14

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Gelling temperature/℃	Specific surface area/（m²·g^-1）	Pore volume/（cm³·g^-1）	Average pore diameter/nm
40	135	0.15	4.69
50	355	0.73	6.33
60	376	0.80	6.92
70	350	0.69	5.91
90	290	0.53	5.65

Gelling temperature/℃	Specific surface area/（m²·g^-1）	Pore volume/（cm³·g^-1）	Average pore diameter/nm
40	135	0.15	4.69
50	355	0.73	6.33
60	376	0.80	6.92
70	350	0.69	5.91
90	290	0.53	5.65

Gelling pH	Specific surface area/（m²·g^-1）	Pore volume/（cm³·g^-1）	Average pore diameter/nm
7~8	173	0.29	5.60
8~9	188	0.40	5.44
9~10	412	0.73	5.10
10~11	413	0.81	6.84
11~12	417	0.77	5.98

Gelling pH	Specific surface area/（m²·g^-1）	Pore volume/（cm³·g^-1）	Average pore diameter/nm
7~8	173	0.29	5.60
8~9	188	0.40	5.44
9~10	412	0.73	5.10
10~11	413	0.81	6.84
11~12	417	0.77	5.98

Aging temperature/℃	Specific surface area/（m²·g^-1）	Pore volume/（cm³·g^-1）	Average pore diameter/nm
50	368	0.65	4.39
70	378	0.71	4.98
90	367	0.78	5.61

Preparation of Pseudo-boehamite from Industrial Materials and Its Application in Selective Hydrogenation of Isophorone

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Figures/Tables 17

References 14

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Aging pH	Specific surface area/（m²·g^-1）	Pore volume/（cm³·g^-1）	Average pore diameter/nm
9.0	327	0.74	5.73
9.5	341	0.73	5.53
10.0	415	0.69	5.42
10.5	413	0.69	5.40
11.0	431	0.68	5.42

Aluminium sulfate dropping speed/（mL·min^-1）	Specific surface area/（m²·g^-1）	Pore volume/（cm³·g^-1）	Average pore diameter/nm
10	475	0.82	6.92
20	413	0.84	6.84
40	412	0.74	5.98
60	421	0.67	5.12
80	416	0.67	4.92

m（（NH₄）₂CO₃）/m（Al₂O₃）（g·100 g^-1）	Specific surface area/（m²·g^-1）	Pore volume/（cm³·g^-1）	Average pore diameter/nm
0	386	0.72	5.61
2.5	404	0.84	6.42
5	429	0.98	7.70
7.5	417	0.87	6.90
10	405	0.84	6.84

m（SiO₂）/m（Al₂O₃）（g·100 g^-1）	Specific surface area/（m²·g^-1）	Pore volume/（cm³·g^-1）	Average pore diameter/nm
0	404	0.72	5.61
2	457	1.07	9.36
4	472	1.17	9.88
6	488	1.31	10.75
8	467	1.53	12.34
10	446	1.43	12.88
12	445	1.28	11.39
16	467	1.27	10.93
20	439	1.21	10.97
25	300	1.03	13.81

m（（NH₄）₂CO₃）/m（Al₂O₃）（g·100 g^-1）	Total acid density/（mmol·g^-1）	Weak acid density/（mmol·g^-1）	Mediate acid density/（mmol·g^-1）
0	0.713	0.407	0.283
2.5	0.770	0.447	0.310
5	0.819	0.457	0.321
7.5	0.752	0.417	0.315
10	0.699	0.397	0.284

m（SiO₂）/m（Al₂O₃）（g·100 g^-1）	Total acid density/（mmol·g^-1）	Weak acid density/ （mmol·g^-1）	Mediate acid density/（mmol·g^-1）
2	0.708	0.456	0.231
4	0.723	0.463	0.239
6	0.772	0.500	0.251
8	0.712	0.435	0.259
10	0.692	0.457	0.215
12	0.567	0.395	0.165
14	0.507	0.427	0.080
16	0.411	0.328	0.078
20	0.385	0.348	0.040
25	0.332	0.286	0.040

Catalysts	Conversion of IP/%	Selectivity/%
Catalysts	Conversion of IP/%	TMCH	TMOL
Cat-0	99.86	99.55	0.45
Cat-1	98.69	99.03	0.97
Cat-2	90.67	100	0
Cat-3	83.80	100	0
Cat-4	45.28	100	0

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Aluminium sulfate concentration/（g·L^-1）	Specific surface area/（m²·g^-1）	Pore volume/（cm³·g^-1）	Average pore diameter/nm
104	406	0.73	5.98
156	435	0.81	5.88
208	443	0.73	5.43
260	441	0.69	5.20
312	447	0.63	4.87

Aluminium sulfate concentration/（g·L^-1）	Specific surface area/（m²·g^-1）	Pore volume/（cm³·g^-1）	Average pore diameter/nm
104	406	0.73	5.98
156	435	0.81	5.88
208	443	0.73	5.43
260	441	0.69	5.20
312	447	0.63	4.87