无机盐工业 ›› 2021, Vol. 53 ›› Issue (2): 94-99.doi: 10.11962/1006-4990.2020-0110
收稿日期:
2020-08-27
出版日期:
2021-02-10
发布日期:
2021-02-06
作者简介:
余天华(1973— ),男,副教授,博士,主要研究方向为多项催化;E-mail: 基金资助:
Yu Tianhua(),Huang Qipeng,Situ Cheng
Received:
2020-08-27
Online:
2021-02-10
Published:
2021-02-06
摘要:
以十六烷基三甲基溴化铵(CTAB)为模板剂,采用溶胶凝胶法合成具有介孔的S-1载体(MS-1),浸渍法制备Cu/MS-1催化剂,用于以双氧水为氧化剂、苯酚直接羟基化合成苯二酚的反应,运用正交实验法[L25(56)]对反应条件进行优化。使用X射线电子能谱(XPS)、N2的等温吸附-脱附和 H2的程序升温还原等方法对催化剂的结构和性能做了表征。结果表明:具有介孔的Cu/MS-1有利于反应物和生成物的快速扩散,催化性能明显优于Cu/S-1;高分散CuO相对质量分数最高的5.5% Cu/MS-1的催化活性最好,在优化条件下,苯二酚的产率达到47.2%,选择性为86.7%。具有介孔和MFI结构的Cu/MS-1稳定性强,重复使用5次后,苯二酚的产率仍达43.2%。
中图分类号:
余天华,黄启朋,司徒成. 介孔Cu/MS-1催化羟基化苯酚合成苯二酚[J]. 无机盐工业, 2021, 53(2): 94-99.
Yu Tianhua,Huang Qipeng,Situ Cheng. Synthesis of dihydroxybenzenes by hydroxylation of phenol over Cu/ MS-1 with mesoporous[J]. Inorganic Chemicals Industry, 2021, 53(2): 94-99.
表3
苯酚直接羟基化生成苯二酚实验条件优化结果
实验 编号 | 因素 | 苯二酚 产率/% | |||||
---|---|---|---|---|---|---|---|
A | B | C | D | E | F | ||
1 | 1 | 1 | 1 | 1 | 1 | 1 | 5.6 |
2 | 1 | 2 | 2 | 2 | 2 | 2 | 15.2 |
3 | 1 | 3 | 3 | 3 | 3 | 3 | 26.4 |
4 | 1 | 4 | 4 | 4 | 4 | 4 | 19.1 |
5 | 1 | 5 | 5 | 5 | 5 | 5 | 8.2 |
6 | 2 | 1 | 2 | 3 | 4 | 5 | 20.9 |
7 | 2 | 2 | 3 | 4 | 5 | 1 | 10.6 |
8 | 2 | 3 | 4 | 5 | 1 | 2 | 15.5 |
9 | 2 | 4 | 5 | 1 | 2 | 3 | 10.8 |
10 | 2 | 5 | 1 | 2 | 3 | 4 | 13.5 |
11 | 3 | 1 | 3 | 5 | 2 | 4 | 11.2 |
12 | 3 | 2 | 4 | 1 | 3 | 5 | 16.5 |
13 | 3 | 3 | 5 | 2 | 4 | 1 | 14.5 |
14 | 3 | 4 | 1 | 3 | 5 | 2 | 9.5 |
15 | 3 | 5 | 2 | 4 | 1 | 3 | 20.5 |
16 | 4 | 1 | 4 | 2 | 5 | 3 | 24.8 |
17 | 4 | 2 | 5 | 3 | 1 | 4 | 35.8 |
18 | 4 | 3 | 1 | 4 | 2 | 5 | 43.7 |
19 | 4 | 4 | 3 | 5 | 3 | 1 | 6.2 |
20 | 4 | 5 | 2 | 1 | 4 | 2 | 9.2 |
21 | 5 | 1 | 5 | 4 | 3 | 2 | 15.7 |
22 | 5 | 2 | 1 | 5 | 4 | 3 | 5.6 |
23 | 5 | 3 | 2 | 1 | 5 | 4 | 20.2 |
24 | 5 | 4 | 3 | 2 | 2 | 5 | 17.2 |
25 | 5 | 5 | 4 | 3 | 1 | 1 | 9.1 |
K1 | 74.5 | 78.2 | 77.9 | 62.3 | 86.5 | 46.0 | ∑Ki=405.5 |
K2 | 71.3 | 83.7 | 86.0 | 85.2 | 98.1 | 65.1 | |
K3 | 72.2 | 120.3 | 71.6 | 101.7 | 78.3 | 88.1 | |
K4 | 119.7 | 62.8 | 85.0 | 109.6 | 69.3 | 99.8 | |
K5 | 67.8 | 60.5 | 85.0 | 46.7 | 73.3 | 106.5 | |
K1/5 | 14.9 | 15.6 | 15.6 | 12.5 | 17.3 | 9.2 | |
K2/5 | 14.3 | 16.7 | 17.2 | 17.0 | 19.6 | 13.0 | |
K3/5 | 14.4 | 24.1 | 14.3 | 20.3 | 15.7 | 17.6 | |
K4/5 | 23.9 | 12.6 | 17.0 | 21.9 | 13.9 | 20.0 | |
K5/5 | 13.6 | 12.1 | 17.0 | 9.3 | 14.7 | 21.3 | |
R | 10.3 | 12.0 | 3.1 | 12.6 | 5.7 | 12.1 |
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