• •
王清莲1,2(), 熊佩芸1, 韩俏飞1,4, 叶长燊1,2, 王红星3, 杨臣1,2(), 邱挺1,2()
收稿日期:
2024-05-23
修回日期:
2024-06-25
出版日期:
2024-07-05
通讯作者:
杨臣,邱挺
作者简介:
王清莲(1989—),女,博士,wqlian@fzu.edu.cn
基金资助:
Qinglian WANG1,2(), Peiyun XIONG1, Qiaofei HAN1,4, changshen YE1,2, Chen YANG3, ting QIU1,2()
Received:
2024-05-23
Revised:
2024-06-25
Online:
2024-07-05
Contact:
ting QIU
摘要:
本研究在聚多巴胺辅助二次生长法制备负载型催化填料(SCP)基础上,通过多次晶化及碱处理协同改性,开发了高性能SCP制备方法。研究结果表明,SCP的活性组分层负载量随晶化次数增加而线性增长,但过密的活性组分层结构限制了活性位点的利用。四甲基氢氧化铵(TMAOH)处理通过溶解硅原子形成介孔,提高了外比表面积和扩散效率,增强了SCP的催化活性和焦炭容纳能力。在优化的改性条件下,即晶化次数为3次、TMAOH溶液浓度为0.05 mol/L、碱处理温度为80 ℃、碱处理时间为120 min,SCP活性提升3.74倍。尽管SCP在乙酸环己酯合成中活性有所下降,但通过焙烧再生可恢复活性。环己烯高温聚合产生的积炭是活性降低的主要原因。
中图分类号:
王清莲, 熊佩芸, 韩俏飞, 叶长燊, 王红星, 杨臣, 邱挺. 高性能负载型催化填料的制备及其性能研究[J]. 化工学报, DOI: 10.11949/0438-1157.20240548.
Qinglian WANG, Peiyun XIONG, Qiaofei HAN, changshen YE, Chen YANG, ting QIU. Preparation and performance investigation of high-performance supported catalytic packing[J]. CIESC Journal, DOI: 10.11949/0438-1157.20240548.
SCP | Smicro① /(m2·g-1) | Sext② /(m2·g-1) | SBET③ / (m2·g-1) | Vmicro④ / (cm3·g-1) | Vmeso⑤ /(cm3·g-1) |
---|---|---|---|---|---|
SCP-PDA-3 | 49.5 | 47.9 | 97.5 | 0.0312 | 0.0102 |
SCP-PDA-3-T | 37.9 | 66.3 | 104.2 | 0.0302 | 0.0114 |
表1 SCP-PDA-3和SCP-PDA-3-T的结构特性
Table 1 Textural properties of SCP-PDA-3 and SCP-PDA-3-T
SCP | Smicro① /(m2·g-1) | Sext② /(m2·g-1) | SBET③ / (m2·g-1) | Vmicro④ / (cm3·g-1) | Vmeso⑤ /(cm3·g-1) |
---|---|---|---|---|---|
SCP-PDA-3 | 49.5 | 47.9 | 97.5 | 0.0312 | 0.0102 |
SCP-PDA-3-T | 37.9 | 66.3 | 104.2 | 0.0302 | 0.0114 |
图10 SCP在间歇稳定性实验前后及焙烧再生后的N2吸-脱附等温线
Fig.10 N2 adsorption and desorption isotherms of SCPs before and after stability tests and after roasting regeneration
SCP | Smicro① / (m2·g-1) | Sext②/ (m2·g-1) | SBET③ /(m2·g-1) | Vmicro④ / (cm3·g-1) | Vmeso⑤ / (cm3·g-1) |
---|---|---|---|---|---|
SCP-PDA-3 | 45.5 | 34.6 | 80.1 | 0.0255 | 0.0071 |
SCP-PDA-3-U | 40.8 | 6.6 | 47.3 | 0.0181 | 0.0025 |
SCP-PDA-3-R | 46.3 | 36.4 | 82.7 | 0.0264 | 0.0076 |
SCP-PDA-3-T | 39.0 | 46.5 | 85.5 | 0.0247 | 0.0082 |
SCP-PDA-3-T-U | 38.1 | 17.2 | 55.6 | 0.0195 | 0.0065 |
SCP-PDA-3-T-R | 37.2 | 43.2 | 80.4 | 0.0232 | 0.0081 |
表2 SCP-PDA-3与SCP-PDA-3-T的结构特性
Table. 2 Textural properties of SCP-PDA-3 and SCP-PDA-3-T
SCP | Smicro① / (m2·g-1) | Sext②/ (m2·g-1) | SBET③ /(m2·g-1) | Vmicro④ / (cm3·g-1) | Vmeso⑤ / (cm3·g-1) |
---|---|---|---|---|---|
SCP-PDA-3 | 45.5 | 34.6 | 80.1 | 0.0255 | 0.0071 |
SCP-PDA-3-U | 40.8 | 6.6 | 47.3 | 0.0181 | 0.0025 |
SCP-PDA-3-R | 46.3 | 36.4 | 82.7 | 0.0264 | 0.0076 |
SCP-PDA-3-T | 39.0 | 46.5 | 85.5 | 0.0247 | 0.0082 |
SCP-PDA-3-T-U | 38.1 | 17.2 | 55.6 | 0.0195 | 0.0065 |
SCP-PDA-3-T-R | 37.2 | 43.2 | 80.4 | 0.0232 | 0.0081 |
图14 SCP-PDA-3-T在乙酸与乙醇酯化反应体系重复性实验前后的N2吸-脱附等温线
Fig. 14 N2 adsorption and desorption isotherms of SCP-PDA-3-T before and after the reusability test in esterification of acetic acid with ethanol
图15 SCP-PDA-3-T在乙酸与乙醇酯化反应中重复性实验前后的实物(左)及SEM照片(右)
Fig. 15 Pictures (left) and SEM (right) images of SCP-PDA-3-T before and after the reusability test in esterification of acetic acid with ethanol
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