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造核-包衣法制备Al2O3小球及其在丙烷直接脱氢反应中的应用研究
Study on preparation of spherical Al2O3 by nucleation-coating method and its application in propane dehydrogenation
- 低碳化学与化工 2024, 49(2): 49-59.
- 作者机构：
大连理工大学 化工学院 精细化工国家重点实验室，辽宁省低碳资源高值化利用国家重点实验室，辽宁 大连 116024
- 作者简介：
陈执（1998—），硕士，研究方向为氧化铝小球的制备工艺及其催化应用，E-mail：chenzhi0927@mail.dlut.edu.cn。
贺雷（1986—），博士，副教授，研究方向为低碳小分子催化转化，E-mail：helei@dlut.edu.cn；
陆安慧（1972—），博士，教授，研究方向为催化新材料的制备、多孔材料设计合成及规模化制备工艺等，E-mail：anhuilu@dlut.edu.cn。
- 基金信息：国家重点研发计划(2018YFA0209404;2021YFA1500300)
DOI：10.12434/j.issn.2097-2547.20230207
中图分类号： TQ426纸质出版日期：2024-02-25，
收稿日期：2023-06-10，
修回日期：2023-08-04，
- 稿件说明：
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陈执,吴凡,高新芊等.造核-包衣法制备Al2O3小球及其在丙烷直接脱氢反应中的应用研究[J].低碳化学与化工,2024,49(02):49-59.
CHEN Zhi,WU Fan,GAO Xinqian,et al.Study on preparation of spherical Al2O3 by nucleation-coating method and its application in propane dehydrogenation[J].Low-carbon Chemistry and Chemical Engineering,2024,49(02):49-59.
陈执,吴凡,高新芊等.造核-包衣法制备Al2O3小球及其在丙烷直接脱氢反应中的应用研究[J].低碳化学与化工,2024,49(02):49-59. DOI： 10.12434/j.issn.2097-2547.20230207.
CHEN Zhi,WU Fan,GAO Xinqian,et al.Study on preparation of spherical Al2O3 by nucleation-coating method and its application in propane dehydrogenation[J].Low-carbon Chemistry and Chemical Engineering,2024,49(02):49-59. DOI： 10.12434/j.issn.2097-2547.20230207.
摘要
氧化铝（Al
2
O
3
）载体是应用最广泛的催化剂的核心材料之一，而球形Al
2
O
3
载体取代条形Al
2
O
3
载体已成为大趋势，因此亟需发展绿色可行的制备球形Al
2
O
3
载体新方法。首先对滚球法进行了优化，以拟薄水铝石粉体为原料，硝酸为胶溶剂，羟丙基甲基纤维素为粘结剂，采用造核-包衣法制备了球形度好、强度高且比表面积大的Al
2
O
3
小球。结合X射线衍射（XRD）、扫描电子显微镜（SEM）等表征手段考察了水粉比（质量比）、酸粉比（质量比）、粘结剂含量（质量分数）和抛丸时间对Al
2
O
3
小球的强度和孔结构的影响。结果表明，控制酸粉比为0.050、水粉比为0.88、粘结剂含量为3%（质量分数）和每次抛丸时间为5 min，能够制备出粒径均匀、成品率高且强度高达43.0 N的Al
2
O
3
小球。在此基础上，制备了球形和粉末PtSn/Al
2
O
3
催化剂，并在温度为618 ℃、H
2
和C
3
H
8
流量分别为3.6 mL/min和6.0 mL/min的条件下应用于丙烷直接脱氢反应，发现球形PtSn/Al
2
O
3
催化剂表现出与粉末PtSn/Al
2
O
3
催化剂接近的反应活性和选择性。造核-包衣法是一种绿色高效的制备球形Al
2
O
3
载体的方法，可为球形Al
2
O
3
载体国产化提供新的思路。
Abstract
Aluminum oxide (Al
2
O
3
) support is one of the most widely used catalytic materials
and replacing linear Al
2
O
3
support with spherical Al
2
O
3
support has become a major trend
so it is urgent to develop novel green and feasible methods for producing spherical Al
2
O
3
support. Firstly
spherical Al
2
O
3
with excellent sphericity
high strength and large specific surface area was prepared by nucleation-coating method: using pseudo boehmite as the raw material
nitric acid as the peptiser and hydroxypropyl methyl cellulose as the binder to optimize the rolling ball method. The effects of water-powder ratio (mass ratio)
acid-powder ratio (mass ratio)
binder content (mass fraction) and blasting time on the strength and pore structure of spherical Al
2
O
3
were investigated by characterization methods such as X-ray diffraction (XRD) and scanning electron microscopy (SEM). The results show that spherical Al
2
O
3
with uniform particle size
high yield and high average compressive strength of 43.0 N can be prepared by controlling the acid-powder ratio of 0.050
water-powder ratio of 0.88
binder content of 3% (mass fraction) and blasting time of 5 min. Furthermore
spherical and powder PtSn/Al
2
O
3
catalysts were prepared and applied to propane dehydrogenation at 618 ℃
H
2
and C
3
H
8
flow rate of 3.6 mL/min and 6.0 mL/min
respectively. The spherical PtSn/Al
2
O
3
catalyst shows similar activity and selectivity as the powder PtSn/Al
2
O
3
catalyst. Nucleation-coating method is green an
d efficient to prepare spherical Al
2
O
3
support
which provides inspirations for localization of spherical Al
2
O
3
support.
关键词
Al2O3小球造核-包衣法Al2O3成型强度丙烷直接脱氢
Keywords
spherical Al2O3nucleation-coating methodAl2O3 moldingstrengthpropane dehydrogenation
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