| 廖正坤,迪丽努尔·艾力,方亚平,苗聪慧,艾沙·努拉洪.钾改性对Au/ZSM-5催化剂上正丁烷裂解性能的影响[J].分子催化,2023,37(2):118-129 |
| 钾改性对Au/ZSM-5催化剂上正丁烷裂解性能的影响 |
| Effect of K+ Modified Au/ZSM-5 Zeolite Catalyst on Cracking Performance of n-Butane |
| 投稿时间：2022-07-21 修订日期：2022-10-25 |
| DOI：10.16084/j.issn1001-3555.2023.02.002 |
| 中文关键词: HZSM-5 正丁烷裂解 Au/HZSM-5 K修饰 |
| 英文关键词:HZSM-5 n-butane cleavage Au/HZSM-5 K modifications |
| 基金项目:2022年自治区自然科学基金面上项目(联合基金2022D01c378) |
| 作者 | 单位 | E-mail | | 廖正坤 | 新疆大学 化工学院省部共建碳基能源资源化学与利用国家重点实验室, 新疆煤碳清洁转化与化工过程重点实验室, 新疆 乌鲁木齐 830017 | | | 迪丽努尔·艾力 | 新疆大学 化工学院省部共建碳基能源资源化学与利用国家重点实验室, 新疆煤碳清洁转化与化工过程重点实验室, 新疆 乌鲁木齐 830017 | | | 方亚平 | 新疆大学 化工学院省部共建碳基能源资源化学与利用国家重点实验室, 新疆煤碳清洁转化与化工过程重点实验室, 新疆 乌鲁木齐 830017 | | | 苗聪慧 | 新疆大学 化工学院省部共建碳基能源资源化学与利用国家重点实验室, 新疆煤碳清洁转化与化工过程重点实验室, 新疆 乌鲁木齐 830017 | | | 艾沙·努拉洪 | 新疆大学 化工学院省部共建碳基能源资源化学与利用国家重点实验室, 新疆煤碳清洁转化与化工过程重点实验室, 新疆 乌鲁木齐 830017 | aisa705@163.com |
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| 中文摘要: |
| 采用负压沉积沉淀法制备了负载型Au/HZSM-5催化剂, 采用X射线衍射(XRD)、 透射电镜(TEM)、 Ｘ射线光电子能谱(XPS)、 NH3-TPD、 紫外可见漫反射(UV-Vis)等技术对催化剂进行了表征分析, 并考察了催化剂对正丁烷裂解性能的影响. 结果表明, Au金属成功负载到HZSM-5催化剂上, 并且金颗粒的尺寸受负载量的影响, 其中1.0%Au/HZSM-5催化剂中的金颗粒粒径最小, 约为5～10 nm. 钾离子作为一种碱性离子可以调节载体酸性, 随着K离子的引入xK-Au/HZSM-5催化剂的酸性逐渐降低, 使Au0的电子结合能更高. 相较于HZSM-5, 2.0Au/HZSM-5催化剂对于正丁烷的转化率从13.1%提升到了37.5%, 对丙烯的选择性从17.2%提升到了52.5%. 随着K离子的引入, 催化剂对于丁烯以及异丁烷的选择性有所提高, 当K离子负荷为0.08%时, 对丁烯的选择性从3.8%提高到36.9%, 负荷为0.1%时, 对异丁烷的选择性由2.8%提升到51.8%. 但原料转化率低于2.0Au/HZSM-5的, 这可能与K的加入降低催化剂酸改性有关. 此外通过研究Au/HZSM-5用K+修饰得知, Au+离子是Au/HZSM-5催化剂转化正丁烷的主要活性中心. |
| 英文摘要: |
| Negative pressure deposition method was used for the preparation of a supported Au/HZSM-5 catalyst. The supported Au/HZSM-5 catalysts were prepared by negative pressure deposition and precipitation method. The catalysts were characterized and analyzed by X-ray diffraction (XRD), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), NH3-TPD, UV-Vis and other technologies. The effect of catalyst on cracking performance of n-butane was also investigated. The results show that Au is successfully loaded onto the HZSM-5 catalyst, and the size of Au particles is affected by the load. The particle size of Au particles of 1.0 Au/HZSM-5 catalyst is the smallest, which is about 5~10 nm. Potassium ion as a kind of basic ion can regulate the carrier acidity, with the introduction of K ions, the acidity of xK-Au/HZSM-5 catalyst is gradually reduce, and the electron binding energy of Au0 is higher. Compared with HZSM-5, the conversion rate of n-butane for 2.0Au/HZSM-5 catalyst increased from 13.1% to 37.5%. The selectivity for propylene increased from 17.2% to 52.5%. With the introduction of K ion, the selectivity of butene and isobutane was improved. When the K ion load was 0.08%, the selectivity of butene increased from 3.8% to 36.9%, and when the K ion load was 0.10%, the selectivity of isobutane increased from 2.8% to 51.8%. However, the conversion rate of raw materials is lower than 2.0Au/HZSM-5, which may be related to the fact that the addition of K reduces the acid modification of catalyst. In addition, the K+ modification of Au/HZSM-5 revealed that Au+ ion was the main active center of n-butane conversion by Au/HZSM-5 catalyst. |
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