论文总字数：21970字

摘 要

本课题以PdCl₂和1, 2-二(三乙氧基硅基)乙烷（BTESE）作为前驱体，通过溶胶-凝胶法制备出Pd掺杂的有机无机杂化SiO₂溶胶。然后采用浸浆法，把制得的溶胶涂覆在自制的γ-Al₂O₃支撑体上，凝胶化后分别在H₂、N₂、H₂ /N₂、Steam和Air的烧成气氛下制备出Pd掺杂的有机无机杂化SiO₂膜（PS膜）。利用XRD、TEM、N₂吸附-脱附(BET)、FT-IR等手段对Pd掺杂的有机无机杂化SiO₂粉体进行表征。结果表明：(1)不同的烧成氛围对Pd的存在状态是有影响的。(2)H₂-400、H₂/N₂-400粉体中金属Pd颗粒粒径分布范围较窄，Steam-400的较宽，可能和高温水蒸汽烧成氛围这一特殊的烧成氛围有关。(3)Air-400粉体性能明显区别于其他四类。

此外，在200 ^oC，0.3 MPa下对有机无机杂化SiO₂膜的单组分气体渗透性能进行测试。综合比较五种不同烧成氛围下得到的膜的气体渗透性能可以得到，Steam-400膜的气体渗透性能较好，其H₂渗透率达到2.47×10^-7 mol·m^-2·s^-1·Pa^-1，H₂/CO₂的理想分离子为9.18。因此证明了烧成气氛对PS膜的气体分离性能有影响。

关键词：Pd 有机无机杂化SiO₂膜 烧成氛围 气体渗透性能

Effects of sintering atmosphere on microstructure and gas permeance of palladium-doped organicsilica membranes

Abstract

A palladium-doped organicsilica sol was successfully synthesized by sol-gel method, 1, 2-bis (triethoxysilyl) ethane (BTESE) and Palladium chloride were used as the organicsilica precursors. The aforementioned sol was dip-coated on γ-Al₂O₃ mesoporous support. Subsequently, calcination process was conducted under five kinds of gas atmosphere (H₂、N₂、H₂ /N₂、Steam and Air). The properties of palladium-doped organic-inorganic hybrid silica powders were characterized by XRD、TEM、N₂ adsorption – desorption. Results showed that different sintering atmosphere is influential on Pd presence status. The size distributions of Pd in powders sintered in H₂ atmosphere and H₂/N₂ atmosphere were narrow, the steam-400 powder was the opposite, which may be related to the special sintering atmosphere. The gas permeance of powder fired in air is different from others.

In addition, single gas permeance of PS membrane was measured under 200 ^oC and 0.3 MPa. Gas permeance of palladium-doped organicsilica membranes sintered in steam was better than in other gas atmospheres. H₂ permeance of palladium-doped organicsilica membranes was 2.47×10^-7 mol·m^-2·s^-1·Pa^-1, while H₂/CO₂ permselectivity was 9.18. This proves that sintering atmosphere is influential on gas permeance of Palladium-doped organicsilica membranes.

Key Words: Palladium; Organicsilica membranes; sintering atmosphere; gas permeance

目 录

摘 要 I

Abstract II

第一章 文献综述 1

1.1 引言 1

1.2 制氢技术 1

1.3 膜分离 2

1.4 膜材料 3

1.5 Pd掺杂的有机无机杂化SiO₂膜的研究 4

1.6 烧成氛围对SiO₂膜的影响 6

1.7 论文研究目的及内容 7

第二章 实验部分 8

2.1 实验装置及试剂 8

2.1.1 实验装置流程图 8

2.1.2 实验仪器与试剂 8

2.2 Pd掺杂的有机无机杂化SiO₂聚合溶胶和粉体的制备 9

2.2.1 实验流程 9

2.2.2 溶胶、粉体及膜制备过程 10

2.3 Pd掺杂的有机无机杂化SiO₂聚合溶胶、粉体及膜的性能表征 11

2.3.1 溶胶表征过程 11

2.3.2 粉体表征过程 11

2.3.3 单组分气体渗透性能测试 11

第三章 结果与讨论 12

3.1 PS溶胶的表征 12

3.2 Pd掺杂的有机无机杂化SiO₂粉体的性能 12

3.2.1 金属Pd的存在状态 13

3.2.2 金属Pd的分散状态及粒径 13

3.2.3 烧成氛围对有机无机杂化SiO₂膜孔结构的影响 15

3.2.4 PS粉体的网络结构 16

3.3 PS膜的气体渗透性能 17

第四章 结论 20

参考文献 21

致 谢 25

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