论文总字数：19570字

摘 要

本文的研究内容为在四通道中空纤维氧化铝载体的外表面上通过晶种诱导，水热合成法制备得到B掺杂的DDR（B-DDR）分子筛膜。将B(硼)掺入分子筛的框架中以期减小分子筛的孔径来分离CO₂和H₂。经过XRD表征，发现随着合成液中Na₂B₄O₇的添加量的增加，衍射角向更大的2θ移动，表明B-DDR分子筛晶胞体积的减小。接着系统地考察了B的掺杂量、进料压力、进料摩尔比以及操作温度对CO₂/H₂双组分气体分离性能的影响。实验结果表明在Na₂B₄O₇的添加量的摩尔比为0.2时，CO₂/H₂的选择性达到最高为11.1；同时随着操作压力从1 bar增加到4 bar，选择性从8.6增加到11.9；选择性随着进料中CO₂的摩尔比的增加而先增加后减小，最大值为8，而当操作温度从298 K增673 K之间时，B-DDR分子筛膜由透CO₂变为透H₂。

关键词： B掺杂的DDR分子筛膜 低温臭氧活化 CO₂/H₂分离

Preparation and Separation of Hollow Fiber Boron Doped DDR Zeolite Membrane

ABSTRACT

The research of this paper was to prepare B-doped DDR (B-DDR) zeolite membrane by seed induction and hydrothermal synthesis on the outer surface of four-channel hollow fiber alumina support. B (boron) was incorporated into the framework of the zeolite to reduce the pore size of the zeolite to separate CO₂ and H₂. XRD results illustrated that as the additive amount of Na₂B₄O₇ in the synthetic solution increased, the diffraction angle shifted to a larger 2θ, indicating the decline of the cell volume of the B-DDR zeolite. Then, the effects of B additive amount, feed pressure, feed molar ratio and operating temperature on the separation performance of binary CO₂/H₂ mixture gas were systematically investigated. The results indicate that the separation selectivity of CO₂/H₂ achieved a maximum value of 11.1 when the molar ratio of Na₂B₄O₇ was 0.2; as the operating pressure raised from 1 bar to 4 bar the selectivity was up from 8.6 to 11.9; the selectivity firstly improved and then declined with a maximum value of 8 as the molar ratio of CO₂ enhanced. When the operating temperature increased from 298 K to 673 K, the B-DDR zeolite membrane changed from CO₂-selective to H₂-selective.

Key words：B doped DDR zeolite membrane; low temperature ozone activation; CO₂/H₂ separation;

目 录

摘 要 I

ABSTRACT II

第一章 文献综述 1

1.1 前言 1

1.2膜分离技术 2

1.2.1 气体分离膜简介 2

1.2.2 膜的分类 2

1.2.2.1有机膜 3

1.2.2.2无机膜 3

1.2.2.3混合基质膜 3

1.3分子筛膜 3

1.3.1简介 3

1.3.2 合成 4

1.4 DDR分子筛膜研究 5

1.4.1 DDR分子筛膜简介 5

1.4.2 DDR分子筛膜研究进展 5

1.5 B掺杂的分子筛膜研究进展 6

1.6 研究内容 7

第二章 实验部分 8

2.1实验试剂与仪器 8

2.2 Sigma-1分子筛 8

2.3 分子筛膜的制备 9

2.3.1 处理载体 9

2.3.2配制晶种液 9

2.3.3涂覆晶种 9

2.3.4合成液的配制 9

2.3.5 水热合成 10

2.3.6 低温臭氧煅烧脱除模板剂 10

2.4表征 11

2.4.1 XRD 11

2.4.2 BET 11

2.4.3 SEM 11

2.4.4 单组分气体 11

2.4.5 双组分气体 12

第三章 结果分析 13

3.1 XRD 13

3.2 BET 14

3.3 SEM 14

3.4单组分气体 15

3.5双组分气体 16

3.5.1 B的掺杂量 16

3.5.2 进料压力 16

3.5.3 进料摩尔比 17

3.5.4温度影响 18

第四章 结论与展望 20

4.1 结论 20

4.2 展望 20

参考文献 22

致 谢 26

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