论文总字数：24291字

摘 要

吸附式制冷技术以低品位热源为驱动力，采用环境友好型制冷剂，具有节能、环保等优势。金属有机骨架材料MIL-101具有比表面积大、水热稳定性强和循环稳定性好等优势，是吸附制冷领域最具应用前景的金属有机骨架材料之一。本文考察了分散液中MIL-101含量、粘结剂含量和单位滴加体积对吸附剂涂层机械强度的影响。在自建水热稳定性装置上测试MIL-101吸附剂涂层的长期循环稳定性。结果表明，当分散液中MIL-101含量为23%，粘结剂含量为25%，滴加体积为4 mL/dm²时，吸附剂涂层超声脱落率较少，吸附剂涂层的机械强度较强。粘结剂含量5%（MIL-101-5MP）和25%（MIL-101-25MP）的吸附剂涂层BET比表面积分别为2895 m²/g和2712 m²/g，比MIL-101下降24.6%和29.4%；MIL-101-5MP和MIL-101-25MP的孔容分别为1.67 cm³/g和1.28 cm³/g，与MIL-101相比分别下降14.4%和34.4%。吸附剂涂层MIL-101-5MP和MIL-101-25MP与MIL-101的脱附性能相近，对异丁烷的脱附峰顶温度为60 ℃，脱附完全温度约90 ℃。吸附剂涂层经过2000次水热稳定性测试后未发生脱落，具有良好的水热稳定性。

关键词：吸附制冷 MIL-101 涂层 机械强度

Works on Preparation and Hydrothermal Stability of MIL-101 Adsorbent Coating

Abstract

Adsorption cooling systems can be driven by the low-grade energy, without consumption for CFCs and electricity, which are energy-saving and environmentally friendly. As a metal-organic framework, MIL-101 has the advantages of large BET specific surface area, high hydrothermal stability and good cycling stability. Thus, MIL-101 has been considered as one of the most prominent adsorbents for adsorption refrigeration. In this work, mechanical properties of the adsorbent coatings were evaluated by rate of falling by ultrasound. The influences of MIL-101 content, binder content and the unit dropping volume on mechanical property were examined. Adsorbent coatings were prepared on stainless steel sheet by the slurry coating method. The adsorbent coating has a low ultrasound falling rate and good mechanical strength when the MIL-101 content is 23 wt%, binder content is 25 wt% and the dropping volume is 4 mL/dm². The BET specific surface area and pore volume of MIL-101-5MP and MIL-101-25MP are 2895 and 2712 m²/g respectively, which decrease by 24.6% and 29.4% compared with MIL-101. The pore volume of MIL-101-5MP and MIL-101-25MP are 1.67 and 1.28 cm³/g, which decrease by 14.4% and 34.4 % respectively. MIL-101-5MP and MIL-101-25MP have a similar desorption performance compared with MIL-101. The desorption peak temperature of isobutane on MIL-101 adsorbent coatings is 60 °C, and the desorption temperature is less than 90 °C. Hydrothermal stability of the MIL-101 adsorbent coatings subjected to 2000 adsorption cycles was success fully verified.

Key Words: Adsorption cooling; MIL-101; Adsorbent coating; Mechanical strength

目 录

摘 要 I

Abstract II

第一章 绪论 1

1.1 课题研究背景 1

1.2 吸附制冷基本原理 1

1.3 吸附制冷工质对 2

1.3.1 传统吸附制冷工质对 2

1.3.2 新型吸附制冷工质对 3

1.4 吸附剂涂层制备 4

1.5 本文主要研究内容 5

第二章 实验 7

2.1 主要原料及试剂 7

2.2 主要仪器和设备 7

2.3 MIL-101放大合成及纯化方法 7

2.3.1 MIL-101放大合成 7

2.3.2 MIL-101纯化方法 8

2.4 浆涂法制备吸附剂涂层 8

2.5 吸附剂涂层机械强度测试 8

2.6 MIL-101涂层结构表征 9

2.7 吸附剂涂层吸附等温线测定 9

2.8 吸附剂涂层水热稳定性测试 10

第三章 结果与讨论 12

3.1 浆涂法制备MIL-101涂层 12

3.1.1 分散液中MIL-101质量分数 12

3.1.2 粘结剂含量 14

3.1.3 单位滴加体积 16

3.2 MIL-101涂层结构表征 16

3.2.1 XRD物相分析 16

3.2.2 SEM形貌分析 17

3.2.3 BET比表面和孔结构分析 18

3.3 MIL-101涂层对异丁烷吸附/脱附性能 19

3.3.1 异丁烷在MIL-101涂层上的吸附等温线 19

3.3.2 MIL-101涂层对异丁烷脱附性能 20

3.4 吸附剂涂层水热稳定性 21

第四章 结论与展望 23

4.1 结论 23

4.2 展望 23

参考文献 25

致 谢 28

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