论文总字数：22262字

摘 要

随着全球工业发展，化石燃料的大量使用使得CO₂的排放量不断增加，全球温室效应愈加严重。氮掺杂多孔碳材料比表面积大、孔结构易调整，在CO₂吸附领域具有较好的应用前景。但是，在制备多孔碳材料过程中，传统碳源会大量蒸发或分解为气体产物，产率较低。通过直接高温焙烧聚离子液体能够高效制备出氮掺杂多孔碳材料，对CO₂捕集具有重要研究意义。

本文报道了一种以咪唑基聚离子液体(PILA)为理想碳源，醋酸锌(Zn(Ac)₂)为模板制备富氮多孔碳纳米片(NDPC)的方法。在热解过程中，不同Zn(Ac)₂的加入量可以调节多孔碳纳米片的孔结构。当Zn(Ac)₂/PILA的质量比x大于1时，NDPC-x出现分级多孔结构(微孔/中孔)，否则为微孔结构。此外，所制得的NDPC-x具有比表面积大(1008-1356m²·g⁻¹)以及N含量高(4.90-7.04wt .%)的优点。在25°C和1.0 bar下，NDPC-1的CO₂吸附量最高为56.74cm³·g⁻¹，是PILA未添加模板制得NCA的2.58倍。这主要是由于其较大的比表面积(1356m²·g⁻¹)、相对较高的N含量(6.48wt .%)和微孔/中孔的协同效应。

关键字：聚离子液体 醋酸锌 氮掺杂多孔碳材料 CO₂吸附

Preparation and CO₂ Adsorption Performance of Porous Carbon Material derived for Imidazolium poly(ionic liquids)

Abstract

With the development of global industry, the extensive use of fossil fuels has increased the emissions of CO₂, and Greenhouse Effect of the world has become more and more serious. Nitrogen-doped porous carbon materials have large specific surface area and easy adjustment of pore structure, so they have a good application prospect in the field of CO₂ adsorption. However, in the prepartion process of porous carbon materials, the traditional carbon source will evaporate or decompose into gas products, and lide to low yield . Nitrogen-doped precursor carbon materials can be prepared efficiently by calcination of poly(ionic liquids) at high temperature directly, which is of great significance for CO₂ trapping.

In this paper, a method for the preparation of nitrogen-rich porous carbon nanoparticles (NDPC) with imidazolium-bised poly(ionic liquids) (PILs) as ideal carbon source and zinc acetate (Zn(Ac)₂) as template has be reported. In the pyrolysis process, the pore structure of porous carbon nanosheets could be adjusted by different amount of Zn(Ac)₂. When the mass ratio of Zn(Ac)₂/PILA is greater than 1, the hierarchically porous structure (micropores/mesoporous) appears in NDPC-x, otherwise it is microporous structure. In addition, the prepared NDPC-x has the advantages of large specific surface areas (1008-1356m²·g^-1) and high N contents (4.90-7.04wt .%). At 25°C and 1.0bar, the highest CO₂ adsorption capacity of NDPC-1 was 56.74cm³·g⁻¹, which was 2.58 times higher that of NCA prepared by PILA without template. This is mainly due to the large specific surface areas (1356m²·g^-1), relatively high N contents (6.48wt .%) and synergistic effect of micropores/mesopores.

Key words: poly(ionic liquid);zinc acetate ; nitrogen dopingporous carbon material,;CO₂ adsorption

目 录

摘 要 I

Abstract II

第一章 文献综述 1

1.1 CO₂捕集技术研究进展 1

1.1.1 CO₂排放现状 1

1.1.2 CO₂捕集技术 1

1.2 CO₂吸附材料 2

1.3 聚离子液体 2

1.3.1 离子液体 2

1.3.2 聚离子液体 3

1.4 聚离子液体衍生多孔碳材料 5

1.5 研究内容及意义 7

第二章 实验部分 9

2.1 实验试剂及仪器 9

2.1.1 实验试剂 9

2.1.2 实验仪器 9

2.2离子液体衍生多孔碳材料制备 10

2.2.1 离子液体单体[C₄DVIM]Br₂的合成 10

2.2.2 聚离子液体材料的合成 10

2.2.3 氮掺杂多孔碳材料的合成 11

2.2.4 碳材料表征 11

2.2.5 CO₂吸附测量测定 12

第三章 结果及讨论 13

3.1 SEM与TEM分析 13

3.2 FT-IR光谱分析 14

3.3 XRD分析 14

3.4 Raman光谱分析 15

3.5 N₂吸附-脱附测试分析 16

3.6 元素分析 18

3.7 XPS分析 19

3.8 CO₂吸附等温线 20

3.9 CO₂吸附循环性能研究 21

第四章 结论与展望 23

4.1结论 23

4.2展望 23

参考文献 24

致谢 28

1. 文献综述

1.1 CO₂捕集技术研究进展

1.1.1 CO₂排放现状

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