氮掺杂柔性块体多孔碳的制备及对CO2/CH4的吸附分离研究

doi:10.11896/cldb.22050326

材料导报

2023, Vol. 37

Issue (22): 22050326-9 https://doi.org/10.11896/cldb.22050326

高分子与聚合物基复合材料

氮掺杂柔性块体多孔碳的制备及对CO₂/CH₄的吸附分离研究

王娅鸽¹, 王彬彬², 杨德威³, 李瑶^1,*

1 河南理工大学安全科学与工程学院,河南焦作 454003
2 河南理工大学材料科学与工程学院,河南焦作 454003
3 河南佰利新能源材料有限公司,河南焦作 454000

Nitrogen-doped Flexible Bulk Porous Carbon: Preparation and Application for CO₂/CH₄ Adsorption and Separation

WANG Yage¹, WANG Binbin², YANG Dewei³, LI Yao^1,*

1 College of Safety Science and Engineering, Henan Polytechnic University, Jiaozuo 454003, Henan, China
2 School of Materials Science and Engineering, Henan Polytechnic University, Jiaozuo 454003, Henan, China
3 Henan Baili New Energy Material Co., Ltd., Jiaozuo 454000, Henan, China

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摘要为开发一种用于CO₂/CH₄吸附和分离的经济、高效、工艺简单的块体多孔碳材料,选取三聚氰胺海绵块为前驱体物质,将其用作块体碳的支撑骨架,同时也作为氮源,引入葡萄糖作为二次碳源,以CO₂气体作为活化剂,经一步碳化-活化制备氮掺杂柔性块体多孔碳,并探讨葡萄糖负载量、活化温度及活化时间对多孔碳孔隙结构形成和化学成分的影响。测试结果表明:葡萄糖负载量为0.5 g、活化温度为800 ℃、活化时间为3 h时,所制备的样品有最大的比表面积(845 m²/g)、最高的总孔体积(0.37 cm³/g)以及最发达的微孔结构,其微孔体积高达0.30 cm³/g,占总孔体积的81%,超微孔体积高达0.26 cm³/g,占总孔体积的百分比高达70%。在25 ℃、0.1 MPa压力下,AMC-800-3展现出最优的CO₂吸附容量,可达2.84 mmol/g;根据亨利定律,利用低压(<0.015 MPa)下的吸附等温线起始斜率计算得出AMC-800-3对CO₂/CH₄的固有选择性系数为2.70,仅次于未活化样品;根据理想溶液吸附理论(IAST),在0.1 MPa压力下,AMC-800-3对二元混合气体CO₂/CH₄(50V/50V)的分离选择性系数为2.35,这主要归因于该样品所具有的优异的微孔结构和一定量氮的协同作用;通过动态穿透实验进一步测试了AMC-800-3对二元混合气体CO₂/CH₄(50V/50V)的选择性,结果与IAST计算相接近。本工作所制备的氮掺杂柔性块体多孔碳在减少碳排放、提高煤层气利用率等方面具有良好的应用前景。

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关键词: 氮掺杂柔性块体多孔碳 CO₂/CH₄吸附分离

Abstract: To develop an economical, efficient and simple prepared bulk porous carbon material for the adsorption and separation of CO₂/CH₄, melamine sponge was selected as both the precursor material for the support framework of bulk porous carbon and the nitrogen source. Glucose was introduced as a secondary carbon source, and CO₂ was used as an active agent to prepare nitrogen-doped flexible bulk porous carbon through one-step carbonization-activation method. The effects of glucose loading, activation temperature, and activation time on the porosity and chemical composition were discussed. The results indicated that at the glucose loading was 0.5 g, the activation temperature was 800 ℃, and the activation time was 3 h, the sample AMC-800-3 exhibited the largest specific surface area of 845 m²/g, the highest total volume of 0.37 cm³/g, and the most developed microporous structure. The micropore volume was up to 0.30 cm³/g, accounting for 81% of the total pore volume, and ultra-micropore volume was up to 0.26 cm³/g, accounting for 70% of the total pore volume. At 25 ℃ and 0.1 MPa, AMC-800-3 exhibited the highest CO₂ adsorption capacity of 2.84 mmol/g. According to Henry's law, the intrinsic selectivity of AMC-800-3 for CO₂/CH₄ calculated via the initial slope of the adsorption isotherm at low pressure (<0.015 MPa), was 2.70, which was the best of all the activated samples. According to ideal adsorption solution theory (IAST), the selectivity of AMC-800-3 for the equimolar binary mixture CO₂/CH₄ (50V/50V) was 2.35 at 0.1 MPa, which is attributed to the synergistic effect of the excellent microporous structure and a certain amount of nitrogen content. Under further dynamic breakthrough experiments, the dynamic selectivity result of AMC-800-3 for CO₂/CH₄ (50V/50V) was close to that calculated by IAST. Therefore, the as-prepared flexible nitrogen-doped bulk porous carbon is expected to be applicable for reducing carbon emissions and improving the utilization rate of coalbed methane.

Key words: nitrogen-doped flexible bulk porous carbon CO₂/CH₄ adsorptive separation

出版日期: 2023-11-25 发布日期: 2023-11-21

ZTFLH:

TE991

基金资助: 国家自然科学基金(42002164;U1804156);河南省自然科学基金(202300410171)

通讯作者: * 李瑶,河南理工大学讲师、硕士研究生导师。2005年毕业于沈阳师范大学获得学士学位,2008年毕业于东北师范大学获得硕士学位,2016年毕业于北京理工大学获得博士学位。主要从事多孔碳的设计、合成及煤层气的吸附分离研究。在国际期刊Carbon、Energy、Journal of Environmental Chemical Engineering等发表论文10余篇,出版专著1部,申请发明专利3项(授权2项)。leayao35@hpu.edu.cn

作者简介: 王娅鸽,2020年毕业于河南理工大学获得学士学位,河南理工大学安全科学与工程学院硕士研究生,主要研究方向为块体多孔碳的制备及CO₂/CH₄吸附分离。

引用本文:

王娅鸽, 王彬彬, 杨德威, 李瑶. 氮掺杂柔性块体多孔碳的制备及对CO₂/CH₄的吸附分离研究[J]. 材料导报, 2023, 37(22): 22050326-9.
WANG Yage, WANG Binbin, YANG Dewei, LI Yao. Nitrogen-doped Flexible Bulk Porous Carbon: Preparation and Application for CO₂/CH₄ Adsorption and Separation. Materials Reports, 2023, 37(22): 22050326-9.

链接本文:

http://www.mater-rep.com/CN/10.11896/cldb.22050326 或 http://www.mater-rep.com/CN/Y2023/V37/I22/22050326

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