Preparation and performance of carbon supported potassium-based CO2 adsorbent derived from hyper-cross linked polymers

doi:10.16085/j.issn.1000-6613.2022-2305

Abstract

Abstract:

In view of the significant demand for reducing the cost of carbon capture and the key problem of developing high-performance adsorbents, a new carbon supported potassium-based CO₂ adsorbent was prepared from a polymer precursor derived from Friedel Crafts alkylation between benzene and dimethyl acetal. By means of solid nuclear magnetic resonance, infrared spectroscopy, electron microscopy, X-ray powder diffraction, N₂ physical adsorption and other characterization methods, it was found that the synthesized polymer precursor had a hyper-crosslinked porous structure, and the modification of a variety of oxygen-containing functional groups could be achieved by surface oxidation modification. These oxygen-containing functional groups had the function of anchoring potassium ions, and thus the surface potassium modification can be achieved by ion exchange. After further high-temperature carbonization, a new carbon supported potassium-based CO₂ adsorbent can be obtained. The potassium sites on the adsorbent had good dispersibility and could react reversibly with CO₂. The CO₂ adsorption capacity of the adsorbent under the simulated flue gas reached 1.63mmol/g with good cyclic stability, which endowed the adsorbent with promising application potential.

Key words: carbon dioxide, capture, carbon materials, emission reduction, carbon neutrality

摘要：

面向降低碳捕集技术成本的重大需求，针对高性能吸附剂开发这一关键问题，以廉价的苯为原料，基于Friedel-Crafts烷基化反应，以二甲醇缩甲醛为交联剂合成了聚合物材料，将其作为前体制备了一种新的碳载钾基CO₂吸附剂。通过固体核磁、红外光谱、电子显微镜、X射线粉末衍射、N₂物理吸附等表征手段，发现所合成的聚合物前体具有超交联多孔结构，通过表面氧化改性的方法可实现多种含氧官能团的修饰，这些含氧官能团具有锚定钾离子的作用，因此可通过离子交换的方式实现表面的钾改性。经过进一步的高温炭化后，可获取全新的碳载钾基CO₂吸附剂。该类吸附剂上的含钾位点具有较好的分散性，能够与CO₂发生可逆化学反应，其在模拟烟气下的CO₂吸附量达到了1.63mmol/g，且循环稳定性良好，具有一定的应用潜力。

关键词: 二氧化碳, 捕集, 碳材料, 减排, 碳中和

CLC Number:

O647.3

CHEN Chongming, ZENG Siming, LUO Xiaona, SONG Guosheng, HAN Zhongge, YU Jinxing, SUN Nannan. Preparation and performance of carbon supported potassium-based CO₂ adsorbent derived from hyper-cross linked polymers[J]. Chemical Industry and Engineering Progress, 2023, 42(3): 1540-1550.

陈崇明, 曾四鸣, 罗小娜, 宋国升, 韩忠阁, 郁金星, 孙楠楠. 基于超交联聚合物前体的碳载钾基CO₂吸附剂制备和性能[J]. 化工进展, 2023, 42(3): 1540-1550.

Figures/Tables 11

References 58

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样品	比表面积/m²·g^-1	微孔比表面积/m²·g^-1	总孔容/cm³·g^-1	微孔孔容/cm³·g^-1	平均孔径/nm	钾质量分数/%
HCP	1186	268	1.634	0.123	0.63	—
HCP-Ox	519	243	0.391	0.102	0.61	—
HCP-K	8	7	0.016	0.003	0.96	6.54
HCP-K650	16	23	0.012	0.008	0.96	14.42
HCP-K750	70	68	0.033	0.026	0.60	18.22
HCP-K850	46	41	0.030	0.016	0.73	21.31

样品	比表面积/m²·g^-1	微孔比表面积/m²·g^-1	总孔容/cm³·g^-1	微孔孔容/cm³·g^-1	平均孔径/nm	钾质量分数/%
HCP	1186	268	1.634	0.123	0.63	—
HCP-Ox	519	243	0.391	0.102	0.61	—
HCP-K	8	7	0.016	0.003	0.96	6.54
HCP-K650	16	23	0.012	0.008	0.96	14.42
HCP-K750	70	68	0.033	0.026	0.60	18.22
HCP-K850	46	41	0.030	0.016	0.73	21.31

样品	40℃下CO₂的吸附量/mmol·g^-1
样品	体积分数15% CO₂/N₂	纯CO₂
HCP	0.83	3.33
HCP-Ox	0.92	3.59
HCP-K	1.13	3.82
HCP-K650	6.14	13.03
HCP-K750	8.89	13.14
HCP-K850	7.38	12.60

样品	40℃下CO₂的吸附量/mmol·g^-1
样品	体积分数15% CO₂/N₂	纯CO₂
HCP	0.83	3.33
HCP-Ox	0.92	3.59
HCP-K	1.13	3.82
HCP-K650	6.14	13.03
HCP-K750	8.89	13.14
HCP-K850	7.38	12.60

样品	温度/℃	CO₂分压/bar	吸附量/mmol·g^-1	测试方法	参考文献
SNS-20	50	0.15	1.15	吸附等温线	[34]
SAC	40	0.15	0.85	吸附等温线	[39]
p-2-973-1.5	50	0.15	1.20	吸附等温线	[40]
C@MF-700	50	0.15	1.30	吸附等温线	[41]
NC-1-500	35	0.15	1.10	热重分析	[42]
RN-450-3	25	0.10	0.94	穿透曲线	[43]
PGC-K	27	0.17	1.10	穿透曲线	[44]
ClCTF-1-650	25	0.10	0.68	穿透曲线	[45]
NGC-650-4	25	0.10	0.84	穿透曲线	[46]
3D-MPCFW-11-18	45	0.15	1.05	吸附等温线	[47]
OTS-1-550	25	0.20	1.51	穿透曲线	[48]
CTS-NaNH₂(1:1)-700	40	0.15	0.60	吸附等温线	[49]
KNC-1-800	40	0.15	1.12	吸附等温线	[50]
ACDES 9	45	0.10	0.49	穿透曲线	[51]
PSK-2-650	40	0.15	1.01	穿透曲线	[52]
HCP-K750	40	0.15	2.02	热重分析	本文
HCP-K750	40	0.15	1.63	穿透曲线	本文

Preparation and performance of carbon supported potassium-based CO₂ adsorbent derived from hyper-cross linked polymers

基于超交联聚合物前体的碳载钾基CO₂吸附剂制备和性能

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Figures/Tables 11

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模式	烟气状态	是否预处理	循环数	进气流速 /mL·min^-1	吸附量 /mmol·g^-1
模式A	干燥烟气	否	1	100	0.37
			2	100	0.38
			3	50	0.48
模式B	潮湿烟气	否	4	100	0.37
			5	100	0.53
			6	100	0.56
模式C	潮湿烟气	是	7	100	1.53
			8	100	1.56
			9	100	1.57
			10	100	1.60
			11	100	1.63

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