木质素浸渍柚子皮生物炭吸附CO2特性

doi:10.16085/j.issn.1000-6613.2023-0143

摘要/Abstract

摘要：

吸附剂的孔隙结构在CO₂捕集过程中起着重要作用。本文为提高生物炭吸附性能，以木质素为前体，采用浸渍法调变了生物炭孔隙结构，并研究了其吸附CO₂特性。结果表明，木质素浸渍后生物炭的比表面积、微孔体积以及碱度分别提高了3.7倍、8.3倍与1.6倍，CO₂吸附容量从43.15mg/g提升至47.36mg/g；线性相关分析表明，比表面积、微孔体积与碱度是决定CO₂吸附容量的关键因素。Avrami模型和Langmuir模型能够较好地拟合生物炭对CO₂的吸附过程，表明该吸附由物理与化学机理共同作用，且以单层吸附为主。当吸附温度由0℃升高至25℃，吸附量降低了46.5%~52.7%，CO₂在生物炭上的吸附为放热过程。10次吸附/解吸循环后，生物炭具有高达97.3%~99.3%的重复利用率，表明浸渍生物炭具有良好的可重复使用性，是一种具有潜力的CO₂吸附剂。

关键词: 生物炭, 二氧化碳捕集, 木质素, 浸渍

Abstract:

The pore structure of adsorbent plays an important role in the process of CO₂ capture. In order to improve the adsorption performance of biochar, the pore structure of biochar was modified by impregnation method using lignin as precursor, and the adsorption properties of CO₂ were studied. The results showed that the specific surface area, micropore volume and alkalinity of biochar after lignin impregnation were increased by 3.7 times, 8.3 times and 1.6 times, respectively, and the CO₂adsorption capacity was increased from 43.15mg/g to 47.36mg/g. The linear correlation analysis showed that specific surface area, micropore volume and alkalinity were the key factors to determine the adsorption capacity of CO₂. The Avrami model and Langmuir model could well fit the adsorption process of CO₂ by biochar, which indicates that the adsorption was mainly monolayer adsorption with the combined action of physical and chemical mechanisms. When the adsorption temperature increased from 0℃ to 25℃, the adsorption capacity decreases by 46.5%—52.7%, and the adsorption of CO₂ on biochar is an exothermic process. After 10 adsorption/desorption cycles, the biochar had a high reuse rate of 97.3%—99.3%, indicating that the impregnated biochar had good reusability and was a potential CO₂ adsorbent.

Key words: biochar, CO₂ capture, lignin, impregnation

中图分类号:

X511

戴欢涛, 曹苓玉, 游新秀, 徐浩亮, 汪涛, 项玮, 张学杨. 木质素浸渍柚子皮生物炭吸附CO₂特性[J]. 化工进展, 2023, 42(S1): 356-363.

DAI Huantao, CAO Lingyu, YOU Xinxiu, XU Haoliang, WANG Tao, XIANG Wei, ZHANG Xueyang. Adsorption properties of CO₂ on pomelo peel biochar impregnated by lignin[J]. Chemical Industry and Engineering Progress, 2023, 42(S1): 356-363.

图/表 9

表1 生物炭理化特征

生物碳名称	比表面积/m²·g^-1	总孔体积/cm³·g^-1	微孔体积/cm³·g^-1	平均孔径/nm	灰分/%	碱度/mmol·g^-1	产率/%
MNa600	19.38	0.0503	0.0083	5.20	24.5	1.32	47.2
MY1.5	13.11	0.0163	0.0054	2.48	12.6	0.74	79.6
MY3	36.98	0.0462	0.0166	2.50	12.8	0.58	87.1
MY5	35.17	0.0405	0.0159	2.30	5.1	0.61	89.5
MY10	47.82	0.0409	0.0215	1.71	6.4	0.53	91.8
MY15	51.15	0.0592	0.0207	2.31	8.4	0.56	91.8
YZP600	13.95	0.0213	0.0025	3.06	5.6	0.45	28.1

图1 生物炭孔径分布、X射线衍射、傅里叶红外光谱

图2 生物炭对CO2的吸附量

图3 生物炭指标与CO2吸附的关系

表2 吸附剂25℃对CO2的吸附动力学参数表

生物炭名称	伪一级动力学模型 $q t = q e 1 - e - k 1 t$			伪二级动力学模型 $q t = k 2 ⋅ q e 2 ⋅ t 1 + k 2 ⋅ q e ⋅ t$			Avrami 模型 $q t = q e 1 - e - k A t n A$				实验吸附量 /mg·g^-1
生物炭名称	q_e/mg·g^-1	k₁/min^-1	R²	q_e/mg·g^-1	k₂/g·mg^-1·min^-1	R²	q_e/mg·g^-1	k_A/min^-1	n_A	R²	实验吸附量 /mg·g^-1
MY1.5	41.59	0.7325	0.9492	44.14	0.0273	0.9561	41.77	0.7262	0.8697	0.9515	42.93
MY3	44.44	0.9203	0.9520	46.68	0.0337	0.9283	44.32	0.9300	1.1780	0.9544	45.51
MY5	43.70	0.8264	0.9510	46.12	0.0301	0.9453	43.72	0.8251	0.9788	0.9510	44.95
MY10	45.28	0.8383	0.9433	47.80	0.0292	0.9450	45.34	0.8348	0.9503	0.9435	46.84
MY15	45.95	0.8984	0.9479	48.35	0.0314	0.9351	45.88	0.9036	1.0890	0.9485	47.36
YZP600	41.18	0.6874	0.9352	43.91	0.0251	0.9615	41.63	0.6720	0.7663	0.9438	43.15

表2 吸附剂25℃对CO2的吸附动力学参数表

生物炭名称	伪一级动力学模型 $q t = q e 1 - e - k 1 t$			伪二级动力学模型 $q t = k 2 ⋅ q e 2 ⋅ t 1 + k 2 ⋅ q e ⋅ t$			Avrami 模型 $q t = q e 1 - e - k A t n A$				实验吸附量 /mg·g^-1
生物炭名称	q_e/mg·g^-1	k₁/min^-1	R²	q_e/mg·g^-1	k₂/g·mg^-1·min^-1	R²	q_e/mg·g^-1	k_A/min^-1	n_A	R²	实验吸附量 /mg·g^-1
MY1.5	41.59	0.7325	0.9492	44.14	0.0273	0.9561	41.77	0.7262	0.8697	0.9515	42.93
MY3	44.44	0.9203	0.9520	46.68	0.0337	0.9283	44.32	0.9300	1.1780	0.9544	45.51
MY5	43.70	0.8264	0.9510	46.12	0.0301	0.9453	43.72	0.8251	0.9788	0.9510	44.95
MY10	45.28	0.8383	0.9433	47.80	0.0292	0.9450	45.34	0.8348	0.9503	0.9435	46.84
MY15	45.95	0.8984	0.9479	48.35	0.0314	0.9351	45.88	0.9036	1.0890	0.9485	47.36
YZP600	41.18	0.6874	0.9352	43.91	0.0251	0.9615	41.63	0.6720	0.7663	0.9438	43.15

图4 生物炭在25℃的吸附动力学拟合曲线

表3 吸附剂0℃吸附CO2等温线参数

生物炭名称	Langmuir模型 $q t = q e K l p e / 1 + K l p e$			Freundlich模型 $q t = K f p e 1 / n$
生物炭名称	q_e/mg·g^-1	K_l/kPa^-1	R²	n	K_f/mg·g^-1·(kPa^1/ⁿ )^-1	R²
MNa600	89.81	0.0468	0.9846	2.6319	13.53	0.9914
MY1.5	92.33	0.0586	0.9894	2.7880	16.08	0.9829
MY3	109.87	0.0503	0.9882	2.6406	16.98	0.9880
MY5	97.69	0.0601	0.9901	2.8151	17.35	0.9815
MY10	98.44	0.0609	0.9891	2.8220	17.61	0.9829
MY15	114.66	0.0514	0.9873	2.6579	18.01	0.9885
YZP600	99.67	0.0694	0.9859	3.0149	20.11	0.9806

表3 吸附剂0℃吸附CO2等温线参数

生物炭名称	Langmuir模型 $q t = q e K l p e / 1 + K l p e$			Freundlich模型 $q t = K f p e 1 / n$
生物炭名称	q_e/mg·g^-1	K_l/kPa^-1	R²	n	K_f/mg·g^-1·(kPa^1/ⁿ )^-1	R²
MNa600	89.81	0.0468	0.9846	2.6319	13.53	0.9914
MY1.5	92.33	0.0586	0.9894	2.7880	16.08	0.9829
MY3	109.87	0.0503	0.9882	2.6406	16.98	0.9880
MY5	97.69	0.0601	0.9901	2.8151	17.35	0.9815
MY10	98.44	0.0609	0.9891	2.8220	17.61	0.9829
MY15	114.66	0.0514	0.9873	2.6579	18.01	0.9885
YZP600	99.67	0.0694	0.9859	3.0149	20.11	0.9806

图5 吸附等温拟合曲线

图6 生物炭对CO2的重复利用实验及重复利用效率

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木质素浸渍柚子皮生物炭吸附CO₂特性

Adsorption properties of CO₂ on pomelo peel biochar impregnated by lignin

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