植物基活性炭的制备及吸附应用研究进展

doi:10.16085/j.issn.1000-6613.2019-0093

摘要/Abstract

摘要：

从植物基活性炭的制备及其吸附应用两个部分对国内外的研究进行了综述。介绍了不同生物质原料对活性炭品质和用途的影响，总结了常用活性炭炭化方法，着重阐述了不同活化方法的优缺点和研究现状，并对不同活性炭改性技术的特点和应用进行了比较。植物基活性炭的应用主要包括对硫化氢等工业废气和甲醛等室内废气的吸附净化，对废水中有机染料、有机药物、小分子有机化合物和重金属的吸附，以及被用于制作超级电容器电极材料等。最后针对目前研究中对植物原料的特点考虑不足、制备过程存在环境污染等问题，指出根据植物前体的性质优化制备方法、开发绿色高效制备技术、提高活性炭回收再利用效率将是今后的主要研究方向。

关键词: 生物质, 活性炭, 制备, 吸附, 应用

Abstract:

The preparation of plant-based activated carbon and its application are reviewed in this paper. The effects of different carbon resource on the characteristics and application of activated carbon were summarized. Features of common carbonization methods, activation methods and modification methods were discussed. The use of different preparing methods and related research progress were summarized as well. The general use of plant-based activated carbon includes decontamination of industrial and indoor waste gas, such as hydrogen sulfide and formaldehyde , adsorption of organic dyes, organic drugs, small molecular organic compounds and heavy metals in wastewater, and use as supercapacitor electrode materials. According to the limitations of current research, such as characteristics of plant raw materials being not adequately considered for single preparation

process

and pollution emission during preparation, future perspectives of plant-based active preparation research were provided as follows: preparation method optimization according the nature of plant precursors, environmental-friendly preparation methods development and improvement of activated carbon reuse ratio.

Key words: biomass, activated carbon, preparation, adsorption, application

中图分类号:

TQ424.1

申朋飞,朱颖颖,李信宝,夏振国,陈耿. 植物基活性炭的制备及吸附应用研究进展[J]. 化工进展, 2019, 38(08): 3763-3773.

Pengfei SHEN,Yingying ZHU,Xinbao LI,Zhenguo XIA,Geng CHEN. Review on preparation of plant-based activated carbon and its adsorption application[J]. Chemical Industry and Engineering Progress, 2019, 38(08): 3763-3773.

图/表 5

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原料	制备方法	孔径/nm	BET/m²·g^-1	吸附值/mg·g^-1	应用	举例
桉树锯末	NaOH活化	平均2.27	1120	碘 899	净水	Chen等^[12]制备的桉树锯末活性炭以介孔为主，且符合Ⅳ型吸附等温线
竹子	KOH活化	—	2295	—	直接碳燃料电池	仲兆平等^[13]制备的竹基活性炭经改性处理后，电阻率仅为6963μΩ·m，电化学性能良好
核桃壳杏核开心果壳	微波+H₃PO₄活化	0.4～6	981.5	碘 1162.8	净水	李勇等^[14]制备的果壳活性炭以介孔、微孔为主，亚甲基蓝吸附值和碘吸附值均可达到GB/T 13803.2—1999木质净水用活性炭国家一级标准
红枣核	ZnCl₂活化	3.168	1223	亚甲基蓝352.6	有机废水处理	杨晓霞等^[15]制备的红枣核基活性炭以介孔为主，对亚甲基蓝的吸附过程符合准二级动力学模型
椰壳	NaOH活化	2.27	2825	亚甲基蓝916.26	有机废水处理	Cazetta等^[16]制备的椰壳活性炭以微孔为主，对亚甲基蓝吸附平衡及动力学模型与朗格缪尔吸附等温线模型拟合最好，且以化学吸附为主
烟杆	KOH活化	微孔0.51～1	1657	碘 1198.27	净水	张利波等^[17]用烟杆制备了微孔活性炭，亚甲基蓝吸附值可达国家一级产品标准的3倍（GB/T13803.2—1999）
木质素	KOH活化	2.405	2684	—	水处理	Xiao等^[18]用木质素制备的活性炭以中微孔为主，表面官能团丰富，可用于大气污染控制和废水处理
莲藕皮	KOH活化	—	2961	—	超级电容器碳电极材料	Wang等^[19]制备的莲藕皮活性炭以微孔、介孔为主，具有较高的比电容和能量密度，经过10500个充放电循环后，仍有近100%的电容保留率，表现出良好的吸附稳定性

原料	制备方法	孔径/nm	BET/m²·g^-1	吸附值/mg·g^-1	应用	举例
桉树锯末	NaOH活化	平均2.27	1120	碘 899	净水	Chen等^[12]制备的桉树锯末活性炭以介孔为主，且符合Ⅳ型吸附等温线
竹子	KOH活化	—	2295	—	直接碳燃料电池	仲兆平等^[13]制备的竹基活性炭经改性处理后，电阻率仅为6963μΩ·m，电化学性能良好
核桃壳杏核开心果壳	微波+H₃PO₄活化	0.4～6	981.5	碘 1162.8	净水	李勇等^[14]制备的果壳活性炭以介孔、微孔为主，亚甲基蓝吸附值和碘吸附值均可达到GB/T 13803.2—1999木质净水用活性炭国家一级标准
红枣核	ZnCl₂活化	3.168	1223	亚甲基蓝352.6	有机废水处理	杨晓霞等^[15]制备的红枣核基活性炭以介孔为主，对亚甲基蓝的吸附过程符合准二级动力学模型
椰壳	NaOH活化	2.27	2825	亚甲基蓝916.26	有机废水处理	Cazetta等^[16]制备的椰壳活性炭以微孔为主，对亚甲基蓝吸附平衡及动力学模型与朗格缪尔吸附等温线模型拟合最好，且以化学吸附为主
烟杆	KOH活化	微孔0.51～1	1657	碘 1198.27	净水	张利波等^[17]用烟杆制备了微孔活性炭，亚甲基蓝吸附值可达国家一级产品标准的3倍（GB/T13803.2—1999）
木质素	KOH活化	2.405	2684	—	水处理	Xiao等^[18]用木质素制备的活性炭以中微孔为主，表面官能团丰富，可用于大气污染控制和废水处理
莲藕皮	KOH活化	—	2961	—	超级电容器碳电极材料	Wang等^[19]制备的莲藕皮活性炭以微孔、介孔为主，具有较高的比电容和能量密度，经过10500个充放电循环后，仍有近100%的电容保留率，表现出良好的吸附稳定性

制备方法	活化剂	孔径/nm	BET /m²·g^-1	吸附值/mg·g^-1	应用	举例
物理活化	水蒸气	平均0.96	1210	亚甲基蓝330	处理有机废水	Zhang等^[25]通过制备竹基活性炭得出：较高的活化温度或活化时间不仅可以促进新微孔的形成，拓宽已有微孔的孔径，不影响活性炭表面含氧官能团的种类，但会改变其含量
	CO₂	—	1120	碘 1032	处理重金属、有机废水	以黄麻为原料，Chen等^[26]在800℃下制备的活性炭以微孔为主，可有效吸附水中的重金属和有机物
	CO₂	—	2288	—	净水	以椰壳为植物前体，Yang等^[27]使用CO₂活化制备的活性炭比表面积最大，微孔率达77.9%，但相比蒸汽、蒸汽-CO₂混合物活化剂，所用活化时间多出约2.5倍，达210min
化学活化	ZnCl₂	2～6	1557	—	处理含重金属废水	陈诚等^[28]制备的板栗壳活性炭是一种具有较多孔隙的无定型炭材料，对Cu²⁺、Cd²⁺都有较好的吸附效果，均可达到3.3 mg·g^-1
	KOH	1.926	2111	—	—	选取咖啡渣为原料，马承愚等^[29]制备的活性炭为大孔骨架-微孔结构，活化后具有羟基、羧基和醚基官能团
	KOH	0～2	3545	碘 2926	水处理、大气污染治理	以丝瓜络为原料，李园园等^[30]制备的活性炭以微孔为主，存在少量中孔，没有大孔，亚甲基蓝吸附值为528.58mg·g^-1，可用于水处理、大气污染治理等领域
	H₃PO₄	0.6～4	1474	碘 1128	—	以芦苇叶为原料，Xu等^[31]在N₂气氛下制得了具有大量含氧和含磷表面基团的活性炭，H₃PO₄作为活化剂可以改变芦苇叶片的热降解性能、稳定纤维素结构，形成丰富的微孔和中孔
	H₃PO₄	4.7	1626.45	碘1043.29	—	以油茶壳残渣为原料，熊道陵等^[32]制备了中孔活性炭，表面存在羧基、羟基等含氧官能团及芳香环结构，亚甲基蓝吸附值达148.5mg·g^-1
物理化学活化	CO₂+磷酸胍	0.5～4	2000	—	—	Tsubota等^[33]先对竹子进行添加磷酸胍等处理，再以CO₂为活化剂制得微孔活性炭，其孔径结构与物理活化法制得活性炭相似，但引入了磷和氮原子。
	CO₂+ H₃PO₄	3.27	1241.81	碘1136.62	—	付国家等^[34]制备的核桃壳活性炭以微孔为主，存在部分中孔和大孔，表面可能有羟基、羧基、醚基、内酯基等官能团，使活性炭具有较强的吸附能力
微波化学活化	微波+KOH	2.434	3341	—	—	以竹废料为前体，Wu等^[35]在微波功率和微波加热时间分别为700W和15min、KOH/C=4的条件下制备活性炭，实验表明微波功率和加热时间对活性炭吸附能力影响显著，孔容最大为2.093cm³·g^-1
微波化学活化	微波+KOH	0～35	3406	碘 2239.1	超级电容器电极	以废弃烟杆为原料，张利波等^[36]通过活性炭实验得出：相比传统加热方式，微波加热可以节约87.5%的加热活化时间，且所得活性炭以微孔、中孔为主，其吸附性能远高于双电层电容器专用活性炭（LY/T1617—2004）的吸附指标

制备方法	活化剂	孔径/nm	BET /m²·g^-1	吸附值/mg·g^-1	应用	举例
物理活化	水蒸气	平均0.96	1210	亚甲基蓝330	处理有机废水	Zhang等^[25]通过制备竹基活性炭得出：较高的活化温度或活化时间不仅可以促进新微孔的形成，拓宽已有微孔的孔径，不影响活性炭表面含氧官能团的种类，但会改变其含量
	CO₂	—	1120	碘 1032	处理重金属、有机废水	以黄麻为原料，Chen等^[26]在800℃下制备的活性炭以微孔为主，可有效吸附水中的重金属和有机物
	CO₂	—	2288	—	净水	以椰壳为植物前体，Yang等^[27]使用CO₂活化制备的活性炭比表面积最大，微孔率达77.9%，但相比蒸汽、蒸汽-CO₂混合物活化剂，所用活化时间多出约2.5倍，达210min
化学活化	ZnCl₂	2～6	1557	—	处理含重金属废水	陈诚等^[28]制备的板栗壳活性炭是一种具有较多孔隙的无定型炭材料，对Cu²⁺、Cd²⁺都有较好的吸附效果，均可达到3.3 mg·g^-1
	KOH	1.926	2111	—	—	选取咖啡渣为原料，马承愚等^[29]制备的活性炭为大孔骨架-微孔结构，活化后具有羟基、羧基和醚基官能团
	KOH	0～2	3545	碘 2926	水处理、大气污染治理	以丝瓜络为原料，李园园等^[30]制备的活性炭以微孔为主，存在少量中孔，没有大孔，亚甲基蓝吸附值为528.58mg·g^-1，可用于水处理、大气污染治理等领域
	H₃PO₄	0.6～4	1474	碘 1128	—	以芦苇叶为原料，Xu等^[31]在N₂气氛下制得了具有大量含氧和含磷表面基团的活性炭，H₃PO₄作为活化剂可以改变芦苇叶片的热降解性能、稳定纤维素结构，形成丰富的微孔和中孔
	H₃PO₄	4.7	1626.45	碘1043.29	—	以油茶壳残渣为原料，熊道陵等^[32]制备了中孔活性炭，表面存在羧基、羟基等含氧官能团及芳香环结构，亚甲基蓝吸附值达148.5mg·g^-1
物理化学活化	CO₂+磷酸胍	0.5～4	2000	—	—	Tsubota等^[33]先对竹子进行添加磷酸胍等处理，再以CO₂为活化剂制得微孔活性炭，其孔径结构与物理活化法制得活性炭相似，但引入了磷和氮原子。
	CO₂+ H₃PO₄	3.27	1241.81	碘1136.62	—	付国家等^[34]制备的核桃壳活性炭以微孔为主，存在部分中孔和大孔，表面可能有羟基、羧基、醚基、内酯基等官能团，使活性炭具有较强的吸附能力
微波化学活化	微波+KOH	2.434	3341	—	—	以竹废料为前体，Wu等^[35]在微波功率和微波加热时间分别为700W和15min、KOH/C=4的条件下制备活性炭，实验表明微波功率和加热时间对活性炭吸附能力影响显著，孔容最大为2.093cm³·g^-1
微波化学活化	微波+KOH	0～35	3406	碘 2239.1	超级电容器电极	以废弃烟杆为原料，张利波等^[36]通过活性炭实验得出：相比传统加热方式，微波加热可以节约87.5%的加热活化时间，且所得活性炭以微孔、中孔为主，其吸附性能远高于双电层电容器专用活性炭（LY/T1617—2004）的吸附指标

改性方法	改性剂	孔径/nm	BET/m²·g^-1	吸附值/mg·g^-1	应用	举例
氧化改性	浓硫酸	2.27	2825	—	吸附丁烷	朱光真等^[40]采用磷酸法制备了杉木屑活性炭，实验表明，添加浓硫酸可以有效提高活性炭的比表面积，所得活性炭的丁烷工作容量可达157.3g·L ^- ¹
	HNO₃	—	802.3	SO₂ 62.21	低温脱硫	黄帮福等^[41]分别采用HNO₃和KOH对椰壳活性炭进行改性并负载镍用于烟气脱硫，通过对比实验得出HNO₃改性可以提高比表面积，脱硫率大于80%
还原改性	NaOH	2.141	332.47	—	—	Cheung等^[42]通过对比试验得出：酸、碱化学改性可以使活性炭微孔表面积有所增加，中孔表面积和体积稍减少，NaOH碱改性的效果明显更好一些，微孔率达65%
负载改性	Fe³⁺、Fe²⁺	—	125.77	Pb（Ⅱ）15.78 Cr(Ⅲ)12.9	处理多种金属离子废水	汪婷等^[43]通过改性制备的磁性活性炭对Pb(Ⅱ)去除率为70.5%，Cr(Ⅲ)去除率为77.4%，经过3次重复再生实验后，其吸附性能几乎没有变化
	FeSO₄	2.44	1086	苯酚 91.491	吸附苯酚	王贵珍等^[44]通过制备毛竹活性炭得出：添加FeSO₄促进了中孔的生成，有利于苯酚分子进入孔隙，提高扩散速度，可加快到达液相吸附平衡，去除率可达90.8%
物理改性	热改性	0.5～7.25	1167.45	二氯乙烷500	吸附有机气体	李立清等^[45]分别以甲苯、甲醇、二氯乙烷、丙酮为吸附质，考察了热改性对商品活性炭吸附性能的影响，得出热改性可以改变活性炭的孔径分布、增加碱性官能团的含量和种类，显著提高其对有机挥发性气体的吸附性能
	微波	1.766	783	SO₂ 22.36	烟气脱硫	李洲等^[46]以椰壳活性炭为例，通过实验分析得出：微波辐照改性能丰富活性炭表面孔隙结构，增加表面含氧官能团，对SO₂的吸附能力也显著增强