氮掺杂生物炭的制备与应用研究进展

doi:10.16085/j.issn.1000-6613.2022-1563

化工进展 ›› 2023, Vol. 42 ›› Issue (7): 3720-3735.DOI: 10.16085/j.issn.1000-6613.2022-1563

氮掺杂生物炭的制备与应用研究进展

李艳玲¹(), 卓振¹, 池亮², 陈曦¹, 孙堂磊¹, 刘鹏¹(), 雷廷宙¹()

^1.常州大学城乡矿山研究院，常州市生物质绿色安全高值利用技术重点实验室，江苏常州 213164
^2.中国石油吉林石化公司乙烯厂，吉林吉林 132022

收稿日期:2022-08-23 修回日期:2022-12-21 出版日期:2023-07-15 发布日期:2023-08-14
通讯作者: 刘鹏,雷廷宙
作者简介:李艳玲（1992—），女，博士研究生，硕士生导师，研究方向为生物质资源化利用。E-mail：liyl@cczu.edu.cn。
基金资助:
常州市科技项目应用基础研究计划(CJ20220138);国家自然科学基金(51906021);现代农业-碳达峰碳中和科技创新专项资金（农业农村领域重大关键技术攻关）(BE2022426)

Research progress on preparation and application of nitrogen-doped biochar

LI Yanling¹(), ZHUO Zhen¹, CHI Liang², CHEN Xi¹, SUN Tanglei¹, LIU Peng¹(), LEI Tingzhou¹()

^1.Institute of Urban and Rural Mining, Changzhou Key Laboratory of Green Safe and High Value Utilization Technology of Biomass, Changzhou University, Changzhou 213164, Jiangsu, China
^2.Ethylene Plant, PetroChina Jilin Petrochemical Company, Jilin 132022, Jilin, China

Received:2022-08-23 Revised:2022-12-21 Online:2023-07-15 Published:2023-08-14
Contact: LIU Peng, LEI Tingzhou

摘要/Abstract

摘要：

生物质不仅储量丰富、分布广泛且可再生，是一种亟待高值化利用的资源。将其炭化后制备的生物炭具有良好的理化性质，常被用于吸附污染物、制作电极材料。但与活性炭相比，生物炭存在孔隙结构欠发达、表面官能团种类和数量稀少等问题，其应用受到了很大限制。通过对生物炭进行N元素掺杂改性制成N掺杂生物炭（NBC）可丰富生物炭孔隙结构和表面活性位点，提高吸附、导电和催化性能。本文综述了国内外近几年来关于NBC的制备/改性方法（热解法、活化法、水热法、模板法和后处理法等）及其优点和局限性，梳理了各方法得到的NBC的形貌结构及表面化学特征，概括了氮掺杂对NBC的催化、吸附、电化学性能的影响及NBC在各领域的应用。以“制备-结构-性能及应用”相结合的思路，从NBC的应用角度逆向出发，思考如何通过探究N掺杂机理和优化制备方法，来充分发挥NBC在各领域中的应用价值，并对今后该领域的研究发展提出了展望。

关键词: 氮掺杂, 生物炭, 活化, 催化, 吸附, 储能

Abstract:

Biomass is abundant, widely distributed and renewable, and can be used in high value resources. The biochar obtained after carbonization of biomass has good physical and chemical properties, and is often used to adsorb pollutants and make electrode materials. Compared with activated carbon, there are many problems such as underdeveloped pore structure and scarcity of surface functional groups, limits the application of biochar. Nitrogen doping can enrich biochar pore structure and surface activity sites, and endow the N-doped biochar (NBC) with improved adsorption, conductivity and catalytic performance. In this paper, preparation/modification methods of NBC, such as pyrolysis, activation, hydrothermal, template and post-treatment method, along with their benefits and drawbacks were reviewed. The morphological structure and surface chemical characteristics of NBC obtained by each method were summarized. And the applications of NBCs in catalysis, adsorption and electrochemical energy storage fields were generalized. With the "preparation-structure-characteristics and application" combined conception, started from the perspective of NBC application, this paper discussed how to maximize the application value of NBC by investigating the N-doping mechanism and improving the preparation method, and then presented references and recommendations for further research and development in this field.

Key words: nitrogen-doping, biochar, activation, catalysis, adsorption, energy storage

中图分类号:

TQ424.1

李艳玲, 卓振, 池亮, 陈曦, 孙堂磊, 刘鹏, 雷廷宙. 氮掺杂生物炭的制备与应用研究进展[J]. 化工进展, 2023, 42(7): 3720-3735.

LI Yanling, ZHUO Zhen, CHI Liang, CHEN Xi, SUN Tanglei, LIU Peng, LEI Tingzhou. Research progress on preparation and application of nitrogen-doped biochar[J]. Chemical Industry and Engineering Progress, 2023, 42(7): 3720-3735.

图/表 15

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制备方法	优点	缺点
原位掺杂法
活化	造孔性能优异、孔隙多为微孔	活化剂具有腐蚀性、工艺要求高、污染环境、反应机理复杂
水热	通过控制反应温度可以很好的调控含N官能团的种类和数量	孔隙少且多为中孔、结构不发达
热解	温度可调范围大、操作简单、炭产率高、N-Q含量高，最为常用	孔隙结构单一、比表面积有限、表面特征不理想
模板	可有效促进和严格把控NBC的孔隙结构和表面形态	去除模板剂造成浪费
后处理法	N掺杂量较高、操作简单	N掺杂不均匀、含N官能团数量少、掺杂效果不理想

制备方法	优点	缺点
原位掺杂法
活化	造孔性能优异、孔隙多为微孔	活化剂具有腐蚀性、工艺要求高、污染环境、反应机理复杂
水热	通过控制反应温度可以很好的调控含N官能团的种类和数量	孔隙少且多为中孔、结构不发达
热解	温度可调范围大、操作简单、炭产率高、N-Q含量高，最为常用	孔隙结构单一、比表面积有限、表面特征不理想
模板	可有效促进和严格把控NBC的孔隙结构和表面形态	去除模板剂造成浪费
后处理法	N掺杂量较高、操作简单	N掺杂不均匀、含N官能团数量少、掺杂效果不理想

原料	制备方法	S_BET/m²·g^-1	S_mic/m²·g^-1	V_total/cm³·g^-1	V_mic/cm³·g^-1	d/nm	文献
柚子皮	900℃热解	627.5	444.7	0.355	0.236	2.26	[51]
豆浆	CO₂活化、热解	558.2	317.3	0.346	0.142	3.23	[50]
芦苇	活化、热解	1074.0	489.0	0.996	0.543	1.85	[52]
稻草	水热、活化、热解	2788.7	—	1.597	0.913	—	[10]
稻草	活化、热解	2537.0	—	1.561	—	—	[31]
椰壳	ZnCl₂活化、热解	1291.0	—	0.785	0.463	2.43	[33]

原料	制备方法	S_BET/m²·g^-1	S_mic/m²·g^-1	V_total/cm³·g^-1	V_mic/cm³·g^-1	d/nm	文献
柚子皮	900℃热解	627.5	444.7	0.355	0.236	2.26	[51]
豆浆	CO₂活化、热解	558.2	317.3	0.346	0.142	3.23	[50]
芦苇	活化、热解	1074.0	489.0	0.996	0.543	1.85	[52]
稻草	水热、活化、热解	2788.7	—	1.597	0.913	—	[10]
稻草	活化、热解	2537.0	—	1.561	—	—	[31]
椰壳	ZnCl₂活化、热解	1291.0	—	0.785	0.463	2.43	[33]

原料	温度 /℃	吡啶氮 /%	吡咯氮 /%	石墨化氮 /%	吡啶型氧化氮 /%	文献
玉米秸秆	700	29.9	17.2	43.1	9.8	[25]
竹渣	800	14.2	71.0	14.8	—	[58]
木浆	900	44.3	19.5	36.2	—	[59]
竹子	800	37.7	25.6	27.6	9.1	[60]
水葫芦	800	43.2	—	56.8	—	[61]
香蕉皮	600	26.2	38.5	35.3	—	[62]
樟子松	600	37.7	46.5	15.8	—	[63]

氮掺杂生物炭的制备与应用研究进展

Research progress on preparation and application of nitrogen-doped biochar

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炭源	氮源	制备工艺	N组分/%	N类型	作用	文献
竹子	NH₃	热解	3.42	N-5、N-6、N-Q、N-X	NBC作催化剂促进了苯酚的生成同时抑制了乙酸的产生，提高了产物产量和生物油的质量	[68]
木屑	双氰胺	热解	20.32	N-6、N-Q	NBC丰富的缺陷结构和N-Q、N-6表现出了较好的催化活性，可以有效降解苯酚、对乙酰氨基酚、磺胺甲𫫇唑	[69]
玉米芯	三聚氰胺	水热炭化、热解	27.19	N-5、N-6、N-Q	氮掺杂技术提高了石墨化水平和N-5相对含量，从而促进了电导率，提高了微生物生物制氢的效率	[25]
玉米芯	吡咯	热解、CO₂活化	6.17	N-Q、N-6	大量的N-Q提高了导电率和电催化活性，丰富的孔隙结构有效负载了Fe₂O₃，使其ORR催化性能优于商业的Pt/C催化剂	[70]
苎麻树皮	尿素	活化、热解	2.12	N-Q、N-5、N-6	NBC中的N-Q、缺陷位点提供了四环素催化降解的活性位点，低阻抗和高的电子转移速率也是催化性高的关键	[71]
葡萄糖	三聚氰胺	热解法	—	N-Q	NBC负载Cu用作还原对硝基苯酚的催化剂，N-Q的π-π键促进了催化降解	[72]
柚皮	三聚氰胺	NaHCO₃活化、热解	13.54	N-5、N-Q	NBC的N结构作为过硫酸氢盐活化的活性中心，催化去除了磺胺甲𫫇唑等抗生素污染物	[73]

炭源	氮源	吸附质	制备工艺	比表面积 /m²·g^-1	孔容 /cm³·g^-1	N类型	机理	文献
蓝藻	蓝藻	CO₂	热解	1148	0.52	N-5、N-6、N-Q	孔隙结构与N-Q提供了吸附CO₂所需的活性位点	[21]
椰壳	椰壳	SO₂	CO₂活化、水热炭化	706	0.45	N-5、N-6、N-Q	SO₂分子与含N官能团的静电作用N掺杂增强了炭基表面对SO₂的吸附	[36]
椰壳	尿素	CO₂	K₂CO₃活化、后处理	1324	0.51	N-5、N-6、N-Q	高的比表面积和多种含N官能团共同促进了对CO₂的吸附	[20]
竹子	尿素	苯酚、亚甲基蓝	KHCO₃活化、热解	1693	0.90	N-5、N-6、N-X	含N官能团的引入增强了生物炭的表面活性，提高了对苯酚、亚甲基蓝的吸附量	[40]
玉米秸秆	尿素	苯酚	NaHCO₃活化、热解	619	0.38	N-6、N-Q	微孔填充作用、N-6与苯酚分子间的Lewis酸碱相互作用、N-Q与苯酚分子形成π-π键	[38]
玉米秸秆	NH₃	Cu²⁺、Cd²⁺	热解	418	0.28	N-Q	阳离子π键和与炭表面N-Q和—OH的络合	[74]
茶树	尿素	Cu²⁺、Pb²⁺	ZnCl₂活化、水热炭化	63	0.30	N-6、N-Q	氢键、螯合作用、N-Q和—OH的表面络合作用提高了对重金属离子的吸附	[28]
莲藕	莲藕	甲基橙	N₂氛围900℃热解4h	693	0.38	N-5、N-6、N-Q	通过官能团和孔隙吸附作用吸附甲基橙	[75]
腐殖酸	尿素	Cd²⁺、As³⁺、As⁶⁺	N₂氛围700℃热解2h	526	—	N-Q、N-6	阳离子π键、N-Q和—OH的络合	[76]

炭源	氮源	制备工艺	比表面积 /m²·g^-1	孔容 /cm³·g^-1	储能器类型	产品特性	文献
麦秸秆	三聚氰胺	KCl和ZnCl₂作为盐模板	1201	1.02	超级电容器	可逆比电容223F/g（0.5A/g），次循电容保持率91.4%（10000）	[24]
稻秸秆	尿素	K₂CO₃活化、水热、热解	2800	1.60	超级电容器	可逆比电容380F/g（0.5A/g），电容保持率95.4%（10000）	[10]
漆籽纤维	铁氰化钾	预炭化、高温活化	407	0.39	超级电容器	可逆比电容324F/g（0.2A/g），3000电容保持率97.0%（3000）	[87]
香菇	香菇	KOH活化、浸泡	1930	0.86	超级电容器	比电容为325F/g（0.5A/g），电容保持率为97.7%（5000）	[88]
菜籽饼	三聚氰胺	K₂CO₃活化、热解	2050	1.13	超级电容器	比电容274F/g（0.05A/g），电容保持率96.0%（10000）	[89]
头发	头发	热解、活化	1617	0.70	钠离子电池	可逆比电容为700mAh/g（0.13C）	[79]
木耳	木耳	冻干、热解	1568	—	锂硫电池	可逆比电容为875mAh/g（0.20C）	[90]
木材	三聚氰胺	熔融盐模板、热解	621	0.34	锂氧电池	放电比电容为9.44mA·h/cm²（0.05mA/cm²），可循环113次（0.5mA/cm²）	[55]

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