煤基零维纳米碳材料的合成、性能及其在能源转换和存储应用中的研究进展

doi:10.11949/0438-1157.20220868

化工学报 ›› 2022, Vol. 73 ›› Issue (11): 4791-4813.DOI: 10.11949/0438-1157.20220868

煤基零维纳米碳材料的合成、性能及其在能源转换和存储应用中的研究进展

侯旺君¹^,²(), 闫翎鹏²^,³, 曹哲勇¹, 郑静霞¹^,²(), 杨永珍¹^,²()

^1.太原理工大学新材料界面科学与工程教育部重点实验室，山西太原 030024
^2.山西浙大新材料与化工研究院，山西太原 030032
^3.太原理工大学材料科学与工程学院，山西太原 030024

收稿日期:2022-06-21 修回日期:2022-09-05 出版日期:2022-11-05 发布日期:2022-12-06
通讯作者: 郑静霞,杨永珍
作者简介:侯旺君（1998—），男，硕士研究生， hwj980307@163.com
基金资助:
国家自然科学基金项目(51972221);山西省基础研究计划项目(20210302124604);山西浙大新材料与化工研究院科技研发项目(2021SX-TD012);山西省回国留学人员科研资助项目(2020-051)

Research progress of synthesis and properties of coal-based zero-dimensional nanocarbon materials and their applications in energy conversion and storage

Wangjun HOU¹^,²(), Lingpeng YAN²^,³, Zheyong CAO¹, Jingxia ZHENG¹^,²(), Yongzhen YANG¹^,²()

^1.Key Laboratory of Interface Science and Engineering in Advanced Materials, Ministry of Education, Taiyuan University of Technology, Taiyuan 030024, Shanxi, China
^2.Shanxi-Zheda Institute of Advanced Materials and Chemical Engineering, Taiyuan 030032, Shanxi, China
^3.College of Materials Science and Engineering, Taiyuan University of Technology, Taiyuan 030024, Shanxi, China

Received:2022-06-21 Revised:2022-09-05 Online:2022-11-05 Published:2022-12-06
Contact: Jingxia ZHENG, Yongzhen YANG

摘要/Abstract

摘要：

煤是自然界中分布最广、储量最丰富的含碳资源，其分子结构与纳米碳材料具有天然的相似性，是优质的纳米碳材料前体。多年来，以煤为前体制备的各种纳米碳材料已被广泛应用于能源、信息、环境和生物医学等领域。其中，煤基零维纳米碳材料如纳米金刚石、富勒烯、碳纳米洋葱、碳点等，因其具有小的纳米尺寸、大的比表面积、独特的球形结构等，表现出优异的荧光特性、电化学性能以及催化性能等，在能源转化和存储等领域展现出极大的应用潜力。本文综述了基于煤炭及其衍生物为前驱体的各类零维纳米碳材料的制备方法和性能，并对其在照明显示、电化学储能、光/电催化等方面的应用进展进行总结，指出目前存在的问题与挑战及其解决策略，最后对其未来发展进行了展望。这为促进煤炭的高附加值转化和利用以及大规模制备煤基零维纳米碳材料提供理论和实践支持。

关键词: 煤及其衍生物, 零维纳米碳材料, 合成, 能源转换和存储, 荧光, 电化学, 催化

Abstract:

Coal is the most widely distributed and abundant carbon-containing resource in nature. Its molecular structure has natural similarity with nano-carbon materials, and it is a high-quality nano-carbon material precursor. Over the years, various nanocarbon materials prepared from coal have been widely used in the fields of energy, information, environment, and biomedicine, etc. Among them, coal-based zero-dimensional nanocarbon materials, such as nanodiamonds, fullerenes, carbon nano-onions, and carbon dots, show excellent fluorescence, electrochemical, and catalytic performances due to their small nanometer size, large specific surface area, and unique spherical structure, showing great application potential in the fields of energy conversion and storage. This paper reviews the preparation methods and properties of various zero-dimensional nanocarbon materials based on coal and its derivatives as precursors. This review summarizes the application research progresses of zero-dimensional nanocarbon materials in lighting display, electrochemical energy storage, photo/electrocatalysis, etc. Moreover, this review proposes the current problems, challenges, and improvement strategies of coal-based zero-dimensional nanocarbon materials, and further prospects their future development. This work provides the theoretical and practical support for promoting the high value-added conversion and utilization of coal as well as the large-scale preparation of coal-based zero-dimensional nanocarbon materials.

Key words: coal and its derivatives, zero-dimensional nanocarbon materials, synthesis, energy conversion and storage, fluorescence, electrochemistry, catalysis

中图分类号:

O 613.71

侯旺君, 闫翎鹏, 曹哲勇, 郑静霞, 杨永珍. 煤基零维纳米碳材料的合成、性能及其在能源转换和存储应用中的研究进展[J]. 化工学报, 2022, 73(11): 4791-4813.

Wangjun HOU, Lingpeng YAN, Zheyong CAO, Jingxia ZHENG, Yongzhen YANG. Research progress of synthesis and properties of coal-based zero-dimensional nanocarbon materials and their applications in energy conversion and storage[J]. CIESC Journal, 2022, 73(11): 4791-4813.

图/表 14

图1 四种煤基零维纳米碳材料TEM图 [12-16]

Fig.1 TEM images of four coal-based zero-dimensional nanocarbon materials [12-16]

表1 煤基NDs、C60、CNOs和CDs的合成、性能及应用研究进展

Table 1 Research progress on synthesis， properties and applications of coal-based NDs， C60， CNOs and CDs

产物	前体	合成方法	粒径	产率/荧光量子产率（QY）	性能	应用领域	文献
NDs	煤	超声法	4~15 nm	—	紫外光下激发为明亮蓝色荧光	生物成像，光伏工程	[7]
	无烟煤	激光烧蚀法	3~5 nm	产率6.2%	在420 nm激发下在乙醇溶液中为绿色荧光，在水溶液中为蓝色荧光	生物成像，光伏，光电子学	[31]
	焦炭	激光烧蚀法	3.2 nm	产率6%	在420 nm激发下在乙醇溶液中为绿色荧光，在水溶液中为蓝色荧光	生物成像，光伏，光电子学	[31]
	煤	化学氧化法	2.1~6.6 nm	产率4%~6%	—	生物传感，药物运输	[32]
C₆₀	褐煤	电弧放电法	—	产率4.5%	—	—	[33]
	烟煤	电弧放电法	—	产率0.67%~2.38%	—	—	[34]
	无烟煤	电弧放电法	—	产率5.96%	—	电化学储能	[34]
CNOs	煤	化学氧化法	5~20 nm	产率76.25%	自然光下，作为催化剂对2-硝基苯酚降解效率很高	光催化降解	[35]
	煤层气	CVD法	5~200 nm	产率70%	内嵌催化剂CNOs具有铁磁性；比容量达到142.31 F/g；电化学性能良好	超级电容器，气敏传感器	[29]
	煤	射频等离子法	10~35 nm	—	CNOs具有空心多面体或准球形形态，化学性能稳定	—	[15]
CDs	煤	激光烧蚀法	9.75~30.25 nm	—	紫外光下激发为绿色荧光；优异的光稳定性、低毒性和生物相容性	生物成像	[36]
	焦煤	激光烧蚀法	约35 nm	QY 34%	蓝色荧光，激发依赖性；随着粒径减小，最强发射峰蓝移	—	[37]
	焦炭	超声法	5.0~6.0 nm	QY 9.2%	蓝色荧光，最佳发射波长为410 nm	照明显示，LED	[38]
	无烟煤	溶剂热法	3.0~6.5 nm	产率25.6%，QY 47%	在紫外激发下显示蓝色荧光	光动力治疗，生物成像	[39]
	煤焦油	溶剂热法	1.5~4.5 nm	QY 29.7%	激发依赖；495~575 nm激发波长下发出橙色荧光，发射波长红移为598~612 nm	生物成像	[40]
	煤焦油沥青	溶剂热法	1.9~5.8 nm	产率18%~23%	结晶度高，分散性好；粒径可控，光吸附能力强	光催化制氢	[41]
	煤焦油中喹啉不溶物	化学氧化法	1.0~14.0 nm	QY 8.5%	紫外光激发下发出绿色荧光，最佳发射波长为578 nm	光学照明，生物成像	[42]
	褐煤	化学氧化/超声法	35 nm	QY 7%	激发依赖，分别在435和403 nm处观察到最佳发射峰；室温磷光	传感	[43]

表1 煤基NDs、C60、CNOs和CDs的合成、性能及应用研究进展

Table 1 Research progress on synthesis， properties and applications of coal-based NDs， C60， CNOs and CDs

产物	前体	合成方法	粒径	产率/荧光量子产率（QY）	性能	应用领域	文献
NDs	煤	超声法	4~15 nm	—	紫外光下激发为明亮蓝色荧光	生物成像，光伏工程	[7]
	无烟煤	激光烧蚀法	3~5 nm	产率6.2%	在420 nm激发下在乙醇溶液中为绿色荧光，在水溶液中为蓝色荧光	生物成像，光伏，光电子学	[31]
	焦炭	激光烧蚀法	3.2 nm	产率6%	在420 nm激发下在乙醇溶液中为绿色荧光，在水溶液中为蓝色荧光	生物成像，光伏，光电子学	[31]
	煤	化学氧化法	2.1~6.6 nm	产率4%~6%	—	生物传感，药物运输	[32]
C₆₀	褐煤	电弧放电法	—	产率4.5%	—	—	[33]
	烟煤	电弧放电法	—	产率0.67%~2.38%	—	—	[34]
	无烟煤	电弧放电法	—	产率5.96%	—	电化学储能	[34]
CNOs	煤	化学氧化法	5~20 nm	产率76.25%	自然光下，作为催化剂对2-硝基苯酚降解效率很高	光催化降解	[35]
	煤层气	CVD法	5~200 nm	产率70%	内嵌催化剂CNOs具有铁磁性；比容量达到142.31 F/g；电化学性能良好	超级电容器，气敏传感器	[29]
	煤	射频等离子法	10~35 nm	—	CNOs具有空心多面体或准球形形态，化学性能稳定	—	[15]
CDs	煤	激光烧蚀法	9.75~30.25 nm	—	紫外光下激发为绿色荧光；优异的光稳定性、低毒性和生物相容性	生物成像	[36]
	焦煤	激光烧蚀法	约35 nm	QY 34%	蓝色荧光，激发依赖性；随着粒径减小，最强发射峰蓝移	—	[37]
	焦炭	超声法	5.0~6.0 nm	QY 9.2%	蓝色荧光，最佳发射波长为410 nm	照明显示，LED	[38]
	无烟煤	溶剂热法	3.0~6.5 nm	产率25.6%，QY 47%	在紫外激发下显示蓝色荧光	光动力治疗，生物成像	[39]
	煤焦油	溶剂热法	1.5~4.5 nm	QY 29.7%	激发依赖；495~575 nm激发波长下发出橙色荧光，发射波长红移为598~612 nm	生物成像	[40]
	煤焦油沥青	溶剂热法	1.9~5.8 nm	产率18%~23%	结晶度高，分散性好；粒径可控，光吸附能力强	光催化制氢	[41]
	煤焦油中喹啉不溶物	化学氧化法	1.0~14.0 nm	QY 8.5%	紫外光激发下发出绿色荧光，最佳发射波长为578 nm	光学照明，生物成像	[42]
	褐煤	化学氧化/超声法	35 nm	QY 7%	激发依赖，分别在435和403 nm处观察到最佳发射峰；室温磷光	传感	[43]

图2 CNOs 的制备、纯化及活化技术路线图(a) [29]; CVD法制备碳包覆催化剂颗粒和空心CNOs的生长过程示意图(b) [30]

Fig.2 Technology road-mapping of the synthesis, purification and functionalization of CNOs (a) [29]; Schematic diagram of the growth process of carbon coated catalyst particles and hollow CNOs prepared by CVD (b) [30]

图3 烟煤为碳源合成GQDs的示意图(a) [14]; H2O2作氧化剂合成煤基CDs的示意图(b) [45]

Fig.3 Schematic representation of the synthesis of GQDs from bituminous coal (a) [14]; Schematic diagram of the synthesis of coal-based CDs with H2O2 as oxidant (b) [45]

图4 DMF作溶剂合成煤基CDs的示意图(a) [39]; 制备煤基FCNPs的路线示意图(b) [43]

Fig.4 Schematic diagram of the synthesis of coal-based CDs using DMF as solvent (a) [39]; Schematic diagram of the route to prepare coal-based FCNPs (b) [43]

图5 低品质煤在H2O2溶剂中超声法合成NDs示意图(a)[12]; 煤在DMF溶剂中超声法合成GQDs示意图(b) [47]

Fig.5 Schematic diagram of NDs synthesized by ultrasonication of low quality coal in H2O2 solvent (a) [12]; Schematic diagram of GQDs synthesized by ultrasonication of coal in DMF solvent (b) [47]

图6 热处理法合成煤基GQDs的示意图[58]

Fig.6 Schematic diagram of coal-based GQDs synthesized by heat treatment [58]

图7 射频等离子体法合成煤基CNOs的生长机理示意图[15]

Fig.7 The growth mechanism diagram of coal-based CNOs synthesized by radiofrequency plasma method[15]

表2 目前制备煤基NDs、C60、CNOs和CDs各种方法的优缺点

Table 2 The advantages and disadvantages of various preparation methods for coal-based NDs， C60， CNOs and CDs

合成方法	主要前体	主要产物	优点	缺点
CVD法	煤层气（甲烷），乙炔，煤沥青	C₆₀，CDs，CNOs	操作简单，成本低，易于大批量生产	伴随有杂质相（无定形碳、石墨、催化剂），纯化困难
化学氧化法	褐煤，烟煤，无烟煤，焦炭	NDs，GQDs，CDs	设备简单，能耗低，操作简便	含有杂质，纯化困难
溶剂热法	煤焦油，烟煤，无烟煤	GQDs，CDs	操作简单，能耗低，不需要特殊的反应条件和设备	产量低，伴随着有毒气体的释放
超声法	烟煤，无烟煤	NDs，CQDs	反应速率快，操作简便	加热效率低，能耗高
电化学氧化法	焦炭或无烟煤混合煤焦油	C₆₀，CNOs，CDs	成本低，效率高，产量高	含有杂质相（金属杂质、无定形碳），设备复杂，原料需力学性能好
电弧放电法	焦炭，无烟煤，石墨	C₆₀，CNOs，CDs	产物结晶性好，能够大量制备，易于收集	含有大量含碳杂质（无定形碳、碳纳米管及金属杂质等），设备复杂
等离子体法	烟煤，无烟煤	CNOs，CDs	成本低，能大量制备	含有金属杂质及无定形碳
热解法	炭黑，纳米金刚石	C₆₀，CNOs	可大量制备，操作简便	产物纯净度低，纯化困难
微波法	褐煤，烟煤，无烟煤	NDs，CDs	反应速率快，高效	产量不高，纯化过程复杂
热处理法	烟煤，无烟煤，石墨	CNOs，CDs	可大量制备，操作简单	能耗高，产物纯净度低，纯化困难

图8 PVA和PVA/GQDs薄膜在紫外灯(波长为365 nm)下的照片(a) [79];CQDs基LED器件的横截面视图(b);在3.2 V下工作的LED及其发射光谱图(c);白光LED的CIE色度图(d) [38]

Fig.8 Photographs of PVA and PVA/GQDs films under UV lamp (wavelength of 365 nm) (a) [79]; Cross-sectional view of CQDs-based LED devices (b); LEDs operating at 3.2 V and their emission spectra plots (c); CIE chromaticity plots of white LEDs (d) [38]

图9 在PBS缓冲液中CDs作为金属离子探针的选择性(a) [80]; 基于GQDs作为纳米猝灭器的DNA传感策略示意图(b) [81]

Fig.9 Selectivity of CDs as metal ion probes in PBS buffer (a) [80]; Schematic of DNA sensing strategy based on GQDs as nano-quenchers (b) [81]

图10 C-GQDs/α-Fe2O3复合材料的合成路线[86]

Fig.10 Preparation of C-GQDs/α-Fe2O3 composites[86]

图11 CoDC-0.5在三电极系统中的CV曲线(a)和恒流充放电曲线(b); CoDC-0.5在10 A/g时的循环性能(c); CoDC-0.5、活性炭和还原氧化石墨烯在不同质量负载下的电容(d); CoDC-0.5在4~25 mg/cm2不同负载下的Nyquist图(e); CoDC-0.5、活性炭和还原氧化石墨烯在20 mg/cm2负荷下的Bode图(f) [90]

Fig.11 CV curves (a) and galvanostatic charge-discharge curves (b) of the CoDC-0.5 in three-electrode system; Cycle performance of the CoDC-0.5 at 10 A/g (c); Areal capacitances of the CoDC-0.5, activated carbon, and reduced graphene oxide with different mass loadings (d); Nyquist plots of the CoDC-0.5 with various mass loadings from 4 to 25 mg/cm (e); Bode plots of the CoDC-0.5, activated carbon, and reduced graphene oxide under a mass loading of 20 mg/cm (f) [90]

图12 BN-GQD/G复合材料的制备示意图(a);样品的电催化活性(b) [101]

Fig.12 Schematic illustration of the preparation of the BN-GQD/G nanocomposite (a); Electrocatalytic activity of samples (b) [101]

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煤基零维纳米碳材料的合成、性能及其在能源转换和存储应用中的研究进展

Research progress of synthesis and properties of coal-based zero-dimensional nanocarbon materials and their applications in energy conversion and storage

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