Citation: SU Xiangxiang, YANG Rong, LI Lan, LI Runqiu, WANG Liqing, LEI Ying. Research Progress of Preparation of Nitrogen-doped Graphene and Its Application in Chemical Energy Storage[J]. Chinese Journal of Applied Chemistry, ;2018, 35(2): 137-146. doi: 10.11944/j.issn.1000-0518.2018.02.170036 shu

Research Progress of Preparation of Nitrogen-doped Graphene and Its Application in Chemical Energy Storage

SU Xiangxiang ^a ,
YANG Rong ^a,, ,
LI Lan ^a ,
LI Runqiu ^b ,
WANG Liqing ^a ,
LEI Ying ^a

a.
School of Science, Xi'an University of Technology, Xi'an 710048, China
b.
State Grid Shaanxi Electric Power Company, Xi'an 710065, China

Corresponding author: YANG Rong, yangrong@xaut.edu.cn
Received Date: 16 February 2017
Revised Date: 19 May 2017
Accepted Date: 27 June 2017

Fund Project: the International Science Technology Cooperation Program of China 2015DFR50350the Innovation and Entrepreneurship Training Program of the Provincial College Students in 2016 1168Supported by the International Science Technology Cooperation Program of China(No.2015DFR50350), the National Natural Science Foundation of China(No.21503166), the Innovation and Entrepreneurship Training Program of the Provincial College Students in 2016(No.1168), the Science and Technology Project of Shaanxi Province(No.2017GY-160), the Innovation Project of Xi'an University of Technology(No.2015CX011)the National Natural Science Foundation of China 21503166the Innovation Project of Xi'an University of Technology 2015CX011the Science and Technology Project of Shaanxi Province 2017GY-160

Figures(2)

The unique two-dimensional spatial structure gives graphene excellent chemical and physical properties and huge specific surface area, which makes graphene a very promising material for energy storage applications and a research hotspot recently. Irreversible agglomeration, smooth surface and inertness result in the dramatic reduction of the available active surface of graphene, which limits its blending with other materials. In recent years, doping graphene with nitrogen reforms its electronic structure and increases surface active sites, promoting its electrochemical performance in the field of energy storage. This paper reviews the current status of nitrogen-doped graphene synthesis and recent progress in the use of nitrogen-doped graphene in chemical energy storage, including supercapacitors, Li-ion batteries, Li-air batteries and Li-S batteries. Finally, key issues related to preparations and applications of nitrogen-doped graphene are briefly discussed as well, and the development prospect of nitrogen-doped graphene is prospected as well.
- nitrogen-doped grapheme,
- preparation,
- chemical energy storage,
- supercapacitor,
- lithium ion batteries
1. [1]
  Novoselov K S, Geim A K, Morozov S V. Electric Field Effect in Atomically Thin Carbon Films[J]. Science, 2004,306(5696):666-669. doi: 10.1126/science.1102896
2. [2]
  Son Y W, Cohen M L, Louie S G. Half-metallic Graphene Nanoribbons[J]. Nature, 2006,444(7117):347-349. doi: 10.1038/nature05180
3. [3]
  Yang X J, Zheng A B, Wang X L. Graphene Nanosheet and Carbon Layer Co-decorated Li₄Ti₅O₁₂ as High-performance Anode Material for Rechargeable Lithium-Ion Batteries[J]. Ceram Int, 2017,43(3):3252-3258. doi: 10.1016/j.ceramint.2016.11.154
4. [4]
  YANG Rong, WANG Liqing, LV Mengni. Progress in Synthesis of Graphene and Graphene-based Materials by Microwave Method[J]. Chem Bull, 2016,79(6):503-508.
5. [5]
  Min J H, Seo T H, Choi S B. Effect of p-GaN Hole Concentration on the Stabilization and Performance of a Graphene Current Spreading Layer in Near-ultraviolet Light-emitting Diodes[J]. Curr Appl Phys, 2016,16(10):1382-1387. doi: 10.1016/j.cap.2016.08.006
6. [6]
  Park S, Shehzad M A, Khan M F. Effect of Grain Boundaries on Electrical Properties of Polycrystalline[J]. Carbon, 2017,112:142-148. doi: 10.1016/j.carbon.2016.11.010
7. [7]
  Wu Z Q, Lu Y H, Xu W L. Surface Plasmon Enhanced Graphene/p-GaN Heterostructure Light-emitting-diode by Ag Nano-particles[J]. Nano Energy, 2016,30:362-367. doi: 10.1016/j.nanoen.2016.10.028
8. [8]
  Wang Q Q, Huang J B, Li G R. A Facile and Scalable Method to Prepare Carbon Nanotube-grafted-graphene for High Performance Li-S Battery[J]. J Power Sources, 2017,339:20-26. doi: 10.1016/j.jpowsour.2016.11.038
9. [9]
  Hao J T, Shu D, Guo S T. Preparation of Three-dimensional Nitrogen-doped Graphene Layers by Gas Foaming Method and Its Electrochemical Capactive Behavior[J]. Electrochim Acta, 2016,193:293-301. doi: 10.1016/j.electacta.2016.02.048
10. [10]
  HU Rongyan, JIA Kunpeng, CHEN Yang. Research Progress of Graphene Doping[J]. Micronanoelectron Technol, 2015,52(11):692-700.
11. [11]
  Rao C N R, Gopalakrishnan K, Govindaraj A. Synthesis, Properties and Applications of Graphene Doped with Boron, Nitrogen and Other Elements[J]. Nano Today, 2014,9(3):324-343. doi: 10.1016/j.nantod.2014.04.010
12. [12]
  Li S H, Yang S Y, Wang Y S. N-Doped Structures and Surface Functional Groups of Reduced Graphene Oxide and Their Effect on the Electrochemical Performance of Supercapacitor with Organic Electrolyte[J]. J Power Sources, 2015,278(4):218-229.
13. [13]
  Tian G Y, Liu L, Meng Q G. Facile Synthesis of Laminated Graphene for Advanced Supercapacitor Electrode Material via Simultaneous Reduction and N-Doping[J]. J Power Sources, 2015,274:851-861. doi: 10.1016/j.jpowsour.2014.10.171
14. [14]
  Wang D W, Min Y G, Yu Y H. A General Approach for Fabrication of Nitrogen-doped Graphene Sheets and Its Application in Supercapacitors[J]. Science, 2014,417(3):270-277.
15. [15]
  Yang Y C, Shi W, Zhang R H. Electrochemical Exfoliation of Graphite into Nitrogen-doped Graphene in Glycine Solution and Its Energy Storage Properties[J]. Electrochim Acta, 2016,204:100-107. doi: 10.1016/j.electacta.2016.04.063
16. [16]
  Liu J, Wang Z H, Zhu J F. Binder-free Nitrogen-doped Carbon Paper Electrodes Derived from Polypyrrole/Cellulose Composite for Li-O₂ Batteries[J]. J Power Sources, 2016,306:559-566. doi: 10.1016/j.jpowsour.2015.12.074
17. [17]
  Sui Y P, Zhu B, Zhang H R. Temperature-dependent Nitrogen Configuration of N-Doped Graphene by Chemical Vapor Deposition[J]. Carbon, 2015,81(1):814-820.
18. [18]
  Bao J F, Kishi N, Soga T. Synthesis of Nitrogen-doped Graphene by the Thermal Chemical Vapor Deposition Method from a Single Liquid Precursor[J]. Mater Lett, 2014,117(1):199-203.
19. [19]
  Kano E, Kalita G, Shinde S M. Grain Structures of Nitrogen-doped Graphene Synthesized by Solid Source-based Chemical Vapor Deposition[J]. Carbon, 2016,96:448-453. doi: 10.1016/j.carbon.2015.09.086
20. [20]
  Deng D H, Pan X L, Yu L. Toward N-Doped Graphene via Solvothermal Synthesis[J]. Chem Mater, 2011,23(5):1188-1193. doi: 10.1021/cm102666r
21. [21]
  Zhang H, Kuila T, Kim N H. Simultaneous Reduction, Exfoliation, and Nitrogen Doping of Graphene Oxide via a Hydrothermal Reaction for Energy Storage Electrode Materials[J]. Carbon, 2014,69(6):66-78.
22. [22]
  Jeony H M, Lee J W, Shin W H. Nitrogen-Doped Graphene for High-Performance Ultracapacitors and the Importance of Nitrogen-Doped Sites at Basal Planes[J]. Nano Lett, 2011,11(6):2472-2477. doi: 10.1021/nl2009058
23. [23]
  Li N, Wang Z Y, Zhao K K. Large Scale Synthesis of N-Doped Multi-layered Graphene Sheets by Simple Arc-discharge Method[J]. Carbon, 2010,48(1):25-259. doi: 10.1016/j.carbon.2009.06.060
24. [24]
  Guo B D, Liu Q, Chen E D. Controllable N-Doping of Graphene[J]. Nano Lett, 2010,12(10):4975-4980.
25. [25]
  Lin Z Y, Waller G, Liu Y. Facile Synthesis of Nitrogen-doped Graphene via Pyrolysis of Graphene Oxide and Urea, and Its Electrocatalytic Activity Toward the Oxygen-reduction Reaction[J]. Adv Energy Mater, 2012,7(2):884-888.
26. [26]
  Sari F N I, Lin H M, Ting J M. Surface Modified Catalytically Grown Carbon Nanofibers/MnO₂ Composites for Use in Supercapacitor[J]. Thin Solid Films, 2016,620:54-63. doi: 10.1016/j.tsf.2016.07.085
27. [27]
  Zheng B J, Chen Y F, Li P J. Ultrafast Ammonia-driven, Microwave-assisted Synthesis of Nitrogen-doped Graphene Quantum Dots and Their Optical Properties[J]. J Nanophoton, 2016,6(1):259-267.
28. [28]
  Chang Y Z, Han G Y, Yuan J P. Using Hydroxylamine as a Reducer to Prepare N-Doped Garphene Hydrogels Used in High-performance Energy Storage[J]. J Power Sources, 2013,238(28):492-500.
29. [29]
  Jiang Z J, Jiang Z Q, Chen W H. The Role of Holes in Improving the Performance of Nitrogen-doped Holey Graphene as an Active Electrode Material for Supercapacitor and Oxygen Reduction Reaction[J]. J Power Sources, 2014,251:55-65. doi: 10.1016/j.jpowsour.2013.11.031
30. [30]
  GUO Huilin, SU Peng, PENG San. Preparation of Nitrogen-Doped Graphene and Its Supercapacitive Properties[J]. Acta Phys-Chim Sin, 2012,28(11):2745-2753. doi: 10.3866/PKU.WHXB201208221
31. [31]
  Liao Y Q, Huang Y L, Shu D. Three-dimensional Nitrogen-doped Graphene Hydrogels Prepared via Hydrothermal Synthesis as High-performance Supercapacitor Materials[J]. Electrochim Acta, 2016,194:136-142. doi: 10.1016/j.electacta.2016.02.067
32. [32]
  ZHONG Wenbin, TAN Xiyi. Synthesis of 3D N-Doped Graphene Networks with High Electrochemical Performance[J]. J Hunan Univ(Nat Sci), 2016,43(6):53-57.
33. [33]
  Jiang M, Xing L B, Zhang J L. Carbohydrazide-dependent Reductant for Preparing Nitrogen-doped Graphene Hydrogels as Electrode Materials in Supercapacitor[J]. Science, 2016,368:388-394.
34. [34]
  ZHONG Qineng, LI Zelong, LI Xinlu. Preparation and Supercapacitor Performance of a Flexible Nitrogen-doped Graphene Film[J]. Surf Technol, 2015,44(1):51-63.
35. [35]
  Jiang B J, Tian C G, Wang L. Highly Concentrated, Stable Nitrogen-doped Graphene for Supercapacitors:Simultaneous Doping and Reduction[J]. Science, 2012,258(8):3438-3443.
36. [36]
  Wang B H, Qin Y, Tan W H. Smartly Designed 3D N-Doped Mesoporous Graphene for High-performance Supercapacitor Electrodes[J]. Electrochim Acta, 2017,241:1-9. doi: 10.1016/j.electacta.2017.04.120
37. [37]
  Zhao X, Dong H, Xiao Y. Three-dimensional Nitrogen-doped Graphene as Binder-free Electrode Materials for Supercapacitors with High Volumetric Capacitance and the Synergistic Effect Between Nitrogen Configuration and Supercapacitive Performance[J]. Electrochim Acta, 2016,218:32-40. doi: 10.1016/j.electacta.2016.09.096
38. [38]
  Du X S, Liu H Y, Mai Y W. Facile Chemical Synthesis of Nitrogen-doped Graphene Sheets and their Electrochemical Capacitance[J]. J Power Sources, 2013,241(241):460-466.
39. [39]
  Lee J W, Ko J M, Kim J D. Hydrothermal Preparation of Nitrogen-doped Graphene Sheets via Hexamethylenetetramine for Application as Supercapacitor Electrodes[J]. Electrochim Acta, 2012,85(1):459-466.
40. [40]
  Cai D D, Wang S Q, Lian P C. Superhigh Capacity and Rate Capability of High-level Nitrogen-doped Graphene Sheets as Anode Materials for Lithium-Ion Batteries[J]. Electrochim Acta, 2013,90(5):492-497.
41. [41]
  GAO Yunlei, ZHAO Donglin, BAI Lizhong. Electrochemical Performance of Nitrogen-doped Graphene as Anode Material for Lithium Ion Batteries[J]. China Sciencepaper, 2012,7(6):413-441.
42. [42]
  Liu X W, Wu Y, Yang Z Z. Nitrogen-doped 3D Macroporous Graphene Frameworks as Anode for High Performance Lithium-Ion Batteries[J]. J Power Sources, 2015,293:799-805. doi: 10.1016/j.jpowsour.2015.05.074
43. [43]
  Jiang Z Q, Jiang Z J, Tian X N. Nitrogen-doped Graphene Hollow Microspheres as an Efficient Electrode Material for Lithium Ion Batteries[J]. Electrochim Acta, 2014,146:455-463. doi: 10.1016/j.electacta.2014.09.069
44. [44]
  Yang C N, Qing Y Q, An K. Facile Synthesis of the N-Doped Graphene/Nickel Oxide with Enhanced Electrochemical Performance for Rechargeable Lithium-Ion Batteries[J]. Mater Chem Phys, 2017,195:149-156. doi: 10.1016/j.matchemphys.2017.04.029
45. [45]
  Wang G X, Su D W, Kim H S. A Study of Pt_xCo_y Alloy Nanoparticles as Cathode Catalysts for Lithium-Air Batteries with Improved Catalytic Activity[J]. J Power Sources, 2013,244(4):488-493.
46. [46]
  Wang J J, Li Y J, Sun X L. Challenges and Opportunities of Nanostructured Materials for Aprotic Rechargeable Lithium-Air Batteries[J]. Nano Energy, 2013,2(4):443-467. doi: 10.1016/j.nanoen.2012.11.014
47. [47]
  Li Y L, Wang J J, Li X F. Nitrogen-doped Graphene Nanosheets as Cathode Materials with Excellent Electrocatalytic Activity for High Capacity Lithium-oxygen Batteries[J]. Electrochem Commun, 2012,18(1):12-15.
48. [48]
  Leng L M, Li J, Zeng X Y. Enhancing the Cyclability of Li-O₂ Batteries using PdM Alloy Nanoparticles Anchored on Nitrogen-doped Reduced Graphene as the Cathode Catalyst[J]. J Power Sources, 2017,337:173-179. doi: 10.1016/j.jpowsour.2016.10.089
49. [49]
  Williford R E, Zhang J G. Air Electrode Design for Sustained High Power Operation of Li/Air Batteries[J]. J Power Sources, 2009,194(2):1164-1170. doi: 10.1016/j.jpowsour.2009.06.005
50. [50]
  Wang M Y, Huang Y, Chen X F. Synthesis of Nitrogen and Sulfur Co-doped Graphene Supported Hollow ZnFe₂O₄ Nanosphere Composites for Application in Lithium-Ion Batteries[J]. J Alloys Compd, 2017,691:407-415. doi: 10.1016/j.jallcom.2016.08.285
51. [51]
  Xiang M W, Wang Y, Wu J H. Natural Silk Cocoon Derived Nitrogen-doped Porous Carbon Nanosheets for High Performance Lithium-Sulfur Batteries[J]. Electrochim Acta, 2017,227:7-16. doi: 10.1016/j.electacta.2016.11.139
52. [52]
  Li L, Zhou G M, Yin L C. Stabilizing Sulfur Cathodes Using Nitrogen-doped Graphene as a Chemical Immobilizer for Li-S Batteries[J]. Carbon, 2016,108:120-126. doi: 10.1016/j.carbon.2016.07.008
53. [53]
  Yin L C, Liang J, Zhou G M. Understanding the Interactions Between Lithium Polysulfides and N-Doped Graphene Using Density Functional Theory Calculations[J]. Nano Energy, 2016,25:203-210.
1. [1]
  Zhaomei LIU , Wenshi ZHONG , Jiaxin LI , Gengshen HU . Preparation of nitrogen-doped porous carbons with ultra-high surface areas for high-performance supercapacitors. Chinese Journal of Inorganic Chemistry, 2024, 40(4): 677-685. doi: 10.11862/CJIC.20230404
2. [2]
  Jin CHANG . Supercapacitor performance and first-principles calculation study of Co-doping Ni(OH)₂. Chinese Journal of Inorganic Chemistry, 2024, 40(9): 1697-1707. doi: 10.11862/CJIC.20240108
3. [3]
  Qiqi Li , Su Zhang , Yuting Jiang , Linna Zhu , Nannan Guo , Jing Zhang , Yutong Li , Tong Wei , Zhuangjun Fan . 前驱体机械压实制备高密度活性炭及其致密电容储能性能. Acta Physico-Chimica Sinica, 2025, 41(3): 2406009-. doi: 10.3866/PKU.WHXB202406009
4. [4]
  Qingtang ZHANG , Xiaoyu WU , Zheng WANG , Xiaomei WANG . Performance of nano Li₂FeSiO₄/C cathode material co-doped by potassium and chlorine ions. Chinese Journal of Inorganic Chemistry, 2024, 40(9): 1689-1696. doi: 10.11862/CJIC.20240115
5. [5]
  Zhihuan XU , Qing KANG , Yuzhen LONG , Qian YUAN , Cidong LIU , Xin LI , Genghuai TANG , Yuqing LIAO . Effect of graphene oxide concentration on the electrochemical properties of reduced graphene oxide/ZnS. Chinese Journal of Inorganic Chemistry, 2024, 40(7): 1329-1336. doi: 10.11862/CJIC.20230447
6. [6]
  Jiahong ZHENG , Jingyun YANG . Preparation and electrochemical properties of hollow dodecahedral CoNi₂S₄ supported by MnO₂ nanowires. Chinese Journal of Inorganic Chemistry, 2024, 40(10): 1881-1891. doi: 10.11862/CJIC.20240170
7. [7]
  Yanhui XUE , Shaofei CHAO , Man XU , Qiong WU , Fufa WU , Sufyan Javed Muhammad . Construction of high energy density hexagonal hole MXene aqueous supercapacitor by vacancy defect control strategy. Chinese Journal of Inorganic Chemistry, 2024, 40(9): 1640-1652. doi: 10.11862/CJIC.20240183
8. [8]
  Huayan Liu , Yifei Chen , Mengzhao Yang , Jiajun Gu . 二维材料基超级电容器的容量与倍率性能提升策略. Acta Physico-Chimica Sinica, 2025, 41(6): 100063-. doi: 10.1016/j.actphy.2025.100063
9. [9]
  Yuting ZHANG , Zunyi LIU , Ning LI , Dongqiang ZHANG , Shiling ZHAO , Yu ZHAO . Nickel vanadate anode material with high specific surface area through improved co-precipitation method: Preparation and electrochemical properties. Chinese Journal of Inorganic Chemistry, 2024, 40(11): 2163-2174. doi: 10.11862/CJIC.20240204
10. [10]
  Jiahong ZHENG , Jiajun SHEN , Xin BAI . Preparation and electrochemical properties of nickel foam loaded NiMoO₄/NiMoS₄ composites. Chinese Journal of Inorganic Chemistry, 2024, 40(3): 581-590. doi: 10.11862/CJIC.20230253
11. [11]
  Yifeng Xu , Jiquan Liu , Bin Cui , Yan Li , Gang Xie , Ying Yang . “Xiao Li’s School Adventures: The Working Principles and Safety Risks of Lithium-ion Batteries”. University Chemistry, 2024, 39(9): 259-265. doi: 10.12461/PKU.DXHX202404009
12. [12]
  Siyu Zhang , Kunhong Gu , Bing'an Lu , Junwei Han , Jiang Zhou . Hydrometallurgical Processes on Recycling of Spent Lithium-lon Battery Cathode: Advances and Applications in Sustainable Technologies. Acta Physico-Chimica Sinica, 2024, 40(10): 2309028-. doi: 10.3866/PKU.WHXB202309028
13. [13]
  Qi Li , Pingan Li , Zetong Liu , Jiahui Zhang , Hao Zhang , Weilai Yu , Xianluo Hu . Fabricating Micro/Nanostructured Separators and Electrode Materials by Coaxial Electrospinning for Lithium-Ion Batteries: From Fundamentals to Applications. Acta Physico-Chimica Sinica, 2024, 40(10): 2311030-. doi: 10.3866/PKU.WHXB202311030
14. [14]
  Aoyu Huang , Jun Xu , Yu Huang , Gui Chu , Mao Wang , Lili Wang , Yongqi Sun , Zhen Jiang , Xiaobo Zhu . Tailoring Electrode-Electrolyte Interfaces via a Simple Slurry Additive for Stable High-Voltage Lithium-Ion Batteries. Acta Physico-Chimica Sinica, 2025, 41(4): 100037-. doi: 10.3866/PKU.WHXB202408007
15. [15]
  Kuaibing Wang , Honglin Zhang , Wenjie Lu , Weihua Zhang . Experimental Design and Practice for Recycling and Nickel Content Detection from Waste Nickel-Metal Hydride Batteries. University Chemistry, 2024, 39(11): 335-341. doi: 10.12461/PKU.DXHX202403084
16. [16]
  Xueyu Lin , Ruiqi Wang , Wujie Dong , Fuqiang Huang . 高性能双金属氧化物负极的理性设计及储锂特性. Acta Physico-Chimica Sinica, 2025, 41(3): 2311005-. doi: 10.3866/PKU.WHXB202311005
17. [17]
  Junke LIU , Kungui ZHENG , Wenjing SUN , Gaoyang BAI , Guodong BAI , Zuwei YIN , Yao ZHOU , Juntao LI . Preparation of modified high-nickel layered cathode with LiAlO₂/cyclopolyacrylonitrile dual-functional coating. Chinese Journal of Inorganic Chemistry, 2024, 40(8): 1461-1473. doi: 10.11862/CJIC.20240189
18. [18]
  Yuanchao LI , Weifeng HUANG , Pengchao LIANG , Zifang ZHAO , Baoyan XING , Dongliang YAN , Li YANG , Songlin WANG . Effect of heterogeneous dual carbon sources on electrochemical properties of LiMn_0.8Fe_0.2PO₄/C composites. Chinese Journal of Inorganic Chemistry, 2024, 40(4): 751-760. doi: 10.11862/CJIC.20230252
19. [19]
  Xinpeng LIU , Liuyang ZHAO , Hongyi LI , Yatu CHEN , Aimin WU , Aikui LI , Hao HUANG . Ga₂O₃ coated modification and electrochemical performance of Li_1.2Mn_0.54Ni_0.13Co_0.13O₂ cathode material. Chinese Journal of Inorganic Chemistry, 2024, 40(6): 1105-1113. doi: 10.11862/CJIC.20230488
20. [20]
  Guanghui SUI , Yanyan CHENG . Application of rice husk-based activated carbon-loaded MgO composite for symmetric supercapacitors. Chinese Journal of Inorganic Chemistry, 2025, 41(3): 521-530. doi: 10.11862/CJIC.20240221

Get Citation

PDF

XML

Metrics

PDF Downloads(3)
Abstract views(1669)
HTML views(124)

通讯作者: 陈斌, bchen63@163.com

1.
沈阳化工大学材料科学与工程学院沈阳 110142