Conductive polypyrrole incorporated nanocellulose/MoS₂ film for preparing flexible supercapacitor electrodes

Abstract

Conductive films have emerged as appealing electrode materials in flexible supercapacitors owing to their conductivity and mechanical flexibility. However, the unsatisfactory electrode structure induced poor output performance and undesirable cycling stability limited their application. Herein, a well-designed film was manufactured by the vacuum filtration and in-situ polymerization method from cellulose nanofibrils (CNFs), molybdenum disulfide (MoS₂), and polypyrrole. The electrode presented an outstanding mechanical strength (21.3 MPa) and electrical conductivity (9.70 S·cm⁻¹). Meanwhile, the introduce of hydrophilic CNFs induced a desirable increase in diffusion path of electrons and ions, along with the synergistic effect among the three components, further endowed the electrode with excellent specific capacitance (0.734 F·cm⁻²) and good cycling stability (84.50% after 2000 charge/discharge cycles). More importantly, the flexible all-solid-state symmetric supercapacitor delivered a high specific capacitance (1.39 F·cm⁻² at 1 mA·cm⁻²) and a volumetric energy density (6.36 mW·h·cm⁻³ at the power density of 16.35 mW·cm⁻³). This work provided a method for preparing composite films with desired mechanical and electrochemical performance, which can broaden the high-value applications of nanocellulose.

Graphical abstract

Keywords

cellulose nanofibril / molybdenum disulfide / polypyrrole / flexible supercapacitor

References

[1] Wang T, Chen S, Pang H, . MoS₂-based nanocomposites for electrochemical energy storage. Advanced Science, 2017, 4(2): 1600289

[2] Dubal D P C, Chodankar N R, Kim D H, . Towards flexible solid-state supercapacitors for smart and wearable electronics. Chemical Society Reviews, 2018, 47(6): 2065–2129

[3] Pendashteh A, Mousavi M F, Rahmanifar M S. Fabrication of anchored copper oxide nanoparticles on graphene oxide nanosheets via an electrostatic coprecipitation and its application as supercapacitor. Electrochimica Acta, 2013, 88: 347–357

[4] Li S, Huang D, Yang J, . Freestanding bacterial cellulose–polypyrrole nanofibres paper electrodes for advanced energy storage devices. Nano Energy, 2014, 9: 309–317

[5] Salanne M, Rotenberg B, Naoi K, . Efficient storage mechanisms for building better supercapacitors. Nature Energy, 2016, 1(6): 16070

[6] Nyholm L, Nyström G, Mihranyan A, . Toward flexible polymer and paper-based energy storage devices. Advanced Materials, 2011, 23(33): 3751–3769

[7] Matte H S S R, Gomathi A, Manna A K, . MoS₂ and WS₂ analogues of graphene. Angewandte Chemie International Edition, 2010, 49(24): 4059–4062

[8] Wang G, Bi X, Yue H, . Sacrificial template synthesis of hollow C@MoS₂@PPy nanocomposites as anodes for enhanced sodium storage performance. Nano Energy, 2019, 60: 362–370

[9] Ma G, Peng H, Mu J, . In situ intercalative polymerization of pyrrole in graphene analogue of MoS₂ as advanced electrode material in supercapacitor. Journal of Power Sources, 2013, 229: 72–78

[10] Tian Y, Song X, Liu J, . Generation of monolayer MoS₂ with 1T Phase by spatial-confinement-induced ultrathin PPy anchoring for high-performance supercapacitor. Advanced Materials Interfaces, 2019, 6(10): 1900162

[11] Cao W, Ma C, Tan S, . Ultrathin and flexible CNTs/MXene/cellulose nanofibrils composite paper for electromagnetic interference shielding. Nano-Micro Letters, 2019, 11(1): 72

[12] Cao W T, Chen F F, Zhu Y J, . Binary strengthening and toughening of MXene cellulose nanofiber composite paper with nacre-inspired structure and superior electromagnetic interference shielding properties. ACS Nano, 2018, 12(5): 4583–4593

[13] Cao W, Ma C, Mao D, . MXene-reinforced cellulose nanofibril inks for 3D-printed smart fibres and textiles. Advanced Functional Materials, 2019, 29(51): 1905898

[14] Zhang F, Tang Y, Yang Y, . In-situ assembly of three-dimensional MoS₂ nanoleaves/carbon nanofiber composites derived from bacterial cellulose as flexible and binder-free anodes for enhanced lithium-ion batteries. Electrochimica Acta, 2016, 211: 404–410

[15] Yang L, Mukhopadhyay A, Jiao Y, . Ultralight, highly thermally insulating and fire resistant aerogel by encapsulating cellulose nanofibers with two-dimensional MoS₂. Nanoscale, 2017, 9(32): 11452–11462

[16] Du X, Zhang Z, Liu W, . Nanocellulose-based conductive materials and their emerging applications in energy devices — A review. Nano Energy, 2017, 35: 299–320

[17] Wang Z, Tammela P, Strømme M, . Cellulose-based supercapacitors: material and performance considerations. Advanced Energy Materials, 2017, 7(18): 1700130

[18] Wan C, Jiao Y, Li J. Flexible, highly conductive, and free-standing reduced graphene oxide/polypyrrole/cellulose hybrid papers for supercapacitor electrodes. Journal of Materials Chemistry A: Materials for Energy and Sustainability, 2017, 5(8): 3819–3831

[19] Ma C, Cao W, Xin W, . Flexible and free-standing reduced graphene oxide and polypyrrole coated air-laid paper-based supercapacitor electrodes. Industrial & Engineering Chemistry Research, 2019, 58(27): 12018–12027

[20] Fu Q, Wang Y, Liang S, . High-performance flexible freestanding polypyrrole-coated CNF film electrodes for all-solid-state supercapacitors. Journal of Solid State Electrochemistry, 2020, 24(3): 533–544

[21] Huang K, Wang L, Liu Y, . Synthesis of polyaniline/2-dimensional graphene analog MoS₂ composites for high-perform-ance supercapacitor. Electrochimica Acta, 2013, 109: 587–594

[22] Wang D, Li Y X, Shi Z, . Spontaneous growth of free-standing polypyrrole films at an air/ionic liquid interface. Langmuir, 2010, 26(18): 14405–14408

[23] Xu J, Wang D, Yuan Y, . Polypyrrole/reduced graphene oxide coated fabric electrodes for supercapacitor application. Organic Electronics, 2015, 24: 153–159

[24] Oh S Y, Yoo D I, Shin Y, . Crystalline structure analysis of cellulose treated with sodium hydroxide and carbon dioxide by means of X-ray diffraction and FTIR spectroscopy. Carbohydrate Research, 2005, 340(15): 2376–2391

[25] Lei J, Lu X, Nie G, . One-pot synthesis of algae-like MoS₂/PPy nanocomposite: A synergistic catalyst with superior peroxi-dase-like catalytic activity for H₂O₂ detection. Particle & Particle Systems Characterization, 2015, 32(9): 886–892

[26] Yuan L, Yao B, Hu B, . Polypyrrole-coated paper for flexible solid-state energy storage. Energy & Environmental Science, 2013, 6(2): 470

[27] Omastova M, Trchova M, Kovarova J, . Synthesis and structural study of polypyrroles prepared in the presence of surfactants. Synthetic Metals, 2003, 138(3): 447–455

[28] Peng H, Ma G, Ying W, . In situ synthesis of polyaniline/sodium carboxymethyl cellulose nanorods for high-performance redox supercapacitors. Journal of Power Sources, 2012, 211: 40–45

[29] Cadot S, Renault O, Frégnaux M, . A novel 2-step ALD route to ultra-thin MoS₂ films on SiO₂ through a surface organometallic intermediate. Nanoscale, 2017, 9(2): 538–546

[30] Yuan L, Yao B, Hu B, . Polypyrrole-coated paper for flexible solid-state energy storage. Energy & Environmental Science, 2013, 6(2): 470

[31] Guan S, Fu X, Lao Z, . NiS–MoS₂ hetero-nanosheet arrays on carbon cloth for high-performance flexible hybrid energy storage devices. ACS Sustainable Chemistry & Engineering, 2019, 7(13): 11672–11681

[32] Peng S, Fan L, Wei C, . Flexible polypyrrole/copper sulfide/bacterial cellulose nanofibrous composite membranes as supercapacitor electrodes. Carbohydrate Polymers, 2017, 157: 344–352

[33] Wang G, Bi X, Yue H, . Sacrificial template synthesis of hollow C@MoS₂@PPy nanocomposites as anodes for enhanced sodium storage performance. Nano Energy, 2019, 60: 362–370

[34] Wang Z, Carlsson D O, Tammela P, . Surface modified nanocellulose fibers yield conducting polymer-based flexible supercapacitors with enhanced capacitances. ACS Nano, 2015, 9(7): 7563–7571

[35] Ge Y, Jalili R, Wang C, . A robust free-standing MoS₂/poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) film for supercapacitor applications. Electrochimica Acta, 2017, 235: 348–355

[36] Yao B, Yuan L, Xiao X, . Paper-based solid-state supercapacitors with pencil-drawing graphite/polyaniline networks hybrid electrodes. Nano Energy, 2013, 2(6): 1071–1078

[37] Wang L, Yang H, Liu X, . Constructing hierarchical tectorum-like α-Fe₂O₃/PPy nanoarrays on carbon cloth for solid-state asymmetric supercapacitors. Angewandte Chemie International Edition, 2017, 56(4): 1105–1110

[38] VahidMohammadi A, Mojtabavi M, Caffrey N M, . Assembling 2D MXenes into highly stable pseudocapacitive electrodes with high power and energy densities. Advanced Materials, 2019, 31(8): 1806931

[39] Xiao Y, Huang L, Zhang Q, . Gravure printing of hybrid MoS₂@S-rGO interdigitated electrodes for flexible microsupercapacitors. Applied Physics Letters, 2015, 107(1): 013906

Acknowledgements

Financial supports from the National Key R&D Program of China (2019YFC1905901), the Beijing Forestry University Outstanding Young Talent Cultivation Project (2019JQ03014), and the Key Production Innovative Development Plan of the Southern Bingtuan (2019DB007) are gratefully acknowledged.

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