In Situ Synthesis of Nitrogen- and Sulfur-Enriched Hierarchical Porous

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In Situ Synthesis of Nitrogen and Sulfur enriched Hierarchical Porous Carbon for high-Performance Supercapacitor Rupali Shaligram Mehare, Suresha P. Ranganath, Vikash Chaturvedi, Manohar V. Badiger, and Manjusha V. Shelke Energy Fuels, Just Accepted Manuscript • DOI: 10.1021/acs.energyfuels.7b02305 • Publication Date (Web): 05 Dec 2017 Downloaded from http://pubs.acs.org on December 8, 2017

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Energy & Fuels

In Situ Synthesis of Nitrogen and Sulfur enriched Hierarchical Porous Carbon for high-Performance Supercapacitor Rupali S. Mehare†, §, Suresha P.Ranganath ‡, Vikash Chaturvedi†, Manohar. V. Badiger‡, § and Manjusha V. Shelke*†, §, ┴ †

Physical and Materials Chemistry Division, CSIR-National Chemical Laboratory, Pune-

411008, MH, India. §

Academy of Scientific and Innovative Research (AcSIR), Chennai 600113, TN, India.



Polymer Science and Engineering Division, CSIR-National Chemical Laboratory, Pune-411008,

MH, India. ┴

CSIR-Network Institute for Solar Energy, CSIR-National Chemical Laboratory, Pune-411008,

MH, India. E-mail: [email protected] KEYWORDS 3D sponge; Polymer; Pyrolysis; N and S doped porous carbon; Capacitance; Energy storage.

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ABSTRACT

In this work, we present a simple and facile method for the Nitrogen (N) and Sulfur (S) doped porous three-dimensional (3D) sponge-like carbon materials via direct pyrolysis of N and S containing polymer N,N'- Methylene-bis-acrylamide cross-linked Poly(Acrylamide-co-2acrylamido-2-methyl-1-propanesulfonic acid) at varying temperatures under inert atmosphere. The obtained nitrogen and sulfur doped porous carbons (NSPCs) possess 3D hierarchical porous structure and contain significantly high amount of N and S species. The concurrent incorporation of N and S successfully modified the surface properties of carbon materials and lead to enhanced capacitive performance. The presented NSPC exhibits specific capacitance of 230 Fg-1 at a current density of 1 Ag-1 and showed excellent cycling stability, depicting as a promising material for energy storage devices.

1. INTRODUCTION Electrochemical supercapacitors or ultracapacitors are one of the energy storage devices that store energy in the form of electrical charges and much appreciated because of their simple working principle, high power density, rapid charging-discharging rate and long cycle life1–6, As compared to the batteries and conventional capacitors, supercapacitor has higher power densities and energy densities respectively7. According to the electrical energy storage mechanisms, the supercapacitor can be categorized into electrical double layer capacitor (EDLC), wherein the charges are stored in the double layer at the interface between electrode and electrolyte8,9. EDLCs mostly use carbon materials like porous activated carbons10, carbon aerogels11, and

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carbon nanotubes12 etc as an electrode material. Another charge storage mechanism in these devices is based on the reversible faradaic redox reactions of electroactive species present on the electrode surface13,14. Electrode materials involved in this are transition metal oxides, nitrides, carbides15,16 and conducting polymers17. In spite of the much popularity of porous carbonaceous materials as high surface area electrode materials, their specific capacity is restricted as the charges are stored only by adsorption/desorption of electrolyte ions at the electrode surface. Well developed pore structure can increase surface area as well as specific capacity of porous carbon up to certain extent. Though the specific capacitance of porous carbon normally increases with increase in surface area, it is not a linear relation always and pore size distribution affects their specific capacitance significantly18. It is also demonstrated that presence of micropores (