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Smart Pillared Carbon Materials for Supercapacitors: from fundamental understanding of ion transport to device testing – SPICS

An all-solid supercapacitor enabled by pillared graphene

A gain in capacity of EDLC is expected to be enabled by the use of pillared graphene with controlled 2D porosities, in standard electrolyte medium, but also in ionic liquid, opening the way to manufacture an all-solid-state supercapacitor with enhanced storage properties.

Pillared graphene for all-solid EDLC: between optimization and understanding of charge transfer phenomena, in standard electrolytes up to ionogels

The objectives of the SPICS project are to develop and characterize 3D carbon materials for supercapacitors, designed from graphene sheets assembled using molecular pillars playing an active role in storage processes. The properties of polarity, redox or the poly-electrolytic nature of these pillars, will decrease the resistance of ionic transport and promote the adsorption of electrolytic species. The study of electrochemical performances will be carried out in standard electrolytes, then in ionic liquids. The materials will be studied with several advanced characterization techniques (some of which are operando or in-situ) in order to answer new questions concerning the kinetics of charge transfer according to the nature of the pillars. These combined advanced characterizations will enable to further optimize the materials and will lead to the selection of the best material-electrolyte pair, based on the capacitance values, the ionic and electronic transfer rate constants, etc. This material-electrolyte pair will be used to develop a complete all-solid device consisting of an electrode / electrolyte material embedded in a solid matrix (ionogel).

The 1st tasks of the project will deal with the preparation and characterization of expanded graphene materials made from new pillars, as well as with the development of SECM observation procedures on standard materials.
In a second step, the first materials will be tested electrochemically in aqueous-, CH3CN-based electrolytes, and then in electrolytes based on ionic liquids.
Advanced characterization studies will then be started on reference samples derived from graphene, then on pillared graphenes, and will continue throughout the project, in standard or LI electrolytes.
The physicochemical, morphological and mechanistic information acquired will, in turn, help to optimize further the materials or their formulations.
The electrochemical results enable to select the most efficient material-electrolyte pair, on the basis of the highest capacitance values, ionic and electronic transfer rate constants, etc. This material-electrolyte pair will be used to develop a complete all-solid device consisting of an electrode / electrolyte material embedded in a solid matrix (ionogel).

After 6 months, the scientific part of the project started according to the planned schedule with the following achievements: 1) the first pillared graphene samples were produced, 2) a study on the reduction of graphene oxide is conducted, and will be transferred to the reduction of pillared graphene, and 3) the reference sample SECM observation conditions have been developed.

The perspectives will follow the course defined initially, with in particular in the short term the first electrochemical studies on pillared graphene.

Poster Graphene 2021

The wide goal of SPICS project is to provide enhanced electrode materials for supercapacitor application.
SPICS aims at developing innovative 2D carbon layered materials with enhanced storage capability thanks to the use of redox active pillars. We aim to reach volumetric capacitance of about 400 F/cm3. The original idea of SPICS is to go beyond the use of simple mechanical pillars and to introduce redox functionality to enhance specific interactions with the electrolyte leading to improved charge storage capability. To achieve this goal, an important part of the project will be devoted to an in-depth analysis of the charge compensation mechanisms through the use and development of cutting-edge characterization techniques. Indeed, these fundamental investigations based on ss-NMR and DNP, SECM (Scanning Electrochemical Microscope) and QCM derived techniques (conventional EQCM, QCM coupled with EIS and QCM coupled to electroacoustic impedance) will be undertaken to understand the impact of these active pillars on the dynamics of ion transfer at the electrode/electrolyte interface, on kinetic rate transfer constants and on faradic reactions occurrences, and will also allow to evaluate the electromechanical and structural stress experienced by the material during cycling. For the electrochemical evaluations, different electrolytes will be tested (from ammoniums salt in CH3CN to ionic liquids-based electrolytes). This tight relation between material development, advanced characterization and electrochemical evaluation will lead to the establishment of a virtuous circle resulting in a major breakthrough in correlating electroadsorption/charge transfer phenomena to smart 2D carbon materials properties, enabling the design of refined material and the selection of the most promising ones. The best material will also be tested with a solid-state electrolyte based on the use of ionogel. Supercapacitors with performances at the state of the art are expected to be achieved with these innovative 2D smart carbon materials, capacitances as high as 300 F/g and 400 F/cm3 with 90% charge retention over 10 000 cycles. Hence SPICS bridges fundamental mechanisms understandings efforts to preliminary tests responding to an important societal demand.
The development and optimization of these next generation active pillared graphene materials will be enabled a close partnership between CEA, CIRIMAT and LISE. The expertise and complementarity of the 3 partners - in graphene–based materials developments, ss-NMR analysis of modified samples, electrochemical material characterization, advanced and SECM techniques - are fundamental to the success of the project. Indeed, the skills and know-how of each partners are highly relevant and necessary to address the project WPs inter-connexion, to allow an efficient project progression, to finally achieve the objectives stated above.

Project coordination


The author of this summary is the project coordinator, who is responsible for the content of this summary. The ANR declines any responsibility as for its contents.


CSE Chimie du solide et énergie

Help of the ANR 600,221 euros
Beginning and duration of the scientific project: January 2020 - 48 Months

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