Performance, stability and operation voltage optimization of screen-printed aqueous supercapacitors

Harvesting micropower energy from the ambient environment requires an intermediate energy storage, for which printed aqueous supercapacitors are well suited due to their low cost and environmental friendliness. In this work, a systematic study of a large set of devices is used to investigate the effect of process variability and operating voltage on the performance and stability of screen printed aqueous supercapacitors. The current collectors and active layers are printed with graphite and activated carbon inks, respectively, and aqueous NaCl used as the electrolyte. The devices are characterized through galvanostatic discharge measurements for quantitative determination of capacitance and equivalent series resistance (ESR), as well as impedance spectroscopy for a detailed study of the factors contributing to ESR. The capacitances are 200–360 mF and the ESRs 7.9–12.7 Ω, depending on the layer thicknesses. The ESR is found to be dominated by the resistance of the graphite current collectors and is compatible with applications in low-power distributed electronics. The effects of different operating voltages on the capacitance, leakage and aging rate of the supercapacitors are tested, and 1.0 V found to be the optimal choice for using the devices in energy harvesting applications.

[1]  Meryl D. Stoller,et al.  Review of Best Practice Methods for Determining an Electrode Material's Performance for Ultracapacitors , 2010 .

[2]  Roberto Passerone,et al.  Towards Extending Sensor Node Lifetime with Printed Supercapacitors , 2012, EWSN.

[3]  Yi Cui,et al.  Printed energy storage devices by integration of electrodes and separators into single sheets of paper , 2010 .

[4]  F. Smits.  Measurement of sheet resistivities with the four-point probe , 1958 .

[5]  P. Taberna,et al.  Anomalous Increase in Carbon Capacitance at Pore Sizes Less Than 1 Nanometer , 2006, Science.

[6]  H. Andreas,et al.  Self-Discharge in Electrochemical Capacitors: A Perspective Article , 2015 .

[7]  J. Vanhala,et al.  Screen-Printed Stretchable Interconnects , 2016, 2016 IEEE 66th Electronic Components and Technology Conference (ECTC).

[8]  Young Hee Lee,et al.  Electrochemical Properties of High-Power Supercapacitors Using Single-Walled Carbon Nanotube Electrodes , 2001 .

[9]  Sunghun Cho,et al.  Screen-Printable and Flexible RuO2 Nanoparticle-Decorated PEDOT:PSS/Graphene Nanocomposite with Enhanced Electrical and Electrochemical Performances for High-Capacity Supercapacitor. , 2015, ACS applied materials & interfaces.

[10]  F. Béguin,et al.  Carbon materials for the electrochemical storage of energy in capacitors , 2001 .

[11]  Sampo Tuukkanen,et al.  Flexible Piezoelectric Energy Harvesting Circuit With Printable Supercapacitor and Diodes , 2014, IEEE Transactions on Electron Devices.

[12]  V. Ruiz,et al.  Long-term cycling of carbon-based supercapacitors in aqueous media , 2009 .

[13]  Alicia M. Oickle,et al.  Examination of Water Electrolysis and Oxygen Reduction As Self-Discharge Mechanisms for Carbon-Based, Aqueous Electrolyte Electrochemical Capacitors , 2011 .

[14]  Lei Zhang,et al.  A review of electrode materials for electrochemical supercapacitors. , 2012, Chemical Society reviews.

[15]  B. Conway.  Electrochemical Supercapacitors: Scientific Fundamentals and Technological Applications , 1999 .

[16]  James W. Evans,et al.  Organic solar cells and fully printed super-capacitors optimized for indoor light energy harvesting , 2016 .

[17]  John B. Goodenough,et al.  Supercapacitor Behavior with KCl Electrolyte , 1999 .

[18]  F. Béguin,et al.  A symmetric carbon/carbon supercapacitor operating at 1.6 V by using a neutral aqueous solution , 2010 .

[19]  Kirsi Tappura,et al.  Printed environmentally friendly supercapacitors with ionic liquid electrolytes on paper , 2014 .

[20]  Daniel A. Steingart,et al.  Tailoring Electrochemical Capacitor Energy Storage Using Direct Write Dispenser Printing , 2008 .

[21]  L. Nyholm,et al.  Asymmetric and symmetric supercapacitors based on polypyrrole and activated carbon electrodes , 2015 .

[22]  R. Kötz,et al.  Cycle versus voltage hold – Which is the better stability test for electrochemical double layer capacitors? , 2013 .

[23]  Qiao Chen,et al.  Effect of different gel electrolytes on graphene-based solid-state supercapacitors , 2014 .

[24]  Jari Suikkola.  Printed Stretchable Interconnects for Wearable Health and Wellbeing Applications , 2015 .

[25]  R. Kötz,et al.  Principles and applications of electrochemical capacitors , 2000 .

[26]  Pierre-Louis Taberna,et al.  Modification of Al current collector surface by sol–gel deposit for carbon–carbon supercapacitor applications , 2004 .

[27]  Sampo Tuukkanen,et al.  Low-cost, solution processable carbon nanotube supercapacitors and their characterization , 2014 .

[28]  A. Lewandowski,et al.  Performance of carbon–carbon supercapacitors based on organic, aqueous and ionic liquid electrolytes , 2010 .

[29]  Kari Halonen,et al.  Performance of printable supercapacitors in an RF energy harvesting circuit , 2014 .

[30]  P. Taberna,et al.  Electrochemical Characteristics and Impedance Spectroscopy Studies of Carbon-Carbon Supercapacitors , 2003 .

[31]  K. Lian,et al.  Knitted and screen printed carbon-fiber supercapacitors for applications in wearable electronics , 2013 .

[32]  Salme Jussila,et al.  Printed supercapacitors on paperboard substrate , 2012 .

[33]  Rudolf Holze,et al.  Screen Printed Asymmetric Supercapacitors based on LiCoO2 and Graphene Oxide , 2014 .

[34]  Sampo Tuukkanen,et al.  Architectural modifications for flexible supercapacitor performance optimization , 2016, Electronic Materials Letters.

[35]  E. Lust,et al.  Physical and electrochemical characteristics of supercapacitors based on carbide derived carbon electrodes in aqueous electrolytes , 2011 .

[36]  V. Ruiz,et al.  Voltage dependence of carbon-based supercapacitors for pseudocapacitance quantification , 2013 .

[37]  F. Béguin,et al.  Exploring the large voltage range of carbon/carbon supercapacitors in aqueous lithium sulfate electrolyte , 2012 .