PL440516A1 - Electrochemical capacitor with high cyclic durability - Google Patents

Electrochemical capacitor with high cyclic durability Download PDF

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PL440516A1
PL440516A1 PL440516A PL44051622A PL440516A1 PL 440516 A1 PL440516 A1 PL 440516A1 PL 440516 A PL440516 A PL 440516A PL 44051622 A PL44051622 A PL 44051622A PL 440516 A1 PL440516 A1 PL 440516A1
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mol
electrolyte
electrochemical capacitor
urea
capacitor
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PL440516A
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PL246396B1 (en
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Elżbieta FRĄCKOWIAK
Sara Azmi
Amelia Klimek
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Politechnika Poznanska
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    • HELECTRICITY
    • H01ELECTRIC ELEMENTS
    • H01GCAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES, LIGHT-SENSITIVE OR TEMPERATURE-SENSITIVE DEVICES OF THE ELECTROLYTIC TYPE
    • H01G9/00Electrolytic capacitors, rectifiers, detectors, switching devices, light-sensitive or temperature-sensitive devices; Processes of their manufacture
    • H01G9/004Details
    • H01G9/022Electrolytes; Absorbents
    • HELECTRICITY
    • H01ELECTRIC ELEMENTS
    • H01GCAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES, LIGHT-SENSITIVE OR TEMPERATURE-SENSITIVE DEVICES OF THE ELECTROLYTIC TYPE
    • H01G11/00Hybrid capacitors, i.e. capacitors having different positive and negative electrodes; Electric double-layer [EDL] capacitors; Processes for the manufacture thereof or of parts thereof
    • H01G11/54Electrolytes
    • H01G11/58Liquid electrolytes
    • H01G11/62Liquid electrolytes characterised by the solute, e.g. salts, anions or cations therein
    • HELECTRICITY
    • H01ELECTRIC ELEMENTS
    • H01GCAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES, LIGHT-SENSITIVE OR TEMPERATURE-SENSITIVE DEVICES OF THE ELECTROLYTIC TYPE
    • H01G9/00Electrolytic capacitors, rectifiers, detectors, switching devices, light-sensitive or temperature-sensitive devices; Processes of their manufacture
    • H01G9/004Details
    • H01G9/022Electrolytes; Absorbents
    • H01G9/035Liquid electrolytes, e.g. impregnating materials
    • YGENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02EREDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/13Energy storage using capacitors

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  • Engineering & Computer Science (AREA)
  • Power Engineering (AREA)
  • Chemical & Material Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • Microelectronics & Electronic Packaging (AREA)
  • Electric Double-Layer Capacitors Or The Like (AREA)

Abstract

Przedmiotem zgłoszenia jest kondensator elektrochemiczny o wysokiej trwałości cyklicznej zawierający elektrody z materiału węglowego o rozwiniętej powierzchni właściwej 100 - 2000 m<sup>2</sup>/g oddzielone separatorem i pracujący w elektrolicie stanowiącym roztwór siarczanu litu o stężeniu 1 mol/L. Przy czym elektrolit zawiera dodatek mocznika o stężeniach w zakresie od 0,1 mol/L do 10 mol/L, korzystnie 2 mol/L.The subject of the application is an electrochemical capacitor with high cyclic durability, containing electrodes made of carbon material with a developed specific surface of 100 - 2000 m<sup>2</sup>/g, separated by a separator and operating in an electrolyte consisting of a lithium sulfate solution with a concentration of 1 mol/L. The electrolyte contains the addition of urea with concentrations ranging from 0.1 mol/L to 10 mol/L, preferably 2 mol/L.

Description

Kondensator elektrochemiczny o wysokiej trwalosci cyklicznej Przedmiotem wynalazku jest kondensator elektrochemiczny o wysokiej trwalosci cyklicznej operujacy w roztworze neutralnego elektrolitu (siarczanu litu) z dodatkiem mocznika jako srodka antykorozyjnego i przeciwdzialajacego starzeniu kondensatora. Kondensatory elektrochemiczne (superkondensatory) to uklady gromadzace ladunek na skutek przyciagania elektrostatycznego jonów na granicy faz elektroda/elektrolit Charakteryzuja sie one wysoka moca i dluga zywotnoscia. Sa one odpowiednim zródlem energii wymaganym w krótkim czasie, np. w samolotach (Airbus A380), do zasilania samochodów elektrycznych hybrydowych, windach. Kondensatory pozwalaja takze na odzyskiwanie energii podczas regeneracyjnego hamowania. Moga sluzyc jako zródlo zasilania w przenosneJ elektronice. Kondensatory elektrochemiczne charakteryzuja sie szybkimi procesami ladowania/wyladowania rzedu sekund oraz doskonala cyklicznoscia bez znacznych spadków pojemnosci [lR. Miller, A Burke "Electrochemical capacitors: Challenges and opportunities for real-world applications" Electrochemical Society Interface 17 (2008) 53-57]. Sa one wykorzystywane przede wszystkim w zastosowaniach gdzie wymagana jest duza moc i wzglednie wysoka energia Energia wlasciwa superkondensatora wyrazona wzorem E=lcu" 2 gdzie C to pojemnosc kondensatora elektrochemicznego, a U - nap1ec1e pracy tego urzadzenia, jest kilkukrotnie mniej sza niz energia akumulatora litowo­ j onowego. Stad, prowadzone sa liczne prace nad zwiekszeniem energn kondensatora poprzez poprawe pojemnosci i zwiekszenie napiecia ukladu [Elzbieta Frackowiak "Carbon materialsfor supercapacitor application" Physical Chemistry Chemical Physics 15 (2007) 1774-1785]. Napiecie kondensatora (U) jest determinowane stabilnoscia elektrochemiczna elektrolitu. PL 440516 A1 2/10W srodowisku wodnego elektrolitu (alkalicznego lub kwasowego) napiecie ukladu W)'nosi okolo 1 V. W elektrolicie o neutralnym pH, napiecie kondensatora osiaga wartosci 1,6 V, natomiast w organicznym elektrolicie 2,5 V-2, 7 V. Wykorzystanie materialów elektrodowych i elektrolitów o róznej stabilnosci opisano przez [Krzysztof Fic, Anetta Platek, Justyna Piwek, Elzbieta Frackowiak "Sustainah/e materia/sfor electrochemzca/ capacztors" Materials Today 21 (2018) 437-454]. Wybór elektrolitu oraz optymalnego napiecia pracy kondensatora ma duze znaczenie dla pracy cyklicznej urzadzenia. Po przekroczeniu limitu napiecia obserwuje sie wydzielanie ubocznych produktów gazowych co opisano przez [Minglong He, Krzysztof Fic, Elzbieta Frackowiak, Petr Novak, Erik J. Berg "lttfluem:e uf aqueuus e/ec:t,·u~yte concentratiun on parasitic reaclions in high­ voltage e/ectrochemzcaf capacitors" Energy Storage Materials 5 (2016) 111- 115]. Podczas dzialania kazdego zródla energii obserwujemy stopniowe starzenie sie ukladu. Kondensatory elektrochemiczne równiez charakteryzuja sie spadkiem charakterystyk elektrycznych zwiazanym ze starzeniem [R. German, A. Sari, P. Venet and Y Zitouni "Predictiun lf supercapacitorsjloating ageing with swface electrude inte1:face-based ageing law" Microelectronics Reliability 54 (2014) 1813-1817]. Degradacja kondensatora wiaze sie z wydzielaniem substancji lotnych jako W)'nik rozkladu elektrolitu, formowaniem sie grup fonkcyjnych na powierzchni elektrod, tworzeniem sie osadu nierozpuszczalnych soli, wzrostem oporu i korozja kolektorów pradowych. Dlugotrwala praca cykliczna i przekroczenie limitu napiecia kondensatora czy potencjalu poszczególnych elektrod powoduje przyspieszone starzenie superkondensatora oraz korozje. Organiczne elektrolity oraz ciecze jonowe spelniaja wymagania dlugotrwalej cyklicznosci aczkolwiek posiadaja wiele wad. Sa toksyczne, palne, drogie, wymagaja inertnej atmosfery podczas montazu superkondensatora. Stad tez idea wynalazcza jest wykorzystanie dodatku o dzialaniu antykorozyjnym i przeciwstarzeniowym do elektrolitu wodnego o neutralnym pH. PL 440516 A1 3/10W ten sposób kondensator operujacy na bazie roztworu siarczanu litu z dodatkiem mocznika spelnia cechy ekologicznego, taniego urzadzenia do magazynowania energii. Dodatek mocznika do elektrolitu nie byl dotychczas wykorzystywany w kondensatorach elektrochemicznych. Istota wynalazku jest kondensator elektrochemiczny o wysokiej trwalosci cyklicznej zawierajacy elektrody z materialu weglowego o rozwinietej powierzchni wlasciwej 100 - 2000 m 2 /g oddzielone separatorem i pracujacy w elektrolicie stanowiacym roztwór siarczanu litu o stezeniu 1 mol/L Przy czym elektrolit zawiera dodatek mocznika o stezeniach w zakresie od O, 1 mol/L do 1 O mol/L, korzystnie 2 mol/L. Kondensator wedlug wynalazku jest tani, ekologiczny, me ulega korozji dzieki charakterystycznym cechom elektrolitu, umozliwiajac tym samym dlugotrwala. prace cykliczna. kondensatora. Dzieki zastosowaniu rozwiazania wedlug wynalazku uzyskano nastepujace efekty techniczno-uzytkowe: • napiecie kondensatora równe 1,6-1,8 V; • wysoka cyklicznosc przy zachowaniu stabilnej pojemnosci podczas stalonapieciowej polaryzacji dzieki antykorozyjnemu dzialaniu elektrolitu (10% spadek pojemnosci po 250 h polaryzacji): • bezpieczne uzytkowanie poniewaz elektrolit jest nielotny i niepalny; • uklad jest symetryczny, latwy w konstrukcji me wymaga atmosfery ochronnej, co niezmiernie ulatwia montaz; • neutralne pH elektrolitu pozwala na szeroki wybór kolektorów pradowych, co znacznie redukuje koszt produkcji kondensatora. Wynalazek w przykladzie realizacji przedstawiono na rysunku, gdzie fig. 1 pokazuje schemat ideowy kondensatora elektrochemicznego o wysokiej trwalosci cyklicznej; fig. 2 pokazuje wynik badania cyklicznej woltamperometrii dla ukladu o skladzie elektrolitu I mol/L Li 2S0 4 z dodatkiem mocznika I mol/L; fig. 3 przedstawia wykres dla galwanostatycznego ladowania/wyladowania I A g- 1 w PL 440516 A1 4/10zakresie napiecia od 1,0V do 1,6V dla elektrolitów z róznymi dodatkami mocznika od 0,5 mol/L do 1 O mol/L a fig. 4 pokazuje charakterystyki pracy cyklicznej i retencji pojemnosci dla elektrolitów z róznymi dodatkami mocznika od 0,5 mol/L do 10 mol/L. Kondensator elektrochemiczny o wysokiej trwalosci cyklicznej - co pokazano na fig. I - zawiera dodatnia I i ujemna 2 elektrode Przy czym elektrody I i 2 sa wykonane z materialu weglowego o rozwinietej powierzchni wlasciwej 100 - 2000 m 2 /g i oddzielone separatorem 4. Pracuja one w roztworze 3 siarczanu litu 1 mol/L Li2SO. z dodatkiem mocznika o stezeniach w zakresie od O, 1 mol/L do 10 mol/L, korzystnie 2 mol/L. Przyklad I Elektrody kondensatora elektrochemicznego wykonano z wegla aktywnego, którego powierzchnia wlasciwa wynosila 1500 m 2 g- 1 . Tabletki o srednicy I O mm i grubosci ok 0,2 mm uzyskano przez sprasowanie mieszaniny: 85% wag. materialu weglowego, 1 O~o wag. srodka wiazacego (PTFE) oraz 5°--ó wag. sadzy weglowej (C65). Tak przygotowane i wysuszone elektrody nasaczono elektrolitem w postaci roztworu siarczanu litu 1 mol/L Li2 SO 4 z dodatkiem mocznika od 0,5 do mol/L. Elektrody rozdzielono separatorem z wlókniny szklanej i umieszczono w naczyniu elektrochemicznym. Kondensator elektrochemicznv o skladzie elektrolitu I mol/L Li2SO4 z dodatkiem mocznika 1 mol/L poddano badaniom cyklicznej woltamperometrii 5 mV s- 1 co przedstawiono na fig. 2. Kondensatory elektrochemiczne operujace z róznymi dodatkami mocznika od 0,5 mol/L do 1 O mol/L poddano galwanostatycznemu ladowaniu/wyladowaniu 1 A g- 1 w zakresie napiecia od 1,0V do 1,6V co przedstawiono na fig. 3. Kondensatory wykazywaly wyzsze pojemnosci dla elektrolitu z dodatkiem mocznika. Przyklad II Elektrody kondensatora elektrochemicznego wykonano z wegla aktywnego, PL 440516 A1 /10którego powierzchnia wlasciwa wynosila 1500 m 2 g- 1 . Tabletki o srednicy 1 O mm i grnbosci ok. 0,2 mm uzyskano przez sprasowanie mieszaniny: 85°-ó wag. materialu weglowego, I O~ o wag. srodka wiazacego (PTFE) oraz 5% wag. sadzy weglowej (C65). Tak przygotowane i wysuszone elektrody nasaczono elektrolitem w postaci roztworn siarczanu litu l mol/L Li2SO4 z dodatkiem mocznika w ilosci od 0,5 do I O mol/L. Elektrody rozdzielono separatorem z wlókniny szklanej i umieszczono w naczyniu elektrochemicznym. Kondensator elektrochemiczny poddano badaniom stalonapieciowej polaryzacji 1,6 V przy regularnej kontroli pojemnosci za pomoca badania galwanostatycznego IA g- 1 . Uklad z dodatkiem mocznika w ilosci 2 mol/L charakteryzowal sie najlepsza dlugotrwala praca cykliczna i wysoka retencja pojemnosci. Charakterystyki sa przedstawione na fig. 4. PL 440516 A1 6/10Zastrzezenie patentowe Kondensator elektrochemiczny o wysokiej trwalosci cyklicznej zawierajacy elektrody z materialu weglowego o rozwinietej powierzchni wlasciwej 100 - 2000 m 2 /g oddzielone separatorem i pracujacy w elektrolicie stanowiacym roztwór siarczanu litu o stezeniu I mol/L znamienny tym, ze elektrolit zawiera dodatek mocznika o stezeniach w zakresie od 0,1 mol/L do 10 mol/L, korzystnie 2 mol/L. PL 440516 A1 7/104 1 3 2 fig. l 250 200 150 100 '": Cl 50 u.. c5 o -50 -100 -150 -0.2 o.o 0.2 0.4 0.6 0.8 1.0 1.2 1.4 1.6 1.8 2.0 U{V) fig. 2 PL 440516 A1 8/10 -- :J - c o o o 1.8 -1M Li,SO 4 : -1M Li 1 S0, 1 + O.SM CH 4 N 2 O; -··- 1M Li 7S0, 1 + 1M CH 4N,p· 1.6 -1M Li 2S0 4 + 2M CH 4N 20; - ~ 1M Li 2S0 4+ 5M CH 4 N 20; -----w 1M Li 2S0 4 + 10M CH 4 N 2 0 1.4 1.2 1.0 0.8 0.6 0.4 0.2 O.O---~-~--......,------~.,..._ ____ .,..... __ --< 120 100 80 60 40 -100 -80 -60 -40 -20 fig. 3 o t(s) " 1M Li 2 SO 4 ; ,;, 1M Li 2 SO 4 + O.SM CH 4 N 2 O; .,, 1M Li 2 SO 4 + 2M CH 4 N 2 O; 1M Li 2 SO 4 + SM CH 4 N 2 O; 40 60 80 100 1M Li 2 SO 4 + 1M CH 4 N 2 O; 1M Li 2 SO 4+ 10M CH 4 N 2 O; O 20 40 60 80 100 120 140 160 180 200 220 240 260 t(h) fig.4 PL 440516 A1 9/10URZAD PATENTOWY RZECZYPOSPOLITEJ POLSKIEJ al. Niepodleglosci 188/192 00-950 Warszawa, skr. poczt 203 tel.: (+48) 22 579 05 55 I fax: (+48) 22 579 00 01 e-mail: kontakt@uprp.gov.pl I www.uprp.gov.pl SPRAWOZDANIE O STANIE TECHNIKI ZGLOSZENIA NR P.440516 Klasyfikacja zgloszenia: H0lG 9/022 (2006.01), H0lG 9/035 (2006.01), H0lG 11/62 (2013.01) Poszukiwania prowadzone w klasach: H0lG 9/022, H0lG 9/035, H0lG 11/62 Bazy komputerowe, w których prowadzono poszukiwania: UPRP, STN, Espacenet, Epoquenet Kategoria Dokumenty - z podana identyfikacja Odniesienie dokumentu do zastrz. A PL 418 568 A 1, 12.03.2018 R. zastrzezenie A PL 425 071 A 1, 7.10.2019 R. zastrzezenie A PL 428 354 A 1, 29.06.2020 R. zastrzezenie ? Dalszy ciag wykazu dokumentów na nastepnej stronie A - dokument okreslajacy ogólny stan techniki, który nie jest uwazany za posiadajacy szczególne znaczenie, E - dokument stano\\'iacy wczesniejsze zgloszenie lub patent, ale opublikowany w lub po dacie zgloszenia, L - dokument, który moze poddawac w watpliwosc zastrzegane pierwszehstwo(-wa), lub przytoczony w celu ustalenia claty publikacji innego L')'tcnvanego doku1nentu lub z innego szczególnego pcnvoclu, O - dokument odnoszaty sie do ujawnienia ustnego przez zastosowanie, wystawienie lub ujawnienie w inny sposób, r - dokument opublikowany przed data zgloszenia, ale pózniej niz zastrzegana data pierwsze11stwa, T - dokument pózniejszy, opublikowany po dacie zgloszenia lub w dacie pierwszefotwa i niebedacy w konflikcie ze zgloszeniem, ale cytowany w celu zrozumienia rnsad lub teorii lezacych u podstaw \\ynal8zku, X - dokument o szczególnym znaczeniu; zastrzegany wynalazek nie moze byc uwazany za no\\Y lub nie moze byc uwazany za posiadajacy poziom wynalazczy, jezeli ten dokument brany jest pod uwage samodzielnie, y dokument o szczególnym znaczeniu; zastrzegany ,rynalazek nie moze byc uwazany za posiadajacy poziom ,\ynalazczy, jezeli ten dokument zostanie polaczony z jednym lub kilkoma tego typu dokumentami, a takie polaczenie bedzie oczywiste dla znawcy, & - dokument nalezacy do tej samej rodziny patentowej. Sprawozdanie wykonali-a: Andrzej Jurkiewicz data 21.04.2022r. /-podpisano kwalifikowanym podpisem elektronicznym-/ Pismo wydane w formie doknmentn elektroniczne_go Uwagi do zgloszenia Sprawozdanie zostalo wykonane w oparciu o wersje zastrzezen patentowych z 1.03.2022 r. PL 440516 A1 /10 PLElectrochemical Capacitor with High Cyclic Stability. The invention concerns an electrochemical capacitor with high cyclic stability operating in a neutral electrolyte solution (lithium sulfate) with the addition of urea as an anti-corrosion and anti-aging agent. Electrochemical capacitors (supercapacitors) are systems that accumulate charge through the electrostatic attraction of ions at the electrode/electrolyte interface. They are characterized by high power and long service life. They are a suitable source of energy required for short periods of time, for example, in aircraft (Airbus A380), for powering hybrid electric cars, and elevators. Capacitors also enable energy recovery during regenerative braking and can be used as a power source in portable electronics. Electrochemical capacitors are characterized by fast charge/discharge processes of the order of seconds and excellent cyclic behavior without significant capacitance drops [lR. Miller, A Burke "Electrochemical capacitors: Challenges and opportunities for real-world applications" Electrochemical Society Interface 17 (2008) 53-57]. They are used primarily in applications requiring high power and relatively high energy. The specific energy of a supercapacitor, expressed by the formula E=lcu"2 where C is the capacitance of the electrochemical capacitor and U is the operating voltage of this device, is several times smaller than the energy of a lithium-ion battery. Therefore, numerous studies are being carried out on increasing the energy of the capacitor by improving the capacitance and increasing the system voltage [Elzbieta Frackowiak "Carbon materials for supercapacitor application" Physical Chemistry Chemical Physics 15 (2007) 1774-1785]. The capacitor voltage (U) is determined by the electrochemical stability of the electrolyte. PL 440516 A1 2/10 In an aqueous electrolyte environment (alkaline or acidic), the system voltage W)' is approximately 1 V. In the electrolyte with a neutral pH, the capacitor voltage reaches 1.6 V, while in an organic electrolyte it is 2.5 V-2.7 V. The use of electrode materials and electrolytes with different stability has been described by [Krzysztof Fic, Anetta Platek, Justyna Piwek, Elzbieta Frackowiak "Sustainable material for electrochemzca/capacztors" Materials Today 21 (2018) 437-454]. The choice of electrolyte and optimal capacitor operating voltage is of great importance for the cyclic operation of the device. When the voltage limit is exceeded, the release of gaseous by-products is observed, as described by [Minglong He, Krzysztof Fic, Elzbieta Frackowiak, Petr Novak, Erik J. Berg "lttfluem:e uf aqueuus e/ec:t, u~~yte concentratiun on parasitic reactions in high voltage [R. German, A. Sari, P. Venet and Y. Zitouni "Predicting supercapacitors aging with swface electtrude inte1:face-based aging law" Microelectronics Reliability 54 (2014) 1813-1817]. Capacitor degradation is associated with the release of volatile substances as a result of electrolyte decomposition, the formation of functional groups on the electrode surfaces, the formation of insoluble salt deposits, an increase in resistance and corrosion of current collectors. Long-term cyclic operation and exceeding the capacitor voltage limit or the potential of individual electrodes causes accelerated aging of the supercapacitor and corrosion. Organic electrolytes and ionic liquids meet the requirements for long-term cyclic operation, but they have many disadvantages. They are toxic, flammable, expensive, and require an inert atmosphere during supercapacitor assembly. Hence, the inventive idea is to use an anti-corrosion and anti-aging additive to a pH-neutral aqueous electrolyte. PL 440516 A1 3/10 In this way, a capacitor operating on the basis of a lithium sulfate solution with the addition of urea fulfills the characteristics of an ecological, low-cost energy storage device. The addition of urea to the electrolyte has not been used in electrochemical capacitors to date. The essence of the invention is an electrochemical capacitor with high cyclic durability containing electrodes made of carbon material with a developed specific surface area of 100-2000 m2/g, separated by a separator, and operating in an electrolyte consisting of a solution lithium sulfate at a concentration of 1 mol/L. The electrolyte contains an addition of urea at concentrations ranging from 0.1 mol/L to 10 mol/L, preferably 2 mol/L. The capacitor according to the invention is cheap, ecological, and non-corrosive due to the characteristic properties of the electrolyte, thus enabling long-term cyclic operation of the capacitor. Thanks to the solution according to the invention, the following technical and operational effects were achieved: • capacitor voltage of 1.6-1.8 V; • high cyclicity while maintaining stable capacitance during constant voltage polarization thanks to the anti-corrosion effect of the electrolyte (10% capacity decrease after 250 h of polarization): • safe use because the electrolyte is non-volatile and non-flammable; • the system is symmetrical, easy to construct, and does not require a protective atmosphere, which greatly facilitates installation; • The neutral pH of the electrolyte allows for a wide selection of current collectors, which significantly reduces the cost of capacitor production. The invention is presented in an example embodiment in the drawing, where Fig. 1 shows a schematic diagram of an electrochemical capacitor with high cyclic durability; Fig. 2 shows the result of a cyclic voltammetry test for a system with an electrolyte composition of I mol/L Li 2 SO 4 with an addition of I mol/L urea; Fig. 3 shows a graph for galvanostatic charge/discharge I A g- 1 in the voltage range from 1.0V to 1.6V for electrolytes with various urea additives from 0.5 mol/L to 10 mol/L, and Fig. 4 shows the cyclic operation and capacity retention characteristics for electrolytes with various urea additives from 0.5 mol/L to 10 mol/L. An electrochemical capacitor with high cyclic durability - as shown in Fig. I - comprises a positive I and a negative 2 electrode. The electrodes I and 2 are made of a carbon material with a developed specific surface area of 100 - 2000 m2/g and separated by a separator 4. They operate in a solution of lithium sulfate 1 mol/L Li2SO3 with the addition of urea at concentrations ranging from 0.1 mol/L to 10 mol/L, preferably 2 mol/L. Example I Electrode electrochemical capacitor was made of activated carbon with a specific surface area of 1500 m2 g-1. Tablets with a diameter of 10 mm and a thickness of about 0.2 mm were obtained by pressing a mixture of: 85% by weight of carbon material, 10% by weight of binder (PTFE) and 5% by weight of carbon black (C65). The prepared and dried electrodes were soaked in an electrolyte in the form of a 1 mol/L Li2 SO4 lithium sulfate solution with a urea addition of 0.5 to 10 mol/L. The electrodes were separated with a glass fiber separator and placed in an electrochemical vessel. An electrochemical capacitor with an electrolyte composition of 1 mol/L Li2 SO4 with a urea addition of 1 mol/L was subjected to cyclic voltammetry at 5 mV s-1, as shown in Fig. 2. Electrochemical capacitors operating with various urea additions from 0.5 mol/L to 10 mol/L were subjected to galvanostatic charge/discharge of 1 A g-1 in the voltage range from 1.0 V to 1.6 V, as shown in Fig. 3. The capacitors showed higher capacitances for the electrolyte with the addition of urea. Example II Electrode electrodes of an electrochemical capacitor were made of activated carbon, PL 440516 A1 /10, with a specific surface area of 1500 m2 g-1. Tablets with a diameter of 10 mm and a thickness of approximately 0.2 mm were obtained by compressing a mixture of: 85% by weight of carbon material, 10% by weight of binding agent (PTFE), and 5% by weight of carbon black (C65). The electrodes thus prepared and dried were impregnated with an electrolyte in the form of a 1 mol/L lithium sulfate solution with the addition of urea in an amount from 0.5 to 10 mol/L. The electrodes were separated with a glass fiber separator and placed in an electrochemical vessel. The electrochemical capacitor was tested 1.6 V constant voltage polarization with regular capacity control by means of galvanostatic test IA g- 1 . The system with urea added in the amount of 2 mol/L was characterized by the best long-term cyclic operation and high capacitance retention. The characteristics are shown in Fig. 4. PL 440516 A1 6/10 Patent claim Electrochemical capacitor with high cyclic durability containing electrodes made of carbon material with a developed specific surface area of 100 - 2000 m2/g separated by a separator and operating in an electrolyte consisting of a lithium sulfate solution with a concentration of 1 mol/L, characterized in that the electrolyte contains urea additive in concentrations ranging from 0.1 mol/L to 10 mol/L, preferably 2 mol/L. PL 440516 A1 7/104 1 3 2 fig. l 250 200 150 100 '": Cl 50 u.. c5 o -50 -100 -150 -0.2 o.o 0.2 0.4 0.6 0.8 1.0 1.2 1.4 1.6 1.8 2.0 U{V) fig. 2 PL 440516 A1 8/10 -- :J - c o o o 1.8 -1M Li,SO 4 : -1M Li 1 S0, 1 + O.SM CH 4 N 2 O; -··- 1M Li 7S0, 1 + 1M CH 4N,p· 1.6 -1M Li 2S0 4 + 2M CH 4N 20; 20; -----w 1M Li 2S0 4 + 10M CH 4 N 2 0 1.4 1.2 1.0 0.8 0.6 0.4 0.2 O.O---~-~--......,------~.,..._ ____ .,..... __ --< 120 100 80 60 40 -100 -80 -60 -40 -20 fig. 3 o t(s) " 1M Li 2 SO 4 ; ,;, 1M Li 2 SO 4 + O.SM CH 4 N 2 O; .,, 1M Li 2 SO 4 + 2M CH 4 N 2 O; 1M Li 2 SO 4 + SM CH 4 N 2 O; 40 60 80 100 1M Li 2 SO 4 + 1M CH 4 N 2 O; 1M Li 2 SO 4+ 10M CH 4 N 2 O; O 20 40 60 80 100 120 140 160 180 200 220 240 260 t(h) fig.4 PL 440516 A1 9/10 PATENT OFFICE OF THE REPUBLIC OF POLAND al. Niepodległosci 188/192 00-950 Warsaw, PO Box 203 tel.: (+48) 22 579 05 55 I fax: (+48) 22 579 00 01 e-mail: kontakt@uprp.gov.pl I www.uprp.gov.pl REPORT ON THE STATE OF TECHNOLOGY APPLICATION NO. P.440516 Classification applications: H0lG 9/022 (2006.01), H0lG 9/035 (2006.01), H0lG 11/62 (2013.01) Searches conducted in classes: H0lG 9/022, H0lG 9/035, H0lG 11/62 Computer databases in which the searches were conducted: UPRP, STN, Espacenet, Epoquenet Category Documents - with given identification Document reference to claim A PL 418 568 A 1, 12/03/2018 R. claim A PL 425 071 A 1, 7/10/2019 R. claim A PL 428 354 A 1, 29/06/2020 R. claim ? List of documents continued on the next page page A - a document defining the general prior art which is not considered to be of particular importance, E - a document constituting an earlier application or patent but published on or after the date of filing, L - a document which may cast doubt on the claimed priority(s), or cited in order to establish the date of publication of another claimed document or from another specific reference, O - a document relating to oral disclosure by use, exhibition or other means of disclosure, r - a document published before the date of filing but after the claimed date of priority, T - a later document, published after the date of filing or on the date of first application and not in conflict with the application but cited for the purpose of understanding the principles or theories underlying the invention, X - a document of particular importance; the claimed invention cannot be considered as No or cannot be considered as involving an inventive step if this document is considered on its own, a document of particular significance; the claimed invention cannot be considered as involving an inventive step if this document is combined with one or more such documents, and such combination is obvious to a person skilled in the art, and - a document belonging to the same patent family. Report prepared by: Andrzej Jurkiewicz, dated April 21, 2022 /- signed with a qualified electronic signature-/ Letter issued in the form of an electronic document. Comments on the application: The report was prepared based on the version of the patent claims of March 1, 2022. PL 440516 A1 /10 PL

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PL452421A1 (en) * 2025-06-20 2026-03-30 Politechnika Poznańska Symmetrical electrochemical capacitor

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* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
PL452421A1 (en) * 2025-06-20 2026-03-30 Politechnika Poznańska Symmetrical electrochemical capacitor

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