Fasta polymera elektrolyter (FPE) är av stort intresse att använda i litiumbat-terier, då flytande elektrolyter är både brandfarliga, giftiga samt sliter hårt på batteriets samtliga komponenter, vilket i sin tur påverkar batteriets livslängd och prestanda. FPE skulle även kunna tillföra mekaniska egenskaper, vilket potentiellt skulle medföra nya möjligheter när man designar batterier i forma av att man inte behöver en separator mellan elektroderna, och på sätt ökar batteriets energidensitet. Det är flera parametrar som måste tas hänsyn till när man designar en ny elektrolyt, mekaniska egenskaper, jonledning, jonselekti-vitet samt elektrokemisk stabilitet är de viktigaste. Det största problemet med polymera elektrolyter är deras dåliga jonledning i förhållande till deras meka-niska egenskaper; ofta måste man välja mellan dessa två egenskaper. FPE li-der emellertid fortfarande av för låg prestanda för praktiska tillämpningar vid rumstemperatur, och temperaturen måste upp till 60 °C-90 °C för att få till en praktisk prestanda. Nackdelen med att höja temperaturen är dock att olika ty-per av sidreaktioner kan accelerera och bli märkbara, vilket påverkar batteriets livslängd och prestanda på ett negativt sätt. Ett sätt att kombinera både meka-niska egenskaper och elektrokemisk prestanda är att polymerisera blocksam-polymerer (BSP), det vill säga blocksam-polymerer som kombinerar ett joniskt ledande block med ett mekaniskt block i en polymer. Genom att variera monomerkom-positionen och strukturen hos BSP är det möjligt att tillverka elektrolyter med olika batteriprestanda. I artikel I och artikel II syntetiserades två typer av metakrylatbaserade BSP:er med olika mekaniska block för att utvärdera mor-fologin, den elektrokemiska stabiliteten och batteriförmågan. Denna avhand-ling började med att syntetisera en serie sampolymerer av metylmetakrylat (MMA) och metylmetakrylat med etylenoxid som sidogrupper. Det visade sig att den jonledande förmågan var hög, så nästa naturliga steg var att polymeri-sera BSP:er, i ett försök att ytterligare öka den jonledande förmågan med hy-potesen att mikrofasseparerade BSP:er kan kombinera både hög jonisk kon-duktivitet och mekanisk integritet. Men som framgår i artikel I visade det sig att elektrolyterna inte fasseparerade. I artikel II ersättas MMA:n med ben-zylmetakrylat (BMA), och då fasseparerade elektrolyterna. Tyvärr visade det sig att de metakrylatbaserade elektrolyerna inte är elektrokemiskt stabila, och batteriprestanda var begränsad.
I artikel III och artikel IV antogs en ny strategi, och fokus förflyttades till diblocksampolymerer, i vilka den jonkoordinerande gruppen byttes från ety-lenoxid till ester- och karbonatgrupper. Det visade sig att batteriprestandan för dessa elektrolyter var överlägsen de metakrylatbaserade elektrolyterna. Det var möjligt att cykla halvceller med konfigurationen Li | elektrolyt | LiFePO4
vid 40 °C och med hög kapacitet under en längre tid. När BMA användes som mekaniskt block i kombination med kaprolakton och trimetylkarbonat erhölls en BSP som visade sig vara ett attraktivt alternativ till etylenoxid som poly-merelektrolyt, då elektrolyten kombinerade elektrokemisk stabilitet med hög jonkonduktivitet och transporttal, samt mekanisk integritet. Genom att växla till polyester- och polykarbonatbaserade elektrolyter uppnåddes alltså inte bara hög jonledningsförmåga utan även höga transporttal, god elektrokemisk kompatibilitet och lovande mekaniska egenskaper. De lovande mekaniska egenskaperna tillsammans med att BSP:erna verkar mycket pålitliga som elektrolytmaterial, de drabbas inte av några plötsliga kortslutningar, gör dessa BSP:er till intressanta kandidater för fortsatta studier som elektrolyter för strukturella batterier.
Figur 12. De två studerade blocksampolymererna i artikel I (vänster) och II (höger).
Figur 2. Bilden visar blocksampolymeren som studerades i artikel IV, som är en kom-bination av benzylmetakrylat som mekaniskt block samt ett jonledande block av kapro-lakton och trimetylenkarbonat.
Acknowledgements
As Ramiro said when a were about to start at Uppsala, enjoy the ride! Truly it has been a ride, both emotionally and in life. Not to mention the ride between Stockholm and Uppsala... I guess I have to acknowledge SJ for (mostly) taking me home to Stockholm late evenings, and the fact that this thesis actually was written (mostly) on the train.
To my supervisors: thank you for giving me an amazing once in a lifetime opportunity to freely explore the world of polymers, I believe that this freedom will be hard to find again. Laurent, thank you for taking your time helping me with the SAXS analysis and all the time you spent on discussing science with me. I’m grateful to have had the opportunity to meet such a friendly and help-ful person. Adrian! Thank you for introducing me to the world of neutrons, a truly amazing but at the same time daunting world. The trip to NIST was an eye-opener for me, it was great to meet so many friendly and enthusiastic peo-ple that really wants to contribute. I will remember this trip for the rest of my life.
All members of the polymer chemistry and PUB-group throughout the years, thank you for the friendly atmosphere and being the people you are! Special thanks to Fabian, Ronnie and Matthew who helped me with the battery chemistry part, without you guys life had been really hard. I really appreciate your friendliness and your enthusiasm to science (and beer drinking), thank you for these years.
I have had a couple of project workers throughout the years helping me with various stuff in the lab. Maybe everything wasn’t that organized and planned in detail, but it was great fun and I’m truly grateful for the help, thank you so much! Special thanks to Jonas Hedman and Guiomar Hernández, with-out your help in the end I would not have made it, at the time I was too tired to do all the lab-work myself.
Daniel Bermejo and Fabian Jeschull, you have been great friends and nice companions in the lab, so well as at the pub. I wish you the best of luck what-ever you do in life.
To my family and friends, it is hard to explain what I’m been doing in Upp-sala, but it doesn’t matter, thank you for supporting me anyways and balanced my life, with football, orchestra, and just having fun! And Martina, I hope that we will have more time for each other and our small family know, exciting new times lie ahead.
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