本研究之核心目標是基於聯合國在2015年通過的可持續發展目標（SDGs）的第七項以及第十二項指標，利用綠色材料提供更清潔、更便宜的能源。幾丁聚醣（CS）是地球上最豐富的陽離子生物聚合物，被用作膠態聚電解質於水系擬固態超級電容器中。但目前水系擬固態超級電容有兩個主要問題限制了商業應用。第一個問題是低溫效應，水分子在零下溫度下會遭受凍結過程，並產生嚴重的電解質鹽類締和析出現象。由於雙離子性修飾官能基團可以降低冰點並協助離子解離，CS在pH值為6、8和10的條件下，分別進行了羧酸化處理以得到CCS6、CCS8和CCS10，通過傅立葉轉換紅外線光譜和核磁共振光譜（NMR）計算，其羧酸度（DC）為108.2%、20%和17.8%。此外，通過拉曼光譜分析，具有最高DC的CCS6在2M Na2SO4電解質達飽和膨潤後也擁有較高的結合水比例68.8%。因此，CCS6作為聚合物電解質用於水系擬固態超級電容器，通過定電流電充放電分析（GCD），在-7℃下的比電容保持率為常溫電容之57.2%。為了更進一步緩解低溫效應，將水系黏著劑羧甲基纖維素（CMC）與甲基丙烯酸磺酸鈉（SBMA）進行oxa-Michael加成反應製備CMC-SBMA，通過FTIR與NMR計算CMC-SBMA之接枝率為40.5%。經過雙離子修飾後，CMC-SBMA作為雙離子黏著劑用於擬固態超級電容器通過GCD分析，在-15℃下比電容保持率為常溫電容之72%。第二個問題是水系擬固態超級電容器過小的電位視窗（EW）。由於雙離子會與水分子形成強烈的離子-偶極交互作用以避免水電解並提高EW，因此CCS6作為膠態電解質用於擬固態超級電容器，通過循環伏安法分析顯示EW可以提高到1.8V。為了再進一步擴大EW，CCS6與SBMA進行oxa-Michael加成，通過NMR計算CCS-SBMA的接枝率為45.7%。之後，CCS-SBMA膠態電解質在2M LiClO4中達飽和膨潤後進行脫水處理，將保水率從100%降到90%，自由水比例從37.9%下降到32.7%，使離子電導率從30.4mS/cm上升到32.6mS/cm，EW從1.6V上升到2.05V。最終，CCS-SBMA擬固態超級電容器在保水率為100%和90%時的比電容分別計算為145.6F/g和441.3F/g。
此外，前述CMC-SBMA雙離子水系黏著劑也被應用於鋰離子電池的石墨負極，顯示出3.35V的額外充放電平台和140 mAh/g的高比電容量。同時，在固體電解質界面形成過程中，觀察到了較小的電解質分解和低的還原電位。此外，從掃描電子顯微鏡圖像中觀察到，包裹的CMC-SBMA可以適當穩定鋰離子插層/脫層過程中石墨顆粒的膨脹/收縮。本研究論文首次展示了聚合物電解質和電極黏著劑上的雙離子改性，以同時（i）幫助電解質解離、（ii）防低溫凍結、（iii）降低水電化學活性、(iv)擴大電位視窗以及（iv）接待電子和鋰離子於介面處遷移，以實現儲能設備的卓越性能。

The core objective of this study is to provide cleaner and cheaper energy with sustainable materials, based on the scope 7 and scope 12 of Sustainable Development Goals (SDGs) adopted by the United Nations in 2015. Accordingly, chitosan (CS), the most abundant cationic biopolymer on earth, is applied as polymer matrix to intake aqueous based electrolyte. The aqueous based pseudo solid state supercapacitor possesses advantages including low cost and easily processed, but there are two major issues that restrict the commercial application in present. The first issue is low temperature effect, water molecule will suffer from freezing process and render severe electrolyte association at subzero temperature. Since zwitterionic segment can serve as antifreeze agent and dissociation enhancer, CS is subjected to carboxylation at pH of 6. 8, and 10, for CCS6, CCS8, and CCS10 respectively with the degree of carboxylation (DC) as 108.2%, 20%, and 17.8% calculated by Fourier-transform infrared (FTIR) and Nuclear magnetic resonance (NMR) spectra. Furthermore, CCS6 with high DC also possessed high bound water proportion of 68.8% after 2M Na2SO4 electrolyte intake analyzed by Raman spectra. Therefore, CCS6 as polymer electrolyte for AC//AC symmetric pseudo solid-state supercapacitors showed the specific capacitance retention of 57.2% at -7℃ via Galvanostatic charge-discharge (GCD) analysis. To further alleviate low temperature effect, binder material, carboxymethyl cellulose (CMC), was subjected to oxa-Michael addition with sulfobetaine methacrylate (SBMA) to fabricate CMC-SBMA as zwitterionic binders with the grafting fraction of 40.5% calculated by NMR spectra. After zwitterionic modification, CMC-SBMA hydrogel with 2M Na2SO4 electrolyte intake showed low freezing temperature of -23℃. Therefore, CMC-SBMA as zwitterionic binder for AC//AC symmetric pseudo solid-state supercapacitors showed the specific capacitance retention of 72% at -15℃ via GCD analysis. The second issue is small electrochemical window (EW). Since zwitterionic segment will form strong ion-dipole interaction with water molecules to reduce water splitting process and improve EW, CCS6 with high DC as polymer electrolyte for AC//AC symmetric pseudo solid-state supercapacitors showed improved EW of 1.8V via Cyclic voltammetry (CV) analysis. To further widen EW, CCS-SBMA is subjected to oxa-Michael addition with SBMA for CCS-SBMA with grafting fraction of 45.7% calculated by NMR spectra. Afterward, CCS-SBMA polymer electrolyte with 2M LiClO4 electrolyte intake is subjected to dehydration process from 100% water retention to 90%, the free water proportion decreases from 37.9% to 32.7% rendering the increase in ionic conductivity from 30.4 mS/cm to 32.6 mS/cm, and the EW from 1.6V to 2.05V. Eventually, the specific capacitance of CCS-SBMA supercapacitor with water retention of 100% and 90% are respectively calculated as 145.6F/g and 441.3F/g. Since zwitterion segment can simultaneously provide quaternary ammonium and sulfonic group respectively for electron and lithium-ion receptions, CMC-SBMA applied as zwitterionic binder of graphite anode for lithium-ion battery shows an extra discharging voltage plateau at 3.35V and high specific capacitance of 140 mAh/g. Meanwhile, both less decomposition of electrolyte and low reduction potential during solid electrolyte interface formation process are observed. Furthermore, the wrapping CMC-SBMA can stabilize expansion/shrinkage of graphite particles during lithium-ion intercalation/deintercalation, being observed from scanning electron microscope images. This study is the first to demonstrate zwitterionic modification on electrolyte and binder to serve as (i) dissociation enhancer, (ii) antifreeze agent, (iii) water activity restriction, and (iv) electron and ion reception for superior performance.

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