Summary: | Water-processable natural polymers represent a valuable alternative for the sustainable manufacturing of electrical double layer capacitors (EDLCs). Here, we demonstrate for the first time the feasibility of the use of pullulan to produce high mass loading electrodes (>10 mg cm<sup>−2</sup>) at low binder content (10%) for ionic-liquid based EDLCs. Pullulan has also been processed as a porous separator by electrospinning. Its ionic resistance and thermal stability have been evaluated in different electrolytes and were found to be superior compared to those of a cellulose triacetate electrospun separator. Pullulan-ionic liquid EDLCs were, thus, assembled and charged up to 3.2 V. The EDLCs delivered specific energy and power of 7.2 Wh kg<sup>−1</sup> and 3.7 kW kg<sup>−1</sup> and featured good cycling stability over 5000 cycles.
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