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Sensors 2020, 20, 506 6 of 14 The corresponding specific capacitance value is obtained by calculating the area of the CV curve. Figure 3i and Table 1 show that the specific capacitance of the friction layer changes greatly after the addition of PA6, PVDF and BaTiO3. Specifically, after adding PA6, the specific capacitance of the friction layer is greatly increased. At 20 mV s−1, the specific capacitance increased from 66.225 mF cm−2 to 77.896 mF cm−2, which is increase by 1.176 times. At a sweep speed of 500 mV s−1, the specific capacitance increased from 28.156 mF cm−2 to 39.212 mF cm−2, which is increase by 1.393 times. Due to the certain redox reaction and the internal ion migration rate of each friction layer, the specific capacitance cannot increase with the increase of the scanning rate as the sweep speed increases, and the capacitance value of each friction layer decreases. On this basis, the friction layer is greatly reduced in specific capacitance after the addition of BaTiO3. At 20 mV s−1 sweep speed, the specific capacitance is reduced from 77.896 mF cm−2 to 67.252 mF cm−2, which is reduced to 0.863 times. At 500 mV s−1 sweep speed, the specific capacitance decreased from 39.212 mF cm−2 to 22.654 mF cm−2, which is reduced to 0.578 times. After adding PVDF, the specific capacitance of the friction layer is reduced. At 20 mV s−1, the specific capacitance decreases from 66.225 mF cm−2 to 65.509 mF cm−2, which is reduced to 0.989 times. At a sweep speed of 500 mV s−1, the specific capacitance decreases from 39.212 mF cm−2 to 27.078 mF cm−2, which is reduced to 0.962 times. On this basis, after adding BaTiO3, the friction layer ratio is reduced at low sweep speed. At 20 mV s−1, the specific capacitance decreases from 66.225 mF cm−2 to 65.293 mF cm−2, which is reduced to 0.997 times. At 500 mV s−1, the specific capacitance increases from 27.078 mF cm−2 to 29.488 mF cm−2, which increases by 1.089 times. Since the friction layer specific capacitance is related to its internal charge capacity and ion permeability, after adding PA6, the internal area of the friction layer increases, and the charge capacity increases, which cause the specific capacitance rises. After adding PVDF and BaTiO3, the specific capacitance of PVDF and BaTiO3-based cellulose films are lower than that of cellulose composite films. On the one hand, PVDF can easily obtain electrons by friction and is used as a negative material. Although its piezoelectric performance can make it a dopant, it can improve the performance of friction generators. But because it is easy to get electrons, the specific capacitance will be lower than that of pure cellulose film. On the other hand, it is because during the electrochemical test, the sample film is not squeezed without generating a dipole moment and producing a piezoelectric effect, and then its specific capacitance is reduced. 3.3. EIS and GCD Test Analysis Electrochemical alternating current impedance spectroscopy (EIS) is an effective method for studying electrochemical processes. The AC impedance characteristics of cellulose-based friction film materials can reflect various kinds of information such as ion diffusion and charge transfer. The equivalent circuit parameters (Figure 4a) Cdl and ionic conductivity σ are calculated by Equations (2) and (3), as follows: Cdl = 1 (2) ω·Rct σ= L (3) Rct · A where ω is the highest angular frequency of the arc, L is the thickness of the sample, and A is the surface area of the ionic electrolyte film. The EIS curves of different types of friction layers are conducted at 105 Hz–10−2 Hz (Figure 4a). The EIS graph curve is roughly divided into three sections: high, medium and low. The three sections are associated with the parameters of Re, W0, R1 and Cdl in the equivalent circuit. The semi-arc of the high frequency band is remarkable, indicating that each friction layer has stable and good electrochemical characteristics, and the arcs are different in size due to different materials. The equivalent resistance Re is obtained by the intersection of the high-frequency arc area and the left side of the real axis, and Re reflects the overall internal resistance of the friction layer. When other conditions are constant, the thickness of the friction layer increases and Re increases after addingPDF Image | Green Triboelectric Nano-Generator Composite of Degradable Cellulose, Piezoelectric Polymers of PVDF PA6
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