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Sensors 2020, 20, 506 2 of 14 electromagnetic [30–32] and other nano-generators, which can convert and store the collected energy or provide power for mobile electronic devices after a certain period of time. With the rise of the concept of green environmental protection, there is an urgent need to develop a green, environment-friendly and bio-degradable nano-generator. In 2016, the first biodegradable TENG was made from a synthetic polymer, polylactic acid-glycolic acid (PLGA), 3-hydroxybutyrate 3-hydroxyvalerate (PHBV) and polycaprolactone (PCL). Ding [33] et al. designed a novel solar-driven regenerative electrochemical system for simultaneous photoelectric energy harvesting and storage. With rational screening of redox species and comprehensive electrochemical study, a high Seebeck coefficient of −1.8 mV K−1 is achieved by solely exploiting earth-abundant materials based on the thermogalvanic effect. In 2019, the effect of piezoelectricity, internal resistance, and surface treatment on output is explained experimentally and theoretically, which illustrates that the extent of charge transfer has a strong connection with the piezoelectricity, internal resistance, and surface treatment of the composite [34]. However, these polymers are often expensive and contain certain harmful chemicals. Natural bio-materials which are compared with these synthetic polymers usually have low cost, wide distribution, easy processing, good biocompatibility, degradability and good film-forming properties. Simultaneously, they are appropriate for the construction of TENG [35–38], which has extensive application prospect in the fields of biomedicine, electronic sensing, etc. In this study we propose a kind of environmentally friendly triboelectric nano-generator based on natural degradable cellulose, which is compared to some developed polymer-generators. At present, chitosan and cellulose are abundant in many natural vegetation sources and organisms. By utilizing the dissolution and regeneration characteristics of cellulose and ionic liquids, the regenerated cellulose film can be obtained as a friction layer, which can generate electricity by extrusion and friction, and test output electrical performance. At this foundation, PA6/PVDF with different electronegativity, and BaTiO3 with high dielectric constant and low dielectric loss, are added for performance optimization. For theoretically explain the effect of piezoelectric and internal resistance on the output, different types of triboelectric layer films are carried out test of electrochemical performance and characterization. The effect of piezoelectricity, internal resistance on output is explained theoretically by electrochemical performance, which illustrates that the extent of charge transfer has a strong connection with the piezoelectricity, internal resistance of the composite. In addition, the electrical output performance is tested after rectifying multiple assemblies. Then, the capacitor is powered for testing its charging and discharging performance within 1000 s. After that, power is supplied to microcontroller, and then drives SFM-27 buzzer and LCD screen. The nano-generator device proposed in this paper has good stability and reliability, and can be widely used in the field of energy harvesting, which greatly promotes the development of natural biomaterials in TENG and other miniature electronic sensor devices. 2. Experimental Preparation and Operating Principle 2.1. Experimental Materials α-Cellulose (99.5) was purchased from Aladdin Chemical Company (Shanghai, China). The ionic liquid 1-butyl-3-methylimidazolium chloride ([Bmim]Cl, molecular weight 174.67 kDa, melting point 70 ◦C) was purchased from the Physical Chemistry Institute of Lanzhou (Lanzhou, China). Barium titanate (BaTiO3) (content not less than 99%, molecular weight 233.19 kDa), polyamide powder (PA6, (C6H11NO)n), polyvinylidene fluoride (PVDF, content not less than 99.5%, and molecular weight 825000) were purchased from Macleans Company (Harbin, China). Some commonly used chemical reagents (distilled water, etc.) were purchased from Yongchang Reagent Co. Ltd. (Harbin, China). 2.2. The Preparation of Different Types of Composite Cellulose Layers [Bmim]Cl (5 g) is added to q beaker, and then stirred at 85 ◦C for 10 min. Then, α-cellulose (0.5 g) weighed by using an analytical balance, is added into the [Bmim]Cl, and the mixture is stirred at a low speed for 60 min at a temperature of 85 ◦C. A certain amount of PA6, PVDF and BaTiO3 are addedPDF Image | Green Triboelectric Nano-Generator Composite of Degradable Cellulose, Piezoelectric Polymers of PVDF PA6
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