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Hybrid All-Solid-State Thin-Film Micro-supercapacitor Based on a Pseudocapacitive Amorphous TiO2 Electrode
ACS Applied Energy Materials ( IF 5.4 ) Pub Date : 2022-12-21 , DOI: 10.1021/acsaem.2c02742 Valentin Sallaz 1 , Sylvain Poulet 2 , Jouhaiz Rouchou 2 , Jean-Marc Boissel 2 , Isabelle Chevalier 2 , Frédéric Voiron 1 , Yann Lamy 2 , Sami Oukassi 2
ACS Applied Energy Materials ( IF 5.4 ) Pub Date : 2022-12-21 , DOI: 10.1021/acsaem.2c02742 Valentin Sallaz 1 , Sylvain Poulet 2 , Jouhaiz Rouchou 2 , Jean-Marc Boissel 2 , Isabelle Chevalier 2 , Frédéric Voiron 1 , Yann Lamy 2 , Sami Oukassi 2
Affiliation
In this work, nanometric (6–21 nm thick) amorphous TiO2 films have been elaborated and characterized in liquid- and solid-state electrolyte (LiPON) half-cell architectures. For all considered configurations, the volumetric capacity extracted from cyclic voltammetry and galvanostatic cycling within the 0.5–3 V potential range almost corresponds to the theoretical value expected for the LixTiO2 (x ∼ 1) phase at low current density. Interestingly, TiO2 films after LiPON deposition exhibited a thickness-independent constant initial amount of intercalated lithium ions and did not require a first activation process, in comparison to the liquid electrolyte configuration. Furthermore, the cooperative effects of high Li+ intercalation kinetics and low interfacial charge transfer resistance for a 6 nm TiO2 electrode led to an outstanding surface capacity of 0.7 μAh cm–2 at 1 μA cm–2 and high rate performance with 60% capacity holding ratio at 1 mA cm–2, thus highlighting the extrinsic pseudocapacitive behavior of our sub-10 nm TiO2 electrodes. A LixTiO2 6 nm/LiPON 100 nm/Pt hybrid micro-supercapacitor has been successfully fabricated, achieving an operating voltage window of 3 V and a surface capacitance of 94 μF cm–2 at 50 mV s–1. In addition, the device also exhibited 97% coulombic efficiency upon cycling for 10,000 continuous charge–discharge cycles. This work proposes an approach that allows us to adjust the Li-ion storage properties of TiO2 by nanoengineering and gives insights into the electrochemical performance enhancement by taking advantage of the pseudocapacitance-assisted lithium storage mechanism.
中文翻译:
基于赝电容非晶二氧化钛电极的混合全固态薄膜微型超级电容器
在这项工作中,纳米(6–21 nm 厚)非晶 TiO 2薄膜在液态和固态电解质 (LiPON) 半电池结构中得到了阐述和表征。对于所有考虑的配置,在 0.5-3 V 电位范围内从循环伏安法和恒电流循环中提取的体积容量几乎对应于低电流密度下 Li x TiO 2 ( x ∼ 1) 相的理论值。有趣的是,TiO 2与液体电解质配置相比,LiPON 沉积后的薄膜表现出与厚度无关的恒定初始嵌入锂离子量,并且不需要第一个激活过程。此外,6 nm TiO 2电极的高 Li +嵌入动力学和低界面电荷转移电阻的协同效应导致在 1 μA cm –2时具有 0.7 μAh cm –2的出色表面容量和 60% 容量的高倍率性能在 1 mA cm –2时的保持率,从而突出我们的亚 10 nm TiO 2电极的外在赝电容行为。Li x TiO 26 nm/LiPON 100 nm/Pt 混合微型超级电容器已成功制造,在 50 mV s –1下实现了 3 V 的工作电压窗口和 94 μF cm –2的表面电容。此外,该器件在循环 10,000 次连续充放电循环后还表现出 97% 的库仑效率。这项工作提出了一种方法,使我们能够通过纳米工程调整 TiO 2的锂离子存储特性,并通过利用赝电容辅助锂存储机制深入了解电化学性能增强。
更新日期:2022-12-21
中文翻译:
基于赝电容非晶二氧化钛电极的混合全固态薄膜微型超级电容器
在这项工作中,纳米(6–21 nm 厚)非晶 TiO 2薄膜在液态和固态电解质 (LiPON) 半电池结构中得到了阐述和表征。对于所有考虑的配置,在 0.5-3 V 电位范围内从循环伏安法和恒电流循环中提取的体积容量几乎对应于低电流密度下 Li x TiO 2 ( x ∼ 1) 相的理论值。有趣的是,TiO 2与液体电解质配置相比,LiPON 沉积后的薄膜表现出与厚度无关的恒定初始嵌入锂离子量,并且不需要第一个激活过程。此外,6 nm TiO 2电极的高 Li +嵌入动力学和低界面电荷转移电阻的协同效应导致在 1 μA cm –2时具有 0.7 μAh cm –2的出色表面容量和 60% 容量的高倍率性能在 1 mA cm –2时的保持率,从而突出我们的亚 10 nm TiO 2电极的外在赝电容行为。Li x TiO 26 nm/LiPON 100 nm/Pt 混合微型超级电容器已成功制造,在 50 mV s –1下实现了 3 V 的工作电压窗口和 94 μF cm –2的表面电容。此外,该器件在循环 10,000 次连续充放电循环后还表现出 97% 的库仑效率。这项工作提出了一种方法,使我们能够通过纳米工程调整 TiO 2的锂离子存储特性,并通过利用赝电容辅助锂存储机制深入了解电化学性能增强。