南方科技大学知识苑(SUSTech KC): FeCN3-/4-溶液基离子热电器件的电极界面效应和离子输运研究

题名	FeCN3-/4-溶液基离子热电器件的电极界面效应和离子输运研究
其他题名	INTERFACE EFFECT AND ION TRANSPORT OF THE FeCN3-/4- SOLUTION BASED IONIC THERMOELECTRIC DEVICE
姓名	王帅华
姓名拼音	WANG Shuaihua
学号	12132079
学位类型	硕士
学位专业	070205 凝聚态物理
学科门类/专业学位类别	07 理学
导师	刘玮书
导师单位	材料科学与工程系
论文答辩日期	2024-04-25
论文提交日期	2024-06-28
学位授予单位	南方科技大学
学位授予地点	深圳
摘要	离子热电器件提供了一种小温差下的热能利用技术方案。本论文针对FeCN^3-/4-基水溶液离子热电器件在0°C以下发电性能较差的技术挑战，围绕电极的界面效应和低温下的离子输运科学，系统地开展了电极亲水镀金处理优化电荷转移性能，溶剂共晶策略优化低温离子输运，以及溶液对流调控优化器件输出性能等研究工作，大幅提高了器件在低温环境下的瞬时功率和能量密度。本文研究了亲水性以及金纳米颗粒涂敷对电极界面效应的影响，利用等离子刻蚀获取完全润湿的电极表面，随着接触角从 114 °减小到 0 °，短路电流密度从 40.2 A m^-2 提高到了 146.2 A m^-2。利用磁控溅射获得了纳米颗粒涂敷的电极表面，随着金纳米颗粒镀层厚度从 30 nm 增加到 180 nm，短路电流密度进一步增加到 223.9 A m^-2。通过改善电极的界面效应，电极界面的电荷转移电阻和物质转移电阻大幅降低，器件的瞬时功率密度提高达 6 倍。本文揭示了离子溶液的冰点与器件服役下限温度的关联性，并通过引入（甲酰胺/水）二元共晶溶剂，阻止水分子间形成氢键网络，降低了离子溶液的冰点。当甲酰胺体积分数为 50%时，器件的服役下限温度从 0°C 降低到了 -35°C，并且实现了在低温下 14.4 W m^-2 的高瞬时功率密度，开拓了离子热电器件在冬季或严寒地区的应用场景。本文研究了温度场下溶液介质对流对器件输出性能的调控作用，利用COMSOL 模拟研究发现：降低电极间距会降低对流速度，而隔膜的增设会改变温度场分布，通过两者的协同优化，实现了器件的瞬时功率密度从 14.4 增加到 17.5 W m^-2，并获得 2h 放电能量密度 27 kJ m^-2，该值为目前文献报道最高值，验证了离子热电器件的可实用性。
其他摘要	Ionic thermoelectric devices provide a technological solution for waste heat recovery near room temperature. This thesis addresses the technical challenge of poor power generation performance of FeCN3-/4- based aqueous ionic thermoelectric device below 0°C. It systematically investigates the interfacial effects of electrodes and the ion transport at low temperatures. The thesis encompasses the optimization of electrode with hydrophilic and gold coating treatments to enhance charge transfer performance, solvent eutectic strategies to optimize low-temperature ion transport, and solution convection regulation to improve device output performance, significantly increasing the device’s instantaneous power and energy density in cold environments. The thesis examines the impact of hydrophilicity and gold nanoparticle coating on electrode interfacial effects. Plasma etching was utilized to achieve fully wetted electrode surfaces, and as the contact angle decreased from 114 ° to 0 °, the short-circuit current density increased from 40.2 A m-2 to 146.2 A m-2 . Magnetron sputtering yielded nanoparticle-coated electrode surfaces, and as the thickness of the gold nanoparticle coating increased from 30 nm to 180 nm, the short-circuit current density further increased to 223.9 A m-2 . By improving the electrode’s interfacial effects, the charge transfer resistance and mass transfer resistance at the electrode interface were significantly reduced, and the device’s instantaneous power density was increased by sixfold. The thesis reveals the correlation between the freezing point of the ionic solution and the lower operational temperature limit of the device. By introducinga binary eutectic solvent of formamide/water, the formation of a hydrogen bond network among water molecules is prevented, lowering the freezing point of the ionic solution. With a formamide volume fraction of 50%, the device’s operational lower temperature limit was reduced from 0°C to -35°C, achieving a high instantaneous power density of 14.4 W m-2 at low temperatures, thus expanding the application scenarios of ionic thermoelectric devices in winter or extremely cold regions. The thesis also investigates the regulatory effect of solution mediumconvection on device output performance under a temperature field. Using COMSOL simulations, it was found that reducing the electrode spacing decreases the convection speed, while the addition of a diaphragm can alter the temperature field distribution. Through the synergistic optimization of both, the device’s instantaneous power density was increased from 14.4 to 17.5 W m-2 , and a 2-hour discharge energy density of 27 kJ m-2 was obtained. This value is the highest reported in the literature to date, validating the practicality of ionic thermoelectric devices.
关键词	离子热电器件输出功率服役下限温度共晶溶剂亲水电极
其他关键词	Ionic Thermoelectric Devices Output Power Service Lower Temperature Eutectic Solvent Hydrophilic Electrode
语种	中文
培养类别	独立培养
入学年份	2021
学位授予年份	2024-07
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所在学位评定分委会	物理学
国内图书分类号	TB34
来源库	人工提交
成果类型	学位论文
条目标识符	http://sustech.caswiz.com/handle/2SGJ60CL/778924
专题	工学院_材料科学与工程系
推荐引用方式 GB/T 7714	王帅华. FeCN3-/4-溶液基离子热电器件的电极界面效应和离子输运研究[D]. 深圳. 南方科技大学,2024.

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