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利用交流阻抗分析鉛酸電池的老化機制

為了解決Fit Hybrid 0-100的問題，作者周昀宣 這樣論述：

　　本論文利用電化學阻抗圖譜（Electrochemical Impedance Spectra, EIS）分析法，對商用鉛酸電池之老化行為進行研究。首先建立最佳之等效電路模型，應用於鉛酸電池之交流阻抗分析之擬合，同時拆解與分析老化鉛酸電池，利用SEM、EDS、ICP與XRD分析電極材料的性質。　　利用本論文中建立的三種等效電路，擬合在不同充電狀態下之鉛酸電池之EIS，發現以第三種等效電路最為合適，並將其應用於電池在不同老化狀態下所得EIS之擬合，與探討電池之老化機制。最合適的等效電路模型以電路元件符號表示為：（Rn+Wn）/Qn+Re+（Rp+Wp）/Qp，以＂+ ＂代表串聯結構，＂/ ＂

則表示為並聯結構，其中Re為電解液與電極之串聯阻抗，Rn為負極之電荷轉移阻抗，Rp為正極之電荷轉移阻抗，Qn為負極考慮電極表面粗糙度之電雙層電容，Qp為正極考量電及表面粗糙係數之電雙層電容，Wn為負極之Warburg質傳阻抗，Wp為正極之Warburg質傳阻抗。　　在本論文中利用三種模式進行鉛酸電池的老化，首先以0.056 C充放電速率，在0 ~ 100 % SOC（State Of Charge）之間對電池進行充放電，發現當充放電136次後，電池的電容量衰退至15.3 %，經EIS的分析與材料分析發現，使電池老化最重要的因素為正極之質傳阻抗，比較活化與老化後電池，其值由1.02x10-3增加

至0.034  s-1/2，增加了3233 %；造成老化的次要因素為正極之電荷轉移阻抗，老化前後由0.1302增加至3.1 Ω，增加了2280 %，第三個重要因素為負極 之電荷轉移阻抗，老化前後由8.132x10-3增加至0.157 Ω，增加了1830 %。　　接著以0.2 C充放電速率，在0 ~ 100 % SOC之間對電池進行充放電，在經過41次充放電後，電池的電容量衰退至15.2 %，在EIS的分析結果中，造成電池老化之主要因素，以正極之質傳阻抗增加幅度最大，由1.02x10-3增加至9.0x10-3 Ω s-1/2，增加了782.4 %；其次則為正極之電荷轉移阻抗，由0.1302增加

至0.688 Ω，增加了428.4 %，第三重要因素為負極之電荷轉移阻抗，隨著電池老化過程中，由活化電池8.132x10-3增加至0.0242 Ω，增加了197.6 %。　　第三種老化方式為使用0.056 C，對全新電池進行淺度（80 ~ 90 % SOC）充放電，模擬動力車上啟動電池之充放電行為，在循環240次之後，其電容量衰退至49.1 %。於EIS之分析結果中發現，老化最重要的因素是正極之電荷轉移阻抗，由活化狀態之0.1012增加至老化之1.68 Ω，增加了1560 %；其次為正極之質傳阻抗，由3.22x10-3 Ω s-1/2增加至0.0268 Ω s-1/2，增加了732.3 %；而

第三重要因素是負極之質傳阻抗，由活化電池5.064x10-3 Ω s-1/2，隨著電池老化增加至0.0232 Ω s-1/2，共增加了358.1 %。　　在三種老化條件下之電池，主要之衰退機制皆發生於正極，當電池在循環過程中，於電極表面生成粒徑較大之不可逆硫酸鹽，導致活性物間之孔隙縮小，增加質傳阻抗，且非導電性之不可逆硫酸鹽晶體，覆蓋於電極表面上，導致電化學活性面積下降，使電荷轉移阻抗增加。在淺度充放電循環老化電池中發現，電池正極活性物的脫落為主要的老化原因。

Upconversion Nanohybrids for Intracellular pH Imaging and Broadband Photodetection

為了解決Fit Hybrid 0-100的問題，作者高聖禹 這樣論述：

Nanohybrids or nanocomposites (NC) offer a wider scope in materials engineering andapplications by utilizing the extended range properties of the individual component materials,and those from the novel interfacial properties. An intriguing aspect of such NC is the chargetransfer that happens among

the components. Synthetic techniques are plenty; however,choosing the correct combination for the NC is important depending on target applications,such as intracellular pH sensing and photodetection, in particular. Previously reportedfluorescent nanoprobes for intracellular pH sensing had drawbacks,

such as shallow penetrationdepth of the excitation light, background autofluorescence, poor photostability, andbiocompatibility. On the other hand, pure or single material-based photodetector devices,although having a fast response, either lacked broadband response, have poorphotoresponsivity, or b

oth. Through this thesis, we have attempted to design and synthesizetwo novels NC of upconversion nanoparticles (UCNPs): i) with mOrange (mO) fluorescentprotein (FP) for fluorescence-based intracellular pH sensing; ii) with molybdenum disulfide(MoS2) for ultrasensitive broadband photodetection, that

overcomes the above-mentionedissues.First, we have constructed a Forster Resonance Energy Transfer (FRET) based pH nanoprobeutilizing the charge transfer between the UCNP donor and the mOrange FP acceptor forintracellular pH sensing. The UCNP-mOrange nanoprobes (on a coverslip or uptaken in asingle

HeLa cell) could be fluorescently imaged with 980 nm excitation. The FRET probesshow FRET efficiency of ~20% at pH = 7.0 and show pH-sensitive simultaneous selfratiometric and ratiometric features. Nigericin-mediated intracellular pH (3.0, 5.0, and 7.0)could be accurately estimated from the fluores

cence-derived FRET ratio. The nanoprobeiiiexhibits good accuracy, reversibility, and stability over a wide range of pH (3.0–8.0), eveninside a cell. The fluorescence intensity ratio from UCNP and mOrange could be used toestimate the pH inside a single HeLa cell.In the second case, we have fabricated

a photodetector (PD) device with a single flake of MoS2electrostatically conjugated with the UCNPs. The idea was to extend the conventional workingrange of the MoS2, within 200-680 nm, to the near-infrared (NIR) regime. The device wasirradiated with power-dependent 325-1064 nm illumination to study

its broadbandphotosensitivity. The highest responsivity of 1254 A W-1 is reported for 980 nm at 1.0 V bias.An unprecedented normalized gain of 7.12 x 104 cm2 V-1, and Detectivity of 1.05 x 1015 Jones(@980 nm, 1 V) was obtained. The real application of the PD device was demonstrated usingnon-laser d

omestic appliances such as sodium vapor lamp, mobile phone flashlight, and aircondition remote controller.