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標題: | 含碲之鎳錳雙金屬結構與碳材修飾其複合物應用於超級電容器 Synthesis and Characterizations of Tellurium-based Bimetallic Nickel Manganese Chalcogenides and their Carbon Composites for Supercapacitors Application |
作者: | 戴博彥 Po-Yen Tai |
指導教授: | 何國川 Kuo-Chuan Ho |
關鍵字: | 鎳錳雙金屬碲化物,無黏著劑電極,摻入異質元素之中空碳球,混合型電容器,二維金屬碳化物, Bimetallic nickel manganese telluride,binder-free electrode,heteroatoms doped graphene hollow balls,hybrid supercapacitors device,MXene, |
出版年 : | 2023 |
學位: | 碩士 |
摘要: | 本文旨在研究含碲之鎳錳雙金屬結構與碳材修飾其複合物應用於超級電容器。本論文主要分為兩大部分:鎳錳雙金屬碲化物複合多重元素摻入之中空碳球應用於超級電容器(第三章)、摻碲之鎳錳雙金屬雙氫氧化物原位生長於高分子修飾二維過渡金屬碳化物(MXene)導電層應用於無黏著劑超電容電極製備(第四章)。此兩方面應用將被介紹在引言(第一章),而實驗流程(第二章)將包含化學藥品、實驗方法及元件量測。
在第三章中,鎳錳金屬碲化物將透過水熱法與所製備摻入異質元素之中空碳球複合。由於碳材中空的特性,其可以防止在充放電過程中材料體積膨脹導致結構塌陷因而壽命降低的問題。其次,透過摻入不同電負度異質元素於中空碳球可以增加結構表面電子活躍性進而促進電解液中離子的吸附。另一方面,以鎳錳為基底的雙金屬雙氫氧化合物是良好的電容器材料之一,原因是因為其有豐富的氧化還原對、較強的偶極矩以及穩定的晶格結構。透過最後的碲化步驟,其有效提升金屬架構之電子雲密度進而增加結構的活性位點。鎳錳雙金屬碲化物複合異質元素摻入之中空碳球在電流密度為1 A/g時能達到最大電容值(1,450 F/g)。其與活性碳電極所組成之混合性電容器於1 A/g時能達到最大電容值(147.3 F/g),在功率密度為772 W/kg 下,能達到最大的能量密度47.8 Wh/kg,並且在電流密度(3 A/g)的10,000圈充放電下,能維持82.0%初始比電容值。 在第四章中,以高分子修飾二維過渡金屬碳化物(MXene),並且將其擇為電極導電層並在其表面原位生長鎳錳雙金屬雙氫氧化物並在隨後摻入碲元素形成無黏著劑之超電容電極。首先,二維過渡金屬碳化物與高分子溶液於攝氏40度反應時,能展現最大的層與層之間的距離以及最佳的導電度。其二,將修飾過之二維過渡金屬碳化物直接附著在鎳網上能降低整體的電阻抗。最後摻入碲的步驟能增加金屬架構之電子雲密度並且提升其氧化態,進而形成良好的超級電容器材料。其電容值可以在2 A/g的電流密度下達到1,920 F/g,與活性碳電極所組成的混合式超級電容器裝置,在功率密度為1,500 W/kg 下,能達到最大的能量密度62.6 Wh/kg並且於10,000圈的充放電測試下,能維持77.3%初始比電容值。 This thesis mainly focuses on two different but related parts, namely, layered double hydroxide derived NiMnTe structure on heteroatoms doped graphene hollow ball for supercapacitors application (Chapter 3), and Tellurium doped NiMn LDH in-situ grown on CTAB modified MXene conductive layer for binder-free supercapacitors application (Chapter 4). The overview of these two applications will be displayed in the introduction (Chapter 1). Moreover, the experimental procedures (Chapter 2) include the chemical reagent, material characterization, and the principle of device analysis. In Chapter 3, novel bimetallic nickel manganese telluride (NiMnTe) is synthesized through a practical hydrothermal way combined with a new carbon material named heteroatoms doped graphene hollow balls (HGHB). Firstly, benefiting from the hollow property of HGHB, it prevents the composite from collapsing and thus enhances the cycling life. Secondly, doping atoms with different electronegativity onto the graphene hollow balls structure modulates the electronic activities and ion adsorption. Thirdly, nickel and manganese-based LDH structures have multiple valance types, more significant dipole moment, and strong crystal structures, which indicate that they are the excellent choice for supercapacitors materials. Final tellurization increases the metal structure’s electron density and supplies more active sites in the LDH structure. The NiMnTe decorated HGHB (NiMnTe/HGHB) delivers high specific capacitance (1,450 F/g) at the current density of 1 A/g. The hybrid supercapacitors device (NiMnTe/HGHB//AC) exhibits a high specific capacitance (147.3 F/g) with reasonable energy density (47.8 Wh/kg) and good power density (772 W/kg). Moreover, this device exhibits good cycling life at 3 A/g (82.0% capacitance retention) after 10,000 cycles. In Chapter 4, this study presents the synthesis process of tellurium-doped NiMn layered double hydroxide (Te-NiMn LDH) grown directly on the hexadecyl trimethylammonium bromide (CTAB) modified MXene layer (C-MXene) anchored on the UV-Ozone-treated nickel foam (Te-NiMn LDH/C-MXene/NF). Firstly, modifying MXene with CTAB-contained ethanol solution at 40 ˚C of reaction temperature presents the most significant interlayer space and highest conductivity. Secondly, C-MXene on the NF acts as the conductive layer for the latter LDH structure growing and the Te doping processes, which prevents undesired resistance and unnecessary cost because of no binder or additive. Finally, the Te doping enhances the electron density of LDH metal structure and further increases the valance types, which improves the capacitance. The binder-free Te-NiMn LDH/C-MXene/NF exhibits an excellent specific capacitance of 1,920 F/g at 2 A/g. Moreover, the hybrid supercapacitor (Te-NiMn LDH/C-MXene/NF//AC) device exhibits a capacitance of 202.0 F/g at 2 A/g and energy density of 62.6 W/kg at a power density of 1,500 Wh/kg with good cycle stability of 77.3% up to 10,000 cycles. |
URI: | http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/88705 |
DOI: | 10.6342/NTU202302581 |
全文授權: | 未授權 |
顯示於系所單位: | 化學工程學系 |
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