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  本文選題：超級電容器 + 多組元化合物�。� 參考：《華中科技大學》2014年博士論文

【摘要】：電化學電容器(又叫超級電容器)因其較高的功率密度、優(yōu)良的循環(huán)穩(wěn)定性、能夠快速充放電等優(yōu)點,在大功率設備、電動車、電子設備等領域廣闊的應用前景而備受關注。目前所報導的各類電極活性材料中,金屬化合物已經(jīng)實現(xiàn)了較高的比容量及優(yōu)良的循環(huán)穩(wěn)定性,是最有希望實現(xiàn)高能量密度超級電容器的一類電極活性材料。本研究以鎳鈷基化合物為研究對象,通過改變鎳與鈷的成分比例及配位陰離子的種類構筑出一系列多元鎳鉆基化合物,如鎳鉆氫氧化物、鎳鉆氧化物、鎳鉆硫化物及鎳鈷硒化物,系統(tǒng)地研究了鎳鉆基化合物的超級電容性能。主要研究結果如下： 提出了一種簡易的混合溶劑熱法,成功地用于制備不同鎳鈷組分的a相層狀鎳鈷氫氧化物,并且可以引入基底用于制備鎳鈷氫氧化物陣列結構。a相鎳鈷氫氧化物作為超級電容器電極活性材料獲得了比a相Ni(OH)2更高的比容量、倍率特性及循環(huán)穩(wěn)定性,表明鎳及鈷離子配位化合形成氫氧化物可以明顯提高其電化學活性并且改善a相結構的電化學穩(wěn)定性。采用泡沫鎳承載形成陣列結構可以進一步提高鎳鈷氫氧化物的比容量,并且實現(xiàn)了良好的循環(huán)穩(wěn)定性。 高溫熱分解a相鎳鈷氫氧化物及其泡沫鎳承載的陣列樣品,可以獲得不同鎳鈷比例的鎳鈷氧化物及泡沫鎳承載陣列結構樣品。鎳鈷雙金屬氧化物樣品表現(xiàn)出比CO3C4及NiO樣品更高的比容量、倍率性能及循環(huán)穩(wěn)定性。利用泡沫鎳承載形成陣列結構可以進一步提高鎳鈷氧化物的比容量,并且實現(xiàn)了優(yōu)良的循環(huán)穩(wěn)定性。同時,采用一種簡單的水解結合高溫熱處理方法制備出具有多孔結構的花狀NiCo2O4納米結構,NiCo2O4納米結構具有比C0304和NiO高兩個數(shù)量級以上的導電性,用作超級電容器電極活性材料時具有較高的比容量、優(yōu)良的倍率特性及超長的循環(huán)穩(wěn)定性。 率先將鎳鉆雙金屬硫化物用作超級電容器電極活性材料,獲得了優(yōu)異的電化學性能�；陉庪x子交換反應,提出一種簡易的制備NiCo2S4海膽狀納米結構和泡沫鎳承載的NiCo2S4納米管陣列結構。NiCo2S4樣品具有比相同形貌及結構的NiCo2O4更低的光學帶隙寬度和更高的導電性,這有助于改善其用作電極活性材料時其電化學過程中的動力學特性。NiCo2S4海膽狀納米結構比相同形貌及結構的NiCo2O4及相同制備方法制備出的Co9S8和NiS具有更高的比容量及倍率性能。泡沫鎳承載的NiCo2S4納米管陣列結構在較高的單載量(6mg/cm2)下實現(xiàn)了超高的電極材料利用率,從而實現(xiàn)了超高的比容量。同時,采用多元醇法制備出不同鎳鈷比例的鎳鉆硫化物,率先研究了鎳鈷成分與鎳鈷雙金屬硫化物電化學性能的關系,鎳鉆雙金屬硫化物樣品具有比相同條件制備出的單金屬硫化物Co3S4和NiS更高的比容量及倍率性能,并且表現(xiàn)出比NiS更高的循環(huán)穩(wěn)定性。 采用一種簡單的溶劑熱法制備出CoSe、Co9Se8、NiSe和NiCo2Se4樣品,率先將其用作電極活性材料獲得了良好的超級電容性能。CoSe及Co9Se8樣品具有超高的循環(huán)穩(wěn)定性,分別經(jīng)過7,000及10,000次循環(huán)后其比容量沒發(fā)生任何衰減。NiSe最有較高的比容量,電流密度為1A/g時實現(xiàn)了高達808.45F/g的比容量。NiCo2Se4樣品綜合具有較高的比容量、倍率特性及循環(huán)穩(wěn)定性,電流密度為1A/g時實現(xiàn)了高達535.7F/g的比容量,電流密度增加50倍后仍可保持最初的67.0%,并且經(jīng)過7,000次充放電循環(huán)后其比容量仍可保持最初的94.92%。
[Abstract]:Electrochemical capacitors (also called supercapacitors) have attracted much attention because of their high power density, excellent cycling stability, fast charging and discharging, etc., which have been widely used in the fields of high power equipment, electric vehicles, electronic equipment and other fields. The specific capacity and excellent cyclic stability are the most promising type of electrode active materials for high energy density supercapacitors. In this study, a series of nickel drilling based compounds, such as nickel drill hydroxide and nickel drilling oxygen, were constructed by changing the composition ratio of nickel and cobalt and the types of coordination anions. The supercapacitor properties of nickel based compounds were systematically studied.
A simple mixed solvent thermal method was proposed, which was successfully used in the preparation of a phase layered nickel cobalt hydroxide with different nickel and cobalt components, and the substrate was introduced to prepare nickel cobalt hydroxide array structure.A phase nickel cobalt hydroxide as the supercapacitor electrode active material to obtain higher specific capacity than a phase Ni (OH) 2. The cyclic stability shows that the formation of hydroxides with nickel and cobalt complexes can obviously improve the electrochemical activity and improve the electrochemical stability of the a phase structure. The specific capacity of Ni Co hydroxides can be further improved by the formation of an array structure with nickel foam, and a good cyclic stability is achieved.
The nickel cobalt oxide and nickel foam bearing array structure samples with different nickel and cobalt ratio can be obtained by thermal decomposition of a phase nickel cobalt hydroxide and the array samples loaded with nickel foam. The nickel cobalt bimetallic oxide sample shows higher specific capacity, multiplying performance and cyclic stability than CO3C4 and NiO samples. The column structure can further improve the specific capacity of nickel cobalt oxide and achieve excellent cyclic stability. At the same time, a simple NiCo2O4 nanostructure with porous structure is prepared by a simple hydrolysis combined with high temperature heat treatment. The NiCo2O4 nanostructure has more than two orders of magnitude higher than C0304 and NiO. The electrode material of super capacitor has higher specific capacity, excellent magnification characteristic and super long cycle stability.
The nickel drilled bimetallic sulfide was first used as a supercapacitor electrode active material and excellent electrochemical performance was obtained. Based on anionic exchange reaction, a simple preparation of NiCo2S4 sea urchin like nanostructures and NiCo2S4 nanotube arrays loaded with nickel foam had a lower NiCo2O4 than the same morphology and structure. The width of the optical band gap and the higher conductivity are helpful to improve the kinetic characteristics of its electrochemical process as the active material of the electrode..NiCo2S4 sea urchin like nanostructures have higher specific capacity and multiple ratio properties than the same morphology and structure of NiCo2O4 and the same preparation method of Co9S8 and NiS. NiCo 2S4 nanotube arrays have achieved ultra-high utilization of electrode materials at a high single load (6mg/cm2), thus achieving super high specific capacity. At the same time, nickel cobalt sulfide with different nickel and cobalt ratios was prepared by polyol method. The relationship between nickel and cobalt composition and the electrochemical properties of nickel cobalt sulfide sulfide was first studied. The samples have higher specific capacity and multiple rate properties than the single metal sulfide Co3S4 and NiS prepared from the same conditions, and exhibit higher cyclic stability than NiS.
CoSe, Co9Se8, NiSe and NiCo2Se4 samples were prepared by a simple solvothermal method. They were first used as electrode active materials to obtain excellent supercapacitor performance,.CoSe and Co9Se8 samples have super high cyclic stability. After 7000 and 10000 cycles, the specific capacity of.NiSe has not occurred any attenuation of.NiSe. When the current density is 1A/g, the.NiCo2Se4 sample with a specific capacity of up to 808.45F/g has a higher specific capacity, multiple rate characteristic and cyclic stability. When the current density is 1A/g, the specific capacity is up to 535.7F/g, and the current density increases 50 times, and it can still maintain the initial 67%, and the specific capacity after the 7000 charge discharge cycle. It is still possible to keep the original 94.92%.

【學位授予單位】：華中科技大學
【學位級別】：博士
【學位授予年份】：2014
【分類號】：TM53

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