本文選題：吸附劑　切入點：催化劑　出處：《吉林大學(xué)》2017年博士論文

【摘要】：隨著城市化和生活水平的不斷提高,全球能源消耗和環(huán)境負(fù)擔(dān)急劇增加。用可再生能源代替?zhèn)鹘y(tǒng)能源是解決能源和相應(yīng)環(huán)境問題的一種重要方法,既能減少污染物的產(chǎn)生又能滿足能源需求。含有有機(jī)染料污染物廢水的數(shù)量已經(jīng)遠(yuǎn)遠(yuǎn)超出了生態(tài)系統(tǒng)的自我修復(fù)能力。迄今為止,一些物理,化學(xué)和生物類的處理方法已經(jīng)被廣泛研究,其中涌現(xiàn)出了大量具有實際應(yīng)用潛力的候選材料。然而實驗研究與實際應(yīng)用之間仍然存在極大的差距,例如,制備工藝昂貴和制備過程的復(fù)雜性,以及低的降解效率,同時也有可能引起二次污染。此外,隨著對高能量和功率密度存儲器件不斷增長的需求,有必要在充電電池和超級電容器的科學(xué)技術(shù)上獲得突破性進(jìn)展,來滿足未來低碳和可持續(xù)經(jīng)濟(jì)的發(fā)展目標(biāo)。針對以上的挑戰(zhàn),本文制備了幾種鐵族合金和其復(fù)合物材料來緩解面臨的環(huán)境問題和能源危機(jī)。本文系統(tǒng)的對材料的結(jié)構(gòu),形貌以及反應(yīng)機(jī)理和性能等進(jìn)行了研究。主要研究內(nèi)容如下:(1)八面體結(jié)構(gòu)的CoFe/CoFe_2O_4亞微米級復(fù)合物通過一種靈巧的一步水熱法制備,作為催化過一硫酸鹽(PMS)的異質(zhì)催化劑,能將污水中含有的有機(jī)污染物降解。經(jīng)過本實驗的研究,在“CoFe/CoFe2O4+PMS”體系的氧化反應(yīng)過程中硫酸根(SO4·-)和羥基自由基(·OH)同時參與降解有機(jī)污染物。無毒性的CoFe/CoFe2O4亞微米復(fù)合物能高效降解溶液中的橙黃II。并對CoFe/CoFe2O4作為PMS催化劑的催化機(jī)理進(jìn)行了系統(tǒng)的分析。CoFe/CoFe2O4復(fù)合物出眾的催化性能,優(yōu)異的重復(fù)利用性和穩(wěn)定性,更廣泛的普遍適用性和磁回收性能使其成為環(huán)境矯正中的候選催化劑材料。(2)通過簡單的室溫硼氫化鈉還原法制備了一系列室溫穩(wěn)定的Co_xNi_(1-x)(x=0,0.2,0.4,0.6,0.8 and 1)雙金屬合金納米顆粒。通過調(diào)節(jié)制備的Co_xNi_(1-x)雙金屬納米顆粒的化學(xué)組成,研究了樣品對含有剛果紅的污水的吸附能力。具有鐵磁性能的Co_xNi_(1-x)合金納米顆粒能夠?qū)⑷芤褐械膭偣t快速高效的移除,在吸附過程結(jié)束后,可以用磁體將吸附后的物質(zhì)從水溶液中快速分離出來�；瘜W(xué)組成為Co0.6Ni0.4的雙金屬合金納米顆粒顯示了最高的吸附效率。并且吸附過程中,化學(xué)吸附與靜電吸附同時發(fā)生,其中化學(xué)吸附占主導(dǎo)地位。此外,應(yīng)用密度泛函理論計算的輔助,對Co0.6Ni0.4雙金屬合金的優(yōu)異吸附效率進(jìn)行了深入研究。在計算中,建立了一系列的表面模型用以對比表面能、功函數(shù)、態(tài)密度和表面電子差分密度之間的差異。通過對表面電子結(jié)構(gòu)的進(jìn)一步研究,表明化學(xué)組成和表面缺陷對d帶中心具有重要的影響,恰當(dāng)?shù)膁帶結(jié)構(gòu)對吸附性能有直接的影響。結(jié)合實驗和理論計算的結(jié)果進(jìn)一步證明了Co0.6Ni0.4合金比單金屬具有優(yōu)秀吸附性能的原因,也表明Co0.6Ni0.4合金可以作為商業(yè)化大規(guī)模的磁性吸附劑使用。(3)本工作中,通過一種新奇的方法制備了一系列的鈷鎳雙金屬/鈷-鎳氧化物@碳(M/MO@C)結(jié)構(gòu)的復(fù)合物。以吸附剛果紅分子的CoNi納米顆粒復(fù)合物作為前驅(qū)體,經(jīng)高溫氮氣氣氛下的煅燒制備了M/MO@C復(fù)合物。以制得的復(fù)合物作為超級電容器的電極材料,通過電化學(xué)性能測試,確定了具有最佳電化學(xué)性能的材料中Co_xNi_(1-x)合金的最佳化學(xué)組成是Co0.2Ni0.8,最佳煅燒溫度為600oC。在最佳制備條件下獲得的具有薄片狀結(jié)構(gòu)的M/MO@C-600復(fù)合物在1 A g~(-1)的電流密度下的比容量可達(dá)1134.9 F g~(-1),在10 A g~(-1)的電流密度下循環(huán)充放電2000圈后,其容量可保留初始容量的66%。此外,以M/MO@C-600復(fù)合物為正極,商用活性炭作為負(fù)極組裝了非對稱電容器。非對稱電容器在0.5 A g~(-1)的電流密度下比容量可達(dá)111.2 F g~(-1),在功率密度為0.425 Kw kg~(-1)時其能量密度可達(dá)44.6 Wh kg~(-1)。在6 A g~(-1)的電流密度下循環(huán)充放電10000圈后非對稱電容器的比容量可基本保持100%。本文提出的制備方法摒棄了傳統(tǒng)方法中使用的碳源,以有機(jī)染料剛果紅分子作為碳源成功制備出的M/MO@C-600復(fù)合物可用作超級電容器的電極材料,實現(xiàn)了污水處理產(chǎn)生的副產(chǎn)物作為綠色能源存儲材料的二次利用,這種經(jīng)濟(jì)綠色環(huán)保的制備方法可同時緩解來自于環(huán)境和能源方面的壓力。
[Abstract]:With the city and the continuous improvement of living standards, the global energy consumption and environmental burden increased dramatically. With the renewable energy to replace traditional energy is an important way to solve the energy and environmental problems, which can not only reduce the generation of pollutants and can meet the demand for energy. There are a number of wastewater containing organic dye pollutants has far exceeded the self repair the capacity of the ecological system. So far, some physical, chemical and biological treatment methods of the class has been extensively studied, including the emergence of a large number of candidate materials has application potential. However, experimental research of great gap still exists between the research and practical application for example, the complexity of preparation process of preparation process and expensive system, and low degradation efficiency, but also may cause two pollution. In addition, with the continuous growth of high energy and power density memory requirements, it is necessary to Breakthrough in battery and super capacitor in science and technology, to meet the objectives of the future development of low carbon and sustainable economy. In view of the above challenges, this paper prepared several iron group alloys and its composites to ease the energy crisis and environment problem. In this paper the structure of material. The morphology and the reaction mechanism and properties were studied. The main contents are as follows: (1) CoFe/CoFe_2O_4 sub micron composite eight surface structure by a one-step hydrothermal method to prepare as smart, a catalytic sulfate (PMS) heterogeneous catalyst can decompose organic pollutants in wastewater. After the experiment, in the oxidation process of CoFe/CoFe2O4+PMS system in sulfate (SO4 -) and hydroxyl radical (- OH) are also involved in the degradation of organic pollutants. The non-toxic CoFe/ CoFe2O4 submicron complex Compound capable of degrading solution of orange II. and CoFe/CoFe2O4 as the catalytic mechanism of PMS catalyst for the catalytic performance of complex.CoFe/CoFe2O4 system analysis outstanding, excellent reusability and stability, wide universality and magnetic recovery performance has been corrected in the environment (2) candidate catalyst material. A series of room temperature stable Co_xNi_ were prepared at room temperature by a simple reduction of sodium borohydride (1-x) (x=0,0.2,0.4,0.6,0.8 and 1) bimetallic alloy nanoparticles. By adjusting the preparation of Co_xNi_ (1-x) chemical composition of bimetallic nanoparticles, were studied with Congo red sewage adsorption capacity with iron. The magnetic properties of Co_xNi_ (1-x) alloy nanoparticles in solution can be fast and efficient removal of Congo red, in the adsorption process is finished, can be adsorbed from aqueous solution with magnet material Fast separation. The chemical composition of bimetallic alloy nanoparticles of Co0.6Ni0.4 showed the highest adsorption efficiency and adsorption process, chemical adsorption and electrostatic adsorption occurred at the same time, the chemical adsorption is dominant. In addition, the auxiliary calculation using density functional theory, excellent adsorption efficiency of Co0.6Ni0.4 bimetallic alloy are studied in the calculation, set up a series of surface model is used to compare the surface energy, work function, state density and surface electron density difference between. Through further research of surface electronic structure, chemical composition and surface defects that have important effect on the D center, d with the proper structure directly the influence on the adsorption performance. Combined with the experimental and theoretical results prove that Co0.6Ni0.4 alloy has excellent adsorption properties than the single metal, also shows that Co0.6Ni0 As a commercial magnetic adsorbent mass using.4 alloy. (3) this work, through a novel method to prepare a series of double metal cobalt and nickel / cobalt - nickel oxide @ carbon (M/MO@C) composite structure. The CoNi nano particle compound molecules for adsorption of Congo red the precursor and calcined at high temperature under nitrogen atmosphere to prepare M/MO@C composites. The composites prepared as electrode material for supercapacitor, by electrochemical performance test, to determine the Co_xNi_ has the best electrochemical performance of the materials (1-x) the best chemical composition of the alloy is Co0.2Ni0.8, the optimum calcination temperature for 600oC. in the best the preparation conditions for M/MO@C-600 composite materials with lamellar structure at 1 A g~ (-1) of the current density is lower than the capacity of up to 1134.9 F g~ (-1), A g~ (-1) 10 in the current density cycle after 2000 charge discharge cycles, the capacity retention In addition to the initial capacity of 66%., M/MO@C-600 composite cathode and commercial activated carbon as anode assembly of asymmetric capacitor. The asymmetric capacitor at 0.5 A g~ (-1) of the current density than the capacity of up to 111.2 F g~ (-1), the power density is 0.425 Kw kg~ (-1) when the energy the density of up to 44.6 Wh kg~ (-1). In 6 A g~ (-1) of the current density cycle after 10000 charge discharge cycles asymmetric capacitance can basically keep the preparation method of 100%. is proposed in this paper to abandon the use of traditional methods of organic carbon source, with Congo red dye molecules as the electrode materials of M/MO@C-600 composite material prepared can be used as a carbon source for the super capacitor, the by-product of wastewater treatment as the two use of green energy storage material and preparation method of the green economy can also relieve pressure on the environment and energy aspects.

【學(xué)位授予單位】：吉林大學(xué)
【學(xué)位級別】：博士
【學(xué)位授予年份】：2017
【分類號】：TG139;TB33

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