新型改性銀基半導(dǎo)體材料的制備及光催化性能研究
本文選題:鎢酸銀 + 碳酸銀; 參考:《江蘇大學(xué)》2017年碩士論文
【摘要】:Ag~+擁有d10全滿或者全空的特殊電子結(jié)構(gòu)和具有較寬的可見光吸收范圍,且會產(chǎn)生獨(dú)特的自穩(wěn)定系統(tǒng)而在光催化領(lǐng)域可作為重要的可見光催化材料。然而銀基化合物材料在催化過程中會發(fā)生光化學(xué)腐蝕而產(chǎn)生銀單質(zhì),進(jìn)而降低了光催化活性,限制了其在能源、環(huán)境等領(lǐng)域的實(shí)際應(yīng)用。因此尋找有效的方法來改善銀基材料的穩(wěn)定性和催化性能成為了研究的重點(diǎn)。本論文主要從新型催化劑的制備和合成方法上入手,采用不同的方法合成了Ag_2CO_3/AC、Ag_2WO_4/RGO、Ag_2WO_4/WO_3異質(zhì)結(jié)、Ag/Ag_2WO_4/g-C3N4三元等離子體和RGO/ZnFe2O_4/Ag_2WO_4光催化劑,從而提高了銀系材料的光催化活性與穩(wěn)定性。通過FT-IR、UV-Vis、XRD、Raman、SEM、TEM和XPS等表征方法,對樣品的結(jié)構(gòu)、形貌、光吸收性質(zhì)及光催化性能進(jìn)行了分析。本論文的主要研究內(nèi)容如下:(1)通過一步簡單沉淀法,合成了一系列不同質(zhì)量比的Ag_2CO_3/AC(Activated carbon)復(fù)合材料;將其應(yīng)用于去除含羅丹明B(RhB)有機(jī)染料廢水處理,探討了不同AC含量對復(fù)合材料光催化性能的影響。實(shí)驗結(jié)果表明Ag_2CO_3/AC(20%)時,催化材料對RhB的去除效率達(dá)到96.6%。并且AC含量為20%的樣品的降解速率是純Ag_2CO_3的10.22倍。(2)通過一步水熱法,對Ag_2WO_4進(jìn)行石墨烯摻雜,以改善其表面結(jié)構(gòu)及物理性能。考察了不同含量的RGO制備的光催化劑的光催化性能。實(shí)驗結(jié)果表明,RGO片層能有效地轉(zhuǎn)移光生電子,抑制Ag_2WO_4的光腐蝕,從而使得復(fù)合材料具有更優(yōu)異的催化活性和穩(wěn)定性,尤其是樣品AR-3具有最好可見光催化活性。(3)首先以水熱-酸化-煅燒法合成空心球狀的WO_3,通過Ag_2CO_3與WO_3不同比例混合煅燒得到一系列Ag_2WO_4/WO_3異質(zhì)結(jié)復(fù)合材料。結(jié)果表明,在可見光照射下最高活性可達(dá)到94%。并且Ag_2WO_4/WO_3異質(zhì)結(jié)光催化劑顯示出優(yōu)異的穩(wěn)定性。其動力學(xué)反應(yīng)速率幾乎是純WO_3和Ag_2WO_4的17.0和7.5倍。(4)首先煅燒三聚氰胺得到塊狀g-C3N4,通過酸化超聲得到單層g-C3N4,再通過一步水熱合成不同比例的Ag/Ag_2WO_4/g-C3N4三元等離子體催化劑。以RhB或Tetracycline(TC)為目標(biāo)降解物,研究了Ag/Ag_2WO_4/g-C3N4的光催化活性,結(jié)合表征探討機(jī)理。實(shí)驗結(jié)果表明,Ag/Ag_2WO_4均勻分散在g-C3N4納米片的表面。并且Ag納米粒子作為電荷分離中心對光催化活性和穩(wěn)定性起到了重要的作用。復(fù)合材料的光催化活性要明顯優(yōu)于g-C3N4和Ag_2WO_4,且動力學(xué)常數(shù)(0.0125 min-1)高于Ag_2WO_4和Ag/Ag_2WO_4。(5)水熱合成納米球狀結(jié)構(gòu)的RGO/ZnFe2O_4,再通過一步共沉淀法合成RGO/ZnFe2O_4/Ag_2WO_4;表征用其結(jié)構(gòu)形態(tài)、化學(xué)組成、可見光吸收能力和光學(xué)性質(zhì)。采用RhB對其催化性進(jìn)行評價。結(jié)果表明,復(fù)合材料比單一樣品具有更高的催化能力,其中RGO/ZFO/AWO-2(1:6)催化效率最高(近90%),其動力學(xué)常數(shù)為0.012 min-1。
[Abstract]:Ag~ has a special electronic structure of d _ (10) full or empty and has a wide range of visible light absorption. It also produces a unique self-stabilization system and can be used as an important visible photocatalytic material in the field of photocatalysis. However, the photochemical corrosion of silver-based compound materials will occur in the process of photochemical corrosion, which will reduce the photocatalytic activity and limit its practical application in the fields of energy, environment and so on. Therefore, to find effective methods to improve the stability and catalytic performance of silver-based materials has become the focus of research. In this paper, the preparation and synthesis methods of new catalysts are discussed, and the Ag2CO3 / AAC / Ag2WO / AW _ 4 photocatalysts have been synthesized by different methods. The photocatalytic activity and stability of Ag / Ag-2WO _ 3N _ 4 ternary plasma and RGO-ZnFe _ 2O _ 4 / Ag _ 2WO _ 4 photocatalysts have been improved by using different methods in the synthesis of Ag2CO3 / AAC / Ag-2WO _ 4 photocatalysts, thus increasing the photocatalytic activity and stability of the Ag / Ag _ 2WO _ 3N _ 4 heterojunction as well as the RGO-ZnFe2O4 / Ag2WO _ 4 photocatalyst. The structure, morphology, photoabsorption properties and photocatalytic properties of the samples were characterized by FTIR UV-Vis-XRDX (XRDX) Ramande SEMU TEM and XPS. The structure, morphology, photoabsorption properties and photocatalytic properties of the samples were analyzed by means of TEM and XPS. The main contents of this thesis are as follows: (1) A series of Ag2CO3 / AC (Activated carbon) composites with different mass ratios have been synthesized by one step simple precipitation method and applied to the treatment of organic dyestuff wastewater containing Rhodamine B (RhB). The effect of different AC content on the photocatalytic properties of composites was discussed. The experimental results show that when Ag2CO3 / AC (20%), the removal efficiency of RhB by the catalytic material reaches 96.6. And the degradation rate of the sample with 20% AC content is 10.22 times that of the pure Ag2COST3. (2) Ag2WO4 is doped with graphene by one step hydrothermal method to improve its surface structure and physical properties. The photocatalytic properties of the photocatalysts prepared by RGO were investigated. The experimental results show that the RGO layer can effectively transfer photogenerated electrons and inhibit the photocorrosion of Ag2WOS _ 4, which makes the composite have better catalytic activity and stability. Especially, the sample AR-3 has the best visible photocatalytic activity. (3) first, hollow spherical WO _ S _ 3s were synthesized by hydrothermal acidification-calcination method, and a series of Ag2WO _ 4 / WO _ 3 heterojunction composites were obtained by calcination of AgStud _ 2CO _ 3 and WO _ S _ 3 in different proportions. The results showed that the highest activity could reach 94g under visible light irradiation. And AgSZ / WO\ +\ {3\}\ ^ 3 heterojunction photocatalysts show excellent stability. The kinetic reaction rate is almost 17.0 and 7.5 times of that of pure WO _ S _ 3 and Ag_ 2WOS _ 4. (4) the bulk g-C _ 3N _ 4 is obtained by calcination of melamine, the monolayer g-C _ 3N _ 4 is obtained by acidizing ultrasound, and then the agg / g _ 2W _ 2W _ 2W _ 2W _ 2W _ 3N _ 4 ternary plasma catalyst is synthesized by one step hydrothermal treatment. With RhB or Tetracycline (TC) as the target degradation material, the photocatalytic activity of Ag / Ag2WOT _ 4 / g-C _ 3N _ 4 was studied and the mechanism was discussed. The experimental results show that Ag / Ag2WO _ 4 is uniformly dispersed on the surface of g-C _ 3N _ 4 nanoparticles. And Ag nanoparticles as charge separation centers play an important role in photocatalytic activity and stability. The photocatalytic activity of the composite is significantly better than that of g-C _ 3N _ 4 and AgS _ 2WO _ 4, and the kinetic constant (0.0125 min-1) is higher than that of Ag2W _ 2W _ 2O _ 4 and AgS _ 2W _ 2O _ 4. (5) hydrothermal synthesis of spherical RGO-ZnFe _ 2O _ 2O _ 4, and synthesis of RGO-ZnFe _ 2O _ 4 / Ag _ 2WO _ 4 by one-step coprecipitation. Visible light absorption capacity and optical properties. RhB was used to evaluate its catalytic properties. The results show that the composite has higher catalytic activity than the single sample, among which RGO / ZFOP AWO-2 (1:6) has the highest catalytic efficiency (nearly 90%), and its kinetic constant is 0.012 min-1.
【學(xué)位授予單位】:江蘇大學(xué)
【學(xué)位級別】:碩士
【學(xué)位授予年份】:2017
【分類號】:O643.36
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