磷酸銀基光催化分解水復(fù)合材料的設(shè)計(jì)合成和性能研究
本文選題:磷酸銀 + 石墨相氮化碳; 參考:《江蘇大學(xué)》2017年碩士論文
【摘要】:近年來,能源緊缺和環(huán)境污染形勢越來越嚴(yán)重,也是人類所面臨的重大挑戰(zhàn)。如何有效解決這兩大問題已成為全社會關(guān)注的焦點(diǎn),也是當(dāng)前科學(xué)研究領(lǐng)域亟需解決的關(guān)鍵問題。太陽能是一種清潔、可持續(xù)利用和無污染的能源,具有一定能帶位置的半導(dǎo)體材料能夠有效利用太陽能光催化分解水產(chǎn)生氫氣和氧氣,將光能轉(zhuǎn)換為化學(xué)能,因此基于半導(dǎo)體材料的太陽能光催化技術(shù)被認(rèn)為是解決環(huán)境污染和能源緊缺最有效的方法之一。設(shè)計(jì)合成新型高效的復(fù)合材料應(yīng)用于太陽能光催化分解水研究成為當(dāng)前研究的熱點(diǎn)和難點(diǎn)問題。本論文主要通過將半導(dǎo)體材料(如C_3N_4、MoS_2)和磷酸銀半導(dǎo)體材料有效復(fù)合,制備出具有固定組成和微觀形貌的復(fù)合材料并應(yīng)用于太陽能光催化分解水研究:(1)充分結(jié)合前驅(qū)體共聚改性、高溫?zé)Y(jié)、靜電驅(qū)動(dòng)自組裝及原位反應(yīng)等手段方法,將帶正電荷的銀離子吸附在在非金屬元素改性氮化碳納米結(jié)構(gòu)材料上,后通過添加的磷酸鹽與吸附在氮化碳基體上銀離子的原位反應(yīng),實(shí)現(xiàn)改性氮化碳/磷酸銀復(fù)合材料的可控制備。復(fù)合材料的組成、結(jié)構(gòu)、形貌等測試分析結(jié)果表明其具有相對固定的化學(xué)組成、晶體及化學(xué)結(jié)構(gòu)、可控的形貌及界面。光催化評價(jià)結(jié)果顯示:復(fù)合材料的太陽能光催化分解水產(chǎn)氧活性相對于純的磷酸銀材料來說提升較多。(2)基于超聲剝離技術(shù)獲得少層結(jié)構(gòu)的片狀二硫化鉬材料,將其與磷酸銀材料有效組裝,獲得片狀二硫化鉬/磷酸銀復(fù)合材料;利用水熱合成技術(shù)、靜電驅(qū)動(dòng)自組裝及原位反應(yīng)等手段,制備出花狀二硫化鉬/磷酸銀復(fù)合材料。掃描電鏡及透射電鏡等分析結(jié)果顯示:兩體系復(fù)合材料均具有較好的微觀形貌和界面復(fù)合;化學(xué)組成、晶體結(jié)構(gòu)以及光譜測試結(jié)果表明:復(fù)合材料的化學(xué)組成相對固定,微觀形貌及界面可控;對可見光的吸收和利用效果好。光解水測試結(jié)果表明:復(fù)合材料在模擬太陽光下光催化分解水產(chǎn)氧效率要遠(yuǎn)遠(yuǎn)高于純磷酸銀;所獲得的花狀二硫化鉬/磷酸銀復(fù)合材料相對于片狀二硫化鉬/磷酸銀復(fù)合材料而言,可見光催化分解水產(chǎn)氧效率要更高。(3)進(jìn)一步采用電子自旋共振(ESR)的原位檢測技術(shù),實(shí)時(shí)監(jiān)測不同材料在可見光驅(qū)動(dòng)下光催化分解水實(shí)驗(yàn)過程中產(chǎn)生的活性含氧自由基種類及濃度,通過不同含氧自由基種類和濃度的分析,確定不同復(fù)合材料光催化分解水過程中起主導(dǎo)作用的活性基團(tuán),并結(jié)合其他分析測試結(jié)果合理推測各系列復(fù)合材料的光催化反應(yīng)機(jī)理。
[Abstract]:In recent years, energy shortage and environmental pollution are becoming more and more serious. How to solve these two problems effectively has become the focus of attention of the whole society, and is also the key problem that needs to be solved in the field of scientific research. Solar energy is a clean, sustainable and pollution-free energy source. Semiconductor materials with certain energy positions can effectively use solar energy to catalyze the decomposition of water to produce hydrogen and oxygen, and convert light energy into chemical energy. Therefore, solar photocatalysis based on semiconductor materials is considered to be one of the most effective methods to solve environmental pollution and energy shortage. It has become a hot and difficult problem to design and synthesize new and efficient composite materials for solar photocatalytic decomposition of water. In this thesis, the composite with fixed composition and micro-morphology was prepared by effectively compounding semiconductor materials (such as C _ S _ 3N _ 4MoS _ 2) with silver phosphate semiconductors and applied to the study of photocatalytic decomposition of water by solar energy. By means of high temperature sintering, electrostatic self-assembly and in-situ reaction, silver ions with positive charge were adsorbed on non-metallic elements modified carbon nitride nanostructures. The controllable preparation of the modified carbon nitride / silver phosphate composite was realized by the in-situ reaction of the added phosphate and the silver ion adsorbed on the carbon nitride matrix. The composition, structure and morphology of the composite show that the composite has relatively fixed chemical composition, crystal and chemical structure, controllable morphology and interface. The results of photocatalytic evaluation showed that the photocatalytic activity of the composite was much higher than that of pure silver phosphate) the lamellar molybdenum disulfide material with less layer structure was obtained based on ultrasonic stripping technology. The flake molybdenum disulfide / silver phosphate composite was prepared by hydrothermal synthesis, electrostatic self-assembly and in-situ reaction. The results of scanning electron microscopy and transmission electron microscopy show that the composites have good microstructure and interfacial compounding, and the chemical composition, crystal structure and spectrum of the composites are relatively fixed. The microstructure and interface are controllable, and the absorption and utilization of visible light are good. The results of photolysis water test showed that the efficiency of photocatalytic decomposition of aquatic oxygen was much higher than that of pure silver phosphate under simulated sunlight. Compared with the flake molybdenum disulfide / silver phosphate composite, the visible photocatalytic decomposition efficiency of aquatic oxygen is higher than that of the flake molybdenum disulfide / silver phosphate composite. The kinds and concentrations of active oxygen free radicals produced by different materials in the process of photocatalytic decomposition of water under visible light were monitored in real time, and the types and concentrations of different oxygen free radicals were analyzed. The active groups which play a leading role in the process of photocatalytic decomposition of water in different composite materials were determined, and the photocatalytic reaction mechanism of each series of composite materials was reasonably inferred in combination with other analytical results.
【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】:TB33;O643.36
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