纖維負(fù)載錳氧化物催化劑的制備及其室溫降解甲醛性能研究
發(fā)布時(shí)間：2018-10-12 16:48
【摘要】：甲醛(HCHO)是室內(nèi)主要污染物之一,主要來(lái)源于室內(nèi)裝修用的膠合板、細(xì)木工板、中密度纖維板和刨花板等人造板材。甲醛是世界衛(wèi)生組織公認(rèn)的致癌物之一,長(zhǎng)期暴露在高濃度甲醛環(huán)境中對(duì)人的身體健康危害很大。所以,一直以來(lái)室內(nèi)甲醛的去除都是環(huán)境工程領(lǐng)域的研究熱點(diǎn)。目前室內(nèi)甲醛的去除方法有物理吸附法、化學(xué)反應(yīng)法、生物降解法、光催化及催化氧化法等,其中過(guò)渡金屬氧化物因其價(jià)格低廉,氧化甲醛效果好且氧化過(guò)程無(wú)有害副產(chǎn)物生成而受到人們的青睞。在過(guò)渡金屬氧化物中,錳氧化物對(duì)甲醛的氧化性能優(yōu)異,甚至優(yōu)于貴金屬負(fù)載的催化劑材料。而纖維負(fù)載錳氧化物型催化材料因其成本低、效果好、易應(yīng)用于實(shí)際等優(yōu)點(diǎn),近年來(lái)成為人們研究的焦點(diǎn)之一。本文選用過(guò)濾棉和絲瓜絡(luò)兩種纖維作為載體,通過(guò)氧化還原法制備了兩種纖維負(fù)載錳氧化物的復(fù)合材料。研究了原料濃度、浸漬時(shí)間等制備條件對(duì)甲醛凈化效果的影響。利用掃描電鏡(SEM)、X射線衍射(XRD)、拉曼光譜(Raman)研究了制備的錳氧化物的形貌、晶型和物相,對(duì)纖維負(fù)載錳氧化物復(fù)合材料在室溫下對(duì)甲醛的降解性能進(jìn)行了測(cè)試,通過(guò)氣相色譜(GC)分析甲醛降解后的產(chǎn)物,原位紅外(in-situ FTIR)分析材料失活的機(jī)制。采用甲醇還原高錳酸鉀(KMn O4)的方法,室溫條件下原位制備了過(guò)濾棉負(fù)載錳氧化物(Mn Ox/PET)復(fù)合材料。研究了高錳酸鉀濃度、甲醇濃度以及十六烷基三甲基溴化銨(CTAB)濃度對(duì)錳氧化物負(fù)載量的影響。Mn Ox/PET材料室溫去除甲醛的性能測(cè)試結(jié)果表明,當(dāng)甲醛濃度為105mg/m3時(shí),Mn Ox/PET在2 h內(nèi)將甲醛全部降解為二氧化碳。Mn Ox/PET材料的表征結(jié)果表明,制備的錳氧化物為無(wú)定形態(tài)與水鈉錳礦型的混合物,形貌為100~200 nm尺寸的顆粒狀。以載體絲瓜絡(luò)為還原劑,高錳酸鉀為氧化劑,在室溫條件下振蕩不同時(shí)間,制備了絲瓜絡(luò)負(fù)載錳氧化物(Mn Ox/LF)復(fù)合材料。研究了高錳酸鉀濃度和制備時(shí)間對(duì)材料去除甲醛活性的影響,獲得室溫下去除甲醛性能最優(yōu)的材料。最優(yōu)的制備條件是0.2 g KMn O4+20 m L水+0.2 g絲瓜絡(luò)于搖床上室溫下反應(yīng)16 h。Mn Ox/LF材料室溫下去除甲醛性能測(cè)試結(jié)果表明,當(dāng)甲醛濃度為320 mg/m3時(shí),Mn Ox/LF復(fù)合材料在5 h后對(duì)甲醛的去除率達(dá)90%以上,降解的甲醛全部氧化為二氧化碳。Mn Ox/LF材料的表征結(jié)果表明,絲瓜絡(luò)上負(fù)載的錳氧化物顆粒尺寸為~50 nm,絲瓜絡(luò)與高錳酸鉀反應(yīng)前后晶型結(jié)構(gòu)發(fā)生了改變,表明其與高錳酸鉀發(fā)生了氧化還原反應(yīng)。此外,研究發(fā)現(xiàn)纖維負(fù)載錳氧化物復(fù)合材料降解甲醛的機(jī)制為載體的吸附于錳氧化物的氧化協(xié)同作用。
[Abstract]:Formaldehyde (HCHO) is one of the main indoor pollutants, mainly from plywood, woodboard, MDF and particleboard. Formaldehyde is one of the carcinogens recognized by the World Health Organization (WHO). Therefore, the removal of indoor formaldehyde has always been a research hotspot in the field of environmental engineering. At present, the removal methods of indoor formaldehyde include physical adsorption, chemical reaction, biodegradation, photocatalysis and catalytic oxidation, among which transition metal oxides are cheap. Formaldehyde oxidation is favored by people because of its good effect and no harmful byproducts in the oxidation process. Among transition metal oxides, manganese oxide has excellent oxidation performance for formaldehyde, even better than noble metal supported catalyst material. Because of its low cost, good effect and easy to be applied in practice, fiber supported manganese oxide catalytic material has become one of the focuses of research in recent years. In this paper, two kinds of fibers, filter cotton and luffa, were used as carriers to prepare manganese oxide composites by redox method. The effects of raw material concentration, impregnation time and other preparation conditions on the purification of formaldehyde were studied. The morphology, crystal form and phase of manganese oxide were studied by scanning electron microscope (SEM), X) (SEM), X ray diffraction (XRD), Raman spectroscopy. The degradation of formaldehyde in fiber supported manganese oxide composites at room temperature was tested. The products of formaldehyde degradation were analyzed by gas chromatography (GC) and the mechanism of material inactivation was analyzed by in situ infrared (in-situ FTIR). Filtration cotton loaded manganese oxide (Mn Ox/PET) composites were prepared by methanol reduction of potassium permanganate (KMn O 4) at room temperature. The effects of potassium permanganate concentration, methanol concentration and cetyltrimethylammonium bromide (CTAB) concentration on the loading amount of manganese oxide were studied. When formaldehyde concentration is 105mg/m3, Mn Ox/PET degrades all formaldehyde to carbon dioxide in 2 h. The results of characterization of Mn Ox/PET material show that the prepared manganese oxide is a mixture of amorphous form and sodium manganite type, and its morphology is 100 ~ 200 nm granular. Mn Ox/LF composites were prepared by oscillating at room temperature with luffa complex as reducing agent and potassium permanganate as oxidant. The effects of potassium permanganate concentration and preparation time on the formaldehyde removal activity of the materials were studied. The best material for formaldehyde removal at room temperature was obtained. The optimum preparation condition is 0.2 g KMn O 4 20 mL water 0.2 g luffa lucifera under the room temperature reaction 16 h.Mn Ox/LF material on the rocker. When formaldehyde concentration was 320 mg/m3, the removal rate of formaldehyde in Mn Ox/LF composite was more than 90% after 5 h, and all the degraded formaldehyde was oxidized to carbon dioxide. The results of characterization of Mn Ox/LF material showed that the content of formaldehyde was more than 90%. The grain size of manganese oxide loaded on the loofah was about 50 nm, and the crystal structure changed before and after the reaction with potassium permanganate, which indicated that it redox with potassium permanganate. In addition, the mechanism of degradation of formaldehyde by fiber supported manganese oxide composite was found to be the synergistic effect of adsorption on manganese oxide.
【學(xué)位授予單位】：北京建筑大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2015
【分類號(hào)】：X51;O643.36
本文編號(hào)：2266869
[Abstract]:Formaldehyde (HCHO) is one of the main indoor pollutants, mainly from plywood, woodboard, MDF and particleboard. Formaldehyde is one of the carcinogens recognized by the World Health Organization (WHO). Therefore, the removal of indoor formaldehyde has always been a research hotspot in the field of environmental engineering. At present, the removal methods of indoor formaldehyde include physical adsorption, chemical reaction, biodegradation, photocatalysis and catalytic oxidation, among which transition metal oxides are cheap. Formaldehyde oxidation is favored by people because of its good effect and no harmful byproducts in the oxidation process. Among transition metal oxides, manganese oxide has excellent oxidation performance for formaldehyde, even better than noble metal supported catalyst material. Because of its low cost, good effect and easy to be applied in practice, fiber supported manganese oxide catalytic material has become one of the focuses of research in recent years. In this paper, two kinds of fibers, filter cotton and luffa, were used as carriers to prepare manganese oxide composites by redox method. The effects of raw material concentration, impregnation time and other preparation conditions on the purification of formaldehyde were studied. The morphology, crystal form and phase of manganese oxide were studied by scanning electron microscope (SEM), X) (SEM), X ray diffraction (XRD), Raman spectroscopy. The degradation of formaldehyde in fiber supported manganese oxide composites at room temperature was tested. The products of formaldehyde degradation were analyzed by gas chromatography (GC) and the mechanism of material inactivation was analyzed by in situ infrared (in-situ FTIR). Filtration cotton loaded manganese oxide (Mn Ox/PET) composites were prepared by methanol reduction of potassium permanganate (KMn O 4) at room temperature. The effects of potassium permanganate concentration, methanol concentration and cetyltrimethylammonium bromide (CTAB) concentration on the loading amount of manganese oxide were studied. When formaldehyde concentration is 105mg/m3, Mn Ox/PET degrades all formaldehyde to carbon dioxide in 2 h. The results of characterization of Mn Ox/PET material show that the prepared manganese oxide is a mixture of amorphous form and sodium manganite type, and its morphology is 100 ~ 200 nm granular. Mn Ox/LF composites were prepared by oscillating at room temperature with luffa complex as reducing agent and potassium permanganate as oxidant. The effects of potassium permanganate concentration and preparation time on the formaldehyde removal activity of the materials were studied. The best material for formaldehyde removal at room temperature was obtained. The optimum preparation condition is 0.2 g KMn O 4 20 mL water 0.2 g luffa lucifera under the room temperature reaction 16 h.Mn Ox/LF material on the rocker. When formaldehyde concentration was 320 mg/m3, the removal rate of formaldehyde in Mn Ox/LF composite was more than 90% after 5 h, and all the degraded formaldehyde was oxidized to carbon dioxide. The results of characterization of Mn Ox/LF material showed that the content of formaldehyde was more than 90%. The grain size of manganese oxide loaded on the loofah was about 50 nm, and the crystal structure changed before and after the reaction with potassium permanganate, which indicated that it redox with potassium permanganate. In addition, the mechanism of degradation of formaldehyde by fiber supported manganese oxide composite was found to be the synergistic effect of adsorption on manganese oxide.
【學(xué)位授予單位】：北京建筑大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2015
【分類號(hào)】：X51;O643.36
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