含鉍配位聚合物的制備、改性及其光催化性能研究
發(fā)布時(shí)間：2018-08-08 17:42
【摘要】：光催化技術(shù)作為一項(xiàng)具有重要應(yīng)用前景的綠色技術(shù),被廣泛用于處理印染廢水。目前,配位聚合物憑借其種類多樣、結(jié)構(gòu)可控、熱穩(wěn)定性高及比表面積大等優(yōu)點(diǎn)廣泛應(yīng)用于光催化領(lǐng)域研究。此外,鉍系氧化物由于具有較窄的禁帶寬度而成為極具發(fā)展前景的可見光響應(yīng)光催化劑。近年來(lái),石墨烯作為一種具有優(yōu)異導(dǎo)電性能和吸附性能的新材料,常被用來(lái)與其他材料制備成復(fù)合物,其復(fù)合物通常具有更好的光催化性能,使光催化技術(shù)得到快速發(fā)展。鑒于含鉍配位聚合物極少報(bào)道,且并未對(duì)其光催化性能進(jìn)行過深入的探討,本文將針對(duì)這些問題展開研究。具體內(nèi)容如下:首先,通過水熱法合成一種新型二維結(jié)構(gòu)鈷鉍雙金屬配位聚合物(簡(jiǎn)稱:24pCoBi),其分子式為BiCoC_(21)H_(17)N_3O_(16)。對(duì)24pCoBi進(jìn)行高溫煅燒得到一復(fù)合物(簡(jiǎn)稱:24pCoBi500)。分別對(duì)兩種材料進(jìn)行多種表征,并通過計(jì)算得到材料的禁帶寬度近似值。在模擬太陽(yáng)光下,兩種材料降解亞甲基藍(lán)(MB)的能力強(qiáng)弱順序?yàn)?24pCoBi50024pCoBi;可見光下降解羅丹明B(RhB)的能力強(qiáng)弱順序?yàn)?24pCoBi24pCoBi500。設(shè)計(jì)實(shí)驗(yàn)改變RhB溶液的pH得出結(jié)論:24pCoBi在強(qiáng)酸條件下對(duì)RhB的降解效果最佳,強(qiáng)堿條件下(pH12.40)則發(fā)生變性。其次,用水熱法合成了一種已知結(jié)構(gòu)的銅鉍雙金屬配位聚合物(簡(jiǎn)稱:35pCuBi)并對(duì)其進(jìn)行高溫煅燒得到一種復(fù)合物(簡(jiǎn)稱:35pCuBi500),同時(shí)用水熱法合成了銅鉍雙金屬配位聚合物與石墨烯的復(fù)合物(簡(jiǎn)稱:35pCuBi/Gr)。分別對(duì)三種材料進(jìn)行多種表征,并通過計(jì)算得到材料的禁帶寬度近似值。通過在模擬太陽(yáng)光下降解MB、可見光下降解RhB考察了三種材料的光催化性能強(qiáng)弱順序?yàn)?35pCuBi50035pCuBi/Gr35pCuBi。設(shè)計(jì)實(shí)驗(yàn)改變RhB溶液的pH得出結(jié)論:35pCuBi在強(qiáng)酸條件下對(duì)RhB的降解效果明顯提升,其較適宜反應(yīng)pH為1.82。最后,探討了35pCuBi/Gr的光催化反應(yīng)機(jī)理。在35pCuBi/Gr的結(jié)構(gòu)中,石墨烯優(yōu)良的導(dǎo)電性能可以加快光生電子的轉(zhuǎn)移速度,從而降低光生電子空穴對(duì)的復(fù)合率、提高太陽(yáng)光利用率。同時(shí)石墨烯的強(qiáng)吸附作用可使有機(jī)分子與光催化劑充分接觸,加速光催化反應(yīng)的進(jìn)行。實(shí)驗(yàn)結(jié)果顯示,可見光下35pCuBi/Gr對(duì)pH 1.82的RhB溶液的兩次循環(huán)降解中,其降解率均可在10分鐘內(nèi)達(dá)到97%以上,且材料結(jié)構(gòu)不發(fā)生改變。
[Abstract]:As a green technology with important application prospect, photocatalytic technology is widely used in the treatment of printing and dyeing wastewater. At present, coordination polymers are widely used in the field of photocatalysis due to their various types, controllable structure, high thermal stability and large specific surface area. In addition, bismuth oxide is a promising photocatalyst for visible light response due to its narrow band gap. In recent years, graphene, as a new material with excellent conductivity and adsorption properties, is often used to prepare composites with other materials. The complexes usually have better photocatalytic properties, which make the photocatalytic technology develop rapidly. Since the coordination polymers containing bismuth are rarely reported and their photocatalytic properties have not been thoroughly discussed, these problems will be studied in this paper. The main contents are as follows: firstly, a novel two-dimensional cobalt-bismuth bimetallic coordination polymer was synthesized by hydrothermal method. Its molecular formula is BiCoC21 H17 N3O16. 24pCoBi was calcined at high temperature to obtain a complex (: 24pCoBi500). Two kinds of materials were characterized and the approximate band gap of the materials was obtained by calculation. Under simulated solar light, the degradation ability of methylene blue (MB) was in the order of: 24pCoBi50024pCoBiand that of visible light descending solution of Rhodamine B (RhB) was: 24pCoBi24pCoBi500. By changing the pH of RhB solution, it is concluded that the degradation effect of RhB is the best under strong acid condition, and denaturation occurs in strong base condition (pH12.40). Secondly, A copper-bismuth bimetallic coordination polymer with known structure (: 35pCuBi) was synthesized by hydrothermal method and calcined at high temperature to obtain a complex (w / 35pCuBi500). At the same time, copper-bismuth bimetallic coordination polymer and graphite were synthesized by hydrothermal method. A complex of alkenes (called: 35 pCuBir / Gr). The three kinds of materials were characterized in different ways, and the approximate band gap of the materials was obtained by calculation. The photocatalytic properties of the three materials were investigated in the order of: 35pCuBi50035pCuBi-Gr35pCuBiR / Gr35pCuBiR by degradation of MBB in simulated solar light and degradation of RhB under visible light in the order of: 35pCuBi50035pCuBi-Gr35pCuBi. The pH of RhB solution was changed by designing experiments. It was concluded that the degradation effect of RhB was obviously improved under the condition of strong acid, and the optimum reaction pH was 1.82. Finally, the photocatalytic reaction mechanism of 35pCuBi/Gr was discussed. In the structure of 35pCuBi/Gr, the excellent conductivity of graphene can accelerate the transfer rate of photogenerated electrons, thus reducing the recombination rate of photogenerated electron hole pairs and increasing the utilization ratio of sunlight. At the same time, the strong adsorption of graphene can make organic molecules fully contact with photocatalyst and accelerate the photocatalytic reaction. The experimental results show that the degradation rate of RhB solution with pH 1.82 can reach more than 97% in 10 minutes after two cycles of 35pCuBi/Gr degradation under visible light, and the structure of the material does not change.
【學(xué)位授予單位】：沈陽(yáng)工業(yè)大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2017
【分類號(hào)】：O641.4
本文編號(hào)：2172536
[Abstract]:As a green technology with important application prospect, photocatalytic technology is widely used in the treatment of printing and dyeing wastewater. At present, coordination polymers are widely used in the field of photocatalysis due to their various types, controllable structure, high thermal stability and large specific surface area. In addition, bismuth oxide is a promising photocatalyst for visible light response due to its narrow band gap. In recent years, graphene, as a new material with excellent conductivity and adsorption properties, is often used to prepare composites with other materials. The complexes usually have better photocatalytic properties, which make the photocatalytic technology develop rapidly. Since the coordination polymers containing bismuth are rarely reported and their photocatalytic properties have not been thoroughly discussed, these problems will be studied in this paper. The main contents are as follows: firstly, a novel two-dimensional cobalt-bismuth bimetallic coordination polymer was synthesized by hydrothermal method. Its molecular formula is BiCoC21 H17 N3O16. 24pCoBi was calcined at high temperature to obtain a complex (: 24pCoBi500). Two kinds of materials were characterized and the approximate band gap of the materials was obtained by calculation. Under simulated solar light, the degradation ability of methylene blue (MB) was in the order of: 24pCoBi50024pCoBiand that of visible light descending solution of Rhodamine B (RhB) was: 24pCoBi24pCoBi500. By changing the pH of RhB solution, it is concluded that the degradation effect of RhB is the best under strong acid condition, and denaturation occurs in strong base condition (pH12.40). Secondly, A copper-bismuth bimetallic coordination polymer with known structure (: 35pCuBi) was synthesized by hydrothermal method and calcined at high temperature to obtain a complex (w / 35pCuBi500). At the same time, copper-bismuth bimetallic coordination polymer and graphite were synthesized by hydrothermal method. A complex of alkenes (called: 35 pCuBir / Gr). The three kinds of materials were characterized in different ways, and the approximate band gap of the materials was obtained by calculation. The photocatalytic properties of the three materials were investigated in the order of: 35pCuBi50035pCuBi-Gr35pCuBiR / Gr35pCuBiR by degradation of MBB in simulated solar light and degradation of RhB under visible light in the order of: 35pCuBi50035pCuBi-Gr35pCuBi. The pH of RhB solution was changed by designing experiments. It was concluded that the degradation effect of RhB was obviously improved under the condition of strong acid, and the optimum reaction pH was 1.82. Finally, the photocatalytic reaction mechanism of 35pCuBi/Gr was discussed. In the structure of 35pCuBi/Gr, the excellent conductivity of graphene can accelerate the transfer rate of photogenerated electrons, thus reducing the recombination rate of photogenerated electron hole pairs and increasing the utilization ratio of sunlight. At the same time, the strong adsorption of graphene can make organic molecules fully contact with photocatalyst and accelerate the photocatalytic reaction. The experimental results show that the degradation rate of RhB solution with pH 1.82 can reach more than 97% in 10 minutes after two cycles of 35pCuBi/Gr degradation under visible light, and the structure of the material does not change.
【學(xué)位授予單位】：沈陽(yáng)工業(yè)大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2017
【分類號(hào)】：O641.4
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