Ag_3PO_4/Ag_2S/g-C_3N_4复合光催化剂的制备与性能
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摘要
通过沉积法和离子交换法成功地制备了Ag_3PO_4/Ag_2S/g-C_3N_4复合型光催化剂。利用X射线多晶粉末衍射仪(XRD)、扫描电子显微镜(SEM)、透射电子显微镜(TEM)、X射线光电子能谱(XPS)、N_2吸附-脱附等温线、紫外-可见漫反射光谱、荧光光谱等手段对样品进行了表征。通过降解罗丹明B考察其可见光催化活性及稳定性,研究了硫化钠与磷酸银物质的量的比值(n_(Na_2S)/n_(Ag_3PO_4))、g-C_3N_4添加量对所制备复合光催化材料性能的影响,同时对光催化机理进行了探讨。结果表明,随着n_(Na2S)/n_(Ag3PO4)的增加,所得复合催化材料活性先增加后降低;当n_(Na2S)/n_(Ag_3PO_4)为1.5%、g-C_3N_4与Ag_3PO_4的质量比为3∶7时制备的催化剂ASC1.5的光催化活性最好,在可见光照射下,40 min内可将罗丹明B完全降解,且5次循环使用后仍保持较高的催化活性。和Ag_3PO_4相比,Ag_3PO_4/Ag_2S/g-C_3N_4复合型光催化材料的活性与稳定性都得到明显提高,这主要归因于复合催化剂比表面积和孔结构的增加,载流子分离效率的提高。光催化机理研究表明,空穴(h~+)、超氧阴离子自由基(·O~(2-))和羟基自由基(·OH)都是光催化过程中的主要活性物种。三者作用大小依次为:h~+>·O~(2-)>·OH。
Ag_3PO_4/Ag_2S/g-C_3N_4composite photocatalysts were successfully prepared by a deposition-ion exchanged combined method.And the obtained samples were characterized by X-ray powder diffractometer(XRD),scanning electron microscope(SEM),transmission electron microscope(TEM),X-ray photoelectron spectroscopy(XPS),N_2adsorption and desorption isotherms,UV-visible diffuse reflectance spectroscopy,fluorescence spectrophotometry and so on.The catalytic activity and stability of the catalysts were evaluated by degradation of rhodamine B under visible light.The effect of molar ratio of sodium sulfide to silver phosphate(n_(Na_2S)/n_(Ag_3PO_4))on the photocatalytic performance of the silver phosphate was studied.In addition,the photocatalytic mechanism was also investigated.The results show that,with the increase of n_(Na_2S)/n_(Ag_3PO_4),the activity of the obtained composite catalytic material increased firstly and then decreased.When n_(Na_2S)/n_(Ag_3PO_4)was 1.5%,the obtained ASC1.5 catalyst could completely degrade rhodamine B within 40 min under visible light irradiation,and also maintained high activity after five-cycle use.Compared with single silver phosphate,the activity and stability of Ag_3PO_4/Ag_2S/g-C_3N_4composite photocatalytic materials were significantly improved,which was mainly attributed to the increase of surface area and the presence of porous structure that enhanced separating efficiency of electron-hole pairs.The study of photocatalytic mechanism over the composite catalyst have shown that h~+,·O~(2-)and·OH were the main active species in the photocatalytic process.The order of the role of the above three species was:h~+>·O~(2-)>·OH.
Ag_3PO_4/Ag_2S/g-C_3N_4composite photocatalysts were successfully prepared by a deposition-ion exchanged combined method.And the obtained samples were characterized by X-ray powder diffractometer(XRD),scanning electron microscope(SEM),transmission electron microscope(TEM),X-ray photoelectron spectroscopy(XPS),N_2adsorption and desorption isotherms,UV-visible diffuse reflectance spectroscopy,fluorescence spectrophotometry and so on.The catalytic activity and stability of the catalysts were evaluated by degradation of rhodamine B under visible light.The effect of molar ratio of sodium sulfide to silver phosphate(n_(Na_2S)/n_(Ag_3PO_4))on the photocatalytic performance of the silver phosphate was studied.In addition,the photocatalytic mechanism was also investigated.The results show that,with the increase of n_(Na_2S)/n_(Ag_3PO_4),the activity of the obtained composite catalytic material increased firstly and then decreased.When n_(Na_2S)/n_(Ag_3PO_4)was 1.5%,the obtained ASC1.5 catalyst could completely degrade rhodamine B within 40 min under visible light irradiation,and also maintained high activity after five-cycle use.Compared with single silver phosphate,the activity and stability of Ag_3PO_4/Ag_2S/g-C_3N_4composite photocatalytic materials were significantly improved,which was mainly attributed to the increase of surface area and the presence of porous structure that enhanced separating efficiency of electron-hole pairs.The study of photocatalytic mechanism over the composite catalyst have shown that h~+,·O~(2-)and·OH were the main active species in the photocatalytic process.The order of the role of the above three species was:h~+>·O~(2-)>·OH.
引文
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[2] Zhu S Y, Liang S J, Wang Y, et al. Appl. Catal. B, 2016,187:11-18
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[4] LI Yao-Wu(李耀武), HUANG Chen-Xi(黄辰曦), TAO Wei(陶伟), et al. Chinese J. Inorg. Chem.(无机化学学报), 2017,33(3):361-376
[5] Wang X B, Liu J, Leong S, et al. ACS Appl. Mater. Interfaces,2016,8:9080-9087
[6] Wang W N, Huang C X, Zhang C Y, et al. Appl. Catal. B,2018,224:854-862
[7] Zhang F, Zhang C L, Peng H Y, et al. Part. Part. Syst. Char,2016,33(5):248-253
[8] Zhang C Y, Liu H H, Wang W N, et al. Appl. Catal. B,2018,239:309-316
[9] Ge M, Li Z L. Chin. J. Catal., 2017,38(11):1794-1803
[10]Yi Z G, Ye J H, Kikugawa N, et al. Nat. Mater., 2010,9(7):559-564
[11]Wan J, Du X, Liu E Z, et al. J. Catal., 2017,345:281-294
[12]XU Meng-Qiu(徐梦秋), CAI Bo(柴波), YAN Jun-Tao(闫俊涛), et al. Journal of the Chinese Ceramic Society(硅酸盐学报), 2018,46(1):93-100
[13]Zhang M Y, Li L, Liu Y, et al. J. Mol. Catal. A:Chem.,2015,400:154-161
[14]Xie M Y, Zhang T L. Appl. Surf. Sci., 2018,436:90-101
[15]Tian L, Xian X Z, Cui X K, et al. Appl. Surf. Sci., 2018,430:301-308
[16]Xiong W W, Dai W L, Hu X, et al. Mater. Lett., 2018,232:36-39
[17]Liu W, Shen J, Yang X F, et al. Appl. Surf. Sci., 2018,456:369-378
[18]Liu Z Y, Feng H G, Xue S L, et al. Appl. Surf. Sci., 2018,458:880-892
[19]Wang W W, Wang L, Li W B, et al. Mater. Lett., 2019,234:183-186
[20]Bagherzadeh M, Kaveh R. Photochem. Photobiol., 2018,94(6):1210-1224
[21]Wang Y F, Wang H L, Xu A L, et al. J. Mater. Sci.-Mater.Electron., 2018,29(19):16691-16701
[22]Dhanabal R, Shafi P M, Arun T, et al. Chemistry Select,2018,3(34):9920-9932
[23]Song L M, Yang J F, Chen Q, et al. Appl. Organomet. Chem.,2018,32(9):e4472
[24]Niu X J, Ma J L. Front. Mater. Sci., 2018,12(3):264-272
[25]Liu Z N, Liu Y C, Xu P P, et al. ACS Appl. Mater. Interfaces,2017,9(24):20620-20629
[26]Wang F R, Wang J D, Sun H P, et al. J. Mater. Sci., 2016,52(5):2495-2510
[27]Qin Y, Li F, Tu P, et al. RSC Adv., 2018,8(10):5382-5387
[28]Deng J T, Liu L, Niu T J, et al. Appl. Surf. Sci., 2017,403:531-539
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[30]Wang F R, Sun H P, Wang Y, et al. Funct. Mater. Lett.,2017,10(3):1750015
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[33]Amornpitoksuk P, Intarasuwan K, Suwanboon S, et al. Ind.Eng. Chem. Res., 2013,52(49):17369-17375
[34]TANG Chun-Ni(汤春妮), FAN Jun(樊君). Contemporary Chemical Industry(当代化工), 2017,46(2):211-214
[35]LI Rong(李容), ZHENG Ming(郑敏), DUAN Wei-Jia(段为甲), et al. Textile Auxiliaries(印染助剂), 2017,34(3):37-40
[36]Hsieh M S, Su H J, Hsieh P L, et al. ACS Appl. Mater.Interfaces, 2017,9(44):39086-39093
[37]XIAO Ming(肖明), HUANG Zai-Yin(黄在银), TANG HuanFeng(汤焕丰), et al. Acta Phys.-Chim. Sin.(物理化学学报),2017,33(2):399-406
[38]WANG Ru-Yi(王如意), XU Hu-Jia(徐会佳), RU Shi-Jie(茹世杰), et al. Journal of Taiyuan University of Science and Technology(太原科技大学学报), 2017,38(3):243-248
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[40]You M Z, Pan J Q, Chi C Y, et al. J. Mater. Sci., 2017,53(3):1978-1986
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[44]Li H P, Liu J Y, Hou W G, et al. Appl. Catal. B, 2014,160-161:89-97
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[53]Cheng X W, Cheng Q F, Deng X Y, et al. Electrochim.Acta, 2015,184:264-275