酯化改性甜菜粕铁配合物的制备及其催化性能
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摘要
为使用低成本甜菜粕作高效催化剂降解染料废水,使用柠檬酸对脱果胶甜菜粕(DSBP)进行改性以引入羧酸基,然后将酯化改性甜菜粕(CDSBP)与Fe~(3+)进行配位反应,制备了柠檬酸改性甜菜粕纤维铁配合物(CDSBP-Fe)。通过FTIR、XRD和SEM对配合物表面形貌和化学结构进行了表征。将CDSBP-Fe作为非均相Fenton反应光催化剂,用于活性红195染料的降解反应,考察了其催化性能。结果表明:通过酯化反应羧酸基被成功引入纤维表面结构,并与Fe~(3+)进行配位反应制备了羧酸纤维铁配合物。在光辐射条件下,CDSBP-Fe能够促进偶氮染料的降解反应,反应25 min时,染料脱色率已达到95%;在pH=3～9时CDSBP-Fe均具有较好活性,且CDSBP-Fe循环5次使用活性也未明显降低。
To use sugar beet pulp as high-effective catalyst for the degradation of dye wastewater,depectinizedsugar beet pulp(DSBP) was modified using citric acid to introduce the carboxyl groups.Subsequently, the obtained citric acid-esterification sugar beet pulp fiber(CDSBP) was coordinated with Fe~(3+) ions to produce carboxylic fiber iron complex(CDSBP-Fe). The surface morphology and chemical structure were characterized by FTIR, XRD and SEM. Then, the catalytic performance of CDSBP-Fe was evaluated as heterogeneous light Fenton catalysts for oxidative degradation of reactive red 195. The results showed that the carboxyl groups were introduced into the surface of the fiber by esterification reaction and coordinated with Fe~(3+) ions. Under the condition of light radiation, CDSBP-Fe could promote the degradation of azo dyes. The degradation rate was up to 95% after 25 min of reaction. CDSBP-Fe showed good activity at pH range from 3 to 9. Additionally, the activity of CDSBP-Fe was not decreased after five successive runs.
To use sugar beet pulp as high-effective catalyst for the degradation of dye wastewater,depectinizedsugar beet pulp(DSBP) was modified using citric acid to introduce the carboxyl groups.Subsequently, the obtained citric acid-esterification sugar beet pulp fiber(CDSBP) was coordinated with Fe~(3+) ions to produce carboxylic fiber iron complex(CDSBP-Fe). The surface morphology and chemical structure were characterized by FTIR, XRD and SEM. Then, the catalytic performance of CDSBP-Fe was evaluated as heterogeneous light Fenton catalysts for oxidative degradation of reactive red 195. The results showed that the carboxyl groups were introduced into the surface of the fiber by esterification reaction and coordinated with Fe~(3+) ions. Under the condition of light radiation, CDSBP-Fe could promote the degradation of azo dyes. The degradation rate was up to 95% after 25 min of reaction. CDSBP-Fe showed good activity at pH range from 3 to 9. Additionally, the activity of CDSBP-Fe was not decreased after five successive runs.
引文
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[4]Sharma D K,Saini H S,Singh M,et al.Biodegradation of acid blue-15,a textile dye,by an up-flow immobilized cell bioreactor[J].Journal of Industrial Microbiology&Biotechnology,2004,31(3):109-114.
[5]Gogate P R,Pandit A B.A review of imperative technologies for wastewater treatment I:oxidation technologies at ambient conditions[J].Advances in Environmental Research,2004,8(3/4):501-551.
[6]Chen C,Gunawan P,Rong X.Self-assembled Fe3O4-layered double hydroxide colloidal nanohybrids with excellent performance for treatment of organic dyes in water[J].Journal of Materials Chemistry,2011,21(4):1218-1225.
[7]Bethi B,Sonawane S H,Bhanvase B A,et al.Nanomaterials based advanced oxidation processes for waste water treatment:A review[J].Chemical Engineering&Processing Process Intensification,2016,109:178-189.
[8]Parra S,Guasaquillo I,Enea O,et al.Abatement of an azo dye on structured C-nafion/Fe-ion surfaces by photo-fenton reactions leading to carboxylate intermediates with a remarkable biodegradability increase of the treated solution[J].Journal of Physical Chemistry B,2003,107(29):7026-7035.
[9]Liu X,Tang R,He Q,et al.Fe(Ⅲ)-loaded collagen fiber as a heterogeneous catalyst for the photo-assisted decomposition of Malachite Green[J].Journal of Hazardous Materials,2010,174(1/2/3):687-693.
[10]Ishtchenko V V,Vitkovskaya R F,Huddersman K D.Investigation of the mechanical and physico-chemical properties of a modified PANfibrous catalyst[J].Applied Catalysis A:General,2003,242(2):221-231.
[11]Zhao Yi(赵毅),Yu Shujuan(于淑娟),Zhu Siming(朱思明),et al.Adsorption equilibrium and kinetics of Fe3+by sugar beet pulp[J].Modern Food Science and Technology(现代食品科技),2014,30(1):28-32.
[12]Huang Qin(黄琴),Chen Boru(陈博儒),Gao Ziyuan(高梓原),et al.Preparation of modified sugar beet pulp fiber and application in sugar decolorization[J].Journal of Chinese Institute of Food Science and Technology(中国食品学报),2019,19(2):116-124.
[13]Liu Zhanpeng(刘战朋),Guo Xiaoming(郭晓明),Pi Fang(皮芳),et al.Modification of pectin extraction conditions on physiochemical properties of sugar beet pulp[J].Modern Food Science and Technology(现代食品科技),2018,34(1):68-74.
[14]Haikel G,Nicolas M,Bernard W,et al.New method for a two-step hydrolysis and chromatographic analysis of pectin neutral sugar chains[J].Journal of Agricultural&Food Chemistry,2004,52(15):4652-4659.
[15]Parikh D V,Thibodeaux D P,Condon B.X-ray crystallinity of bleached and crosslinked cottons[J].Textile Research Journal,2007,77(8):612-616.
[16]Wu X,Gu X,Lu S,et al.Degradation of trichloroethylene in aqueous solution by persulfate activated with citric acid chelated ferrous ion[J].Chemical Engineering Journal,2014,255(255):585-592.
[17]Cheng M,Song W,Ma W,et al.Catalytic activity of iron species in layered clays for photodegradation of organic dyes under visible irradiation[J].Applied Catalysis B:Environmental,2008,77(3):355-363.
[18]Lin S S,Gurol M D.Catalytic decomposition of hydrogen peroxide on iron oxide:Kinetics,mechanism,and implications[J].Environmental Science&Technology,1998,32(10):1417-1423.
[19]Hu X J,Zhu H Y,Feng J Y,et al.Degradation of azo-dye OrangeⅡby a photoassisted Fenton reaction using a novel composite of iron oxide and silicate nanoparticles as a catalyst[J].Industrial&Engineering Chemistry Research,2003,42(10):2058-2066.