CuO@C催化过二硫酸盐降解盐酸四环素研究
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摘要
采用溶剂热法制备了含铜金属有机骨架材料(Cu-MOFs),并进一步碳化得到了CuO@C催化剂。研究了CuO@C催化过二硫酸盐(PS)降解盐酸四环素的效能,考察了CuO@C投加量、PS投加量、盐酸四环素初始浓度及反应溶液初始pH对PS/CuO@C体系降解盐酸四环素效果的影响。结果表明,当CuO@C投加量、PS投加量、盐酸四环素浓度分别为0.150 g/L、1.00 mmol/L、20μmol/L时,盐酸四环素的去除率可以达到90%。在一定范围内,催化剂和PS投加量增加、盐酸四环素含量降低以及碱性环境更有利于PS-CuO@C体系中盐酸四环素的降解。通过投加叔丁醇和乙醇2种猝灭剂,证实了盐酸四环素的降解主要由SO_4~(·-)及其转化的HO·共同作用的结果。
Cu-metal organic frameworks(Cu-MOFs) was prepared via hydrothermal method, and CuO@C catalyst was obtained by further carbonization. The tetracycline hydrochloride degradation efficiency by CuO@C catalyzed persulfate(PS) was studied, the effect of CuO@C dosage, PS dosage, tetracycline hydrochloride initial concentration, and initial pH on removal efficiency of tetracycline hydrochloride by PS/CuO@C system was investigated. The results indicated that the tetracycline hydrochloride degradation reached 90% when CuO@C dosage, PS dosage and tetracycline hydrochloride initial concentration was 0.150 g/L, 1.00 mmol/L and 20 μmol/L respectively. Increased CuO@C and PS dosage and decreased tetracycline hydrochloride content within limits, and alkaline condition was favored for tetracycline hydrochloride by PS/CuO@C system. By adding different radical scavengers of ethanol(Et OH) and Tert-butyl alcohol identified that sulfate radical(SO_4~(·-)) and its transformed hydroxyl radical(HO·) led to the degradation of tetracycline hydrochloride.
Cu-metal organic frameworks(Cu-MOFs) was prepared via hydrothermal method, and CuO@C catalyst was obtained by further carbonization. The tetracycline hydrochloride degradation efficiency by CuO@C catalyzed persulfate(PS) was studied, the effect of CuO@C dosage, PS dosage, tetracycline hydrochloride initial concentration, and initial pH on removal efficiency of tetracycline hydrochloride by PS/CuO@C system was investigated. The results indicated that the tetracycline hydrochloride degradation reached 90% when CuO@C dosage, PS dosage and tetracycline hydrochloride initial concentration was 0.150 g/L, 1.00 mmol/L and 20 μmol/L respectively. Increased CuO@C and PS dosage and decreased tetracycline hydrochloride content within limits, and alkaline condition was favored for tetracycline hydrochloride by PS/CuO@C system. By adding different radical scavengers of ethanol(Et OH) and Tert-butyl alcohol identified that sulfate radical(SO_4~(·-)) and its transformed hydroxyl radical(HO·) led to the degradation of tetracycline hydrochloride.
引文
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[4]NORZAEE S,TAGHAVI M,DJAHED B,et al.Degradation of penicillin g by heat activated persulfate in aqueous solution[J].Journal of Environmental Management,2018,215:316-323.
[5]KERMANI M,MOHAMMADI F,KAKAVANDI B,et al.Simultaneous catalytic degradation of 2,4-D and MCPA herbicides using sulfate radical-based heterogeneous oxidation over persulfate activated by natural hematite(α-Fe2O3/PS)[J].Journal of Physics and Chemistry of Solids,2018,117:49-59.
[6]LIN S,BEDIAKO J K,CHO C,et al.Selective adsorption of Pd(II)over interfering metal ions(Co(II),Ni(II),Pt(IV))from acidic aqueous phase by metal-organic frameworks[J].Chemical Engineering Journal,2018,345:337-344.
[7]CHOWDHURI A R,LAHA D,CHANDRA S,et al.Synthesis of multifunctional upconversion nmofs for targeted antitumor drug delivery and imaging in triple negative breast cancer cells[J].Chemical Engineering Journal,2017,319:200-211.
[8]XU G,XU G,BAN J,et al.Cobalt and cobalt oxides N-codoped porous carbon derived from metal-organic framework as bifunctional catalyst for oxygen reduction and oxygen evolution reactions[J].Journal of Colloid and Interface Science,2018,521:141-149.
[9]FENG D,WU Y,TAN X,et al.Sensitive detection of melamine by an electrochemiluminescence sensor based on tris(bipyridine)ruthenium(II)-functionalized metal-organic frameworks[J].Sensors and Actuators B:Chemical,2018,265:378-386.
[10]SARKER M,AHMED I,JHUNG S H.Adsorptive removal of herbicides from water over nitrogen-doped carbon obtained from ionic liquid@zif-8[J].Chemical Engineering Journal,2017,323:203-211.
[11]LIN K A,HSU F,LEE W.Magnetic cobalt-graphene nanocomposite derived from self-assembly of mofs with graphene oxide as an activator for peroxymonosulfate[J].Journal of Materials Chemistry A,2015,3(18):9480-9490.
[12]HU L,DENG G,LU W,et al.Peroxymonosulfate activation by Mn3O4/metal-organic framework for degradation of refractory aqueous organic pollutant rhodamine B[J].Chinese Journal of Catalysis,2017,38(8):1360-1372.
[13]RAOOF J,HOSSEINI S R,OJANI R,et al.Mo F-derived Cu/nanoporous carbon composite and its application for electro-catalysis of hydrogen evolution reaction[J].Energy,2015,90:1075-1081.
[14]ZHANG T,CHEN Y,WANG Y,et al.Efficient peroxydisulfate activation process not relying on sulfate radical generation for water pollutant degradation[J].Environmental Science&Technology,2014,48(10):5868-5875.
[15]LIU F,YI P,WANG X,et al.Degradation of acid orange 7 by an ultrasound/Zn O-GAC/persulfate process[J].Separation and Purification Technology,2018,194:181-187.
[16]ZHOU P,ZHANG J,ZHANG Y,et al.Degradation of 2,4-dichlorophenol by activating persulfate and peroxomonosulfate using micron or nanoscale zero-valent copper[J].Journal of Hazardous Materials,2018,344:1209-1219.
[17]WALDEMER R H,TRATNYEK P G,JOHNSON R L,et al.Oxidation of chlorinated ethenes by heat-activated persulfate:kinetics and products[J].Environmental Science&Technology,2007,41(3):1010-1015.
[18]CHANG P,LI Z,JEAN J,et al.Adsorption of tetracycline on 2:1layered non-swelling clay mineral illite[J].Applied Clay Science,2012,67/68:158-163.