Position:Home >> Abstract

Preparation of MXene/C electrocatalytic membrane and study on degradation performance of tetracycline hydrochloride in water
Authors: WANG Hong, SHAO Yanan, YU Di, YIN Zhen
Units: State Key Laboratory of Separation Membranes and Membrane Processes, National Center for International Joint Research on Separation Membranes, Tiangong University, Tianjin 300387, China; Tianjin University of Science and Technology, College of Chemical Engineering and Materials Science, Tianjin Key Laboratory of Brine Chemical Engineering and Resource Eco-utilization, Tianjin 300457, China
KeyWords: MXene; Electrophoretic deposition; MXene/C membrane; Tetracycline hydrochloride wastewater; Electrocatalysis
ClassificationCode:TQ460.9
year,volume(issue):pagination: 2022,42(6):151-158

Abstract:
 Two-dimensional MXene nanosheets were loaded on activated carbon-based microporous carbon membrane by electrophoretic deposition method to prepare MXene/C membranes. Surface micromorphology analysis of carbon membrane and MXene/C membrane by field emission scanning electron microscopy (SEM) and transmission electron microscopy (TEM), X-ray diffraction (XRD) was used for chemical crystal analysis, and X-ray diffraction photoelectron spectroscopy (XPS) was used for elemental valence analysis. The hydrophilicity of the membrane surface was analyzed using an automatic contact Angle measuring instrument, and the electrochemical performance was analyzed using an electrochemical workstation. Electrocatalytic membrane reactors (ECMR) were constructed with carbon membrane and MXene/C membrane as anodes for electrocatalytic oxidation degradation of tetracycline hydrochloride wastewater, and their degradation effects were compared. The results showed that the MXene nanosheets were successfully loaded on the surface of the carbon membrane, and the MXene/C membrane was successfully prepared. Compared with the original carbon membrane, the MXene/C membrane had better hydrophilicity, higher electrochemical activity, and higher removal efficiency of tetracycline hydrochloride. When the temperature was 20 ℃, residence time was 8 min, tetracycline hydrochloride wastewater concentration was 50 mg/L, pH was 7.0, current density of 0.6 mA/cm2 and an electrolyte Na2SO4 concentration of 15 g/L, the removal rates of tetracycline hydrochloride by carbon membrane and MXene/C membrane were 86.4% and 97.76%, respectively, and the TOC removal rates were 40.6 % and 88.57%. Meanwhile, after 10 cycles, the MXene/C membrane showed excellent stability.

Funds:
国家重点研发计划(2020YFA0211002)

AuthorIntro:
王虹(1978—),女,辽宁鞍山人,博士,副教授,主要研究方向为电催化在水处理中的应用

Reference:
 [1] Fiaz A, Zhu D C, Sun J Z. Environmental fate of tetracycline antibiotics: degradation pathway mechanisms, challenges, and perspectives[J]. Environ Sci Eur, 2021, 33(1): 64.
[2] Klein E Y, Van Boeckel T P, Martinez E M, et al. Global increase and geographic convergence in antibiotic consumption between 2000 and 2015[J]. P Natl Acad Sci USA, 2018, 115(15): 3463-3470.
[3] Wang H B, Hu C, Liu L Z, et al. Interaction of ciprofloxacin chlorination products with bacteria in drinking water distribution systems[J]. J Hazard Mater, 2017, 339: 174-181.
[4] Li J N, Cheng W X, Xu L K, et al. Occurrence and removal of antibiotics and the corresponding resistance genes in wastewater treatment plants: effluents’ influence to downstream water environment[J]. Environ Sci Pollut R, 2016, 23(7): 6826-6835.
[5] Watkinson A J, Murby E J, Kolpin D W, et al. The occurrence of antibiotics in an urban watershed: From wastewater to drinking water[J]. Sci Total Environ, 2009, 407(8): 2711-2723.
[6] Sarmah A K, Meyer M T, Boxall A B A. A global perspective on the use, sales, exposure pathways, occurrence, fate and effects of veterinary antibiotics in the environment[J]. Chemosphere, 2006, 65(5): 725-759.
[7] Jones O A, Lester J N, Voulvoulis N. Pharmaceuticals: a threat to drinking water?[J]. Trends Biotechnol, 2005, 23 (4): 163-167.
[8] Long L L , Bai C W, Zhang S R, et al. Staged and efficient removal of tetracycline and Cu2+ combined pollution: A designed double-chamber electrochemistry system using 3D rGO[J]. J Clean Prod, 2021, 305: 127101.
[9] Yang S M, Feng Y, Gao D, et al. Electrocatalysis degradation of tetracycline in a three-dimensional aeration electrocatalysis reactor (3D-AER) with a flotation-tailings particle electrode (FPE): Physicochemical properties, influencing factors and the degradation mechanism [J]. J Hazard Mater, 2021, 407: 124361.
[10] Shi Z, Xu P F, Shen X F, et al. TiO2/MoS2 heterojunctions-decorated carbon fibers with broad-spectrum response as weaveable photocatalyst/photoelectrode[J]. Mater Res Bull, 2019, 112: 354-362.
[11] Zhang S W, Gao H H, Xu X T, et al. MOF-derived CoN/N-C@SiO2 yolk-shell nanoreactor with dual active sites for highly efficient catalytic advanced oxidation processes[J]. Chem Eng J, 2020, 381: 122670.
[12] Misal S N, Lin M H, Mehraeen S, et al. Modeling electrochemical oxidation and reduction of sulfamethoxazole using electrocatalytic reactive electrochemical membranes[J]. J Hazard Mater, 2019, 383: 121420-121428.
[13] Yang K, Liu Y Y, Liu J W, et al. Preparation optimization of multilayer-structured SnO2-Sb-Ce/Ti electrode for efficient electrocatalytic oxidation of tetracycline in water[J]. Chinese J Chem Eng, 2018, 26(12): 2622-2627.
[14] Ren C E, Hatzell K B, Alhabeb M, et al. Charge- and size-selective ion sieving Ti3C2Tx MXene membranes[J]. J Phys Chem Lett, 2015, 6(20): 4026-4031.
[15] Iqbal M A, Ali S I, Amin F, et al. La- and Mn-codoped bismuth ferrite/Ti3C2 MXene composites for efficient photocatalytic degradation of congo red dye[J]. ACS Omega, 2019, 4(5): 8661-8668.
[16] Liu T, Liu X Y, Graham N, et al. Two-dimensional MXene incorporated graphene oxide composite membrane with enhanced water purification performance[J]. J Membrane Sci, 2020, 593: 7.
[17] Ying Y L, Liu Y, Wang X Y et al. Two-dimensional titanium carbide for efficiently reductive removal of highly toxic chrornium(VI) from water[J]. ACS Appl Mater Inter, 2015, 7(3): 1795-1803.
[18] Shahzad A, Rasool K, Miran W, et al. Two-dimensional Ti3C2Tx MXene nanosheets for efficient copper removal from water[J]. ACS Sustain Chem Eng, 2017, 5(12): 11481-11488. 
[19] Srimuk P, Kaasik F, Kruner B, et al. MXene as a novel intercalation-type pseudocapacitive cathode and anode for capacitive deionization[J]. J Mater Chem A, 2016, 4(47): 18265-18271.
[20] 熊鸽, 王虹, 惠洪森, 等. 活性炭基微孔炭膜制备及电化学性能[J]. 膜科学与技术, 2019, 39(05): 37-44.
[21] Deng J J, Lu Z, Ding L, et al. Fast electrophoretic preparation of large-area two-dimensional titanium carbide membranes for ion sieving[J]. Chem Eng J, 2021, 408: 127806.
[22] 王虹, 万勇, 惠洪森, 等. TiO2/Ti 电催化膜电极的制备及其对盐酸四环素废水的处理[J]. 天津工业大学学报, 2021, 40(2): 8-13.
[23] Halim J, Cook K M, Naguib M, et al. X-ray photoelectron spectroscopy of select multi-layered transition metal carbides (MXenes)[J]. Appl Surf Sci, 2016, 362: 406-417.
[24] Huang Y, Yan H J, Tong Y J. Electrocatalytic determination of reduced glutathione using rutin as a mediator at acetylene black spiked carbon paste electrode[J]. J Electroanal Chem, 2015, 743: 25-30.
[25] Mai L Q, Tian X C, Xu X, et al. Nanowire electrodes for electrochemical energy storage devices[J]. Chem Rev, 2014, 114(23): 11828-11862.

Service:
Download】【Collect

《膜科学与技术》编辑部 Address: Bluestar building, 19 east beisanhuan road, chaoyang district, Beijing; 100029 Postal code; Telephone:010-80492417/010-80485372; Fax:010-80485372 ; Email:mkxyjs@163.com

京公网安备11011302000819号