碳化改性ZIF(Co/Zn)@PPy复合流动电极高效分离有机物/无机阴离子Carbonization-modified ZIF(Co/Zn)@PPy for efficient separation of organic compounds and inorganic anions
潘华淳,骆一周,贾颖娜,孙晨,雷乐成,杨彬
摘要(Abstract):
针对流动电极材料在分离有机物/无机阴离子时选择性低、吸附容量有限及循环稳定性差的问题,通过原位生长双金属ZIF(Co/Zn)于聚吡咯(PPy)导电网络上并高温碳化(900℃)的策略,制备了碳化改性ZIF(Co/Zn)@PPy复合材料,并将其作为流动电极用于电容去离子(FCDI)系统,处理含头孢类抗生素的高盐废水。结果表明:碳化后材料相对于碳化前具有更丰富的介孔结构与更优异的电化学性能,电荷传输性能明显改善,电荷效率由74.06%提高至95.50%;对NaCl的吸附容量提升77%,有机/无机阴离子分离因子达13 635,且20次循环后性能保持率超97%。该碳化改性策略显著提升了ZIF@PPy流动电极材料的性能,为开发高效、高选择性分离回收高盐有机废水中有机物的FCDI技术提供了新材料基础和理论支撑。
关键词(KeyWords): 流动电极材料;ZIF(Co/Zn)@PPy;碳化;电化学性能;吸附
基金项目(Foundation): 浙江省领雁研发计划项目(2023C03140)
作者(Author): 潘华淳,骆一周,贾颖娜,孙晨,雷乐成,杨彬
参考文献(References):
- [1]TANG K,ZHENG H,DU P,et al. Simultaneous fractionation,desalination,and dye removal of dye/salt mixtures by carbon clothmodified flow-electrode capacitive deionization[J]. Environmental Science&Technology,2022,56(12):8885-8896.
- [2]WU H, XU L, ZHANG Y, et al. Selective chromium and copper recovery from wastewater using flow-electrode capacitance deionization:In-situ reduction mechanism regulating metal charging characteristics[J]. Separation and Purification Technology,2024,328:124970.
- [3]XU Y,DUAN F,CAO R,et al. Enhanced salt removal performance using nickel hexacyanoferrate/carbon nanotubes as flow cathode in asymmetric flow electrode capacitive deionization[J]. Desalination,2023,566:116929.
- [4]WAN K, YUAN S, ZHANG J, et al. Enhanced seawater uranium extraction via flow capacitive deionization by amidoximefunctionalized MXene/CoZn-MOF heterostructure electrodes[J]. Water Research,2025,285:124149.
- [5]MANSOOR N E,DIAZ L A,SHUCK C E,et al. Removal and recovery of ammonia from simulated wastewater using Ti3C2Tx MXene in flow electrode capacitive deionization[J]. npj Clean Water,2022,5(1):26.
- [6]YAN L, ISSAKA ALHASSAN S, GANG H, et al. Enhancing charge transfer utilizing ternary composite slurry for high-efficient flow-electrode capacitive deionization[J]. Chemical Engineering Journal,2023,468:143413.
- [7]ZHENG F, YANG Y, CHEN Q. High lithium anodic performance of highly nitrogen-doped porous carbon prepared from a metalorganic framework[J]. Nature Communications,2014,5(1):5261.
- [8]WANG K, CHEN J, HOU F, et al. In situ growth-optimized synthesize of Al-MOF@RGO anode materials with long-life capacityenhanced lithium-ion storage[J]. Chemical Engineering Journal,2023,455:140561.
- [9]ILIC I K,OSCHATZ M. The functional chameleon of materials chemistry—Combining carbon structures into all-carbon hybrid nanomaterials with intrinsic porosity to overcome the“Functionality-Conductivity-Dilemma” in electrochemical energy storage and electrocatalysis[J]. Small,2021,17(19):2007508.
- [10]ZHANG C, MA J, WU L, et al. Flow electrode capacitive deionization(FCDI):Recent developments, environmental applications,and future perspectives[J]. Environmental Science&Technology,2021,55(8):4243-4267.
- [11]KUMAR S, ALDAQQA N M, ALHSEINAT E, et al. Electrode materials for desalination of water via capacitive deionization[J].Angewandte Chemie International Edition,2023,62(35):e202302180.
- [12]SUN K, TEBYETEKERWA M, WANG C, et al. Electrocapacitive deionization:mechanisms, electrodes, and cell designs[J].Advanced Functional Materials,2023,33(18):2213578.
- [13]TAN Z,SONG W,MAO X,et al. Efficient capacitive deionization with hierarchical porous carbon flow electrodes[J]. Desalination,2024,591:118051.
- [14]ZHAO Y, LUO G, ZHANG L, et al. Nitrogen-doped porous carbon tubes composites derived from metal-organic framework for highly efficient capacitive deionization[J]. Electrochimica Acta,2020,331:135420.
- [15]ZONG M,HUO S,LIU Y,et al. Hydrangea-like nitrogen-doped porous carbons derived from NH2-MIL-53(Al)for high-performance capacitive deionization[J]. Separation and Purification Technology,2021,256:117818.
- [16]PAN, H, DING, J, CHEN, S, et al. Spider web-inspired ZIF@PPy conductive networks for efficient flow-electrode capacitive desalination of high-salinity antibiotic wastewater[J]. Chemical Engineering Journal,2025:169484.
- [17]PAN H,YAN M,WU B,et al. Revealing critical factors in the separation of organic and inorganic anions through electrodialysis using back propagation neural networks[J]. Desalination,2024,592:118145.
- [18]HWANG I, LEE D, JUNG Y, et al. High-performance asymmetric flow-electrode capacitive mixing with MnO2-coated activated carbon flow-electrode for energy harvesting from salinity gradient power[J]. ACS Materials Letters,2022,4(4):618-625.
- [19]TRAN N A T,KHOI T M,PHUOC N M,et al. A review of recent advances in electrode materials and applications for flow-electrode desalination systems[J]. Desalination,2022,541:116037.
- [20]MINH PHUOC N, ANH THU TRAN N, MINH KHOI T, et al. ZIF-67 metal-organic frameworks and CNTs-derived nanoporous carbon structures as novel electrodes for flow-electrode capacitive deionization[J]. Separation and Purification Technology, 2021,277:119466.
- [21]NAZIR M A, ULLAH S, SHAHID M U, et al. Zeolitic imidazolate frameworks(ZIF-8&ZIF-67):Synthesis and application for wastewater treatment[J]. Separation and Purification Technology,2025,356:129828.
- [22]SI Z,CAI D,LI S,et al. Carbonized ZIF-8 incorporated mixed matrix membrane for stable ABE recovery from fermentation broth[J].Journal of Membrane Science,2019,579:309-317.
- [23]GADIPELLI S, GUO Z X. Tuning of ZIF-Derived Carbon with High Activity, Nitrogen Functionality, and Yield–A Case for Superior CO2 Capture[J]. ChemSusChem,2015,8(12):2123-2132.
- [24]FERRARI A C,ROBERTSON J. Interpretation of Raman spectra of disordered and amorphous carbon[J]. Physical Review B,2000,61(20):14095-14107.
- [25]XU X,WANG M,LIU Y,et al. Metal–organic framework-engaged formation of a hierarchical hybrid with carbon nanotube inserted porous carbon polyhedra for highly efficient capacitive deionization[J]. Journal of Materials Chemistry A,2016,4(15):5467-5473.
- [26]ABBASI Z, SHAMSAEI E, LEONG S K, et al. Effect of carbonization temperature on adsorption property of ZIF-8 derived nanoporous carbon for water treatment[J]. Microporous and Mesoporous Materials,2016,236:28-37.
- [27]GUO X, ZHANG J, YUAN L, et al. Biologically assisted construction of advanced electrode materials for electrochemical energy storage and conversion[J]. Advanced Energy Materials,2023,13(24):2204376.
- [28]XIA C, JOO S W, HOJJATI-NAJAFABADI A, et al. Latest advances in layered covalent organic frameworks for water and wastewater treatment[J]. Chemosphere,2023,329:138580.