具有染料选择吸附性的衍生于沸石咪唑酯骨架-67的NiCo-层状双氢氧化物设计与合成

doi:10.11944/j.issn.1000-0518.2020.06.190330

摘要/Abstract

摘要：

以沸石咪唑类金属有机骨架(ZIF-67)为模板合成了一种新型的中空吸附剂NiCo-LDH@ZIF-67,该吸附剂对甲基橙具有良好的选择吸附性以及可循环性。通过扫描电子显微镜(SEM)、透射电子显微镜(TEM)、X射线粉末衍射仪(XRD)、红外光谱、电子能谱和氮气吸附-脱附等手段对样品进行了表征。研究了溶液的pH值、甲基橙的初始浓度以及染料与吸附剂作用时间对NiCo-LDH@ZIF-67吸附性能的影响。结果表明,该吸附剂对甲基橙的吸附动力学符合准二级动力学模型,且吸附等温线符合朗缪尔方程。当pH值等于4, 吸附时间15 min,吸附剂用量为2400 mg/L时,该吸附剂对甲基橙的最大吸附量可达1766 mg/g,高于之前文献报道的类似吸附剂。此外,NiCo-LDH@ZIF-67能从甲基橙和亚甲基蓝的混合溶液中选择性吸附甲基橙。

关键词: 层状双氢氧化物, 吸附, 染料, 金属有机骨架, 沸石咪唑酯骨架-67

Abstract:

A novel hollow composite of NiCo-layered double hydroxide and zeolitic imidazolate framework-67 (NiCo-LDH@ZIF-67) adsorbent with high adsorption capacity for pollutants, high adsorption selectivity of methyl orange (MO) and great regenerability was synthesized using ZIF-67 as a template. The sample was characterized by using scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray diffraction (XRD), Fourier transform infrared spectrometer (FT-IR), N₂ adsorption desorption and X-ray photoelectron spectroscopy (XPS). The effect of solution pH, the initial MO concentration and the contact time with the mixture solution on the adsorption property of NiCo-LDH@ZIF-67 was studied. The results indicate that its adsorption kinetics for MO can be well simulated by a pseudo-second-order model and its adsorption isotherm for MO follows the Langmuir equation. The optimized adsorption condition is pH=4, contact time of 15 minutes, and adsorbent dosage of 2400 mg/L. Its maximum adsorption capacity for MO can reach as high as 1766 mg/g and is higher than those reported for all similar adsorbents in the literature. In addition, NiCo-LDH@ZIF-67 can selectively adsorb MO from a mixed solution of MO and methylene blue (MB).

Key words: layered double hydroxide, adsorption, dye, metal organic frameworks, zeolitic imidazolate framework-67

林泳岑, 董雪, 马玉芹, 赵朗. 具有染料选择吸附性的衍生于沸石咪唑酯骨架-67的NiCo-层状双氢氧化物设计与合成[J]. 应用化学, 2020, 37(6): 683-694.

LIN Yongcen, DONG Xue, MA Yuqin, ZHAO Lang. Designed Formation of NiCo-Layered Double Hydroxide Derived from Zeolitic Imidazolate Framework-67 with Selective Dye Adsorption Property[J]. Chinese Journal of Applied Chemistry, 2020, 37(6): 683-694.

参考文献

[1]	Akbarnejad S,Amooey A A,Ghasemi S.High Effective Adsorption of Acid Fuchsin Dye Using Magnetic Biodegradable Polymer-Based Nanocomposite from Aqueous Solutions[J]. Microchem J,2019,149:103966.
[2]	Sabarinathan C,Karuppasamy P,Vijayakumar C T,et al. Development of Methylene Blue Removal Methodology by Adsorption Using Molecular Polyoxometalate:Kinetics, Thermodynamics and Mechanistic Study[J]. Microchem J,2019,146:315-326.
[3]	Miandad R,Kumar R,Barakat M A,et al. Untapped Conversion of Plastic Waste Char into Carbon-Metal LDOs for the Adsorption of Congo Red[J]. J Colloid Interface Sci,2018,511:402-410.
[4]	Wang L,Wang A.Adsorption Properties of Congo Red from Aqueous Solution onto Surfactant-Modified Montmorillonite[J]. J Hazard Mater,2008,160(1):173-180.
[5]	Lin H Y,Zhao J,Song G,et al. High Quality and High Performance Adsorption of Congo Red Using As-Grown MWCNTs Synthesized over a Co-MOF as a Catalyst Precursor via the CVD Method[J]. Dalton Trans,2017,46(48):17067-17073.
[6]	Wang J H,Zhang Y,An L C,et al. Sulfonated Hollow Covalent Organic Polymer: Highly-Selective Adsorption Toward Cationic Organic Dyes over Anionic Ones in Aqueous Solution[J]. Chinese J Chem,2018,36(9):826-830.
[7]	Zhao S,Chen D,Wei F,et al. Removal of Congo Red Dye from Aqueous Solution with Nickel-Based Metal-Organic Framework/Graphene Oxide Composites Prepared by Ultrasonic Wave-Assisted Ball Milling[J]. Ultrason Sonochem,2017,39:845-852.
[8]	Yang Q,Wang Y,Wang J,et al. High Effective Adsorption/Removal of Illegal Food Dyes from Contaminated Aqueous Solution by Zr-MOFs(UiO-67)[J]. Food Chem,2018,254:241-248.
[9]	Guan T,Fang L,Lu Y,et al. A Facile Approach to Synthesize 3D Flower-Like Hierarchical NiCo Layered Double Hydroxide Microspheres and Their Enhanced Adsorption Capability[J]. Colloids Surf A,2017,529:907-915.
[10]	Chakraborty A,Acharya H.Facile Synthesis of MgAl-Layered Double Hydroxide Supported Metal Organic Framework Nanocomposite for Adsorptive Removal of Methyl Orange Dye[J]. J Colloid Interface Sci,2018,24:35-39.
[11]	Hu H,Guan B,Xia B,et al. Designed Formation of Co3O4/NiCo2O4 Double-Shelled Nanocages with Enhanced Pseudocapacitive and Electrocatalytic Properties[J]. J Am Chem Soc,2015,137(16):5590-5595.
[12]	Wang H,Fan G L,Zheng C,et al. Facile Sodium Alginate Assisted Assembly of Ni-Al Layered Double Hydroxide Nanostructures[J]. Ind Eng Chem Res,2010,49(6):2759-2767.
[13]	Li C,Wei M,Evans D G,et al. Layered Double Hydroxide-Based Nanomaterials as Highly Efficient Catalysts and Adsorbents[J]. Small,2014,10(22):4469-4486.
[14]	Yang Y,Yan X,Hu X,et al. In-situ Growth of ZIF-8 on Layered Double Hydroxide: Effect of Zn/Al Molar Ratios on Their Structural, Morphological and Adsorption Properties[J]. J Colloid Interface Sci,2017,505:206-212.
[15]	Yao W,Yu S J,Wang J,et al. Enhanced Removal of Methyl Orange on Calcined Glycerol-Modified Nanocrystallined Mg/Al Layered Double Hydroxides[J]. Chem Eng J,2017,307:476-486.
[16]	Tao X, Liu D, Cong W,et al. Controllable Synthesis of Starch-Modified ZnMgAl-LDHs for Adsorption Property Improvement[J]. Appl Surf Sci,2018,457:572-579.
[17]	Robati D,Mirza B,Rajabi M,et al. Removal of Hazardous Dyes-BR 12 and Methyl Orange Using Graphene Oxide as an Adsorbent from Aqueous Phase[J]. Chem Eng J,2016,284:687-697.
[18]	Habiba U,Siddique T A,Joo T C,et al. Synthesis of Chitosan/Polyvinyl Alcohol/Zeolite Composite for Removal of Methyl Orange, Congo Red and Chromium(VI) by Flocculation/Adsorption[J]. Carbohydr Polym,2017,157:1568-1576.
[19]	Huang R H,Liu Q,Huo J,et al. Adsorption of Methyl Orange onto Protonated Cross-Linked Chitosan[J]. Arab J Chem,2017,10(1):24-32.
[20]	Ni Z M,Xia S J,Wang L G,et al. Treatment of Methyl Orange by Calcined Layered Double Hydroxides in Aqueous Solution:Adsorption Property and Kinetic Studies[J]. J Colloid Interface Sci,2007,316(2):284-291.
[21]	Ling F L,Fang L,Lu Y,et al. A novel CoFe Layered Double Hydroxides Adsorbent: High Adsorption Amount for Methyl Orange Dye and Fast Removal of Cr(VI)[J]. Micropor Mesopor Mater,2016,234:230-238.
[22]	Haque E, Lee J E, Jang I T,et al. Adsorptive Removal of Methyl Orange from Aqueous Solution with Metal-Organic Frameworks, Porous Chromium-Benzenedicarboxylates[J]. J Hazard Mater,2010,181:535-542.
[23]	Liu P F,Tao K,Li G C,et al. In situ Growth of ZIF-8 Nanocrystals on Layered Double Hydroxide Nanosheets for Enhanced CO2 Capture[J]. Dalton Trans,2016,45(32):12632-12635.
[24]	Hao L,Qiu Q,Li H.Directional Functionalization of MOF-74 Analogs via Ligand Pre-installation[J]. Chinese J Chem,2016,34(2):220-224.
[25]	Thanh N T,Thien T V,Du P D,et al. Adsorptive Removal of Congo Red from Aqueous Solution Using Zeolitic Imidazolate Framework-67[J]. J Environ Eng,2018,6(2):2269-2280.
[26]	Tian T,Wharmby M T,Parra J B,et al. Role of Crystal Size on Swing-Effect and Adsorption Induced Structure Transition of ZIF-8[J]. Dalton Trans,2016,45(16):6893-6900.
[27]	Gao B,Zhou J,Wang H,et al. Zeolitic Imidazolate Framework 8-Derived Au@ZnO for Efficient and Robust Photocatalytic Degradation of Tetracycline[J]. Chinese J Chem,2019,37(2):148-154.
[28]	Zhang J J,Yan X L,Hu X Y,et al. Direct Carbonization of Zn/Co Zeolitic Imidazolate Frameworks for Efficient Adsorption of Rhodamine B[J]. Chem Eng J,2018,347:640-647.
[29]	Yang Q X,Ren S S,Zhao Q Q,et al. Selective Separation of Methyl Orange from Water Using Magnetic ZIF-67 Composites[J]. Chem Eng J,2018,333:49-57.
[30]	Yu D,Wu B,Ge L,et al. Decorating Nanoporous ZIF-67-derived NiCo2O4 Shells on a Co3O4 Nanowire Array Core for Battery-Type Electrodes with Enhanced Energy Storage Performance[J]. J Mater Chem,2016,4(28):10878-10884.
[31]	Wang Q,Wang X F,Shi C L.LDH Nanoflower Lantern Derived from ZIF-67 and Its Application for Adsorptive Removal of Organics from Water[J]. Ind Eng Chem Res,2018,57(37):12478-12484.
[32]	Chen N N,Chen D,Wei F H,et al. Effect of Structures on the Adsorption Performance of Cobalt Metal Organic Framework Obtained by Microwave-Assisted Ball Milling[J]. Chem Phys Lett,2018,705:23-30.
[33]	Wang L,Wang A.Adsorption Characteristics of Congo Red onto the Chitosan/Montmorillonite Nanocomposite[J]. J Hazard Mater,2007,147(3):979-985.
[34]	He P,Yu X Y,Lou X W.Carbon-Incorporated Nickel-Cobalt Mixed Metal Phosphide Nanoboxes with Enhanced Electrocatalytic Activity for Oxygen Evolution[J]. Angew Chem Int Ed Engl,2017,56(14):3897-3900.
[35]	Zhang J,Hu H,Li Z,et al. Double-Shelled Nanocages with Cobalt Hydroxide Inner Shell and Layered Double Hydroxides Outer Shell as High-Efficiency Polysulfide Mediator for Lithium-Sulfur Batteries[J]. Angew Chem Int Ed Engl,2016,55(12):3982-3986.
[36]	Gao J,Lu Y,Fang L,et al. Efficient Removal of Methyl Orange and Heavy Metal Ion from Aqueous Solution by NiFe-Cl-Layered Double Hydroxide[J]. Environ Eng Sci,2018,35(4):373-381.
[37]	Li Z,Shao M,Zhou L,et al. Directed Growth of Metal-Organic Frameworks and Their Derived Carbon-Based Network for Efficient Electrocatalytic Oxygen Reduction[J]. Adv Mater,2016,28(12):2337-2344.
[38]	Yang Y,Yan X,Hu X,et al. Development of Zeolitic Imidazolate Framework-67 Functionalized Co-Al LDH for CO2 Adsorption[J]. Colloids Surf A,2018,552:16-23.
[39]	Li J,Lu S,Huang H,et al. ZIF-67 as Continuous Self-Sacrifice Template Derived NiCo2O4/Co,N-CNTs Nanocages as Efficient Bifunctional Electrocatalysts for Rechargeable Zn-Air Batteries[J]. ACS Sustain Chem Eng,2018,6(8):10021-10029.
[40]	Chen Y,Jing C,Zhang X,et al. Acid-Aalt Treated CoAl Layered Double Hydroxide Nanosheets with Enhanced Adsorption Capacity of Methyl Orange Dye[J]. J Colloid Interface Sci,2019,548:100-109.
[41]	Du X D,Wang C C,Liu J G,et al. Extensive and Selective Adsorption of ZIF-67 Towards Organic Dyes:Performance and Mechanism[J]. J Colloid Interface Sci,2017,506:437-441.
[42]	Jiang D B,Yuan S,Cai X,et al. Magnetic Nickel Chrysotile Nanotubes Tethered with pH-Sensitive Poly(Methacrylic Acid) Brushes for Cu(II) Adsorption[J]. J Mol Liq,2019,276:611-623.
[43]	Zhang Z,Zhang J,Liu J,et al. Selective and Competitive Adsorption of Azo Dyes on the Metal-Organic Framework ZIF-67[J]. Water Air Soil Pollut,2016,227(12):471.