A pyrazine based metal-organic framework for selective removal of copper from strongly acidic solutions

doi:10.1007/s11783-023-1633-0

Front. Environ. Sci. Eng.

2023, Vol. 17

Issue (3) : 33 https://doi.org/10.1007/s11783-023-1633-0

RESEARCH ARTICLE

A pyrazine based metal-organic framework for selective removal of copper from strongly acidic solutions

Jiachuang Shao¹, Penghui Shao¹(

), Mingming Peng¹, Min Li², Ziwei Yao¹, Xiuqin Xiong¹, Caiting Qiu¹, Yufan Zheng¹, Liming Yang¹, Xubiao Luo¹(

)

¹. Key Laboratory of Jiangxi Province for Persistent Pollutants Control and Resources Recycle, National-Local Joint Engineering Research Center of Heavy Metals Pollutants Control and Resource utilization, Nanchang Hangkong University, Nanchang 330063, China
². Department of Chemical Engineering, Chongqing University of Science and Technology, Chongqing 401331, China

Download: PDF(20460 KB) HTML
Export: BibTeX | EndNote | Reference Manager | ProCite | RefWorks

Abstract

● pz-UiO-66 was synthesized facilely by a solvothermal method.

● Efficient capture of copper from highly acidic solution was achieved by pz-UiO-66.

● pz-UiO-66 exhibited excellent selectivity and capacity for copper capture.

● Pyrazine-N in pz-UiO-66 was shown to be the dominant adsorption site.

The selective capture of copper from strongly acidic solutions is of vital importance from the perspective of sustainable development and environmental protection. Metal organic frameworks (MOFs) have attracted the interest of many scholars for adsorption due to their fascinating physicochemical characteristics, including adjustable structure, strong stability and porosity. Herein, pz-UiO-66 containing a pyrazine structure is successfully synthesized for the efficient separation of copper from strongly acidic conditions. Selective copper removal at low pH values is accomplished by using this material that is not available in previously reported metal–organic frameworks. Furthermore, the material exhibits excellent adsorption capacity, with a theoretical maximum copper uptake of 247 mg/g. As proven by XPS and FT-IR analysis, the coordination of pyrazine nitrogen atoms with copper ions is the dominant adsorption mechanism of copper by pz-UiO-66. This work provides an opportunity for efficient and selective copper removal under strongly acidic conditions, and promises extensive application prospects for the removal of copper in the treatment for acid metallurgical wastewater.

Keywords Pyrazine Metal-organic frameworks Copper removal Strong acidity High selectivity

Corresponding Author(s): Penghui Shao,Xubiao Luo

About author:

Tongcan Cui and Yizhe Hou contributed equally to this work.

Issue Date: 17 October 2022

Cite this article:

Jiachuang Shao,Penghui Shao,Mingming Peng, et al. A pyrazine based metal-organic framework for selective removal of copper from strongly acidic solutions[J]. Front. Environ. Sci. Eng., 2023, 17(3): 33.

URL:

https://academic.hep.com.cn/fese/EN/10.1007/s11783-023-1633-0
https://academic.hep.com.cn/fese/EN/Y2023/V17/I3/33

Scheme1 Schematic diagram of preparation process of pz-UiO-66.

Fig.1 XRD patterns (a) and FT-IR spectrum (b) of UiO-66 and pz-UiO-66, N₂ sorption isotherms (c) and TGA profiles (d) of pz-UiO-66.

Fig.2 Effect of pH on the adsorption of copper ions.

Fig.3 Transformation of pz-UiO-66 after adsorption: (a) SEM images and optical properties of pz-UiO-66 and pz-UiO-66-Cu, (b) Extended scanning electron microscopy image and energy-dispersive X-ray spectroscopy analysis of pz-UiO-66-Cu, (c) PXRD data for pz-UiO-66 and pz-UiO-66-Cu, (d) N₂ sorption isotherms of pz-UiO-66-Cu.

Fig.4 Adsorption capacity of pz-UiO-66 for Cu²⁺ with coexisting Mn²⁺, Li⁺, Co²⁺, Ni²⁺, Fe³⁺ and Cd²⁺ in binary systems (a) and in a mixed solution composed of seven metal ions (b), distribution coefficients (c) of pz-UiO-66 with respect to Cu²⁺ concentration.

Fig.5 Adsorption isotherms (a) for pz-UiO-66 fitted by Langmuir model and Freundlich model and comparative plot (b) of the effect of pH on copper adsorption for pz-UiO-66 and other copper ion sorbents.

Fig.6 Adsorption kinetics data and fitting curves (a), pseudo-first order (b) and pseudo-second order (c) plots of pz-UiO-66 for the adsorption of Cu²⁺.

Fig.7 Adsorption thermodynamics data (a) and plot of ln K_d vs. 1/T (b) for the adsorption of Cu²⁺ by pz-UiO-66.

Fig.8 FTIR spectrum of pz-UiO-66 before and after Cu²⁺ capture.

Fig.9 XPS characterization of pz-UiO-66 before and after Cu²⁺ adsorption: (a) full spectrum, (b) Cu 2p, (c) Zr 3d, (d) O 1s and (e) N 1s.

1	K Ai, C Ruan, M Shen, L Lu. (2016). MoS2 nanosheets with widened interlayer spacing for high-efficiency removal of mercury in aquatic systems. Advanced Functional Materials, 26(30): 5542–5549 https://doi.org/10.1002/adfm.201601338
2	M R Awual. (2019). Novel ligand functionalized composite material for efficient copper (II) capturing from wastewater sample. Composites Part B: Engineering, 172: 387–396 https://doi.org/10.1016/j.compositesb.2019.05.103
3	D C Brady, M S Crowe, M L Turski, G A Hobbs, X Yao, A Chaikuad, S Knapp, K Xiao, S L Campbell, D J Thiele, C M Counter. (2014). Copper is required for oncogenic BRAF signalling and tumorigenesis. Nature, 509(7501): 492–496 https://doi.org/10.1038/nature13180 pmid: 24717435
4	N T Bui, H Kang, S J Teat, G M Su, C W Pao, Y S Liu, E W Zaia, J Guo, J L Chen, K R Meihaus, C Dun, T M Mattox, J R Long, P Fiske, R Kostecki, J J Urban. (2020). A nature-inspired hydrogen-bonded supramolecular complex for selective copper ion removal from water. Nature Communications, 11(1): 1–12 https://doi.org/10.1038/s41467-020-17757-6 pmid: 32769977
5	Y Cao, W Xiao, G Shen, G Ji, Y Zhang, C Gao, L Han. (2019). Carbonization and ball milling on the enhancement of Pb(II) adsorption by wheat straw: competitive effects of ion exchange and precipitation. Bioresource Technology, 273: 70–76 https://doi.org/10.1016/j.biortech.2018.10.065 pmid: 30415071
6	J H Cavka, S Jakobsen, U Olsbye, N Guillou, C Lamberti, S Bordiga, K P Lillerud. (2008). A new zirconium inorganic building brick forming metal organic frameworks with exceptional stability. Journal of the American Chemical Society, 130(42): 13850–13851 https://doi.org/10.1021/ja8057953 pmid: 18817383
7	T Chen, F Liu, C Ling, J Gao, C Xu, L Li, A Li. (2013a). Insight into highly efficient coremoval of copper and p-nitrophenol by a newly synthesized polyamine chelating resin from aqueous media: competition and enhancement effect upon site recognition. Environmental Science & Technology, 47(23): 13652–13660 https://doi.org/10.1021/es4028875 pmid: 24164273
8	X Chen, A Chen, Z Zhao, X Liu, Y Shi, D Wang. (2013b). Removal of Cu from the nickel electrolysis anolyte using nickel thiocarbonate. Hydrometallurgy, 133: 106–110 https://doi.org/10.1016/j.hydromet.2012.12.007
9	Y Chen, B Pan, H Li, W Zhang, L Lv, J Wu. (2010). Selective removal of Cu(II) ions by using cation-exchange resin-supported polyethyleneimine (PEI) nanoclusters. Environmental Science & Technology, 44(9): 3508–3513 https://doi.org/10.1021/es100341x pmid: 20373792
10	M Choudhary, R Kumar, S Neogi. (2020). Activated biochar derived from Opuntia ficus-indica for the efficient adsorption of malachite green dye, Cu2+ and Ni2+ from water. Journal of Hazardous Materials, 392: 122441 https://doi.org/10.1016/j.jhazmat.2020.122441 pmid: 32193109
11	S Daliran, M Ghazagh-Miri, A R Oveisi, M Khajeh, S Navalón, M Âlvaro, M Ghaffari-Moghaddam, Delarami H Samareh, H García. (2020). A pyridyltriazol functionalized zirconium metal-organic framework for selective and highly efficient adsorption of palladium. ACS Applied Materials & Interfaces, 12(22): 25221–25232 https://doi.org/10.1021/acsami.0c06672 pmid: 32368890
12	H Demiral, C Güngör. (2016). Adsorption of copper(II) from aqueous solutions on activated carbon prepared from grape bagasse. Journal of Cleaner Production, 124: 103–113 https://doi.org/10.1016/j.jclepro.2016.02.084
13	H Feng, Y Li, D Luo, G Tan, J Jiang, H Yuan, S Peng, D Qian. (2016). Novel visible-light-responding InVO4-Cu2O-TiO2 ternary nanoheterostructure: preparation and photocatalytic characteristics. Chinese Journal of Catalysis, 37(6): 855–862 https://doi.org/10.1016/S1872-2067(15)61105-6
14	D J Fitzgerald (1998). Safety guidelines for copper in water. The American journal of clinical nutrition, 67(5 Suppl): 1098S–1102S https://doi.org/10.1093/ajcn/67.5.1098S pmid: 9587159
15	E Hosseinpournajjar, A H Kianfar, M Dinari. (2022). Synthesizing and characterization of Cu(II) polymer complex: application for removing heavy metals from aqueous solutions. Journal of the Iranian Chemical Society, 19(5): 1963–1977 https://doi.org/10.1007/s13738-021-02437-z
16	H Irving, R J P Williams. (1953). The stability of transition-metal complexes. Journal of the Chemical Society (Resumed), 3192–3210
17	C Jiang, X Wang, G Wang, C Hao, X Li, T Li. (2019). Adsorption performance of a polysaccharide composite hydrogel based on crosslinked glucan/chitosan for heavy metal ions. Composites Part B: Engineering, 169: 45–54 https://doi.org/10.1016/j.compositesb.2019.03.082
18	V I Kuz’min, D V Kuz’min. (2014). Sorption of nickel and copper from leach pulps of low-grade sulfide ores using Purolite S930 chelating resin. Hydrometallurgy, 141: 76–81 https://doi.org/10.1016/j.hydromet.2013.10.007
19	S Lee, G Barin, C M Ackerman, A Muchenditsi, J Xu, J A Reimer, S Lutsenko, J R Long, C J Chang. (2016). Copper capture in a thioether-functionalized porous polymer applied to the detection of Wilson’s disease. Journal of the American Chemical Society, 138(24): 7603–7609 https://doi.org/10.1021/jacs.6b02515 pmid: 27285482
20	S Lin, D H Kumar Reddy, J K Bediako, M H Song, W Wei, J A Kim, Y S Yun (2017). Effective adsorption of Pd(Ⅱ), Pt(Ⅳ) and Au(Ⅲ) by Zr(Ⅳ)-based metal-organic frameworks from strongly acidic solutions. Journal of Materials Chemistry. A, Materials for Energy and Sustainability, 5(26): 13557–13564 https://doi.org/10.1039/C7TA02518A
21	Y Ma, W Lu, X Han, Y Chen, Silva I da, D Lee, A M Sheveleva, Z Wang, J Li, W Li, M Fan, S Xu, F Tuna, E J L McInnes, Y Cheng, S Rudić, P Manuel, M D Frogley, A J Ramirez-Cuesta, M Schröder, S Yang. (2022). Direct observation of ammonia storage in UiO-66 incorporating Cu(II) binding sites. Journal of the American Chemical Society, 144(19): 8624–8632 https://doi.org/10.1021/jacs.2c00952 pmid: 35533381
22	Y Marcus. (1988). Ionic radii in aqueous solutions. Chemical Reviews, 88(8): 1475–1498 https://doi.org/10.1021/cr00090a003
23	P B Miniyar, P R Murumkar, P S Patil, M A Barmade, K G Bothara. (2013). Unequivocal role of pyrazine ring in medicinally important compounds: a review. Mini reviews in medicinal chemistry, 13(11): 1607–1625 https://doi.org/10.2174/1389557511313110007 pmid: 23544468
24	I Park, C B Tabelin, S Jeon, X Li, K Seno, M Ito, N Hiroyoshi. (2019). A review of recent strategies for acid mine drainage prevention and mine tailings recycling. Chemosphere, 219: 588–606 https://doi.org/10.1016/j.chemosphere.2018.11.053 pmid: 30554047
25	Y Peng, H Huang, Y Zhang, C Kang, S Chen, L Song, D Liu, C Zhong. (2018). A versatile MOF-based trap for heavy metal ion capture and dispersion. Nature Communications, 9(1): 1–9 https://doi.org/10.1038/s41467-017-02600-2 pmid: 29335517
26	P Shao, D Liang, L Yang, H Shi, Z Xiong, L Ding, X Yin, K Zhang, X Luo. (2020). Evaluating the adsorptivity of organo-functionalized silica nanoparticles towards heavy metals: quantitative comparison and mechanistic insight. Journal of Hazardous Materials, 387: 121676 https://doi.org/10.1016/j.jhazmat.2019.121676 pmid: 31759761
27	D B Wang, B H Chen, B Zhang, Y X Ma. (1997). XPS study of aroylhydrazones containing triazole and their chelates. Polyhedron, 16(15): 2625–2629 https://doi.org/10.1016/S0277-5387(96)00606-7
28	L Wang, Y Shi, D Yao, H Pan, H Hou, J Chen, J C Crittenden. (2019). Cd complexation with mercapto-functionalized attapulgite (MATP): adsorption and DFT study. Chemical Engineering Journal, 366: 569–576 https://doi.org/10.1016/j.cej.2019.02.114
29	N Wang, J Feng, W Yan, L Zhang, Y Liu, R Mu. (2022). Dual-functional sites for synergistic adsorption of Cr(VI) and Sb(V) by polyaniline-TiO2 hydrate: adsorption behaviors, sites and mechanisms. Frontiers of Environmental Science & Engineering, 16(8): 1–14
30	L Xie, Z Yu, S M Islam, K Shi, Y Cheng, M Yuan, J Zhao, G Sun, H Li, S Ma, M G Kanatzidis. (2018). Remarkable acid stability of polypyrrole-MoS4: a highly selective and efficient scavenger of heavy metals over a wide pH range. Advanced Functional Materials, 28(20): 1800502 https://doi.org/10.1002/adfm.201800502
31	M Xu, S S Meng, H Liang, Z Y Gu. (2020). A metal-organic framework with tunable exposed facets as a high-affinity artificial receptor for enzyme inhibition. Inorganic Chemistry Frontiers, 7(19): 3687–3694 https://doi.org/10.1039/D0QI00827C
32	Z Yao, P Shao, D Fang, J Shao, D Li, L Liu, Y Huang, Z Yu, L Yang, K Yu, X Luo. (2022). Thiol-rich, porous carbon for the efficient capture of silver: understanding the relationship between the surface groups and transformation pathways of silver. Chemical Engineering Journal, 427: 131470 https://doi.org/10.1016/j.cej.2021.131470
33	H Yu, P Shao, L Fang, J Pei, L Ding, S G Pavlostathis, X Luo. (2019). Palladium ion-imprinted polymers with PHEMA polymer brushes: role of grafting polymerization degree in anti-interference. Chemical Engineering Journal, 359: 176–185 https://doi.org/10.1016/j.cej.2018.11.149
34	X Zhang, S Tong, D Huang, Z Liu, B Shao, Q Liang, T Wu, Y Pan, J Huang, Y Liu, M Cheng, M Chen. (2021). Recent advances of Zr based metal organic frameworks photocatalysis: energy production and environmental remediation. Coordination Chemistry Reviews, 448: 214177 https://doi.org/10.1016/j.ccr.2021.214177
35	Y Zhang, Z Xie, Z Wang, X Feng, Y Wang, A Wu. (2016). Unveiling the adsorption mechanism of zeolitic imidazolate framework-8 with high efficiency for removal of copper ions from aqueous solutions. Dalton Transactions, 45(32): 12653–12660 https://doi.org/10.1039/C6DT01827K pmid: 27396854

[1]

FSE-22085-OF-SJC_suppl_1

Download

[1]	Yali CHEN,Lu XIONG,Weikang WANG,Xing ZHANG,Hanqing YU. Efficient and selective electro-reduction of nitrobenzene by the nano-structured Cu catalyst prepared by an electrodeposited method via tuning applied voltage[J]. Front. Environ. Sci. Eng., 2015, 9(5): 897-904.

Viewed

Full text

Abstract

Cited

Shared

Discussed