Facile synthesis of flake-like dihydrate zinc oxalate particles

Abstract

Monodispersed dihydrated zinc oxalate (ZnC₂O₄·2H₂O) particles with characteristic morphology were synthesized by aging a mixed solution of zinc nitrate (Zn(NO₃)₂) and sodium oxalate (Na₂C₂O₄) in the presence of a citrate ligand, with an average flat size of approximately 10–15 μm. The important parameters, including the solution pH values and the concentration of the zinc ions and citrate ligand, were investigated using a series of experiments. It is verified that the citrate ligand significantly affects the morphology of zinc oxalate particles, probably via its multiple roles of chelating, dispersing, and selective absorption. Thermodynamic equilibrium of the distribution of zinc species in an aqueous solution of Zn(II)-citrate-oxalate-H₂O was estimated to explain the experimental results and to clarify the size and morphological evolution mechanism of the precipitated particles.

Keywords

facile synthesis / zinc oxalate / flaky morphology / citrate ligand / one-pot synthesis

References

[1] Kumar R., Umar A., Kumar G., Nalwa H.S. Antimicrobial properties of ZnO nanomaterials: A review. Ceram. Int., 2017, 43(5): 3940.

[2] Nie Q., Yang L., Cao C., Zeng Y.M., Wang G.Z., Wang C.Z., Lin S.W. Interface optimization of ZnO nanorod/CdS quantum dots heterostructure by a facile two-step low-temperature thermal treatment for improved photoelectrochemical water splitting. Chem. Eng. J., 2017, 325, 151.

[3] Wang L.P., Zhang F., Chen S., Bai Z.H. One-pot synthesis and optical properties of In- and Sn-doped ZnO nanoparticles. Int. J. Miner. Metall. Mater., 2017, 24(4): 455.

[4] Zhou J.H., Pu C.D., Jiao T.Y., Hou X.Q., Peng X.G. A two-step synthetic strategy toward monodisperse colloidal CdSe and CdSe/CdS core/shell nanocrystals. J. Am. Chem. Soc., 2016, 138(20): 6475.

[5] Umar A., Lee J., Dey J., Choi S.M. Seedless synthesis of monodisperse cuboctahedral gold nanoparticles with tunable sizes. Chem. Mater., 2016, 28, 4962.

[6] Hu X.L., Gong J.M., Zhang L.Z., Yu J.C. Continuous size tuning of monodisperse ZnO colloidal nanocrystal clusters by a microwave-polyol process and their application for humidity sensing. Adv. Mater., 2008, 20(24): 4845.

[7] Kanie K., Seino Y., Matsubara M., Muramatsu A. Size-controlled hydrothermal synthesis of monodispersed BaZrO3 sphere particles by seeding. Adv. Powder Technol., 2017, 28, 55.

[8] Wang D.S., Ma X.L., Wang Y.G., Wang L., Wang Z.Y., Zheng W., He X.M., Li J., Peng Q., Li Y.D. Shape control of CoO and LiCoO₂ nanocrystals. Nano Res., 2010, 3(1): 1.

[9] Trandafilović L.V., Whiffen R.K., Dimitrijević-Branković S., Stoiljković M., Luyt A.S., Djoković V. ZnO/Ag hybrid nanocubes in alginate biopolymer: Synthesis and properties. Chem. Eng. J., 2014, 253, 341.

[10] Watanabe S., Ohsaki S., Hanafusa T., Takada K., Tanaka H., Mae K., Miyahara M.T. Synthesis of zeolitic imidazolate framework-8 particles of controlled sizes, shapes, and gate adsorption characteristics using a central collision-type microreactor. Chem. Eng. J., 2017, 313, 724.

[11] LaMer V.K., Dinegar R.H. Theory, production and mechanism of formation of monodispersed hydrosols. J. Am. Chem. Soc., 1950, 72(11): 4847.

[12] von Weimarn P.P. The precipitation laws. Chem. Rev., 1926, 2(2): 217.

[13] Tóth J., Kardos-Fodor A., Halász-Péterfi S. The formation of fine particles by salting-out precipitation. Chem. Eng. Process., 2005, 44(2): 193.

[14] Seyed-Razavi A., Snook I.K., Barnard A.S. Origin of nanomorphology: does a complete theory of nanoparticle evolution exist. J. Mater. Chem., 2010, 20(3): 416.

[15] Nguyen D.T., Kim K.S. Self-development of hollow TiO2 nanoparticles by chemical conversion coupled with Ost wald ripening. Chem. Eng. J., 2016, 286, 266.

[16] Kwon S.G., Hyeon T. Formation mechanisms of uniform nanocrystals via hot-injection and heat-up methods. Small, 2011, 7(19): 2685.

[17] Park J., Joo J., Kwon S.G., Jang Y.J., Hyeon T. Synthesis of monodisperse spherical nanocrystals. Angew. Chem. Int. Ed., 2007, 46, 4630.

[18] Sebastian V., Smith C.D., Jensen K.F. Shape-controlled continuous synthesis of metal nanostructures. Nanoscale, 2016, 8(14): 7534.

[19] Yang L.M., Knowles K.E., Gopalan A., Hughes K.E., James M.C., Gamelin D.R. One-pot synthesis of monodisperse colloidal copper-doped CdSe nanocrystals mediated by ligand-copper interactions. Chem. Mater., 2016, 28(20): 7375.

[20] Wang T., Zhang L.Y., Wang H.Y., Yang W.C., Fu Y.C., Zhou W.L., Yu W.T., Xiang K.S., Su Z., Dai S., Chai L.Y. Controllable synthesis of hierarchical porous Fe3O4 particles mediated by poly(diallyldimethylammonium chloride) and their application in arsenic removal. ACS Appl. Mater. Interfaces, 2013, 5(23): 12449.

[21] Kim S.J., Kim Y.T., Choi J. Facile and rapid synthesis of zinc oxalate nanowires and their decomposition into zinc oxide nanowires. J. Cryst. Growth, 2010, 312(20): 2946.

[22] Kaur J., Bansal S., Singhal S. Photocatalytic degradation of methyl orange using ZnO nanopowders synthesized via thermal decomposition of oxalate precursor method. Physica B, 2013, 416, 33.

[23] Gao Z.J., Gu Y.S., Wang X.Q., Zhang Y. Mechanical properties of Mn-doped ZnO nanowires studied by first-principles calculations. Int. J. Miner. Metall. Mater., 2012, 19(1): 89.

[24] Shamsipur M., Roushani M., Pourmortazavi S.M. Electrochemical synthesis and characterization of zinc oxalate nanoparticles. Mater. Res. Bull., 2013, 48(3): 1275.

[25] Jia Z.G., Yue L.H., Zheng Y.F., Xu Z.D. Rod-like zinc oxide constructed by nanoparticles: synthesis, characterization and optical properties. Mater. Chem. Phys., 2008, 107(1): 137.

[26] Ni L., Wang L., Shao B., Wang Y.J., Zhang W.L., Jiang Y. Synthesis of flower-like zinc oxalate microspheres in ether-water bilayer refluxing systems and their conversion to zinc oxide microspheres. J. Mater. Sci. Technol., 2011, 27(6): 563.

[27] Tang T., Yang T.Z. Fundamental and Technology of Complex Metallurgy, 2011, Changsha, Central South University Press 4.