A two-stage citric acid–sol/gel synthesis of ZnO/SiO2 nanocomposites: study of precursors and final products
Source abstract
Abstract
ZnO nanoparticles, of average size of 10–15 nm, homogeneously dispersed in a silica matrix were prepared by a two stage citric acid/sol–gel process and thermal treatments up to 700 °C. The precursors formed at the early stages of the synthesis and their thermal evolution were investigated by FTIR, 29Si NMR MAS and CPMAS, 13C CPMAS and T1ρ(1H). A unidentate complex was revealed in the gel, together with other complexes in which citrate carboxylate groups are bound to one Zn2+ ion or act as a bridge between two Zn2+ ions. A comparison of the results from nanocomposite and silica samples prepared by the same method showed that chemical interactions between amorphous silica and zinc ions are not present either in the precursors or in the final materials. As a consequence, ZnO particles do not react with silica matrix when they are heated up to 700 °C. This result is ascribed to a nanophase segregation of zinc citrate complexes from the host matrix.
Source: openaire · Quality: candidate unverified · Source record ↗
Research context
OpenAlex topics: Mesoporous Materials and Catalysis · ZnO doping and properties · Layered Double Hydroxides Synthesis and Applications
SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.
References (44)
Show source-provided references
1. Andelman T, Gong Y, Polking M, Yin M, Kuskovsky I, Neumark G, O’Brien S (2005) Morphological control and photoluminescence of zinc oxide nanocrystals. J Phys Chem B 109(30):14314–1431810.1021/jp050540o ↗
2. Cannas C, Casu M, Musinu A, Lai A, Piccaluga G (1999) XRD, TEM and 29Si MAS NMR study of sol-gel ZnO-SiO2 nanocomposites. J Mater Chem 9:1765–176910.1039/a901001g ↗
3. Cannas C, Casu M, Lai A, Musinu A, Piccaluga G (2002) Study of the nanoparticle/matrix interactions in Y2O3-SiO2 samples. Phys Chem Chem Phys 4:2286–229210.1039/b110996k ↗
4. Cannas C, Mainas M, Musinu A, Piccaluga G (2003) ZnO/SiO2 nanocomposites obtained by impregnation of mesoporous silica. Compost Sci Technol 63:1187–119110.1016/S0266-3538(03)00040-X ↗
5. Cannas C, Musinu A, Peddis D, Piccaluga G (2004) New synthesis of ferrite-silica nanocomposites by a sol-gel auto-combustion. J Nanop Res 6:223–23210.1023/B:NANO.0000034679.22546.d7 ↗
6. Cannas C, Musinu A, Peddis D, Piccaluga G (2006) Synthesis and characterization of CoFe2O4 nanoparticles dispersed in a silica matrix by a sol-gel autocombustion method. Chem Mater 18:3835–384210.1021/cm060650n ↗
7. Deng YF, Zhou ZH, Wan HL (2004) pH-dependent isolations and spectroscopic, structural, and thermal studies of Titanium citrate complexes. Inorg Chem 43:6266–627310.1021/ic0496018 ↗
8. Dickinson LC, Yang H, Chu CW, Stein RS, Chien JCW (1987) Limits to compatibility in poly(x-methylstyrene)/poly(2,6-dimethylphenylene oxide) blends by NMR. Macromolecules 20(8):1757–176010.1021/ma00174a007 ↗
9. Engelhardt G (1987) High resolution solid state NMR of silicates and zeolites. Wiley, New York
10. Ennas G, Musinu A, Piccaluga G, Montenero A, Gnappi G (1990) Structure and chemical durability of zinc-containing glasses. J Non-Cryst Solids 125(1–2):181–18510.1016/0022-3093(90)90337-L ↗
11. Fang TT, Wu MS, Tsai JD (2002) 13C NMR study of the solution chemistry of barium titanium citrate gels prepared using the Pechini process. J Am Ceram Soc 85:2984–298810.1111/j.1151-2916.2002.tb00567.x ↗
12. Fischer JW, Merwin LH, Nissan RA (1995) NMR investigation of the thermolysis of citric acid. Appl Spectr 49:120–12610.1366/0003702953963229 ↗
13. Guo L, Yang S, Yang C, Yu P, Wang J, Ge W, Wong GKL (2000) Synthesis and characterization of poly(vinylpyrrolidone)-modified zinc oxide nanoparticles. Chem Mater 12:2268–227310.1021/cm9907817 ↗
14. Kakihana M, Milanova M, Arima M, Yoshima M, Yoshimura M (1996) Polymerized complex route to synthesis of pure Y2Ti2O7 at 750°C using yttrium-titanium mixed-metal citric acid complex. J Am Ceram Soc 79:1673–167610.1111/j.1151-2916.1996.tb08781.x ↗
15. Kakihana M, Arima M, Nakamura Y, Yashima M, Yoshimura M (1999) Spectroscopic characterization of precursors used in the Pechini-type polymerizable complex processing of barium titanate. Chem Mater 11:438–45010.1021/cm9806681 ↗
16. Khouchaf L, Tullier MH, Wark M, Paillaud JJ, Soulard M (1997) Structure of zinc oxide particles inserted in nanopores of microporous materials. J Phys IV 7:C-267–C-268
17. Lipmaa E, Magi M, Samson A, Engelhardt G, Grimmer AR (1980) Structural studies of silicates by solid-state high-resolution silicon-29 NMR. J Am Chem Soc 102:4889–489310.1021/ja00535a008 ↗
18. Lorenz C, Emmerling A, Fricke J, Schmidt T, Hilgendorff M, Spanhel L, Muller G (1998) Aerogel containing strongly photoluminescing zinc oxide nanocrystals. J Non-Cryst Solids 238:1–510.1016/S0022-3093(98)00679-6 ↗
19. Lu S, Liu H, Zhang L, Yao X (1996) Preparation, structure and properties of ZnS-SiO2 nanocomposites. Chin Sci Bull 41:230–233
20. Lu Y, Miller JD (2002) Carboxyl stretching vibrations of spontaneously adsorbed and LB-transferred calcium carboxylates as determined by FTIR internal reflection spectroscopy. J Colloid Interface Sci 256:41–5210.1006/jcis.2001.8112 ↗
21. Maciel GE, Sindorf DW (1980) Silicon-29 NMR study of the surface of silica gel by cross polarization and magic-angle spinning. J Am Chem Soc 102:7606–760710.1021/ja00545a056 ↗
22. Matzapetakis M, Dakanali M, Raptopoulou CP, Taugoulis V, Terris A, Moon N, Giapintzakis J, Salifoglou A (2000) Synthesis, spectroscopic, and structural characterization of the first aqueous cobalt(II)-citrate complex: toward a potentially bioavailable form of cobalt in biologically relevant fluids. JBIC 5:469–47410.1007/PL00021448 ↗
23. Mehrotra RC, Bohra R (1983) Metal carboxylates, Chap. 3. Academic Press, New York
24. Mondelaers D, Vhoyland G, Van den Rul H, D’Haen J, Van Bael MK, Mullens J, Van Poucke LC, Frederix F (2002) Synthesis of ZnO nanopowder via an aqueous acetate–citrate gelation method. Mater Res Bull 37, 901–91410.1016/S0025-5408(02)00727-4 ↗
25. Musinu A, Piccaluga G, Magini M (1988) Coordination of zinc(II) in ZnO-K2O-SiO2 glasses by X-ray diffraction. J Am Ceram Soc 71(5):256–25910.1111/j.1151-2916.1988.tb05073.x ↗
26. Nakamoto K (1997) Infrared and Raman spectroscopy of inorganic and coordination compounds, Part B. Application in coordination, organometallic and bioinorganic chemistry, 5th edn. Wiley, New York
27. Narendar Y, Messing GL (1997) Mechanism of phase separation in gel-based synthesis of multicomponent metal oxides. Catal Today 35:247–26810.1016/S0920-5861(96)00160-5 ↗
28. Oner M, Norwig J, Meyer WH, Wegner G (1998) Control of ZnO crystallization by a PEO-b-PMAA Diblock copolymer. Chem Mater 10:460–46310.1021/cm970450z ↗
29. Polarz S, Neues F, Van den Berg MWE, Grunert W, Khodei L (2005) Mesosynthesis of ZnO-silica composites for methanol nanocatalysis. J Am Chem Soc 127:12028–1203410.1021/ja0516514 ↗
30. Powder Diffraction File, Card No. 36-1451 (1998) International Centre for Diffraction Data, Swarthmore, PA
31. Simonutti R, Comotti A, Neuroni F, Sozzani P (1999) 13C and 29Si Solid-State NMR of rubber-silica composite materials. Chem Mater 11:822–82810.1021/cm9807539 ↗
32. Sindorf DW, Maciel GE (1981) Silicon-29 CP/MAS NMR studies of methylchlorosilane reactions on silica gel. J Am Chem Soc 103:4263–426510.1021/ja00404a055 ↗
33. Takahashi R, Sato S, Sodesawa T, Kawakita M, Ogura K (2000) High surface-area silica with controlled pore size prepared from nanocomposite of silica and citric acid. J Phys Chem B 104:12184–1219110.1021/jp002662g ↗
34. Takahashi R, Sato S, Sodesawa T, Suzuki M, Ichikuni N (2003) Ni/SiO2 prepared by sol-gel process using citric acid. Micropor Mesopor Mat 66:197–20810.1016/j.micromeso.2003.09.007 ↗
35. Turgeman R, Gershevitz O, Deutsch M, Ocko BM, Gedanken A, Sukenik CN (2005) Crystallization of highly oriented ZnO microrods on carboxylic acid-terminated SAMs. Chem Mater 17(20):5048–505610.1021/cm051234q ↗
36. Van Werde K, Mondelaers D, Vanhoyland G, Nelis D, Van Bael MK, Mullens J, Van Poucke C, Van Der Veken B, Desseyn HO (2002) Thermal decomposition of the ammonium zinc acetate citrate precursor for aqueous chemical solution deposition of ZnO. J Mater Sci 37:81–8810.1023/A:1013141723764 ↗
37. Viitanen MM, Jansen WPA, van Welzenis RG, Brongersma HH (1999) Cu/ZnO and Cu/ZnO/SiO2 catalysts studied by low-energy ion scattering. J Phys Chem B 103:6025–602910.1021/jp990375a ↗
38. Walther KL, Wokaun A, Baiker A (1990) Characterization of porous silica gels prepared via the sol-gel process by 29Si CP/MAS solid-state NMR spectroscopy. Mol Phys 71:769–78010.1080/00268979000102101 ↗
39. Xia HL, Tang FQ (2003) Surface synthesis of zinc oxide nanoparticles on silica spheres: preparation and characterization. J Phys Chem B 107(35):9175–917810.1021/jp0261511 ↗
40. Xu CX, Sun XW, Chen BJ, Shum P, Li S, Hu X (2004) Nanostructural ZnO and its electrical and optical properties. J Appl Phys 95:661–66610.1063/1.1632549 ↗
41. Yabuki M, Takahashi R, Sato S, Sodesawa T, Ogura K (2002) Silica-alumina catalysts prepared in sol-gel process of TEOS with organic additives. Phys Chem Chem Phys 4:4830–483710.1039/B205645C ↗
42. Zhang J, Sun L, Yin J, Su H, Liao C, Yan C (2002) Control of ZnO morphology via a simple solution route. Chem Mater 14:4172–417910.1021/cm020077h ↗
43. Zhang WH, Shi JL, Wang LZ, Yan DS (2000) Preparation and characterization of ZnO clusters inside mesoporous silica. Chem Mater 12:1408–141310.1021/cm990740a ↗
44. Zumbulyadis N, O’Reilly JM (1991) Polarization transfer across interfaces. 1. 29Si cross-polarization dynamics at the poly(vinyl alcohol)-silica sol-gel interface. Macromolecules 24:5294–529810.1021/ma00019a012 ↗