Synthesis and Characterization of Lanthanide complexes
Transcription
Synthesis and Characterization of Lanthanide complexes
Synthesis and Characterization of Lanthanide complexes with 1-hydroxy-2-naphthoic acid and Hydrazine as Ligands Karuppannan Parimalagandhi, Sundararajan Vairam* Department of Chemistry, Government College of Technology, Coimbatore 641013, India *Correspondance should be addressed to S. Vairam; [email protected] Six new lanthanide complexes [Ln(N2H4)2{C10H6(1-O)(2-COO)}1.5].3H2O, [where Ln = La(III), Ce(III), Pr(III), Nd(III), Sm(III) and Gd(III)] of 1-hydroxy-2-naphthoic acid with hydrazine as co-ligand, have been synthesized by the reaction of the corresponding metallic nitrates with the 1-hydroxy-2-naphthoic acid and hydrazine in aqueous medium at pH 5. The complexes are characterized by elemental analysis, IR, UV-Visible spectra, Magnetic moment measurement, Simultaneous TG-DTA and Powder X-ray studies. IR spectra of the complexes indicate that the ligands behave as bidentate ligand through COO-. The complexes show the symmetric and asymmetric COO- in the range of 1410-1411 cm-1 and 1557-1559 cm-1 indicating bidental coordination. TG-DTA studies reveal that the compounds undergo endothermic dehydration in the range of 98-110ºC followed by exothermic decomposition to leave the respective metal oxides as the end product through oxalate intermediates. The SEMEDX studies reveal the presence of respective metal oxides in nanosize. X-ray powder patterns show isomorphism among the complexes with similar molecular formulae. 1. Introduction Hydroxy substituted aromatic carboxylic acids, when both -OH and –COOH in ortho positions are important chelating agents in coordination chemistry. They form metal complexes due to the existence of COO- ion held up by hydrogen bonding with hydroxy hydrogen; even in aqueous solutions variety of complexes have been reported [1-3]. Furthermore, using this acid with organic bases, mixed ligand complexes have also been prepared [4-6]. Hydrazine is the simplest diamine and has two donating sites due to which its use as ligand leads to formation of polymeric complexes. In our laboratory we have been synthesizing polymeric metal complexes using aromatic carboxylic acids [7-9] and organic compounds of similar nature, such as squaric acid [10]. Owing to bridging ligation nature of hydrazine and hydroxy aromatic carboxylic acids, we performed this work with an intention of preparing polymeric lanthanide complexes containing 1-hydroxy-2-naphthoic acid and hydrazine as ligands. In this paper, we have presented synthesis and characterization of complexes by IR, UV, TG-DTA, SEM-EDX, powder XRD and magnetic measurements. 1 2. Experimental All the chemicals used were of AR grade. The solvents are distilled prior to use, and double distilled water is used for the preparation and chemical analysis. In all the reactions, 99.99% pure hydrazine hydrate is used as received. 2.1. Preparation of Lanthanide complexes. Lanthanum oxide (0.325 g, 1 mmol) is dissolved in a minimum quantity of 1:1 HNO3, evaporated to eliminate excess of acid, and dissolved in 20 mL of water. This is added slowly to freshly prepare aqueous solution (60 mL) of the ligand containing 1-hydroxy-2-naphthoic acid (0.188 g, 1 mmol) and hydrazine (0.2 g, 4 mmol) stirring the reaction mixture at pH 5. Immediately turbidity developed which turned out to be micro-crystalline solid. Then the complex is filtered, washed with water, alcohol and then with ether and dried. All other lanthanide complexes are prepared by similar procedure by adding the respective metal nitrate solution to the ligand solution in the same molar ratio. 2.2. Physicochemical Techniques. The composition is fixed by chemical analysis. Hydrazine content is determined by titrating against standard KIO3 (0.025 mol L-1) under Andrew’s conditions [11]. The metals, after destroying the hydrazine and organic matter by treatment with concentrated HNO3 and evaporating the excess HNO3 are determined volumetrically by EDTA (0.01 mol L-1) using xylenol orange indicator [11]. IR spectra of the complexes in the region 4000-400 cm-1 were recorded as KBr pellets using a Shimadzu FTIR-8201 (PC)S spectrophotometer. The compounds are insoluble in water and organic solvents, and hence their electronic absorption spectra are recorded for solid samples. Electronic absorption spectra of La(III), Pr(III), Nd(III), Gd(III), Sm(III) & Ce(III) complexes are obtained using a Varian Cary 5000 recording spectrophotometer. The magnetic susceptibility of the complexes was measured using a vibrating sample magnetometer, Lakeshore VSM model 7410 at room temperature. The X-ray powder diffraction patterns of the complexes were recorded using Bruker X-ray diffractometer (model AXS D8 Advance) employing Cu-Kα radiation with nickel filter. The TG-DTA experiments are carried out using Q600 SDT and Q20 DSC instrument, in air atmosphere at a heating rate of 10ºC min-1 using 5 to 10 mg of the samples. Platinum cups are employed as sample holders and alumina as reference. The temperature range is ambient to 800ºC. The elemental analysis is carried out using an Elementar Vario ELIII CHNS elemental analyzer. The SEM with EDX analysis was obtained using JEOL model JSM-6390 LV and JEOL model JED -2300 instrument. 3. RESULTS AND DISSCUSION 3.1. IR Spectra. IR spectra of the complexes are shown in Figures (1-3) and important assignments are given in Table. I & II. The presence of hydrazine in the complexes is revealed from the absorption at 949-981 cm-1 corresponding to (N-N) stretching frequency, which evidence the presence of bidentate bridging ligands [12, 13] and broad absorption peaks in the range of 3550-3575 cm-1 is assigned to O-H vibrations of the associated water 2 molecules. An additional peak observed in the range 578-591 cm-1 is evidence for the presence of lattice water in the complexes [14]. The COO- group coordinated to metal is found by their symmetric (C=O) and asymmetric (C=O) vibration at 1410-1411 cm-1 and 1557-1559 cm-1 respectively. The difference between the above two ranges from 147-149 cm1 implies the bidental coordination [14] to metal. The vN-H stretching is observed in the range of 3394 - 3421 cm-1. The other peaks are common with those of acid. 3.2. Electronic Spectra and Magnetic Susceptibility Measurements. The compounds are insoluble in water and organic solvents, and hence their electronic spectra are recorded for solid samples. The electronic spectra for Pr(III) and Nd(III) complexes shows absorptions at 22831, 21276, 20790, 17667, 16583 cm-1 and 19531, 18975, 15600, 14641, 13605, 12468 which are assigned to 3H4 → 3P2, 3P1, 3P0, 4G5/2, 1D2 and 4I9/2 → 4G9/2, 4G7/2, 2H11/2, 4F9/2, 4F7/2, 4 F5/2 transitions respectively [15, 16]. Magnetic moments from magnetic susceptibility measurements for Pr(III) and Nd(III) are 3.40 BM and 3.55 BM respectively, are in good agreement with the values reported [15]. 3.3. Thermal analysis. TG-DTA of complexes are shown in Figures (4–7) and the thermal data are given in Table-III. All the complexes undergo similar pattern of dehydration. Initially all the water molecules are found to be lost showing endotherms in the range 98ºC to 110ºC. Since they undergo continuous decomposition after dehydration, showing broad exotherms centered at (La-350ºC, Pr-300ºC, Nd-354ºC, Gd-392ºC, Sm-350ºC and Ce-395ºC), the intermediates cannot be indentified clearly. However, stoichiometric calculation indicates that the complexes undergo decomposition via the formation of respective oxalates. This fact is substantiated by comparing [17-19] the decomposition temperatures of oxalate intermediates with those reported in the literature. The final residues are found to be respective oxides [17, 20-22] formed from the decomposition of oxalates showing exotherms at (300ºC to 395ºC). The oxides were further confirmed by their XRD patterns which are comparable with the JCPDS data. While comparing the thermal behavior of similar type of complexes of the same acid with transition metals, it is found that the hydrazine is not eliminated separately in the case of lanthanide complexes. Hydrazine goes along with the decomposition of organic moiety of the complexes. In the case of transition metal complexes, hydrazine is eliminated separately showing clear exothermic peak in the range 260ºC to 300ºC [9]. This may be because of the stability of the complexes lanthanides (hard acid) formed with hydrazine (hard base). Further, the transition metal complexes have coordinated water molecules, whereas in the case of lanthanide complexes water molecules are present in the lattice. Furthermore, the final decomposition is found to happen in almost similar range of temperature viz. (La-710ºC, Pr-720ºC, Nd-720ºC, Gd-740ºC, Sm-750ºC and Ce-710ºC). While the decomposition of complexes is compared with of the pure acid, the complexes undergo decomposition at lower temperature probably because of the fuelling nature of hydrazine and more carbon content of the acid moiety. The Scheme of decomposition reactions are shown in (1). The scheme of decomposition reactions are as follows: 3 [Ln(N2H4)4{C10H6(1-O)(2-COO)}1.5].3H2O [Ln(N2H4)2{C10H6(1-O)(2-COO)}1.5] Ln2(C2O4)3 + 1.5O2 Pr2(C2O4)3 + 1.8O2 98-110 ºC 200-625ºC 600-800ºC 720ºC [Ln(N2H4)2{C10H6(1-O)(2-COO)}1.5] +3H2O Ln2(C2O4)3 Ln2O3 + 6CO2 1/3Pr6O11 + 6CO2 (1) where Ln = La (III),Ce(III),Pr(III),Nd(III),Sm (III) & Gd (III) 3.4. X- ray diffraction Analysis. The X-ray powder diffraction patterns of the complexes [Ln(N2H4)2{C10H6(1-O)(2-COO)}1.5].3H2O,where Ln= La(III) and Nd(III) are given in figure 8 and 9 (representative examples). They show similarity among them, implying isomorphism. 3.5. SEM-EDX Studies. The complexes are calcined in muffle furnace at their decomposition temperature, heating subsequently at the same temperature for one hour and analyzed for their particle size, show that they are in nanoscale (39-42 nm). This fact is further substantiated by their XRD patterns using Scherer’s formula [23] D = Kλ / βcosθ, where λ is the X-ray wavelength, β is the full width of height maximum (FWHM) of a diffraction peak, θ is the diffraction angle, and K is Scherer’s constant of the order of 0.89. The SEM – EDX image of residue obtained from [Nd(N2H4)2{C10H6(1-O)(2-COO)}1.5].3H2O are shown in figures (10,11) as representative examples. From their images, it is understood that the residue is nanosized metal oxides with irregular shape. 4. Conclusion 1-hydroxy-2-naphthoic acid and hydrazine yields the complexes of formulae [Ln(N2H4)2{C10H6(1-O)(2-COO)}1.5].3H2O,where Ln = La(III), Ce(III), Pr(III), Nd(III), Sm(III) & Gd(III) at pH 5. Analytical data confirm their formulations. The hydrazine complexes display an N-N stretching frequency in the range of 949-981 cm-1 showing bidentate bridging nature in the complexes. The complexes undergo thermal decomposition to metal oxide particles of nanosize. All the complexes decompose exothermally in the range 300ºC to 395ºC with elimination of corresponding oxalates. The magnetic and electronic data indicate the presence of metal in the complexes. Powder XRD and SEM –EDX studies confirm the formation of respective metal oxides. References [1] [2] T. Premkumar, and S. 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Analytical data of [Ln(N2H4)2{C10H6(1-O)(2-COO)}1.5].3H2O complexes Table II. Characteristic I.R. bands of [Ln(N2H4)2{C10H6(1-O)(2-COO)}1.5].3H2O complexes Table III. Thermal Analysis of [Ln(N2H4)2{C10H6(1-O)(2-COO)}1.5].3H2O complexes 7 Table I. Analytical data of [Ln(N2H4)2{C10H6(1-O)(2-COO)}1.5].3H2O complexes Complexes [La(N2H4)2{C10H6 (1-O)(2-COO)}1.5].3H2O [Pr(N2H4)2{C10H6 (1-O)(2-COO)}1.5].3H2O [Nd(N2H4)2{C10H6 (1-O)(2-COO)}1.5].3H2O [Gd(N2H4)2{C10H6 (1-O)(2-COO)}1.5].3H2O [Sm(N2H4)2{C10H6 (1-O)(2-COO)}1.5].3H2O [Ce(N2H4)2{C10H6 (1-O)(2-COO)}1.5].3H2O Colour White Light Green Light Violet Dull White Dull White Light Yellow Carbon Found (calc.) Hydrogen Found (calc.) Analytical data (%) Nitrogen Hydrazine Found Found (calc.) (calc.) 36.2 (36.4) 4.4 (4.0) 10.1 (10.4) 11.5 (11.6) 25.6 (25.7) 36.5 (36.3) 4.4 (4.1) 10.5 (10.4) 11.8 (11.9) 26.3 (26.2) 36.1 (36.2) 4.0 (4.1) 10.6 (10.5) 11.5 (11.7) 26.4 (26.3) 35.1 (35.3) 4.0 (3.9) 10.1 (10.2) 11.1 (11.3) 28.1 (28.2) 36.2 (36.3) 4.3 (4.1) 10.2 (10.3) 11.5 (11.6) 27.2 (27.4) 36.2 (36.3) 4.2 (4.3) 10.3 (10.2) 11.7 (11.8) 25.4 (25.5) 8 Metal Found (calc.) Table II. IR data of [Ln(N2H4)2{C10H6(1-O)(2-COO)}1.5].3H2O complexes υN-N cm-1 υC=O Asym cm-1 υC=O sym cm-1 υC=O asym-sym cm-1 υOH cm-1 [La(N2H4)2{C10H6 (1-O)(2-COO)}1.5].3H2O 949 (m) 1441 (s) 141 [Pr(N2H4)2{C10H6 (1-O)(2-COO)}1.5].3H2O 901 (m) 1582 (s) 1582 (s) 1442 (s) [Nd(N2H4)2{C10H6 (1-O)(2-COO)}1.5].3H2O 966 (m) 1557 (s) [Gd(N2H4)2{C10H6 (1-O)(2-COO)}1.5].3H2O 969 (m) [Sm(N2H4)2{C10H6 (1-O)(2-COO)}1.5].3H2O 980 (m) [Ce(N2H4)2{C10H6 (1-O)(2-COO)}1.5].3H2O 966 1582 1438 144 (m) (s) (s) (b): broad, (s):sharp, (m):medium Molecular formula of Complexes υH2O cm-1 υNH cm-1 3407 (b) 591 (s) 3049 140 3420 (b) 583 (s) 3066 1444 (s) 113 3399 (b) 586 (s) 3049 1582 (s) 1442 (s) 140 3400 (b) 578 (s) 3066 1582 (s) 1442 (s) 140 3394 (b) 583 (s) 3049 3392 (b) 583 (s) 3033 9 Table III. Thermal data of [Ln(N2H4)2{C10H6(1-O)(2-COO)}1.5].3H2O complexes Thermogravimetry Temp. Weight loss/ % Range (°C) Obs. Calc. 102(+) 65-228 10.2 10.1 [La(N2H4)2{C10H6 350(-) 228-600 48.9 49.0 (1-O)(2-COO)}1.5].3H2O 710(+) 600-800 66.8 67.0 99.5(+) 63-140 10.1 10.2 [Pr(N2H4)2{C10H6 350(-) 140-625 49.2 49.3 (1-O)(2-COO)}1.5].3H2O 720(+) 625-790 68.1 68.4 102 (+) 65-212 10.0 10.1 [Nd(N2H4)2{C10H6 360(-) 212-620 48.7 48.9 (1-O)(2-COO)}1.5].3H2O 720(+) 620-800 68.7 68.9 110 (+) 75-220 9.7 10.0 [Gd(N2H4)2{C10H6 390(-) 220-582 47.5 47.6 (1-O)(2-COO)}1.5].3H2O 740(+) 582-700 67.1 67.3 98.5(+) 67.8-200 10.1 9.8 [Sm(N2H4)2{C10H6 350(-) 200-480 44.0 43.8 (1-O)(2-COO)}1.5].3H2O 750(+) 480-700 64.0 63.6 125 (+) 75-200 10.3 10.2 [Ce(N2H4)2{C10H6 375(-) 200-500 49.3 49.1 (1-O)(2-COO)}1.5].3H2O 710(+) 500-625 67.9 67.6 (-) = Exotherm, (+) = Endotherm Compound DTA peak Temp (°C) 10 Intermediate/End product Dehydration La2(C2O4)3 La2O3 Dehydration Pr2(C2O4)3 Pr6O11 Dehydration Nd2(C2O4)3 Nd2O3 Dehydration Gd2(C2O4)3 Gd2O3 Dehydration Sm2(C2O4)3 Sm2O3 Dehydration Ce2(C2O4)3 CeO2 Figure Captions Fig.1. IR spectrum of C10H6(1-OH)(2-COOH) Fig.2. IR spectrum of [Gd(N2H4)2{C10H6(1-O)(2-COO)}1.5].3H2O Fig.3. IR spectrum of [Pr(N2H4)2{C10H6(1-O)(2-COO)}1.5].3H2O Fig.4. TG-DTA spectrum of [La(N2H4)2{C10H6(1-O)(2-COO)}1.5].3H2O Fig.5. TG-DTA spectrum [Pr(N2H4)2{C10H6(1-O)(2-COO)}1.5].3H2O Fig.6. TG-DTA spectrum of [Nd(N2H4)2{C10H6(1-O)(2-COO)}1.5].3H2O Fig.7. TG-DTA spectrum of [Gd(N2H4)2{C10H6(1-O)(2-COO)}1.5].3H2O Fig.8. XRD pattern of [La(N2H4)2{C10H6(1-O)(2-COO)}1.5].3H2O Fig.9. XRD pattern of [Nd(N2H4)2{C10H6(1-O)(2-COO)}1.5].3H2O Fig.10. SEM images of Nd2O3 obtained by [Nd(N2H4)2{C10H6(1-O)(2-COO)}1.5].3H2O residue Fig.11. SEM-EDX image of Nd2O3 11 Fig.1. IR spectrum of C10H6(1-OH)(2-COOH) Fig.2. IR spectrum of [Gd(N2H4)2{C10H6(1-O)(2-COO)}1.5].3H2O 12 Fig.3. IR spectrum of [Pr(N2H4)2{C10H6(1-O)(2-COO)}1.5].3H2O Fig.4. TG-DTA spectrum of [La(N2H4)2{C10H6(1-O)(2-COO)}1.5].3H2O 13 Fig.5. TG-DTA spectrum of [Pr(N2H4)2{C10H6(1-O)(2-COO)}1.5].3H2O Fig.6. TG-DTA spectrum of [Nd(N2H4)2{C10H6(1-O)(2-COO)}1.5].3H2O 14 Fig.7. TG-DTA spectrum of [Gd(N2H4)2{C10H6(1-O)(2-COO)}1.5].3H2O Fig.8. XRD pattern of [Ln(N2H4)2{C10H6(1-O)(2-COO)}1.5].3H2O 15 Fig.9. XRD pattern of [Nd(N2H4)2{C10H6(1-O)(2-COO)1.5].3H2O Fig.10. SEM images of Nd2O3 obtained by [Nd(N2H4)2{C10H6(1-O)(2-COO)}1.5].3H2O residue 16 Fig.11. SEM-EDX image of Nd2O3 17