Bond valence and bond strength calculations
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1 Bond valence and bond strength calculations Pauling: bond strength divided equally between bonds. i.e. undistorted polyhedra Elaboration: bond strength depends on bond distances, i.e. individual bond-lengths are used. Bond strength calculated individually for each bond are added. E.g. Brown and Shannon: Empirical bond-strength-bond-length curves for oxides. Needs empirical ionic radii for each oxidation state, but independent of coordination number. Another approach: Bond valence: generalization of bond-order, i.e. assignment of single/double bond. E.g. O Keeffe: The bond valence method in crystal chemistry Needs empirical data for each M-X bond KJM31 V2 Using bond-strength-bond-length curves Relates bond strength to bond length. Several expressions of the form: Donnay and Allman: s s = R R N s: strength or bond valence of a bond of length _ R S : ideal bond strength of the bond of length R N: constant different for each cation-anion pair, and sometimes for each cation KJM31 V2
2 Brown and Shannon s = s R R N The constant s is chosen, and the constants R and N are determined by fitting to a large number of structures so that the sum of the bond strengths are closest possible to the valence. In contrast to earlier work, Brown and Shannon use the equation over the whole range of bond strengths. The same curve is used for all bonds between two atomic species. And a large number of structures are included in determining s, R and N. KJM31 V2 Corrected and uncorrected parameters Corrected for oxygen coordination KJM31 V2
3 Universal bond-strength-bondlengths parameters, R 1, N 1, for isoelectronic cations can be determined. (Comparison between results from uncorrected, corrected and universal parameters in table 4.) KJM31 V2 Calculated valence sums for V5+ in a number of structures. Usually within 5%, but significant deviations is observed: Structural uncertainties? Second-nearest neighbour effects? Other effects? KJM31 V2
4 What is the coordination number??? KJM31 V2 Testing for the correctness of structures Distinguishing the structure suggestions for Zn 3 (BO 3 ) 2 KJM31 V2
5 Determining cation distribution Cation distribution in sanidine, (Na,K)AlSi 3 O 8 Distribution of Al, Si (Not easy be X-ray diffraction) Calculate K/Na ratio (not very precise) KJM31 V2 Prediction of hydrogen positions Determining hydrogen positions is not easy from X-ray diffraction. MgSO 4 4H 2 O: known hydrogen positions KJM31 V2
6 KJM31 V2 The bond valence method in crystal chemistry Michael O Keeffe Uses the bond-valence concept, i.e. a generalization of bond order Used for prediction and interpretation of bond lengths Definition of bond valence: The valence of a bond between two atoms, i and j is ν ij. Bond valences are defined so that the sum of all bond valences of the bonds formed by a given atom, i, is the atom valency, ν i. If Al 3+ forms four equal bonds, the bond valences are ¾. KJM31 V2
7 Correlation between bond length and bond valence: e.g. Pauling, 1947: d ij = R ij b lnν ij. d ij : Bond length R ij : Length of a single bond (ν ij = 1) b: constant, universal parameter ~.37Å Values of Rij can be determined for pairs of atoms, using a variety of coordinations from parameters in experimental crystal structures. May be used for ionic, covalent and metal-metal bonds. KJM31 V2 The Matrix B 2 O 3 High pressure form, B 4-coordinated iv B 2 ii O(1) iii O(2) 2 Numbers per formula unit 2B O(1) 2O(2) 2α β Number of bonds Bond valences Bond valence sums: Horiz: 2α + β = 2V B = Vert: 2α = V O = 2 and β = 2V O = 4 KJM31 V2
8 B 2 O 3, high pressure 2B O(1) 2O(2) 2α β Bond valence sums: Horiz: 2α + β = 2V B = Vert: 2α = V O = 2 and β = 2V O = 4 Solution: α = 1 β = 2/3 2α + β = is the sum of 2α = 2 and β = 4 R BO = 1.37Å d ij = R ij b lnν ij. B-O(1) = 1.37Å B-O(2) = 1.57Å n cations, m anions: m+n-1 independent valence sums Bonds from O(1) are equal, and bonds from O(2) are equal (Equal valence rule) KJM31 V2 SrBe 3 O 4 Sr 2Be(1) Be(2) O(1) 3α 2γ 3O(2) β δ 3ε 5 kinds of bond, valences α, β γ, δ, ε. But only 5-1=4 independent bond valence sums. Browns equal valences rule: bonds between equal atoms have almost the same bond valence In this case: α β = γ δ. (This is the needed extra equation) Better result when using: (a-b)/s SrO = (g-d)/s BeO KJM31 V2
9 More complex: β-ga 2 O 3 Ga(1)Ga(2)O(1)O(2)O(3) O(1) O(2) O(3) Ga(1) α 2β γ Ga(2) 2δ ε ξ parameters 5-1=4 equations 3 extra from the equal valence rule KJM31 V2 Comparison with use of radii β-laof LaOF in crystal Bond valence Sum of radii ( Sum of radii ( vi viii La and La) xii La) La - O La - F KJM31 V2
10 Using the bond valence method Verifying crystal structures Determining atomic valences and locating atoms: Ilmenite: FeTiO 3 Fe(II)Ti(IV)O 3 or Fe(III)Ti(III)O 3? Hypothesis Fe( II ), Ti( IV ) Fe( III ), Ti( III ) V Fe V Ti Distinguishing O 2-, OH -, F - e.g. LaOF KJM31 V2 Using the bond valence method Indications of non-bonded interactions Example: Al 2 O 3 (All oxygen equal, but two Al-O bond lengths) Two garnets: Mg 3 Al 2 Si 3 O 12 and Ca 3 Al 2 Si 3 O 12 KJM31 V2
11 Co Mn 3O(1) α β Co(II), Mn(IV) Co(II) Co(III) Mn(III) 1.7 Mn(IV) d(ij)=r(ij)-b n(ij)=exp(d( Co(II) Mn(IV) Co(III) Mn(III) KJM31 V2 LiAlSiO4 H2O, zeolite Li-A(BW) Li Unit Cell 1.311(1) 8.19(1) 4.995(1) Al Vol Si Z 4 Space Group P n a 21 Li 1 +1 Al 1 +3 Si 1 +4 O O O O O O O O O O O O KJM31 V2 O O O O O
12 Neutron diffraction LiAlSiO4 H2O, zeolite Li-A(BW) Li Unit Cell 1.311(1) 8.19(1) 4.995(1) Al Vol Si Z 4 H Space Group P n a 21 Li 1 +1 Al 1 +3 Si 1 +4 O O O O O O O O O O O O D1 D2 D2' O O1 O O2 O O3 O O4 O O5 KJM31 V2 D1 O O D2 O O Li Al Si H (1) H (2) O(1) ε κ O(2) α φ λ O(3) β ϕ μ O(4) γ η ν O(5) δ π ϖ KJM31 V2
13 O(1) O(2) O(3) O(4) O(5) Li α α α β Al γ δ δ δ Si η λ λ λ H (1) μ H (2) ν KJM31 V2 O(1) O(2) O(3) O(4) O(5) Si(1) 2 Si(2) 2 Si(3) 2 P O(1) O(2) O(3) O(4) O(5) Si(1) α 2 Si(2) β γ 2 Si(3) 2δ ε P η κ λ μ KJM31 V2
14 O(1) O(2) O(3) O(4) O(5) Si(1) α 2 Si(2) β γ 2 Si(3) 2δ ε P η κ λ μ δ=1 α=4/ κ=4/3 ε=1 λ=1 β= γ = 2/3 ν= μ = 4/3 KJM31 V2
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