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EX3 section

BH3

B3LYP/6-31G level

  • Energy = -26.61532 a.u. (5 d.p) In comparison, total energy using 3-21G basis set was -26.46226 a.u. (5 d.p)
 Item               Value     Threshold  Converged?
 Maximum Force            0.000014     0.000450     YES
 RMS     Force            0.000009     0.000300     YES
 Maximum Displacement     0.000057     0.001800     YES
 RMS     Displacement     0.000037     0.001200     YES
 

Link to frequency log file: File:PSL BH3 FREQ.LOG

 Low frequencies ---  -10.0419   -2.9960   -0.0055    0.4925    2.1764    3.7030
 Low frequencies --- 1162.9539 1213.1540 1213.1567
Optimized BH3 structure

Vibrational spectrum for BH3

wavenumber (cm-1) Intensity (arbitrary units) Symmetry IR active? Type
1162.95 92.5526 A1 Yes Out-of-plane Bend
1213.15 14.0531 E Yes (slightly) Bend
1213.16 14.0568 E Yes (slightly) Bend
2582.42 0 A1 No Symmetric Stretch
2715.61 126.3250 E Yes Asymmetric Stretch
2715.61 126.3155 E Yes Asymmetric Stretch

IR Spectrum for BH3

Although there are 6 vibrations, there are only 3 peaks in the IR spectrum. This is because the asymmetric stretches and bends at 1162 and 2715 cm-1 respectively are both degenerate, so only 2 peaks are observed at those frequencies. The third peak is that of the out-of-plane bend. The symmetric stretch is not IR active since there is no change in dipole moment, so no peak is observed.

Molecular Orbitals

The molecular orbital diagram for BH3 is as follows:

The key occupied orbitals, the HOMO and the LUMO predicted using Gaussview are compared to those predicted using LCAO theory:

The overall shape, size and phases of the calculated MOs correspond well with those predicted in the MO diagram, showing that for BH3, LCAO theory gives a very good approximation of the molecular orbitals. However, this is probably because B and H are light atoms and the molecule only has 8 electrons, meaning that there aren't significant relativistic effects.

Ammonia-Borane Association Energy

Key data for Ammonia

B3LYP/6-31G level

Item               Value     Threshold  Converged?
 Maximum Force            0.000006     0.000450     YES
 RMS     Force            0.000004     0.000300     YES
 Maximum Displacement     0.000012     0.001800     YES
 RMS     Displacement     0.000008     0.001200     YES

Link to frequency log file: File:PSL NH3 FREQ.LOG

 Low frequencies ---   -8.5646   -8.5588   -0.0044    0.0454    0.1784   26.4183
 Low frequencies --- 1089.7603 1694.1865 1694.1865
Optimised structure for NH3

Key data for Ammonia-Borane

B3LYP/6-31G level

 Item               Value     Threshold  Converged?
 Maximum Force            0.000122     0.000450     YES
 RMS     Force            0.000058     0.000300     YES
 Maximum Displacement     0.000513     0.001800     YES
 RMS     Displacement     0.000296     0.001200     YES

Link to frequency log file: File:PSL BH3NH3 FREQ 1.LOG

 Low frequencies ---   -0.0010   -0.0006    0.0007   17.5817   27.9112   40.2360
 Low frequencies ---  266.5197  632.3594  639.4724

It is noted that the energy given in the summary table after the frequency calculation is -83.22469057 au, which differs from that of the optimisation calculation by the last 4 decimal places. However, the 'Item table' of the frequency calculation shows that the structure is optimised:

Item               Value     Threshold  Converged?
 Maximum Force            0.000113     0.000450     YES
 RMS     Force            0.000061     0.000300     YES
 Maximum Displacement     0.000660     0.001800     YES
 RMS     Displacement     0.000442     0.001200     YES
Optimised structure for NH3BH3


Calculation of the association energy of the B-N Bond:

  • E(NH3): -56.55777 au
  • E(BH3): -26.61532 au
  • E(NH3BH3): -83.22469 au
  • ΔE = E(NH3BH3)-[E(NH3)+E(BH3)] = -83.22469 - (-56.55777 - 26.61532) = -0.05160 au (5 d.p) = -135 kJ/mol

Smf115 (talk) 08:33, 17 May 2018 (BST)Correct calculation but a comment on the result with comparison to other bond dissociation energies was required.

BBr3 pseudopotential optimisation

To carry out the optimisation, the GEN basis set was used - B3LYP/6-31G level was used for B and pseudo-potential LanL2DZ for Br

         Item               Value     Threshold  Converged?
 Maximum Force            0.000008     0.000450     YES
 RMS     Force            0.000005     0.000300     YES
 Maximum Displacement     0.000036     0.001800     YES
 RMS     Displacement     0.000023     0.001200     YES

Link to frequency optimisation file: DOI:10042/202320

 Low frequencies ---   -0.0137   -0.0064   -0.0046    2.4315    2.4315    4.8421
 Low frequencies ---  155.9631  155.9651  267.7052
Optimized BBr3 structure

Project section

For all the following optimisations, a mixed between pseudo-potentials and basis sets were used via the GEN function. Al and Cl atoms were optimised using B3LYP/6-31G(d,p) and Br atoms were optimised using LanL2DZ pseudo-potentials.

Possible Isomers of AlBr2Cl4 and their symmetries

Isomer 1: Bridging Bromides

Energy of isomer = -2352.40631 a.u. (5 d.p) = -6175067 kJ/mol (nearest integer)

Item               Value     Threshold  Converged?
 Maximum Force            0.000003     0.000450     YES
 RMS     Force            0.000001     0.000300     YES
 Maximum Displacement     0.000040     0.001800     YES
 RMS     Displacement     0.000015     0.001200     YES

Link to frequency file:File:Psl brbridge freq output.log

 Low frequencies ---   -5.1748   -5.0356   -3.1468    0.0027    0.0031    0.0034
 Low frequencies ---   14.8260   63.2702   86.0770
Optimized Isomer 1 structure

Isomer 2: Bridging Chlorides

Energy of isomer = -2352.41630 a.u. (5 d.p) = -6175093 kJ/mol (to nearest integer). This shows that the isomer with the bridging Cl ions is the more stable conformer. This is as expected since Al and Cl are both in the third row, so their orbitals are of more similar size and energy compared to those of Br, leading to more overlap. This means that the Cl lone pairs are more able to relieve Al's electron deficiency, leading to a structure that is overall more stable.

Item               Value     Threshold  Converged?
 Maximum Force            0.000171     0.000450     YES
 RMS     Force            0.000053     0.000300     YES
 Maximum Displacement     0.001613     0.001800     YES
 RMS     Displacement     0.000674     0.001200     YES

Link to frequency file:File:Psl clbridge freq output.log

 Low frequencies ---   -6.1262   -2.0171   -0.0014    0.0026    0.0032    1.3830
 Low frequencies ---   17.8118   49.0588   72.9995
Optimized Isomer 2 structure

AlCl2Br Monomer

Energy of monomer = -1176.19014 a.u. (5 d.p) = -3087499 kJ/mol (to nearest integer)

Item               Value     Threshold  Converged?
 Maximum Force            0.000136     0.000450     YES
 RMS     Force            0.000073     0.000300     YES
 Maximum Displacement     0.000681     0.001800     YES
 RMS     Displacement     0.000497     0.001200     YES

Link to frequency file:File:Psl monomer freq output.log

 Low frequencies ---    0.0039    0.0043    0.0050    1.3569    3.6367    4.2604
 Low frequencies ---  120.5042  133.9178  185.8950
Optimized AlCl2Br structure

Calculation of the dissociation energy of Isomer 2

  • E(Isomer) = -6175093 kJ/mol
  • E(Monomer) = -3087499 kJ/mol
  • Dissociation energy = [2 x E(Monomer)] - E(Isomer) = 95 kJ/mol
  • Since the value is positive, the dimer is more stabilised than the isolated isomers, which is as expected since the dimerisation relieves the electron deficiency of the Al atoms.

Smf115 (talk) 08:39, 17 May 2018 (BST)Correct calculation and consideration given to the accuracy when reporting the result.

Molecular orbitals for Isomer 2

MO 38 (Symmetry: Ag)

MO 43 (Symmetry: Bu)

MO 54 (HOMO, symmetry: Bu)

Smf115 (talk) 08:37, 17 May 2018 (BST)Good MO analysis and nice inclusion of the FO's too. The LCAOs have clear annotations and the nodal planes, strength and character of the interactions are identified and explained. To improve subtler points could have been made, such as the size difference in contributions from Br and Cl in MO 54.


Smf115 (talk) 08:37, 17 May 2018 (BST)Overall a clear report with a very good project section but some missing information and errors throughout the first section.