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Fig 1.

The design of new analogues based on the potent, first generation molecule, donepezil.

Here, D1 was designed from donepezil, while others (D2 to D10) are based on the basic structure of D1.

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Fig 1 Expand

Fig 2.

Most stable optimized structures of all designed analogues along with their parent molecule, donepezil.

All analogues were optimized in the gas phase at B3LYP/SDD level in Gaussian 09.

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Fig 2 Expand

Table 1.

The stoichiometry, electronic energy, enthalpy, Gibbs free energy (in Hartree), and dipole moment (Debye) of donepezil and its designed analogues.

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Table 1 Expand

Fig 3.

Molecular orbital distribution plots of HOMO and LUMO in the ground state of D9 analogue and donepezil at DFT/SDD level of theory in the gas phase.

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Fig 3 Expand

Table 2.

Energy of HOMOs, LUMO, gap, hardness and softness (all units are in Hartree) of the donepezil and its designed analogues.

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Table 2 Expand

Fig 4.

Predicted pose from molecular docking by Autodock Vina.

Here, the stick representations of ligands denote the superimposed view of docked (pink) and co-crystallized ligand (green).

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Fig 4 Expand

Fig 5.

Predicted pose from the docking analysis showed the binding orientation map of important amino acids for analogue D9, showing hydrogen bond interaction (green color), including π–π stacking (pink color).

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Fig 5 Expand

Table 3.

Binding affinity (kcal/mol) and nonbonding interactions of donepezil and its designed analogues.

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Table 3 Expand

Fig 6.

The time series of the RMSD of backbone atoms (C, Cα, and N) for a) protein and b) ligand for each docked complex. Here, red and blue lines denote donepezil and D9 complex respectively.

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Fig 6 Expand

Fig 7.

The structural changes of protein by means of a) solvent accessible surface area (SASA), b) radius of gyration, and c) root means square fluctuations (RMSF) analysis. Here, red and blue lines denote donepezil and D9 complex, respectively.

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Fig 7 Expand

Fig 8.

Total number of hydrogen bonds formed a) within the protein and b) between the protein and ligand in complex state during the simulation. Here, red and blue lines denote donepezil and D9 complex, respectively.

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Fig 8 Expand

Fig 9.

Conformational changes of the D9-AChE complex.

Here, the stick model of the ligand in blue color represents the starting conformation of the complex, while the green color represents the conformation of last step in the 25 ns long MD simulation.

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Fig 9 Expand

Fig 10.

Binding affinities of designed ligands and standard inhibitor, obtained from ensemble based docking analysis.

Here, binding affinities of D8, D9, D10, and donepezil against multiple AChE conformers from a) protein data bank and b) 25 ns MD simulation.

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Fig 10 Expand

Table 4.

Ensemble based docking against all crystal structures of AChE.

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Table 4 Expand

Table 5.

Binding affinity values of donepezil, D8, D9, and D10 docked against multiple AChE conformers generated by 25 ns MD simulation.

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Table 6.

Nonbonding interactions of the best docked complexes obtained from ensemble based docking analysis.

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Table 7.

Selected pharmacokinetic parameters of donepezil and its designed analogues.

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Table 7 Expand