||Computer modeling of microporous materials has been increasingly important. Recently, two new classes of 2-D ALPOs have been synthesized, namely Al3P4O163- and Al2P3O12H2-. In our research, molecular mechanics calculations are employed to study the stability and structural isomerism of these 2-D ALPOs. We have successfully shown that infinite numbers of 2-D ALPOs hypothetical anionic networks with formula Al3P4O163- can be constructed. Calculations show that these hypothetical networks can have similar thermodynamically stability. The ternplating effects of organic cations which allow selection of particular forms of the anionic 2-D sheets are also discussed in detail. We have also studied other major sheet ALPOs family, which has formula Al2P3O123-. We found that Al2P3O123- can be chiral. Indeed, one of the existing crystal structures contains chiral anionic sheets. However, since the crystal structure contains sheets of both handedness, the overall crystal structure is non-chiral. A systematic analysis of the stability of Al2P3O123- isomers has been performed including some chiral networks. Promising results are found in the energy minimization of these hypothetical networks. It is found that all isomers built based on the 6.6.6 net are stable. We can conclude that many chiral networks may be possible to synthesize if suitable templates and reaction condition are used.