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9.2.2.1 30 ,40 Stereoselectivity According to an almost universally accepted opinion, stereoisomers of an organic molecule should be anticipated to frequently exhibit widely different and unpredictable pharmacological effects.18 20 The two chiral centers of suksdor n (1), C-30 and C-40 , both possess R con gurations. Our rst SAR effort was to elucidate the stereochemical requirement of these two positions, as a different con guration changes the orientation and shape of the whole molecule. Huang et al. synthesized a series of khellactone derivatives, including all four stereochemical isomers, 30 , 40 cis or trans (2 38) (Figures 9-2 and 9-3).21,22 Some cis-30 , 40 -substituted compounds showed activity against HIV-1 in H9 lymphocytes, which are listed in Table 9-1. Among them, 30 R,40 R-di-O-( )-camphanoyl-( )-cis-khellactone (DCK, 2) had an EC50 of 2:6 10 4 mM and TI of 137,000, and it was much more potent than the remaining stereo-isomers, 3 (30 S,40 S, EC50 51 mM and TI 33), 4 (30 R,40 S, EC50 6.4 mM and TI 1), and 5 (30 S,40 R) (EC50 32 mM and TI 1). The three-dimensional (3-D) orientations of the four DCK stereochemical isomers (Figure 9-2), generated by Tripos Sybyl software,23 showed different molecular orientations and shapes. Therefore, 30 R,40 R DCK (2) may t the putative receptor, whereas the other three con gurations do not. Thus, the low anti-HIV activity of most synthetic khellactone analogs may be attributed to racemization (Figure 9-3).22 The rigid ( )-camphanoyl moiety in DCK (2) contains the isovaleryl group. An x-ray crystallographic analysis con rms that the isovaleryl group in 1 is more

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analysis is applied to the spatially discretized system (11 15). Details on the numerical methods are given in the Appendix. Figure 3.6 shows codimension-1 singularities in a parameter plane spanned by the activation energy of the anodic reaction A and the activation energy of the electrolyte conductivity , when the total cell current I is used as the bifurcation parameter. Hysteresis and isola varieties are found. The nonlinear behavior becomes increasingly complicated for increasing values of . Steady-state multiplicities even exist for rather small values of , but vanish if the electrolyte s conductivity is temperature-independent, i.e., = 0. This confirms that the multiple steady states are caused not by the electrochemical reaction alone, but by the combination of reaction and varying electrical conductivity. One-parameter continuations for a fixed value of A and increasing values of are shown in Fig. 3.7 (a) (f). In Fig. 3.7 (a), all steady-state solutions are stable and unique. When going from the conditions of Fig. 3.7 (a) to those of Fig. 3.7 (b), the lowest line of isola varieties in Fig. 3.6 is crossed. Therefore, Fig. 3.7 (b) contains an additional isolated branch of solutions. Increasing to the value used in Fig. 3.7 (c) leads to the generation of a hysteresis, as a line of hysteresis varieties is crossed in Fig. 3.6. More isolas and hysteresies are created when the value of is increased further, as can be seen in Fig. 3.7 (c) (f). Finally, up to seven coexisting steady states are found in Fig. 3.7 (f). Figure 3.8 shows the spatial temperature profiles of the seven states. Although the temperature maxima and minima of the coexisting solutions vary strongly, the total cell voltages of the different solutions are found to

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