Optimal design of non-linear Temperature Programmed Reduction (TPR) experiments

摘要

The experimental method of temperature programmed reduction (TPR) is extended by application of non-constant temperature gradients. An optimal control problem is formulated with the D-optimality criterion as the objective function and ordinary differential equations (ODEs) as constraints. The problem is solved for systems with a single reaction and with two consecutive reactions. The results show that optimal nonlinear temperature profiles promise to yield lower variances of the estimated parameters when compared to experiments with the best linear temperature profile. To improve the applicability of this approach under lab conditions, reduced problems are formulated with considerably fewer degrees of freedom that can be solved more reliably. The optima of the reduced problems approximate those of the full problems very well.