Protein design is the design of new protein molecules, either from scratch or by making calculated variations on a known structure.
Therefore, Is it possible to design highly active de novo enzymes for any desired reaction?
If you are really talking about de novo design with no selection or directed evolution component, then the answer is no.
More or less agree with Michael Benedik. The goal of de novo design is generally to get a good enough sequence that directed evolution can take over. While there are several examples of de novo enzymes with new catalytic functions, the number of successful designs is fairly low. For example, in the new Diels-Alder enzyme below it was noted that only 4% of the constructs had measurable activity.
http://www.sciencemag.org/content/329/5989/309.full.html#ref-5
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