What you are looking for is the method Autodesk.Aec.PropertyData.DatabaseServices.PropertySet.SetAt
I am at the airport right now getting ready to board a plane and don't have a code sample ready but it is pretty simple to do. There are several overloaded methods the easiest being just pass in the objectId of the property set definition and then the value to set. Something like this.
pset.SetAt(pset.PropertyNameToId("Name"), "PropertySetDefinitionValue");