I haven't done much assembly in a while, but I was heavily into it once upon a time, and I recall that values with lots of 1s were useful. There is not quick way to generate those here. This means that we can write a single instruction to set any single bit using an inclusive OR and the proper immediate value, but we cannot write a single instruction to clear any single bit.
The reason I think a bit more cleverness might have helped is that there are so many values with multiple encodings. Anything where the 8-bit value ends with 0 has a different encoding as well. For example, a rotation of 0000 and an 8-bit value of 00000100 gives the same result as a rotation of 1111 and an 8-bit value of 00000001 (right?). Perhaps some of the redundant instructions could have been used to represent things ending in lots of 1s?
Regardless, an interesting and informative post. :-)