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Very simple idea that can make locating the basic comparison functions more efficient (first two lines). Changing the order putting each comparison function and his counterpart below him would make easier to find the desired one.
The operations are also well sorted in the original: all binary operations in the first line and all unary operations (with implied zero) in the second line. You are actually scrambling things more in your proposed solution. I would suggest a small correction: at least place all unary operations in the upper right quadrant (move the =0 and !=0 to the fourth column)..
I've always found the existing palette difficult to navigate. Arranging items in vertical pairs feels *so* much better. Kudos for the Altenbach refinement.
In the original way, you align binary and unary on a row, with comparable operators vertically aligned.
In the new way, you group binary and unary in two distinct groups, and keep the order similar.
I prefer the original way. There's more connection between binary and unary. I think it's easier to find the unary functions, because they're located directly under the binary ones with the same functionality.
I.e... it's easier to spot the > and then select the >0 under it, then searching directly for the >0