The point of the 4×2 tiles is exactly to avoid the blockiness artifacts of vector quantization (visible in the article).
Larger tiles increase the average error and entropy because of the way VQ works - it tries to find blocks that look like each other and then encode all similar blocks by referencing a single tile (usually choosing the "average" or "mode" the blocks).
As tiles grow larger, the chance to find highly similar blocks obviously decreases (and deviation from the representative tile increases).
Reducing one of the dimensions is probably better positioned on the quality-speed frontier.