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It depends a bitt of what you think about as best to paint. Easiest to paint, moast funn to paint, or that looks best after little effort. Or one that is just a challenge.
Many of the space marine chapters have colours that where pupular in the early 80s. You can see this on the blood angels for instance. A strong red and yellow on the details. Little subtelty about them. Also you need to keep in mind that some of your models might stand out like centerpiced (big terminators coming to mind) but moast of the other models will be looked upon en mass along with the rest. So you need to think colourschemes on a macro level, that being the army, as well as a micro level, the singel modell.
From a colour theory perspective yellow is a bit hard to work with, since it is a quite dominant colour. Yellow paint also acts very diferently then other colours, it needs more of it. This is even true with the foundations, and it tend to cloth more then the regular colours. The same is true for orange since it has a lott of yellow in it. It is also very hard to shade yellow. One shure way to do it is to blend in purple until it becomes brown and then add black. If you just add black you make green.
The salamanders I do think would make a nice army to paint. The lush green and the orange flames really are good but it does not leave much room for other colours since you are already pretty comitted.
White scars and black templars both look great, but if you are going for the templars then you really need templar parts to make them "crusading". I would recomend both of them. Mind you, white is a hard colour to do right since it requers many layers. However, both the black and the white is quite easy to combine with other colours, leaving you easy to add details. I would recomen "dirtying" both of them up a bitt, deluding them. When painting white the problem is that you cannot go "brighter" so shading needs to be done in reverse (by shading the rest of the modle instead of highlighting the figure) and the same with the black one since you can't just add black to the recesses. However, I do belive both will be a dream to work with.
Edit: If you really wanne look on the whole thing as an exersice then go for grey knights and learn to paint non-metalic metal. It looks really great even when you are starting to learn it. Also, the grey knights codex is good with a low model count. Perfect for the experimentating. I would advice you to do some research intro impresionism. It is a painting mind sett that makes for fats models that looks great once you actualy play. (The level of detail is not that great close up,m but seen from 2 feet away it is amasing.)
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