Sure, I always love giving feedback! Though realistically all I can give you is just a second, equally subjective, data point to work with.
I only managed to replay chapter 0 and chapter 1 this weekend so I can't comment on quite everything yet, but I definitely do have some more impressions to share.

Harper: New portrait is pretty much an exact match with the vibe I already had of her character. The old portraits for her didn't really the same aggressive confidence to them, so I think this set is a huge improvement in every way. Also, combined with Bennett's new portraits, I actually think their interactions are much more enjoyable now. Despite the dialog being the same, it feels much more like they're engaging in mutual banter and less like Bennett is just struggling to keep up with her now.

Luna: Her new portraits (or at least the ones we see in chapter 0) do feel a bit different to me. Her old portraits always looked a little scary and unapproachable to me, like she was already tired of dealing with me 5 minutes before I first met her. She still has a very serious look, but not quite that same death stare. If I was being chased by an insane killer at night and saw her, I wouldn't be afraid to ask her for help now.

For Penny and Cal, I don't think I can comment until I get around to replaying chapter 2. They both look much better and so far they feel right, but they also don't actually say or do all that much in chapter 0, so... not sure yet. Speaking of chapter 0 though, goddamn, the new Anguis is such a MASSIVE improvement. He looks much more scary and fucked up now so the new portraits are a much better match for how freaked out Bennett is. From chapter 1, i think both Kiera and Vincent felt like their usual selves so far, just improved. Not much to say there. And, leaving the star for last of course...

Liebra: Honestly, I think her new portraits make her feel a lot less scary. Part of it may just be because the new style is so much cuter, but I think there's more to it than just that. My best guess is that it comes down to the old portraits having such huge shifts in the different expressions she would make. The differences in looks from her standard "spider watching a prey caught in her web" face, to her excessively punchable smile when she's overly amused with herself, and of course the classic "devilish grin", all of them would feel that bit exaggerated and like such a large change in mood that it would make her feel a bit more abnormal and unpredictable. Her new portraits aren't just cuter, their expressions also feel much more natural. That should be a good thing, and the increase in quality is undeniable, but I think it comes at the cost of some uncanniness in this case.

But again, these are just my personal impressions. Other people might get completely different vibes from the new portraits. At this point I just hope I didn't ramble too much.