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Two problems. 1. Treasuries do not like "hypothecated" taxation. It makes life awkward when you need to divert money in an emergency or to cover up a mistake, and it adds to the total burden of bookkeeping. Not everyone agrees with the amount spent on, say, the army, but you can't vote not to be defended.
2. Those most likely to pay are, sadly, those least able to do so. Nobody gets rich by giving their money away. If you have a very large income, it's cheaper to pay an accountant than the taxman. If you doubt my word, try door-to-door charity collection and assess the ratio of household income to what they put in the tin, or just look at the people queuing up to pay their weekly idiot tax for the lottery.
Nationalised health services are organised as insurance: everyone pays a premium and hopes never to claim, but unlike private health insurance the premium is related to your ability to pay and there's no penalty for claiming.
Free transport is a social benefit to everyone: the more people who use buses, the easier it is for trucks, emergency vehicles and disabled drivers to get around. It's a good idea if it is subsidised by parking or congestion charges, but that's almost the opposite of hypothecation: those who don't use it, pay for it!
Nevertheless, a huge amount of medical research, education and clinical and social care is provided or part-funded by charities, without which the NHS would be in serious trouble.