Simply printing money may seem like the solution to most economic problems to those who do not understand how a country's economy actually works. Obviously a country's central bank has the ability to print money but it this form of quantitative easing has huge impacts on the economy, devaluing the currency and increasing inflation due to the increased supply of notes. If a country did decide on printing money it would most likely only occur when they are trying to reach their inflation targets.

In OP's given scenario, after printing the amount of money required to purchase all of the bitcoin in supply, inflation within the given country would be so high their currency would be worth nothing and the economy would be fully crippled, meaning that there would be no chance for them to buy their desired amount of bitcoin.