All observables admit a spectral decomposition in terms of projectors $P_m$ into the eigenspace corresponding to the eigenvalue $m$. So given for example a collection of kets $|0\rangle, |1\rangle,..., |n\rangle$ with eigenvalues $a_0,a_1,...,a_n$ I can always perform a measurement on a state $|\psi\rangle=\alpha_0|0\rangle+...+\alpha_n|n\rangle$ by a projection such as $$P_0|\psi\rangle=| 0\rangle\langle 0|\psi\rangle=\alpha_0|0\rangle$$ (to be eventually renormalized) with outcome $a_0$. But what if I wanted to see if the system is in a superposition of certain eigenstates? For example, I may wish to apply the projector $$P=\frac{1}{2}(|0\rangle+|1\rangle)(\langle 0|+\langle 1|)=\frac{P_0+|0\rangle\langle1|+|1\rangle\langle 0|+P_1}{2}.$$ Clearly $P$ doesn't belong to the set $\{P_m\}$ as $|0\rangle$ and $|1\rangle$ are associated to different eigenvalues.
My question is: is such a measurement possible, and what would be the outcome of the measurement?