Efforts to enhance signal detection in NMR, such as crosspolarization (CP) and dynamic nuclear polarization (DNP), have been extensively employed to improve the signal-to-noise ratio and address the analytical challenges associated with analyzing C-(A)-S-H, which hosts a plethora of coexisting Si and Al species . CP involves transferring polarization from pro-tons to the nucleus of interest , while DNP facilitates polarization transfer from electrons to nuclear spins .