Zeolites/molecular sieves with uniform, molecular-sized pores are important for many
adsorption-based separation processes. Pore size gaps, however, exist in the current
zeolite family. This leads to a great challenge of separating molecules with size
differences at ~0.01 nm level. Here, we report a novel concept, pore
misalignment, to form a continuously adjustable, molecular-sieving
“gate” at the 5A zeolite pore entrance without sacrificing the
internal capacity. Misalignment of the micropores of the alumina coating with the 5A
zeolite pores was related with and facilely adjusted by the coating thickness. For
the first time, organic molecules with sub-0.01 nm size differences were
effectively distinguished via appropriate misalignment. This novel concept may have
great potential to fill the pore size gaps of the zeolite family and realize
size-selective adsorption separation.