Built‐in Electric Fields in Heterostructured Lamellar Membranes Enable Highly Efficient Rejection of Charged Mass

Abstract Separation membranes with homogeneous charge channels are the mainstream to reject charged mass by forming electrical double layer (EDL). However, the EDL often compresses effective solvent transport space and weakens channel‐ion interaction. Here, built‐in electric fields (BIEFs) are constructed in lamellar membranes by assembling the heterostructured nanosheets, which contain alternate positively‐charged nanodomains and negatively‐charged nanodomains. We demonstrate that the BIEFs are perpendicular to horizontal channel and the direction switches alternately, significantly weakening the EDL effect and forces ions to repeatedly collide with channel walls. Thus, highly efficient rejection for charged mass (salts, dyes, and organic acids/bases) and ultrafast water transport are achieved. Moreover, for desalination on four‐stage filtration option, salt rejection reaches 99.9 % and water permeance reaches 19.2 L m −2 h −1 bar −1 . Such mass transport behavior is quite different from that in homogeneous charge channels. Furthermore, the ion transport behavior in nanochannels is elucidated by validating horizontal projectile motion model.