In nature, hierarchically assembled nanoscale ionic conductors, such as ion channels and ion pumps, become the structural and functional basis of bioelectric phenomena. Recently, ion‐channel‐mimetic nanofluidic systems have been built into reconstructed 2D nanomaterials for energy conversion and storage as effective as the electrogenic cells. Here, a 2D‐material‐based nanofluidic reverse electrodialysis system, containing cascading lamellar nanochannels in oppositely charged graphene oxide membrane (GOM) pairs, is reported for efficient osmotic energy conversion. Through preassembly modification, the surface charge polarity of the 2D nanochannels can be efficiently tuned from negative (−123 mC m−2) to positive (+147 mC m−2), yielding strongly cation‐ or anion‐selective GOMs. The complementary two‐way ion diffusion leads to an efficient charge separation process, creating superposed electrochemical potential difference and ionic flux. An output power density of 0.77 W m−2 is achieved by controlled mixing concentrated (0.5 m) and diluted ionic solutions (0.01 m), which is about 54% higher than using commercial ion exchange membranes. Tandem alternating GOM pairs produce high voltage up to 2.7 V to power electronic devices. Besides simple salt solutions, various complex electrolyte solutions can be used as energy sources. These findings provide insights to construct cascading nanofluidic circuits for energy, environmental, and healthcare applications.

With the advance of chemistry, materials science, and nanotechnology, significant progress has been achieved in the design and application of synthetic nanofluidic devices and materials, mimicking the gating, rectifying, and adaptive functions of biological ion channels. Fundamental physics and chemistry behind these novel transport phenomena on the nanoscale have been explored in depth on single-pore platforms. However, toward real-world applications, one major challenge is to extrapolate these single-pore devices into macroscopic materials. Recently, inspired partially by the layered microstructure of nacre, the material design and large-scale integration of artificial nanofluidic devices have stepped into a completely new stage, termed 2D nanofluidics. Unique advantages of the 2D layered materials have been found, such as facile and scalable fabrication, high flux, efficient chemical modification, tunable channel size, etc. These features enable wide applications in, for example, biomimetic ion transport manipulation, molecular sieving, water treatment, and nanofluidic energy conversion and storage. This review highlights the recent progress, current challenges, and future perspectives in this emerging research field of "2D nanofluidics", with emphasis on the thought of bio-inspiration.

Inspired by the microstructure of nacre, material design, and large-scale integration of artificial nanofluidic devices step into a completely new stage, termed 2D nanofluidics, in which mass and charge transportation are confined in the interstitial space between reconstructed 2D nanomaterials. However, all the existing 2D nanofluidic systems are reconstituted from homogeneous nanobuilding blocks. Herein, this paper reports the bottom-up construction of 2D nanofluidic materials with kaolinite-based Janus nanobuilding blocks, and demonstrates two types of electrokinetic energy conversion through the network of 2D nanochannels. Being different from previous 2D nanofluidic systems, two distinct types of sub-nanometer- and nanometer-wide fluidic channels of about 6.8 and 13.8 Å are identified in the reconstructed kaolinite membranes (RKM), showing prominent surface-governed ion transport behaviors and nearly perfect cation-selectivity. The RKMs exhibit superior capability in osmotic and hydraulic energy conversion, compared to graphene-based membranes. The mineral-based 2D nanofluidic system opens up a new avenue to self-assemble asymmetric 2D nanomaterials for energy, environmental, and healthcare applications.