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.

Recent advances in materials science and nanotechnology have lead to considerable interest in constructing ion-channel-mimetic nanofluidic systems for energy conversion and storage. The conventional viewpoint suggests that to gain high electrical energy, the longitudinal dimension of the nanochannels (L) should be reduced so as to bring down the resistance for ion transport and provide high ionic flux. Here, counterintuitive channel-length dependence is described in nanofluidic osmotic power generation. For short nanochannels (with length L < 400 nm), the converted electric power persistently decreases with the decreasing channel length, showing an anomalous, non-Ohmic response. The combined thermodynamic analysis and numerical simulation prove that the excessively short channel length impairs the charge selectivity of the nanofluidic channels and induces strong ion concentration polarization. These two factors eventually undermine the osmotic power generation and its energy conversion efficiency. Therefore, the optimal channel length should be between 400 and 1000 nm in order to maximize the electric power, while balancing the efficiency. These findings reveal the importance of a long-overlooked element, the channel length, in nanofluidic energy conversion and provide guidance to the design of high-performance nanofluidic energy devices.

Nanopores in ultrathin or atomically thin membranes attract broad interest because the infinitesimal pore depth allows selective transport of ions and molecules with ultimate permeability. Toward large-scale osmotic energy conversion, great challenges remain in extrapolating the promising singlepore demonstration to really powerful macroscopic applications. Herein, the origin of the selective ion transport in ultrathin nanopores is systematically investigated. Based on a precise Poisson and Nernst-Planck model calculation, it is found that the generation of net diffusion current and membrane potential stems from the charge separation within the electric double layer on the outer membrane surface, rather than that on the inner pore wall. To keep the charge selectivity of the entire membrane, a critical surface charged area surrounding each pore orifice is therefore highly demanded. Otherwise, at high pore density, the membrane selectivity and the overall power density would fall down instead, which explains the giant gap between the actual experimental achievements and the single-pore estimation. To maximize the power generation, smaller nanopores (pore diameter ≈1-2 nm) are appropriate for large-scale osmotic energy conversion. With a porosity of ≈10%, the total power density approaches more than 200 W m -2 , anticipating a substantial advance toward high-performance large-scale nanofluidic power sources.

fly. Many of the well-developed structurefunction relationships in biological systems have become the inspiration for the design and application of innovative materials. [2,3] This bioinspired learning process accelerates the continuous evolution of novel man-made materials, circumventing many of the previously insurmountable challenges in, for example, architecture, aerodynamics, and materials science, etc. [4] More intriguingly, by adopting various design strategies from different natural inspirations, synthetic materials and devices keep on evolving and gaining more functions. Taking the development of aircraft for example, the wing curve of the prototype airplane mimics the streamlined shape of bird wings so as to reduce aerodynamic drag. The bat uses supersonic-based pathfinding to avoid obstacles when flying at night. Learning from this skill, modern aircraft use radar navigation systems as their "eyes". The adaptive surface coatings of aircraft mimic the micro-and nanostructures of shark skin, which greatly reduces frictional resistance, saving fuel and preventing damage from ultraviolet irradiation. As human beings constantly get new inspiration from nature, the evolution of bioinspired materials never stops.Research in nanofluidic energy conversion is enlightened by the electrogenic cells that convert transmembrane ion-concentration gradients into the release of electrical impulses by membrane-protein-regulated ion transport through the hierarchically arranged ion channels and ion pumps. [5] One particular example is electric eels (Electrophorus electricus), which are capable of generating electric shocks up to 600 V for predation and self-defense (Figure 1). Toward this goal, one research direction is to build synthetic nanofluidic devices with a minimum set of components, yet can mimic the biological energyconversion process on the nanoscale. [6] Another research direction is the multiscale integration of individual nanofluidic devices into macroscopic materials for practical use. [7] Here, we present an overview of the structural and functional evolution in synthetic one-dimensional (1D) and two-dimensional (2D) nanofluidic systems under the guidance of three different types of biological inspiration: the asymmetric ion-transport behaviors of biological ion channels, the strong bioelectric function of electric eels, and the layered microstructure of nacre. The progress, challenges, and future perspectives in this growing field are highlighted.Well-developed structure-function relationships in living systems have become inspirations for the design and application of innovative materials. Building artificial nanofluidic systems for energy conversion undergoes three essential steps of structural and functional development with the uptake of separate biological inspirations. This research field started from the mimicking of the bioelectric function of electric eels, wherein a transmembrane ion concentration gradient is converted into ultrastrong electrical impulses via membrane-protein-regulated ion tran...

The discovery of ionic current rectification (ICR) phenomena in synthetic nanofluidic systems elicits broad interest from interdisciplinary fields of chemistry, physics, materials science, and nanotechnology; and thus, boosts their applications in, for example, chemical sensing, fluidic pumping, and energy related aspects. So far, it is generally accepted that the ICR effect stems from the broken symmetry either in the nanofluidic structures, or in the environmental conditions. Although this empirical regularity is supported by numerous experimental and theoretical results, great challenge still remains to precisely figure out the correlation between the asymmetric ion transport properties and the degree of symmetry breaking. An appropriate and quantified measure is therefore highly demanded. Herein, taking DNA-stuffed nanopores as a model system, we systematically investigate the evolution of dynamic ICR in between two symmetric states. The fully stuffed and fully opened nanopores are symmetric; therefore, they exhibit linear ion transport behaviors. Once the stuffed DNA superstructures are asymmetrically removed from one end of the nanopore via aptamer-target interaction, the nanofluidic system becomes asymmetric and starts to rectify ionic current. The peak of ICR is found right before the breakthrough of the stuffed DNA forest. After that, the nanofluidic system gradually retrieves symmetry, and becomes non-rectified. Theoretical results by both the coarse-grained Poisson-Nernst-Planck model and the 1D statistic model excellently support the experimental observations, and further establish a quantified correlation between the ICR effect and the degree of asymmetry for different molecular filling configurations. Based on the ICR properties, we develop a proof-of-concept demonstration for sensing ATP, termed the ATP balance. These findings help to clarify the origin of ICR, and show implications to other asymmetric transport phenomena for future innovative nanofluidic devices and materials.

Metal oxides are widely used in many applications such as thermoelectric, solar cells, sensors, transistors, and optoelectronic devices due to their outstanding mechanical, chemical, electrical, and optical properties. For instance, their high Seebeck coefficient, high thermal stability, and earth abundancy make them suitable for thermoelectric power generation, particularly at a high-temperature regime. In this article, we review the recent advances of developing high electrical properties of metal oxides and their applications in thermoelectric, solar cells, sensors, and other optoelectronic devices. The materials examined include both narrow-band-gap (e.g., Na x CoO 2 , Ca 3 Co 4 O 9 , BiCuSeO, CaMnO 3 , SrTiO 3 ) and wide-band-gap materials (e.g., ZnO-based, SnO 2 -based, In 2 O 3 -based). Unlike previous review articles, the focus of this study is on identifying an effective doping mechanism of different metal oxides to reach a high power factor. Effective dopants and doping strategies to achieve high carrier concentration and high electrical conductivities are highlighted in this review to enable the advanced applications of metal oxides in thermoelectric power generation and beyond.