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Since the first exfoliation and identification of graphene in 2004, research on layered ultrathin two-dimensional (2D) nanomaterials has achieved remarkable progress. Realizing the special importance of 2D geometry, we demonstrate that the controlled synthesis of nonlayered nanomaterials in 2D geometry can yield some unique properties that otherwise cannot be achieved in these nonlayered systems. Herein, we report a systematic study involving theoretical and experimental approaches to evaluate the Li-ion storage capability in 2D atomic sheets of nonlayered molybdenum dioxide (MoO2). We develop a novel monomer-assisted reduction process to produce high quality 2D sheets of nonlayered MoO2. When used as lithium-ion battery (LIB) anodes, these ultrathin 2D-MoO2 electrodes demonstrate extraordinary reversible capacity, as high as 1516 mAh g-1 after 100 cycles at the current rate of 100 mA g-1 and 489 mAh g-1 after 1050 cycles at 1000 mA g-1. It is evident that these ultrathin 2D sheets did not follow the normal intercalation-cum-conversion mechanism when used as LIB anodes, which was observed for their bulk analogue. Our ex situ XPS and XRD studies reveal a Li-storage mechanism in these 2D-MoO2 sheets consisting of an intercalation reaction and the formation of metallic Li phase. In addition, the 2D-MoO2 based microsupercapacitors exhibit high areal capacitance (63.1 mF cm-2 at 0.1 mA cm-2), good rate performance (81% retention from 0.1 to 2 mA cm-2), and superior cycle stability (86% retention after 10,000 cycles). We believe that our work identifies a new pathway to make 2D nanostructures from nonlayered compounds, which results in an extremely enhanced energy storage capability. [ABSTRACT FROM AUTHOR]

Enriching the functionality of ferroelectric materials with visible-light sensitivity and multiaxial switching capability would open up new opportunities for their applications in advanced information storage with diverse signal manipulation functions. We report experimental observations of robust intralayer ferroelectricity in two-dimensional (2D) van der Waals layered α-In2Se3 ultrathin flakes at room temperature. Distinct from other 2D and conventional ferroelectrics, In2Se3 exhibits intrinsically intercorrelated out-of-plane and in-plane polarization, where the reversal of the out-of-plane polarization by a vertical electric field also induces the rotation of the in-plane polarization. On the basis of the in-plane switchable diode effect and the narrow bandgap (~1.3 eV) of ferroelectric In2Se3, a prototypical nonvolatile memory device, which can be manipulated both by electric field and visible light illumination, is demonstrated for advancing data storage technologies. [ABSTRACT FROM AUTHOR]

Two-dimensional (2D) lead halide perovskites (LHPs) have garnered incredible attention thanks to their exciting optoelectronic properties and intrinsic strong quantum confinement effect. Herein, we carefully investigate and decipher the charge carrier dynamics at the interface between CsPbBr 3 multiple quantum wells (MQWs) as the photoactive layer and TiO 2 and Spiro-OMeTAD as electron and hole transporting materials, respectively. The fabricated MQWs comprise three monolayers of CsPbBr 3 separated by 2,9-dimethyl-4,7-diphenyl-1,10-phenanthroline (BCP) as barriers. By varying the BCP thickness, we show that charge carrier extraction from MQWs to the corresponding extracting layer occurs through a quantum tunneling effect, as elaborated by steady-state and time-resolved photoluminescence measurements and further verified by femtosecond transient absorption experiments. Ultimately, we have investigated the impact of the barrier-thickness-dependent quantum tunneling effect on the photoelectric behavior of the synthesized QW photodetector devices. Our findings shed light on one of the most promising approaches for efficient carrier extraction in quantum-confined systems.

Aqueous Zn-based batteries are attractive because of the low cost and high theoretical capacity of the Zn metal anode. However, the Zn-based batteries developed so far utilize an excess amount of Zn (i.e., thick Zn metal anode), which decreases the energy density of the whole battery. Herein, we demonstrate an anode-free design (i.e., zero-excess Zn), which is enabled by employing a nanocarbon nucleation layer. Electrochemical studies show that this design allows for uniform Zn electrodeposition with high efficiency and stability over a range of current densities and plating capacities. Using this anode-free configuration, we showcase a Zn-MnO 2 battery prototype, showing 68.2% capacity retention after 80 cycles. Our anode-free design opens a new direction for implementing aqueous Zn-based batteries in energy storage systems.

Aqueous Zn-ion batteries present low-cost, safe, and high-energy battery technology but suffer from the lack of suitable cathode materials because of the sluggish intercalation kinetics associated with the large size of hydrated zinc ions. Herein we report an effective and general strategy to transform inactive intercalation hosts into efficient Zn 2+ storage materials through intercalation energy tuning. Using MoS 2 as a model system, we show both experimentally and theoretically that even hosts with an originally poor Zn 2+ diffusivity can allow fast Zn 2+ diffusion. Through simple interlayer spacing and hydrophilicity engineering that can be experimentally achieved by oxygen incorporation, the Zn 2+ diffusivity is boosted by 3 orders of magnitude, effectively enabling the otherwise barely active MoS 2 to achieve a high capacity of 232 mAh g -1 , which is 10 times that of its pristine form. The strategy developed in our work can be generally applied for enhancing the ion storage capacity of metal chalcogenides and other layered materials, making them promising cathodes for challenging multivalent ion batteries.