Chiral Viologen-Derived Water-Stable Small Band Gap Lead Halides: Synthesis, Characterization, and Optical Properties.

Chiral organic-inorganic metal halides (OIMHs) are attractive for their potential applications in chiral optoelectronics and spintronics, such as circular polarized light emitters, detectors, and chiral-induced spin selectivity. Here, we report three pairs of chiral OIMHs with great water stability constructed from chiral viologens. These OIMHs contain either 1D or 0D structures, however, with small band gaps around 2 eV. Circular dichroism (CD) spectroscopy on transparent thin films of two OIMH pairs showed a wide CD response covering most of the visible light range. Although the chiral center is not directly attached to the pyridinium in these chiral viologens, the chirality is still successfully transferred into both the band gap and the exciton absorption ranges. Liquid and solid CD studies of the chiral viologens further indicate that the chiral induction inside these OIMHs is possibly through chiral crystallization. This work demonstrated the design strategy of water-stable, small band gap chiral OIMHs through chiral viologens. These low-dimensional chiral materials may provide an interesting system to investigate chiral induction, and their broad CD response may enable their potential application as circular photodetectors with a wide detection range.

Predictive Design Model for Low-Dimensional Organic-Inorganic Halide Perovskites Assisted by Machine Learning.

Low-dimensional organic-inorganic halide perovskites have attracted interest for their properties in exciton dynamics, broad-band emission, magnetic spin selectivity. However, there is no quantitative model for predicting the structure-directing effect of organic cations on the dimensionality of these low-dimensional perovskites. Here, we report a machine learning (ML)-assisted approach to predict the dimensionality of lead iodide-based perovskites. A literature review reveals 86 reported amines that are classified into "2D"-forming and "non-2D"-forming based on the dimensionality of their perovskites. Machining learning models were trained and tested based on the classification and descriptor features of these ammonium cations. Four structural features, including steric effect index, eccentricity, largest ring size, and hydrogen-bond donor, have been identified as the key controlling factors. On the basis of these features, a quantified equation is created to calculate the probability of forming 2D perovskite for a selected amine. To further illustrate its predicting capability, the built model is applied to several untested amines, and the predicted dimensionality is verified by growing single crystals of perovskites from these amines. This work represents a step toward predicting the crystal structures of low dimensional hybrid halide perovskites using ML as a tool.

A Lightweight 3D Cu Nanowire Network with Phosphidation Gradient as Current Collector for High-Density Nucleation and Stable Deposition of Lithium.

Lithium metal anodes with high energy density are important for further development of next-generation batteries. However, inhomogeneous Li deposition and dendrite growth hinder their practical utilization. 3D current collectors are widely investigated to suppress dendrite growth, but they usually occupy a large volume and increase the weight of the system, hence decreasing the energy density. Additionally, the nonuniform distribution of Li ions results in low utilization of the porous structure. A lightweight, 3D Cu nanowire current collector with a phosphidation gradient is reported to balance the lithiophilicity with conductivity of the electrode. The phosphide gradient with good lithiophilicity and high ionic conductivity enables dense nucleation of Li and its steady deposition in the porous structure, realizing a high pore utilization. Specifically, the homogenous deposition of Li leads to the formation of an oriented texture on the electrode surface at high capacities. A high mass loading (≈44 wt%) of Li with a capacity of 3 mAh cm-2 and a high average Coulombic efficiency of 97.3% are achieved. A lifespan of 300 h in a symmetrical cell is obtained at 2 mA cm-2 , implying great potential to stabilize lithium metal.

Fast Gelation of Ti3 C2 Tx MXene Initiated by Metal Ions.

Gelation is an effective way to realize the self-assembly of nanomaterials into different macrostructures, and in a typical use, the gelation of graphene oxide (GO) produces various graphene-based carbon materials with different applications. However, the gelation of MXenes, another important type of 2D materials that have different surface chemistry from GO, is difficult to achieve. Here, the first gelation of MXenes in an aqueous dispersion that is initiated by divalent metal ions is reported, where the strong interaction between these ions and OH groups on the MXene surface plays a key role. Typically, Fe2+ ions are introduced in the MXene dispersion which destroys the electrostatic repulsion force between the MXene nanosheets in the dispersion and acts as linkers to bond the nanosheets together, forming a 3D MXene network. The obtained hydrogel effectively avoids the restacking of the MXene nanosheets and greatly improves their surface utilization, resulting in a high rate performance when used as a supercapacitor electrode (≈226 F g-1 at 1 V s-1 ). It is believed that the gelation of MXenes indicates a new way to build various tunable MXene-based structures and develop different applications.

A Nacre-Like Carbon Nanotube Sheet for High Performance Li-Polysulfide Batteries with High Sulfur Loading.

Lithium-sulfur (Li-S) batteries are considered as one of the most promising energy storage systems for next-generation electric vehicles because of their high-energy density. However, the poor cyclic stability, especially at a high sulfur loading, is the major obstacles retarding their practical use. Inspired by the nacre structure of an abalone, a similar configuration consisting of layered carbon nanotube (CNT) matrix and compactly embedded sulfur is designed as the cathode for Li-S batteries, which are realized by a well-designed unidirectional freeze-drying approach. The compact and lamellar configuration with closely contacted neighboring CNT layers and the strong interaction between the highly conductive network and polysulfides have realized a high sulfur loading with significantly restrained polysulfide shuttling, resulting in a superior cyclic stability and an excellent rate performance for the produced Li-S batteries. Typically, with a sulfur loading of 5 mg cm-2, the assembled batteries demonstrate discharge capacities of 1236 mAh g-1 at 0.1 C, 498 mAh g-1 at 2 C and moreover, when the sulfur loading is further increased to 10 mg cm-2 coupling with a carbon-coated separator, a superhigh areal capacity of 11.0 mAh cm-2 is achieved.