Layered perovskites with the formula (R-NH)PbI have excellent environmental stability but poor photovoltaic function due to the preferential orientation of the semiconducting layer parallel to the substrate and the typically insulating nature of the R-NH cation. Here, we report a series of these n = 1 layered perovskites with the form (aromatic- O-linker-NH)PbI where the aromatic moiety is naphthalene, pyrene, or perylene and the linker is ethyl, propyl, or butyl. These materials achieve enhanced conductivity perpendicular to the inorganic layers due to better energy level matching between the inorganic layers and organic galleries. The enhanced conductivity and visible absorption of these materials led to a champion power conversion efficiency of 1.38%, which is the highest value reported for any n = 1 layered perovskite, and it is an order of magnitude higher efficiency than any other n = 1 layered perovskite oriented with layers parallel to the substrate. These findings demonstrate the importance of leveraging the electronic character of the organic cation to improve optoelectronic properties and thus the photovoltaic performance of these chemically stable low n layered perovskites.

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The design of soft matter in which internal fuels or an external energy input can generate locomotion and shape transformations observed in living organisms is a key challenge. Such materials could assist in productive functions that may range from robotics to smart management of chemical reactions and communication with cells. In this context, hydrated matter that can function in aqueous media would be of great interest. Here, we report the design of hydrogels containing a scaffold of high–aspect ratio ferromagnetic nanowires with nematic order dispersed in a polymer network that change shape in response to light and experience torques in rotating magnetic fields. The synergistic response enables fast walking motion of macroscopic objects in water on either flat or inclined surfaces and also guides delivery of cargo through rolling motion and light-driven shape changes. The theoretical description of the response to the external energy input allowed us to program specific trajectories of hydrogel objects that were verified experimentally.

Iron-incorporated nickel-based materials show promise as catalysts for the oxygen evolution reaction (OER) halfreaction of water electrolysis. Nickel has also exhibited high catalytic activity for methanol oxidation, particularly when in the form of a bimetallic catalyst. In this work, bimetallic iron−nickel nanoparticles were synthesized using a multistep procedure in water under ambient conditions. When compared to monometallic iron and nickel nanoparticles, Fe−Ni nanoparticles show enhanced catalytic activity for both OER and methanol oxidation under alkaline conditions. At 1 mA/cm 2 , the overpotential for monometallic iron and nickel nanoparticles was 421 and 476 mV, respectively, while the bimetallic Fe−Ni nanoparticles had a greatly reduced overpotential of 256 mV. At 10 mA/cm 2 , bimetallic Fe−Ni nanoparticles had an overpotential of 311 mV. Spectroscopy characterization suggests that the primary phase of nickel in Fe−Ni nanoparticles is the more disordered alpha phase of nickel hydroxide.

Skeletal muscle provides inspiration on how to achieve reversible, macroscopic, anisotropic motion in soft materials. Here we report on the bottom-up design of macroscopic tubes that exhibit anisotropic actuation driven by a thermal stimulus. The tube is built from a hydrogel in which extremely long supramolecular nanofibers are aligned using weak shear forces, followed by radial growth of thermoresponsive polymers from their surfaces. The hierarchically ordered tube exhibits reversible anisotropic actuation with changes in temperature, with much greater contraction perpendicular to the direction of nanofiber alignment. We identify two critical factors for the anisotropic actuation, macroscopic alignment of the supramolecular scaffold and its covalent bonding to polymer chains. Using finite element analysis and molecular calculations, we conclude polymer chain confinement and mechanical reinforcement by rigid supramolecular nanofibers are responsible for the anisotropic actuation. The work reported suggests strategies to create soft active matter with molecularly encoded capacity to perform complex tasks.

Liquid crystalline hydrogels are an attractive class of soft materials to direct charge transport, mechanical actuation, and cell migration. When such systems contain supramolecular polymers, it is possible in principle to easily shear align nanoscale structures and create bulk anisotropic properties. However, reproducibly fabricating and patterning aligned supramolecular domains in 3D hydrogels remains a challenge using conventional fabrication techniques. Here, a method is reported for 3D printing of ionically crosslinked liquid crystalline hydrogels from aqueous supramolecular polymer inks. Using a combination of experimental techniques and molecular dynamics simulations, it is found that pH and salt concentration govern intermolecular interactions among the self‐assembled structures where lower charge densities on the supramolecular polymers and higher charge screening from the electrolyte result in higher viscosity inks. Enhanced hierarchical interactions among assemblies in high viscosity inks increase the printability and ultimately lead to greater nanoscale alignment in extruded macroscopic filaments when using small nozzle diameters and fast print speeds. The use of this approach is demonstrated to create materials with anisotropic ionic and electronic charge transport as well as scaffolds that trigger the macroscopic alignment of cells due to the synergy of supramolecular self‐assembly and additive manufacturing.

In energy storage materials, large surface areas and oriented structures are key architecture design features for improving performance through enhanced electrolyte access and efficient electron conduction pathways. Layered hydroxides provide a tunable materials platform with opportunities for achieving such nanostructures via bottom-up syntheses. These nanostructures, however, can degrade in the presence of the alkaline electrolytes required for their redox-based energy storage. A layered Co(OH) 2 -organic hybrid material that forms a hierarchical structure consisting of micrometerlong, 30 nm diameter tubes with concentric curved layers of Co(OH) 2 and 1-pyrenebutyric acid is reported. The nanotubular structure offers high surface area as well as macroscopic orientation perpendicular to the substrate for efficient electron transfer. Using a comparison with flat films of the same composition, it is demonstrated that the superior performance of the nanotubular films is the result of a large accessible surface area for redox activity. It is found that the organic molecules used to template nanotubular growth also impart stability to the hybrid when present in the alkaline environments necessary for redox function.supercapacitors that store energy through electric double-layer capacitance (EDLC) in symmetric carbon-based electrodes have only limited energy density compared to currently used batteries. There has been growing interest recently in asymmetric supercapacitors that utilize high-performance EDLC anodes, [6,7] in conjunction with faradaic cathodes that undergo redox reactions and thus have much larger energy densities. [8][9][10] Among the materials investigated for cathodes, cobalt(II) hydroxide (Co(OH) 2 ) is a particularly promising candidate due to its high theoretical specific capacity and electrical conductivity. [11][12][13] This metal hydroxide is known to form a crystalline layered structure that facilitates ion transport, and in the presence of an oxidizing potential and hydroxide ions it will transform into a cobalt(III) oxyhydroxide (CoOOH) phase. [14] This charging transformation is easily reversible in a discharge process that reduces the oxyhydroxide back to the original cobalt hydroxide. This redox reaction offers the potential for high energy storage density and rapid charge/discharge cycles, the two attributes that define a supercapacitive material. While the operating voltage window for Co(OH) 2 electrodes is limited to ≈0.5 V, solid-state asymmetric supercapacitor devices utilizing Co(OH) 2 -based cathodes and EDLC anodes have demonstrated stable potential windows of 1.2 and 1.8 V. [15,16] This electrode Energy Storage

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