MXenes with metallic conductivity, high pseudo-capacitance and 2D structure, are promising flexible electrode materials for supercapacitors, but suffer from the restacking issue, which hinders ion accessibility and causes sluggish ion kinetics. Herein, a simple in situ ice template strategy is proposed to fabricate free-standing, flexible 3D porous Ti 3 C 2 T x /carbon nanotubes (CNTs) film (3D-PMCF) by freeze-drying Ti 3 C 2 T x-based hydro-films without any postprocessing. During the freeze-drying process, small ice grains are in situ transformed from the residual water molecules in the Ti 3 C 2 T x interlayer and then act as a self-sacrifice template to construct a 3D porous network. CNTs introduced in the hydro-film increase the amount of interlayer water and the resultant porosity. The 3D structure of Ti 3 C 2 T x significantly increases the exposed surface active sites and accelerates the ion transport, meanwhile maintaining good flexibility. Consequently, the flexible 3D-PMCF film delivers a capacitance of 375 F g −1 at 5 mV s −1 and retains 251.2 F g −1 at 1000 mV s −1 with excellent cycling stability, much superior to the conventional densely stacked Ti 3 C 2 T x film. Being assembled into a symmetric supercapacitor, an energy density of 9.2 Wh kg −1 is realized. This work demonstrates a simple and efficient route for constructing high-performance and flexible 3D MXene film electrodes for supercapacitors.

Alloy nanoparticles are important in many fields, including catalysis, plasmonics, and electronics, due to the chemical and physical properties that arise from the interactions between their components. Typically, alloy nanoparticles are made by solution-based synthesis; however, scanning-probe-based methods offer the ability to make and position such structures on surfaces with nanometer-scale resolution. In particular, scanning probe block copolymer lithography (SPBCL), which combines elements of block copolymer lithography with scanning probe techniques, allows one to synthesize nanoparticles with control over particle diameter in the 2-50 nm range. Thus far, single-element structures have been studied in detail, but, in principle, one could make a wide variety of multicomponent systems by controlling the composition of the polymer ink, polymer feature size, and metal precursor concentrations. Indeed, it is possible to use this approach to synthesize alloy nanoparticles comprised of combinations of Au, Ag, Pd, Ni, Co, and Pt. Here, such structures have been made with diameters deliberately tailored in the 10-20 nm range and characterized by STEM and EDS for structural and elemental composition. The catalytic activity of one class of AuPd alloy nanoparticles made via this method was evaluated with respect to the reduction of 4-nitrophenol with NaBH4. In addition to being the first catalytic studies of particles made by SPBCL, these proof-of-concept experiments demonstrate the potential for SPBCL as a new method for studying the fundamental science and potential applications of alloy nanoparticles in areas such as heterogeneous catalysis.

The development of a lithographic method that can rapidly define nanoscale features across centimeter-scale surfaces has been a long standing goal of the nanotechnology community. If such a ‘desktop nanofab’ could be implemented in a low-cost format, it would bring the possibility of point-of-use nanofabrication for rapidly prototyping diverse functional structures. Here we report the development of a new tool that is capable of writing arbitrary patterns composed of diffraction-unlimited features over square centimeter areas that are in registry with existing patterns and nanostructures. Importantly, this instrument is based on components that are inexpensive compared to the combination of state-of-the-art nanofabrication tools that approach its capabilities. This tool can be used to prototype functional electronic devices in a mask-free fashion in addition to providing a unique platform for performing high throughput nano- to macroscale photochemistry with relevance to biology and medicine.

Complex-oxide interfaces host a diversity of phenomena not present in traditional semiconductor heterostructures. Despite intense interest, many basic questions remain about the mechanisms that give rise to interfacial conductivity and the role of surface chemistry in dictating these properties. Here we demonstrate a fully reversible >4 order of magnitude conductance change at LaAlO3/SrTiO3 (LAO/STO) interfaces, regulated by LAO surface protonation. Nominally conductive interfaces are rendered insulating by solvent immersion, which deprotonates the hydroxylated LAO surface; interface conductivity is restored by exposure to light, which induces reprotonation via photocatalytic oxidation of adsorbed water. The proposed mechanisms are supported by a coordinated series of electrical measurements, optical/solvent exposures, and X-ray photoelectron spectroscopy. This intimate connection between LAO surface chemistry and LAO/STO interface physics bears far-reaching implications for reconfigurable oxide nanoelectronics and raises the possibility of novel applications in which electronic properties of these materials can be locally tuned using synthetic chemistry.

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