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Highlights The interfacing between SnO2 and MXene alters electronic structures, shifting the d-band center in transition metals, enhancing catalytic efficiency by reducing electron filling in antibonding orbitals. A binder-free, ultrathin, laminar heterostructured interlayer on polypropylene separator is demonstrated. The ionic sieving mechanism and efficient adsorption–catalysis process enable deeper charge/discharge cycle and improved stability. The improved catalytic conversion and suppressed lithium dendrites formation enable a high loading of 7.5 mg cm−2 and an initial area capacity of 7.6 mAh cm−2.

Abstract As the demand for photovoltaic technologies continues to grow, the quest for efficient and sustainable transparent conducting electrodes (TCEs) rapidly rises. Traditional solutions, such as indium tin oxide (ITO), face challenges related to indium scarcity and environmental impact. To tackle these issues, a novel metal mesh rear TCE consisting of gold micro‐meshes is developed as ITO replacement in perovskite solar cells (PSCs). This study reveals that optimized Au meshes can guarantee 75% of the extracted photocurrent compared to reference devices with ITO and a promising power conversion efficiency (PCE) of 8.65%. By utilizing hybrid mesh structures with a 10‐nm ITO layer, the PCE further improves to 12.1%, with the extracted current exceeding 80% of the reference. Metal meshes can even serve to replace the opaque metal contact of PSCs, amplifying their functionality and efficiency through bifacial and multi‐junction applications. Here, aerosol jet‐printed silver meshes serve as front electrodes, combined with either 5–10 nm of Au, achieving efficient semi‐transparent devices (PCE 16.8%), or with 5–10 nm of ITO, providing enhanced bifacial properties while maintaining competitive efficiency. Overall, this work highlights remarkable features of metal meshes, making them promising alternatives to commonly used TCEs in optoelectronic applications.

Mass spectroscopy (MS) is a robust technique for polymer characterization, and it can provide the chemical fingerprint of a complete sample regarding polymer distribution chains. Nevertheless, polymer chemical properties such as polydispersity (Pd), average molecular mass (Mn), weight average molecular mass (Mw) and others are not determined by MS, as they are commonly characterized by gel permeation chromatography (GPC). In order to calculate polymer properties from MS, a Python script was developed to interpret polymer properties from spectroscopic raw data. Polypy script can be considered a peak detection and area distribution method, and represents the result of combining the MS raw data filtered using Root Mean Square (RMS) calculation with molecular classification based on theoretical molar masses. Polypy filters out areas corresponding to repetitive units. This approach facilitates the identification of the polymer chains and calculates their properties. The script also integrates visualization graphic tools for data analysis. In this work, aryl resin (poly(2,2-bis(4-oxy-(2-(methyloxirane)phenyl)propan) was the study case polymer molecule, and is composed of oligomer chains distributed mainly in the range of dimers to tetramers, in some cases presenting traces of pentamers and hexamers in the distribution profile of the oligomeric chains. Epoxy resin has Mn = 607 Da, Mw = 631 Da, and polydispersity (Pd) of 1.015 (data given by GPC). With Polypy script, calculations resulted in Mn = 584.42 Da, Mw = 649.29 Da, and Pd = 1.11, which are consistent results if compared with GPC characterization. Additional information, such as the percentage of oligomer distribution, was also calculated and for this polymer matrix it was not possible to retrieve it from the GPC method. Polypy is an approach to characterizing major polymer chemical properties using only MS raw spectra, and it can be utilized with any MS raw data for any polymer matrix.

Abstract Two‐dimensional (2D) transition metal carbides, and/or nitrides, so‐called MXenes, have triggered intensive research interests in applications ranging from electrochemical energy storage to electronics devices. Producing these functional devices by printing necessitates to match the rheological properties of MXene dispersions to the requirements of various solution processing techniques. In particular, for additive manufacturing such as extrusion‐printing, MXene inks with high solid fraction are typically required, which is commonly achieved by tediously removing excessive free water (top‐down route). Here, the study reports on a bottom‐up route to reach a highly concentrated binary MXene‐water blend, so‐called MXene dough, by controlling the water admixture to freeze‐dried MXene flakes by exposure to water mist. The existence of a critical threshold of MXene solid content (≈60%), beyond which no dough is formed, or formed with compromised ductility is revealed. Such metallic MXene dough possesses high electrical conductivity, excellent oxidation stability, and can withstand a couple of months without apparent decay, providing that the MXene dough is properly stored at low‐temperature with suppressed dehydration environment. Solution processing of the MXene dough into a micro‐supercapacitor with gravimetric capacitance of 161.7 F g−1 is demonstrated. The impressive chemical and physical stability/redispersibility of MXene dough indicate its great promise in future commercialization.

The properties of 2D materials are unparalleled when compared to their 3D counterparts; many of these properties are a consequence of their size reduction to only a couple of atomic layers. Metallic, semiconducting, and insulating types can be found and form a platform for a new generation of devices. Among the possible methods to utilize 2D materials, functional printing has emerged as a strong contender because inks can be directly formulated from dispersions obtained by liquid‐phase exfoliation. Printed graphene‐based devices are shifting from laboratory applications toward real‐world and mass‐producible systems going hand in hand with a good understanding of suitable exfoliation methods for the targeted type of ink. Such a clear picture does not yet exist for hexagonal boron nitride (h‐BN), the transition metal dichalcogenides (TMDs), and black phosphorous (BP). Rather, reports of applications of these 2D materials in printed devices are scattered throughout the literature, not yet adding to a comprehensive and full understanding of the relevant parameters. This perspective starts with a summary of the most important features of inks from exfoliated graphene. For h‐BN, the TMDs, and BP, the characteristic properties when exfoliated from solution and strategies to formulate inks are summarized.

Abstract Rechargeable lithium‐sulfur (Li‐S) batteries have attracted significant research attention due to their high capacity and energy density. However, their commercial applications are still hindered by challenges such as the shuttle effect of soluble lithium sulfide species, the insulating nature of sulfur, and the fast capacity decay of the electrodes. Various efforts are devoted to address these problems through questing more conductive hosts with abundant polysulfide chemisorption sites, as well as modifying the separators to physically/chemically retard the polysulfides migration. Two dimensional transition metal carbides, carbonitrides and nitrides, so‐called MXenes, are ideal for confining the polysulfides shuttling effects due to their high conductivity, layered structure as well as rich surface terminations. As such, MXenes have thus been widely studied in Li‐S batteries, focusing on the conductive sulfur hosts, polysulfides interfaces, and separators. Therefore, in this review, we summarize the significant progresses regarding the design of multifunctional MXene‐based Li‐S batteries and discuss the solutions for improving electrochemical performances in detail. In addition, challenges and perspectives of MXenes for Li‐S batteries are also outlined.

An aerosol jet printing (AJP) printing head built on top of precise motion systems can provide positioning deviation down to 3 μm, printing areas as large as 20 cm × 20 cm × 30 cm, and five-axis freedom of movement. Typical uses of AJP are 2D printing on complex or flexible substrates, primarily for applications in printed electronics. Nearly all commercially available AJP inks for 2D printing are designed and optimized to reach desired electronic properties. In this work, we explore AJP for the 3D printing of free-standing pillar arrays. We utilize aryl epoxy photopolymer as ink coupled with a cross-linking “on the fly” technique. Pillar structures 550 μm in height and with a diameter of 50 μm were 3D printed. Pillar structures were characterized via scanning electron microscopy, where the morphology, number of printed layers and side effects of the AJP technique were investigated. Satellite droplets and over-spray seem to be unavoidable for structures smaller than 70 μm. Nevertheless, reactive ion etching (RIE) as a post-processing step can mitigate AJP side effects. AJP-RIE together with photopolymer-based ink can be promising for the 3D printing of microstructures, offering fast and maskless manufacturing without wet chemistry development and heat treatment post-processing.

The efficiency of ternary organic solar cells relies on the spontaneous establishment of a nanostructured network of donor and acceptor phases during film formation. A fundamental understanding of phase composition and arrangement and correlations to photovoltaic device parameters is of utmost relevance for both science and technology. We demonstrate a general approach to understanding solar cell behavior from simple thermodynamic principles. For two ternary blend systems we construct and model phase diagrams. Details of EQE and solar cell parameters can be understood from the phase behavior. Our blend system is composed of PC70BM, PBDTTT-C and a near-infrared absorbing cyanine dye. Cyanine dyes are accompanied by counterions, which, in a first approximation, do not change the photophysical properties of the dye, but strongly influence the morphology of the ternary blend. We argue that counterion dissociation is responsible for different mixing behavior. For the dye with a hexafluorophosphate counterion a hierarchical morphology develops, the dye phase separates on a large scale from PC70BM and cannot contribute to photocurrent. Differently, a cyanine dye with a TRISPHAT counterion shows partial miscibility with PC70BM. A large two-phase region dictated by the PC70BM: PBDTTT-C mixture is present and the dye greatly contributes to the short-circuit current.

Abstract Supramolecular assemblies from organic dyes forming J‐aggregates are known to exhibit narrowband photoluminescence with full‐width at half maximum of ≈9 nm (260 cm−1). Applications of these high color purity emitters, however, are hampered by the rather low photoluminescence quantum yields reported for cyanine J‐aggregates, even when formed in solution. Here, it is demonstrated that cyanine J‐aggregates can reach an order of magnitude higher photoluminescence quantum yield (increase from 5% to 60%) in blend solutions of water and alkylamines at room temperature. By means of time‐resolved photoluminescence studies, an increase in the exciton lifetime as a result of the suppression of non‐radiative processes is shown. Small‐angle neutron scattering studies suggest a necessary condition for the formation of such highly emissive J‐aggregates: the presence of a sharp water/amine interface for J‐aggregate assembly and the coexistence of nanoscale‐sized water and amine domains to restrict the J‐aggregate size and solubilize monomers, respectively.

Abstract Designing lightweight nanostructured aerogels for high‐performance electromagnetic interference (EMI) shielding is crucial yet challenging. Ultrathin cellulose nanofibrils (CNFs) are employed for assisting in building ultralow‐density, robust, and highly flexible transition metal carbides and nitrides (MXenes) aerogels with oriented biomimetic cell walls. A significant influence of the angles between oriented cell walls and the incident EM wave electric field direction on the EMI shielding performance is revealed, providing an intriguing microstructure design strategy. MXene “bricks” bonded by CNF “mortars” of the nacre‐like cell walls induce high mechanical strength, electrical conductivity, and interfacial polarization, yielding the resultant MXene/CNF aerogels an ultrahigh EMI shielding performance. The EMI shielding effectiveness (SE) of the aerogels reaches 74.6 or 35.5 dB at a density of merely 8.0 or 1.5 mg cm–3, respectively. The normalized surface specific SE is up to 189 400 dB cm2 g–1, significantly exceeding that of other EMI shielding materials reported so far.

Tinted and colour-neutral semitransparent organic photovoltaic elements are of interest for building-integrated applications in windows, on glass roofs or on facades. We demonstrate a semitransparent organic photovoltaic cell with a dry-laminated top electrode that achieves a uniform average visible transmittance of 51% and a power conversion efficiency of 3%. The photo-active material is based on a majority blend composed of a visibly absorbing donor polymer and a fullerene acceptor, to which a selective near-infrared absorbing cyanine dye is added as a minority component. Our results show that organic ternary blends are attractive for the fabrication of semitransparent solar cells in general, because a guest component with a complementary absorption can compensate for the inevitably reduced current generation capability of a high-performing binary blend when applied as a thin, semitransparent film.

Simple bilayer organic solar cells rely on very thin coated films that allow for effective light absorption and charge carrier transport away from the heterojunction at the same time. However, thin films are difficult to coat on rough substrates or over large areas, resulting in adverse shorting and low device fabrication yield. Chemical p-type doping of organic semiconductors can reduce Ohmic losses in thicker transport layers through increased conductivity. By using a Co(III) complex as chemical dopant, we studied doped cyanine dye/C60 bilayer solar cell performance for increasing dye film thickness. For films thicker than 50 nm, doping increased the power conversion efficiency by more than 30%. At the same time, the yield of working cells increased to 80%. We addressed the fate of the doped cyanine dye, and found no influence of doping on solar cell long term stability.

Most all-organic solar cells rely on undoped electron donor–acceptor heterojunctions. Power-conversion efficiencies depend critically on the photoinduced charge generation at these interfaces such as the charge transport through the layers and collection at the electrodes. Hence, the ability to regulate and control these processes would offer advanced device functionality. Mobile ions are able to create internal electric fields similar to conventional, electronic p-n junctions without having the inconvenience of doping, which often leads to carrier recombination and excited state quenching. We demonstrate that at organic heterointerfaces these ionic junctions can shift the electronic orbital energy level, which allows the direction of electron transfer processes to be controlled. Cationic cyanine dyes offer a convenient model system to study the effect of mobile ions systematically. In conjunction with usually strong electron acceptors such as the Buckminsterfullerene C60, and donors such as the poly(p-phenylenevinylene) derivative MEH-PPV, we fabricated bilayer photovoltaic devices to reveal exciting effects due to ionic interfacial space charge. For example, we show that C60 can be turned into an electron donor. Furthermore, oxidative or reductive electron transfer processes can simply be switched on and off with an applied bias, thereby drastically altering device performance and spectral sensitivity.

The controlled fabrication of submicrometer phase-separated morphologies of semiconducting organic materials is attracting considerable interest, for example, in emerging thin-film optoelectronic device applications. For thin films of spin-coated blends of PCBM ([6,6]-phenyl-C 61-butyric acid methyl ester) and cationic cyanine dyes, we used atomic force microscopy scans to infer the structure formation mechanism: The solutions separate into transient bilayers, which further spinodally destabilize because of long-range molecular interactions. A thin layer ruptures earlier than a thick layer, and the earlier instability determines the morphology. Consequently, the resulting morphology type mainly depends on the ratio of the layer thicknesses, whereas the periodicity of structures is determined by the absolute film thickness. These findings allow control of the feature sizes, and nodular domains with diameters well below 50 nm were produced. Films prepared with dyes possessing a mobile counterion were always unstable. To rationalize the findings, we developed a thermodynamic model showing that electrostatic forces induced by the mobile counterions act as destabilizing pressure. [ABSTRACT FROM AUTHOR]