High-energy lithium (Li)-based batteries, especially rechargeable Li-CO2 batteries with CO2 fixation capability and high energy density, are desirable for electrified transportation and other applications. However, the challenges of poor stability, low energy efficiency, and leakage of liquid electrolytes hinder the development of Li-CO2 batteries. Herein, a highly conductive and stable metal-organic framework-encapsulated ionic liquid (IL@MOF) electrolyte system is developed for quasi-solid-state Li-CO2 batteries. Benefiting from the host-guest interaction of MOFs with open micromesopores and internal IL, the optimized IL@MOF electrolytes exhibit a high ionic conductivity of 1.03 mS cm-1 and a high transference number of 0.80 at room temperature. The IL@MOF electrolytes also feature a wide electrochemical stability window (4.71 V versus Li+/Li) and a wide working temperature (-60 °C ∼ 150 °C). The IL@MOF electrolytes also enable Li+ and electrons transport in the carbon nanotubes-IL@MOF (CNT-IL@MOF) solid cathodes in quasi-solid-state Li-CO2 batteries, delivering a high specific capacity of 13,978 mAh g-1 (50 mA g-1), a long cycle life of 441 cycles (500 mA g-1 and 1000 mAh g-1), and a wide operation temperature of -60 to 150 °C. The proposed MOF-encapsulated IL electrolyte system presents a powerful strategy for developing high-energy and highly safe quasi-solid-state batteries.

Flash Joule heating has been used as a versatile solid-state synthesis method in the production of a wide range of products, including organic, inorganic, and ceramic products. Conventional flash Joule heating systems are large and customized, presenting significant barriers in the cost of assembly, the expertise needed to operate, and uniformity of results between different systems. Even laboratory-scale flash Joule heating systems struggle to operate above 10 g capacity, and they suffer from poor temperature controllability. We present here the use of commercial off-the-shelf arc welders as a superior alternative to standard flash Joule heating systems due to their low cost ($120), ease of use, compact size, high temperature controllability, and tunability. We demonstrate the gram-scale synthesis of a variety of organic and ceramic species using these systems. With the addition of another reactor configuration for only $260, we scale up the synthesis of these products to record rates for the laboratory scale, achieving a production rate of 3 kg/h for graphene and kilogram-per-day production rates for SiC, carbon nanotubes, SnSe2, and SnS2.

Photovoltaic devices capable of reversible photovoltaic polarity through external signal modulation may enable multifunctional optoelectronic systems. However, such devices are limited to those induced by gate voltage, electrical poling, or optical wavelength by using complicated device architectures. Here, we show that the photovoltaic polarity is also switchable with the intensity of incident light. The modulation in light intensity induces photovoltaic polarity switching in geometrically asymmetric MoS2 Schottky photodiodes, explained by the asymmetric lowering of the Schottky barrier heights due to the trapping of photogenerated holes at the MoS2/Cr interface states. An applied gate voltage can further modulate the carrier concentration in the MoS2 channel, providing a method to tune the threshold light intensity of polarity switching. Finally, a bidirectional optoelectronic logic gate with "AND" and "OR" functions was demonstrated within a single device.

Chemical exchange saturation transfer magnetic resonance imaging (CEST MRI) enables the imaging of many endogenous and exogenous compounds with exchangeable protons and protons experiencing dipolar coupling by using a label-free approach. This provides an avenue for following interesting molecular events in vivo by detecting the natural protons of molecules, such as the increase in amide protons of proteins in brain tumors and the concentration of drugs reaching the target site. Neither of these detections require metallic or radioactive labels and thus will not perturb the molecular events happening in vivo. Yet, magnetization transfer processes such as chemical exchange and dipolar coupling of protons are sensitive to the local environment. Hence, the use of nanocarriers could enhance the CEST contrast by providing a relatively high local concentration of contrast agents, considering the portion of the protons available for exchange, optimizing the exchange rate, and utilizing molecular interactions. This review provides an overview of these factors to be considered for designing efficient CEST contrast agents (CAs), and the molecular events that can be imaged using CEST MRI during disease progression and treatment, as well as the nanocarriers for drug delivery and distribution for the evaluation of treatments.

Twisted two-dimensional (2D) material heterostructures provide an exciting platform for investigating fundamental physical phenomena. Many of the most interesting behaviors emerge at small twist angles, where the materials reconstruct to form areas of perfectly stacked crystals separated by partial dislocations. However, understanding the properties of these systems is often impossible without correlative imaging of their local reconstructed domain configuration, which exhibits random variations due to disorder and contamination. In particular, visualization of the local domain configuration allows determination of the local twist angle and, hence, the local lattice strain. Here, we demonstrate a simple and widely accessible route to visualize domains in the as-produced twisted transition metal dichalcogenide (TMD) heterostructures using electron channeling contrast imaging (ECCI) in scanning electron microscopy (SEM). This nondestructive approach is compatible with conventional substrates and allows domains to be visualized even when sealed beneath an encapsulation layer. Complementary theoretical calculations reveal how a combination of elastic and inelastic scattering leads to contrast inversions at the specified detector scattering angles and sample tilts. We demonstrate that optimal domain contrast is therefore achieved by maximizing signal collection while avoiding contrast inversion conditions.

Ionic liquids (ILs) are a promising class of electrolytes with a unique combination of properties, such as extremely low vapor pressures and nonflammability. Doping ILs with alkali metal salts creates an electrolyte that is of interest for battery technology. These salt-in-ionic liquids (SiILs) are a class of superconcentrated, strongly correlated, and asymmetric electrolytes. Notably, the transference numbers of the alkali metal cations have been found to be negative. Here, we investigate Na-based SiILs with a surface force apparatus, X-ray scattering, and atomic force microscopy. We find evidence of confinement-induced structural changes, giving rise to long-range interactions. Force curves also reveal an electrolyte structure consistent with our predictions from theory and simulations. The long-range steric interactions in SiILs reflect the high aspect ratio of compressible aggregates at the interfaces rather than the purely electrostatic origin predicted by the classical electrolyte theory. This conclusion is supported by the reported anomalous negative transference numbers, which can be explained within the same aggregation framework. The interfacial nanostructure should impact the formation of the solid electrolyte interphase in SiILs.

The quantum-dot-in-perovskite matrix (DIM) is an emerging class of semiconductors for optoelectronics enabled by their complementary charge transport properties and stability improvements. However, a detailed understanding of the pure electrical properties in DIM is still in its early stage. Here, we developed PbS quantum dot-in-CsSnI3 matrix solids exhibiting improved electrical properties and enhanced stability. PbS incorporation reduces the tensile strain of DIM films compared to that of pristine CsSnI3, consequently increasing the electrical conductivity. Electrical conductivity is tunable between 20 and 130 S/cm as a function of PbS concentration. Notably, a decoupling of electrical conductivity and Seebeck coefficient is observed upon PbS addition into the perovskite matrix, which is attractive for thermoelectric applications. Density functional theory analysis reveals that at low concentrations of PbS, light holes/electrons govern the overall transport properties in DIM, while heavy holes/electrons begin to dominate as the PbS concentration increases. Understanding the electrical properties would help for designing DIMs with specific properties for various technological applications.

Realizing tunable functional materials with built-in nanoscale heat flow directionality represents a significant challenge that could advance thermal management strategies. Here we use spatiotemporally resolved thermoreflectance to visualize lateral thermal transport anisotropy in self-assembled supercrystals of anisotropic Au nanocrystals. Correlative electron and thermoreflectance microscopy reveal that nano- to mesoscale heat predominantly flows along the long-axis of the anisotropic nanocrystals, and does so across grain boundaries and curved assemblies while voids disrupt heat flow. We finely control the anisotropy via the aspect ratio of constituent nanorods, and it exceeds the aspect ratio for nanobipyramid supercrystals and certain nanorod arrangements. Finite element simulations and effective medium modeling rationalize the emergent anisotropic behavior in terms of a simple series resistance model, further providing a framework for estimating thermal anisotropy as a function of material and structural parameters. Self-assembly of colloidal nanocrystals promises an interesting route to direct heat flow in a wide range of applications that utilize this important class of materials.

Silica polymerization from its soluble monomers is fundamental to many chemical processes. Although industrial methods require harsh conditions and concentrated precursors, biological silica precipitation occurs under ambient conditions from dilute solutions. The hallmark of biosilica is the presence of amine-rich organic macromolecules, but their functional role remains elusive. Here, we show a pH-dependent stimulatory effect of such polyamines on silica polymerization. Notably, this process is decoupled from the saturation degree, allowing the synthesis of polymer-silica hybrid products with controlled network morphologies from undersaturated solutions. The data suggest a two-step phase separation process. First, an associative liquid-liquid phase separation forms a micrometer-size dense phase. Second, silica undergoes a liquid-to-solid transition in the supersaturated condensates to form a bicontinuous silica structure. This study can inspire "soft chemistry" routes to design organic-inorganic nanomaterials with regulatory principles optimized by evolution.