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Function convergence of gas sensing and neuromorphic computing is attracting much research attention due to the promising potential in electronic olfactory, artificial intelligence, and internet of everything systems. However, the current neuromorphic gas-sensing systems are either realized via integration of gas detectors and neuromorphic devices or operating with three-terminal synaptic transistors at high voltages, leading to a rather high system complexity or power consumption. Herein, gas-modulated synaptic diodes with lateral structures are developed to converge sensing, processing, and storage functions into a single device. The lateral synaptic diode is based on a p-n junction of an organic semiconductor (OSC) and amorphous In-Ga-Zn-O, in which the upper OSC layer can directly interact with the gas molecules in the atmosphere. Typical synaptic behaviors triggered by ammonia, including inhibitory postsynaptic current and paired-pulse depression, are successfully demonstrated. Meanwhile, a low power consumption of 6.3 pJ per synaptic event has been achieved, which benefits from the simple device structure, the decent chemosensitivity of the OSC, and the low operation voltage. A simulated ammonia analysis in human exhaled breath is further conducted to explore the practical application of the synaptic diode. Therefore, this work provides a gas-modulated synaptic diode for circuit-compact and power-efficient artificial olfactory systems.

Ag2S nanoparticles are the staple for high-resolution preclinical imaging and sensing owing to their photochemical stability, low toxicity, and photoluminescence (PL) in the second near-infrared biological window. Unfortunately, Ag2S nanoparticles exhibit a low PL efficiency attributed to their defective surface chemistry, which curbs their translation into the clinics. To address this shortcoming, we present a simple methodology that allows to improve the PL quantum yield from 2 to 10%, which is accompanied by a PL lifetime lengthening from 0.7 to 3.8 μs. Elemental mapping and X-ray photoelectron spectroscopy indicate that the PL enhancement is related to the partial removal of sulfur atoms from the nanoparticle’s surface, reducing surface traps responsible for nonradiative de-excitation processes. This interpretation is further backed by theoretical modeling. The acquired knowledge about the nanoparticles’ surface chemistry is used to optimize the procedure to transfer the nanoparticles into aqueous media, obtaining water-dispersible Ag2S nanoparticles that maintain excellent PL properties. Finally, we compare the performance of these nanoparticles with other near-infrared luminescent probes in a set of in vitro and in vivo experiments, which demonstrates not only their cytocompatibility but also their superb optical properties when they are used in vivo, affording higher resolution images.

Polymer-derived SiBCN ceramics (PDCs-SiBCN) are promising ultrahigh-temperature ceramics owing to their excellent high-temperature oxidation resistance and electromagnetic wave (EMW)-absorbing capa...

Metallic lithium is one of the most promising anode materials to build next generation electrochemical power sources such as Li-air, Li-sulfur, and solid-state lithium batteries. The implementation of rechargeable Li-based batteries is plagued by issues including dendrites, pulverization, and an unstable solid electrolyte interface (SEI). Herein, we report the use of nanostructured CuO in situ grown on commercial copper foil (CuO@Cu) via chemical etching as a Li-reservoir substrate to stabilize SEI formation and Li stripping/plating. The lithiophilic interconnected CuO layer enhances electrolyte wettability. Besides, a mechanically stable Li2O- and LiF-rich SEI is generated on CuO@Cu during initial discharge, which permits dense and uniform lithium deposition upon subsequent cycling. Compared with bare Cu, the CuO@Cu electrode exhibits superior performance in terms of Coulombic efficiency, discharge/charge overpotentials, and cyclability. By pairing with the Li-CuO@Cu anodes, full cells with LiFePO4 and LiNi1/3Mn1/3Co1/3O2 cathodes sustain 300 cycles with 98.8% capacity retention at 1 C and deliver a specific capacity of 80 mAh g-1 at 10 C, respectively. This work would shed light on the design of advanced current collectors with SEI modulation to upgrade lithium anodes.

Thiocyanate-based perovskite (SCN-PVSK) photodetectors have been fabricated by introducing lead thiocyanate precursor. Incorporating SCN groups into CH3NH3PbI3 can significantly improve the device stability in air. Compared with pure CH3NH3PbI3 films, SCN-PVSK films have larger grain size and reduced trap states. The perovskite layers can be prepared by a simple solution method in air. Solvent effects on the crystallization of SCN-PVSK films have also been investigated. It is found that highly uniform, pinhole-free perovskite films can be obtained utilizing the N,N-dimethylformamide (DMF) solution of Pb(SCN)2. The SCN-PVSK based photodetectors performed a high responsivity of 12.3 A/W and a decent detectivity over 1.3 × 1013 Jones. More important, the SCN-PVSK based two-terminal photodetectors, without encapsulation, have shown great stability with 92% of the initial photocurrent being retained after storage in air (relative humidity >50%) for 10 days, whereas the value is only 10% for pure CH3NH3PbI3 devices tested under the same conditions.

Bacterial vaccines have been widely used to prevent infectious diseases, especially in veterinary medicine. Although there are many reports on bacterin adjuvants, only a few contain innovations in bacterin adjuvants. Taking this into consideration, in this study we designed and synthesized a new aluminum (oxy) hydroxide (AlOOH) nanorod (Al-NR) with a diameter of 200 ± 80 nm and a length of 1.1 ± 0.6 μm. Using whole- Pseudomonas aeruginosa PAO1 as antigens, we showed that the bacterial antigens of P. aeruginosa PAO1 adsorbed on the Al-NRs induced a quick and stronger antigen-specific antibody response than those of the other control groups, especially in the early stage of immunization. Furthermore, the level of antigen-specific IgG was approximately 4-fold higher than that of the no adjuvant group and 2.5-fold higher than those of other adjuvant groups in the first week after the initial immunization. The potent adjuvant activity of the Al-NRs was attributed to the rapid presentation of antigen adsorbed on them by APCs. Additionally, Al-NRs induced a milder local inflammation than the other adjuvants. In short, we confirmed that Al-NRs, enhancing both humoral and cellular immune responses, are a potentially promising vaccine adjuvant delivery system for inhibiting the whole- Pseudomonas aeruginosa infection.

As a novel molecular and functional imaging modality, X-ray luminescence computed tomography (XLCT) has shown its potentials in biomedical and preclinic applications. However, there are still some limitations of X-ray-excited luminescent materials, such as low luminescence efficiency, poor biocompatibility, and cytotoxicity, making in vivo XLCT imaging quite challenging. In this study, for the very first time, we present on using sub-10 nm β-NaGdF4:X% Eu3+ nanoparticles with poly(acrylic acid) (PAA) surface modification, which demonstrate outstanding luminescence efficiency, uniform size distribution, water dispersity, and biosafety, as the luminescent probes for in vivo XLCT application. The pure hexagonal phase (β-) NaGdF4 has been successfully synthesized and characterized by X-ray powder diffraction (XRD) and transmission electron microscopy (TEM), and then the results of X-ray photoelectron spectroscopy (XPS), energy-dispersive X-ray spectrometry (EDX), and elemental mapping further confirm Eu3+ ion...

Stimuli-sensitive hydrogels are ideal candidates for biomedical and bioengineering purposes, although applications of hydrogels may be limited, due in part to the limited choice of suitable materials for constructing hydrogels, the complexity in the synthesis of the source materials, and the undesired fast-then-slow drug-release behaviors of usual hydrogels. Herein, we describe the fabrication of a new supramolecular guanosine (G)-quadruplex hydrogel by multicomponent self-assembly of endogenous guanosine (G), 2-formylboronic acid (2-FPBA), and tris(2-aminoethyl)amine (TAEA) in the presence of KCl in an easy and convenient way. The features of the G-quadruplex hydrogel include (1) versatility and commercial availability of building blocks with different functions, (2) dynamic iminoboronate bonds with pH and glucose responsiveness, and (3) zero-order drug-release behavior because of the superficial peel-off of the hydrogel in response to stimuli. The structure, morphology, and properties of the G-quadruplex hydrogel were well-characterized, and satisfactory zero-order drug release was successfully achieved. This kind of supramolecular G-quadruplex hydrogels may find applications in biological fields.

A facile strategy was designed for the in situ synthesis of MoS2 nanospheres on functionalized graphene nanoplates (MoS2@f-graphene) for use as lithium-ion battery anode materials. A modified Birch reduction was used to exfoliate graphite into few-layer graphene followed by modification with functional groups. Compared to the most common approach of mixing MoS2 and reduced graphene oxide, our approach provides a way to circumvent the harsh oxidation and destruction of the carbon basal planes. In this process, alkylcarboxyl functional groups on the functionalized graphene (f-graphene) serve as sites where MoS2 nanospheres crystallize, and thus create bridges between the MoS2 nanospheres and the graphene layers to effectively facilitate electronic transport and to avoid both the aggregation of MoS2 and the restacking of graphene. As anode materials, this unique MoS2@f-graphene heterostructure has a high specific capacity of 1173 mAh g–1 at a current density of 100 mA g–1 and a good rate capacity (910 mAh g–...

CH3NH3PbI3 perovskite-based optoelectronics have attracted intense research interests recently because of their easy fabrication process and high power conversion efficiency. Herein, we report a novel photodetector based on unique CH3NH3PbI3 perovskite films with island-structured morphology. The light-induced electronic properties of the photodetectors were investigated and compared to those devices based on conventional compact CH3NH3PbI3 films. The island-structured CH3NH3PbI3 photodetectors exhibited a rapid response speed (50 ms), good stability at a temperature of up to 100 °C, a large photocurrent to dark current ratio (Ilight/Idark1 × 10(4) under an incident light of ∼6.59 mW/cm(2), and Ilight/Idark1 × 10(2) under low incident light ∼0.018 mW/cm(2)), and excellent reproducibility. Especially, the performance of the island-structured devices markedly exceed that of the conventional compact CH3NH3PbI3 thin-film devices. These excellent performances render the island-structured device to be potentially applicable for a wide range of optoelectronics.

Metal-organic frameworks (MOFs) represent an emerging class of crystalline materials with well-defined pore structures and hold great potentials in a wide range of important applications. The functionality of MOFs can be further extended by integration with other functional materials, e.g., encapsulating metal nanoparticles, to form hybrid materials with novel properties. In spite of various synthetic approaches that have been developed recently, a facile method to prepare hierarchical hollow MOF nanostructures still remains a challenge. Here we describe a facile emulsion-based interfacial reaction method for the large-scale synthesis of hollow zeolitic imidazolate framework 8 (ZIF-8) nanospheres with controllable shell thickness. We further demonstrate that functional metal nanoparticles such as Pd nanocubes can be encapsulated during the emulsification process and used for heterogeneous catalysis. The inherently porous structure of ZIF-8 shells enables encapsulated catalysts to show size-selective hydrogenation reactions.

Porous cubic Cu microparticles were synthesized by a facile solvothermal method using Cu(CH3COO)(2)center dot H2O as the Cu precursor and NaOH in a solution containing ethanol, ethylene glycol, and water. The synthesis conditions were investigated and a growth process of porous cubic Cu microparticles was proposed. The catalytic properties of the porous Cu microparticles as model copper catalysts for Rochow reaction were explored. The samples were characterized by X-ray diffraction, scanning electron microscopy, transmission electron microscopy, thermogravimetric analysis, temperature-programmed reduction, and nitrogen adsorption. It was found that the morphology and structure of the porous cubic Cu microparticles are highly dependent on the reaction time and temperature as well as on the amount of reactants added. Compared to the commercial Cu microparticles with irregular morphology and dense internal structure, porous cubic Cu microparticles show much higher dimethyldichlorosilane selectivity and Si conversion via Rochow reaction, which are attributed to the enhanced formation of active CuxSi phase and gas transportation in the presence of the pore system within microparticles, demonstrating the significance of the pore structure of the copper catalysts in catalytic reactions of organosilane synthesis.

This document is the Accepted Manuscript version of a Published Work that appeared in final form in ACS Applied Materials and Interfaces, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see: https://pubs.acs.org/doi/10.1021/acsami.9b22827, Ag2S semiconductor nanoparticles (NPs) are near-infrared luminescent probes with outstanding properties (good biocompatibility, optimum spectral operation range, and easy biofunctionalization) that make them ideal probes for in vivo imaging. Ag2S NPs have, indeed, made possible amazing challenges including in vivo brain imaging and advanced diagnosis of the cardiovascular system. Despite the continuous redesign of synthesis routes, the emission quantum yield (QY) of Ag2S NPs is typically below 0.2%. This leads to a low luminescent brightness that avoids their translation into the clinics. In this work, an innovative synthetic methodology that permits a 10-fold increment in the absolute QY from 0.2 up to 2.3% is presented. Such an increment in the QY is accompanied by an enlargement of photoluminescence lifetimes from 184 to 1200 ns. The optimized synthetic route presented here is based on a fine control over both the Ag core and the Ag/S ratio within the NPs. Such control reduces the density of structural defects and decreases the nonradiative pathways. In addition, we demonstrate that the superior performance of the Ag2S NPs allows for high-contrast in vivo bioimaging, This work was partially supported by the Ministerio de Economía y Competitividad de España MAT2017-83111R, MAT2016-75362-C3-1-R, RTI2018-094859-B-100, and CTQ2016-76311 by the Comunidad Autónoma de Madrid (B2017/BMD-3867RENIM-CM) and cofinanced by the European Structural and investment fund. Additional funding was provided by the European Commission, Horizon 2020 project NanoTBTech. RCC acknowledges the funding to the Comunidad de Madrid for the “Atracción de Talento” fellowship with reference no. 2018-T1/IND-10736. D.M.-G. thanks UCM-Santander for a postdoctoral contract (CT17/17-CT18/17)