bluuebunny/crossref_metadata_2025 huggingface dataset:
Antibacterial Triboelectric Nanogenerator for Mite Removal and Intelligent Human Monitoring
Authors: Lu Yanru , Xiang Huijing , Jie Yang , Cao Xia , Wang Zhong Lin
Published: April 2023

Triboelectric nanogenerators (TENGs) stand out for their wearability, portability, and versatility as a promising energy‐harvesting technology and facilitate their wide self‐powered intelligent applications in various medical fields. However, there are few studies on sterilization and mite removal. Herein, a wearable and antibacterial sandwich‐structured single‐electrode chitosan‐hydroxyethyl cellulose‐pectin (CHP) ‐ polypyrrole (PPy) ‐ CHP( CHP‐PPy‐CHP) triboelectric nanogenerator (CPC‐TENG) by utilizing CHP composite film as the triboelectric layer is proposed and developed. The CPC‐TENG exhibits a maximum short‐circuit current density of 12.99 µA cm−2, resulting in a high instantaneous power of 287 µW during one cycle. It is found that the prepared CPC‐TENG with 11 wt% chitosan fillers has an antibacterial effectiveness of 92.86% against Escherichia coli. Moreover, The CPC‐TENG can be used as a self‐powered human motion monitoring sensor with stable and sensitive response to continuous motion. The antimicrobial and sensing properties of CPC‐TENG demonstrate the enormous potential of the intelligent health monitoring for medical and health.
Long‐Term UV Detecting Wearable Patches Enabled by III‐N Compound Semiconductor‐Based Microphotodetectors
Authors: Kim Jeong Hyeon , Park Sang Yoon , Kim Min Kyoo , Park Woo Hyun , Doh Il , Joe Daniel J. , Lee Han Eol
Published: April 2023

UV radiation is considered indispensable from the hygienic, medical, aesthetic, and industrial perspectives. Among the various types of UV radiation, UV‐A (with a wavelength of 315–400 nm) has a significant influence because it adversely affects human skin, leading to damage such as blemishes, freckles, and wrinkles. Although various photosensors are developed for monitoring UV‐A radiation in real time, these devices have critical issues, such as inefficient fabrication processes, insufficient photoresponsivity, and incompatibility with long‐term wearable applications. Here, the authors report on a wearable UV‐detecting patch targeted for long‐term use in the medical and clinical fields. A wearable UV sensor is fabricated by integrating optimized InGaN/GaN microphotodetectors (µPDs) in a 3D porous patch. The optical and electrical properties of the device are intensively investigated under various types of optical radiation and input electrical power and show high photoresponsivity (2.82 A W−1) and excellent external quantum efficiency (897.63%). Long‐term real‐time UV radiation monitoring using the wearable µPDs is demonstrated; moreover, the by‐products can be efficiently removed from human skin surfaces.
Sulfide, Sulfoxide, and Sulfone Substitution: Electron Structure Modulation from Para‐D‐π‐B to Para‐A‐π‐B in Multiple‐Resonance Emitters with Narrowband Emission and High Color Purity
Authors: Li Yanru , Li Wansi , Hu Jinlian , Yao Xiang , Hua Lei , Cai Wanqing , Shi Shiling , Zhang Chan , Liu Zhongwei , Li Shihua , Chen Xing , Sun Zhe , Ren Zhongjie , Tang Man‐Chung , Wei Guodan , Fei Zhuping
Published: April 2023

Multi‐resonance thermally activated delayed fluorescence (MR‐TADF) emitters have been studied to address the issue of the broadband emission in organic light‐emitting diodes (OLEDs). Herein, the authors have systematically investigated the effect of electron‐donating or ‐withdrawing units in the para position of B atom on the optoelectronic emission modulation BCz‐BN MR‐TADF emitters. Due to the enhanced spin‐orbit coupling (SOC) effect, BN(p)SCH3 with electron structure of para‐D‐π‐B is synthesized by introducing a heavy S atom into the para position of B atom of BCz‐BN. By oxidizing BN(p)SCH3, BN(p)SOCH3 and BN(p)SO2CH3 with electron structure of para‐A‐π‐B have been synthesized. The quantum simulations and photophysical studies have illustrated BN(p)SCH3 can exhibit large reverse intersystem crossing rate constant (kRISC) of 6.4 × 104 s−1 due to the large SOC constants and small singlet‐triplet energy splitting (ΔEST) of 0.12 eV. BN(p)SOCH3 and BN(p)SO2CH3 with electron structure of para‐A‐π‐B displayed red‐shift emissions with smaller full‐width at half‐maximum (FWHM) values of ≈21 nm and kRISC values owing to enhanced ΔEST and the low emission contribution of the triplet excitons in contrast to those of BN(p)SCH3 with electron structure of para‐D‐π‐B. Consequently, BN(p)SCH3‐based OLEDs show highly efficient blue emission with an external quantum efficiency (EQE) of 26.2% and excellent color purity.
Realizing Color‐Tunable and Time‐Dependent Ultralong Afterglow Emission in Antimony‐Doped CsCdCl3 Metal Halide for Advanced Anti‐Counterfeiting and Information Encryption
Authors: Ge Shuaigang , Peng Hui , Wei Qilin , Shen Xiaodong , Huang Weiguo , Liang Weizheng , Zhao Jialong , Zou BingSuo
Published: April 2023

Long afterglow luminescent materials have captured intense attention for their unique applications in biological imaging, photodynamic therapy, and optical anti‐counterfeiting. However, achieving highly efficient and tunable ultralong afterglow emission in all‐inorganic metal halides is an open challenge. Herein, Sb3+‐doped hexagonal CsCdCl3 metal halide is reported via hydrothermal reaction. Upon photoabsorption, the as‐synthesized compounds exhibit dual‐emission bands with a photoluminescence quantum yield (PLQY) of 59.6%, which can be attributed to the self‐trapped exciton emission out of the strong electron‐phonon coupling. After ceasing excitation of 365 nm, bright afterglow emission with the longest duration lasting up to 5000 s is witnessed in Sb3+‐doped CsCdCl3. More importantly, the color‐tunable and time‐dependent ultralong afterglow emission is realized via regulating the doping concentration of Sb3+, which should be due to the trap electrons increase gradually under high doping concentration. Given this unusual afterglow emission characteristics, the optical anti‐counterfeiting and information encryption are constructed based on as‐synthesized compounds. These findings not only help further understand the tunable afterglow emission mechanism in all‐inorganic metal halides, but also provide a new strategy for designing novel ultralong afterglow luminescent materials.
Effects of Opposite Atoms on Electronic Structure and Optical Absorption of Two‐Dimensional Hexagonal Boron Nitride
Authors: Lan You‐Zhao
Published: April 2023

The first‐principles many‐body GW and Bethe–Salpeter equation (BSE) calculations on the 2D hexagonal boron nitride (2D‐hBN) to explore the effects of opposite atoms on the electronic structure and linear one‐photon absorption (OPA) are performed. Five AA‐ and AB‐stacked bilayer and eight AAB‐stacked trilayer structures are considered. The AAB‐stacked trilayer hBN (TL‐BN) structures are constructed by mixing the AA‐ and AB‐stacked bilayer hBN (BL‐BN). It is shown that the GW approximation gives rise to different types (i.e., indirect or direct) of fundamental bandgaps from the independent particle approximation for all structures except those dominated by the B–B opposite. The stacking modes dominated by the B–B opposite have a direct fundamental bandgap in both approximations. The OPA spectra are calculated by solving the BSE combined with the GW quasi‐particle correction. The binding energy and Davydov splitting of excitons of TL‐BN strongly depend on the opposite atoms and are related to the role of the stacking BL‐BN substructure. Finally, taking the six‐layer and below AB‐stacked structures as examples, it is shown that the B–B opposite unit is helpful in constructing the turbostratic‐phase‐like stacking structures with a direct fundamental bandgap which are more suitable for optoelectronic applications.
Trimanganese Tetroxide Nanozyme protects Cartilage against Degeneration by Reducing Oxidative Stress in Osteoarthritis
Authors: Wang Wenhan , Duan Jiazhi , Ma Wenjun , Xia Bowei , Liu Feng , Kong Ying , Li Boyan , Zhao Hang , Wang Liang , Li Keyi , Li Yiwei , Lu Xiheng , Feng Zhichao , Sang Yuanhua , Li Gang , Xue Hao , Qiu Jichuan , Liu Hong
Published: April 2023

Osteoarthritis, a chronic degenerative cartilage disease, is the leading cause of movement disorders among humans. Although the specific pathogenesis and associated mechanisms remain unclear, oxidative stress‐induced metabolic imbalance in chondrocytes plays a crucial role in the occurrence and development of osteoarthritis. In this study, a trimanganese tetroxide (Mn3O4) nanozyme with superoxide dismutase (SOD)‐like and catalase (CAT)‐like activities is designed to reduce oxidative stress‐induced damage and its therapeutic effect is investigated. In vitro, Mn3O4 nanozymes are confirmed to reprogram both the imbalance of metabolism in chondrocytes and the uncontrolled inflammatory response stimulated by hydrogen peroxide. In vivo, a cross‐linked chondroitin sulfate (CS) hydrogel is designed as a substrate for Mn3O4 nanozymes to treat osteoarthritis in mouse models. As a result, even in the early stage of OA (4 weeks), the therapeutic effect of the Mn3O4@CS hydrogel is observed in both cartilage metabolism and inflammation. Moreover, the Mn3O4@CS hydrogel maintained its therapeutic effects for at least 7 days, thus revealing a broad scope for future clinical applications. In conclusion, these results suggest that the Mn3O4@CS hydrogel is a potentially effective therapeutic treatment for osteoarthritis, and a novel therapeutic strategy for osteoarthritis based on nanozymes is proposed.
Multiple Valence Bands Convergence and Localized Lattice Engineering Lead to Superhigh Thermoelectric Figure of Merit in MnTe
Authors: Zulkifal Shahzada , Wang Zhichao , Zhang Xuemei , Siddique Suniya , Yu Yuan , Wang Chong , Gong Yaru , Li Shuang , Li Di , Zhang Yongsheng , Wang Peng , Tang Guodong
Published: April 2023

MnTe has been considered a promising candidate for lead‐free mid‐temperature range thermoelectric clean energy conversions. However, the widespread use of this technology is constrained by the relatively low‐cost performance of materials. Developing environmentally friendly thermoelectrics with high performance and earth‐abundant elements is thus an urgent task. MnTe is a candidate, yet a peak ZT of 1.4 achieved so far is less satisfactory. Here, a remarkably high ZT of 1.6 at 873 K in MnTe system is realized by facilitating multiple valence band convergence and localized lattice engineering. It is demonstrated that SbGe incorporation promotes the convergence of multiple electronic valence bands in MnTe. Simultaneously, the carrier concentration can be optimized by SbGeS alloying, which significantly enhances the power factor. Simultaneously, MnS nanorods combined with dislocations and lattice distortions lead to strong phonon scattering, resulting in a markedly low lattice thermal conductivity(κlat) of 0.54 W m K−1, quite close to the amorphous limit. As a consequence, extraordinary thermoelectric performance is achieved by decoupling electron and phonon transport. The vast increase in ZT promotes MnTe as an emerging Pb‐free thermoelectric compound for a wide range of applications in waste heat recovery and power generation.
Bidirectionally Regulating Viral and Cellular Ferroptosis with Metastable Iron Sulfide Against Influenza Virus
Authors: Miao Xinyu , Yin Yinyan , Chen Yulian , Bi Wenhui , Yin Yuncong , Chen Sujuan , Peng Daxin , Gao Lizeng , Qin Tao , Liu Xiufan
Published: April 2023

Influenza virus with numerous subtypes and frequent variation limits the development of high‐efficacy and broad‐spectrum antiviral strategy. Here, a novel multi‐antiviral metastable iron sulfides (mFeS) against various influenza A/B subtype viruses is developed. This work finds that mFeS induces high levels of lipid peroxidation and •OH free radicals in the conservative viral envelope, which depends on Fe2+. This phenomenon, termed as a viral ferroptosis, results in the loss of viral infectibility and pathogenicity in vitro and in vivo, respectively. Furthermore, the decoction of mFeS (Dc(mFeS)) inhibits cellular ferroptosis‐dependent intracellular viral replication by correcting the virus‐induced reprogrammed sulfur metabolism, a conserved cellular metabolism. Notably, personal protective equipment (PPE) that is loaded with mFeS provides good antiviral protection. Aerosol administration of mFeS combined with the decoction (mFeS&Dc) has a potential therapeutic effect against H1N1 lethal infection in mice. Collectively, mFeS represents an antiviral alternative with broad‐spectrum activity against intracellular and extracellular influenza virus.
IL‐1β Is an Androgen‐Responsive Target in Macrophages for Immunotherapy of Prostate Cancer
Authors: Wang Deng , Cheng Chaping , Chen Xinyu , Wang Jinming , Liu Kaiyuan , Jing Na , Xu Penghui , Xi Xialian , Sun Yujiao , Ji Zhongzhong , Zhao Huifang , He Yuman , Zhang Kai , Du Xinxing , Dong Baijun , Fang Yuxiang , Zhang Pengcheng , Qian Xueming , Xue Wei , Gao Wei‐Qiang , Zhu Helen He
Published: April 2023

Great attention is paid to the role of androgen receptor (AR) as a central transcriptional factor in driving the growth of prostate cancer (PCa) epithelial cells. However, the understanding of the role of androgen in PCa‐infiltrated immune cells and the impact of androgen deprivation therapy (ADT), the first‐line treatment for advanced PCa, on the PCa immune microenvironment remains limited. On the other hand, immune checkpoint blockade has revolutionized the treatment of certain cancer types, but fails to achieve any benefit in advanced PCa, due to an immune suppressive environment. In this study, it is reported that AR signaling pathway is evidently activated in tumor‐associated macrophages (TAMs) of PCa both in mice and humans. AR acts as a transcriptional repressor for IL1B in TAMs. ADT releases the restraint of AR on IL1B and therefore leads to an excessive expression and secretion of IL‐1β in TAMs. IL‐1β induces myeloid‐derived suppressor cells (MDSCs) accumulation that inhibits the activation of cytotoxic T cells, leading to the immune suppressive microenvironment. Critically, anti‐IL‐1β antibody coupled with ADT and the immune checkpoint inhibitor anti‐PD‐1 antibody exerts a stronger anticancer effect on PCa following castration. Together, IL‐1β is an important androgen‐responsive immunotherapeutic target for advanced PCa.
A Clinical‐Scale Microfluidic Respiratory Assist Device with 3D Branching Vascular Networks
Authors: Isenberg Brett C. , Vedula Else M. , Santos Jose , Lewis Diana J. , Roberts Teryn R. , Harea George , Sutherland David , Landis Beau , Blumenstiel Samuel , Urban Joseph , Lang Daniel , Teece Bryan , Lai WeiXuan , Keating Rose , Chiang Diana , Batchinsky Andriy I. , Borenstein Jeffrey T.
Published: April 2023

Recent global events such as COVID‐19 pandemic amid rising rates of chronic lung diseases highlight the need for safer, simpler, and more available treatments for respiratory failure, with increasing interest in extracorporeal membrane oxygenation (ECMO). A key factor limiting use of this technology is the complexity of the blood circuit, resulting in clotting and bleeding and necessitating treatment in specialized care centers. Microfluidic oxygenators represent a promising potential solution, but have not reached the scale or performance required for comparison with conventional hollow fiber membrane oxygenators (HFMOs). Here the development and demonstration of the first microfluidic respiratory assist device at a clinical scale is reported, demonstrating efficient oxygen transfer at blood flow rates of 750 mL min⁻1, the highest ever reported for a microfluidic device. The central innovation of this technology is a fully 3D branching network of blood channels mimicking key features of the physiological microcirculation by avoiding anomalous blood flows that lead to thrombus formation and blood damage in conventional oxygenators. Low, stable blood pressure drop, low hemolysis, and consistent oxygen transfer, in 24‐hour pilot large animal experiments are demonstrated – a key step toward translation of this technology to the clinic for treatment of a range of lung diseases.
Remodeling Collagen Microenvironment in Liver Using a Biomimetic Nano‐Regulator for Reversal of Liver Fibrosis
Authors: Liang Yan , Wang Jinjin , Xu Chenlu , Han Wenshuai , Wu Sixuan , Wu Yonghua , Zhang Jingge , Liu Junjie , Zhang Zhenzhong , Shi Jinjin , Zhang Kaixiang
Published: April 2023

Liver fibrosis is a progressive histological manifestation that happens in almost all chronic liver diseases. An unabated liver fibrosis may eventually develop into liver cirrhosis or hepatocellular carcinoma. Yet, the strategy for reversal of liver fibrosis is still limited. Herein, a biomimetic nano‐regulator (P‐ZIF8‐cirDNAzyme) is developed to affect both collagen synthesis and degradation in liver to remodel collagen microenvironment. It is found that Zn (II) interference can efficiently inhibit collagen synthesis in activated hepatic stellate cells (aHSC) by inactivating proline 4 hydroxylase and affecting many fibrosis‐related signaling pathways. Meanwhile, Zn (II)‐dependent circular DNAzymes (cirDNAzymes) are used to efficiently silence tissue inhibitors of metalloproteinase‐1, accelerating the degradation of collagen. They act in concert to recover the balance between collagen deposition and degradation. Additionally, ZIF‐8‐cirDNAzyme is coated by platelet membrane (PM) for precisely targeting aHSC via PM's inflammatory tropism and CD62p–CD44 interaction. In carbon tetrachloride‐induced fibrotic mice, P‐ZIF‐8‐cirDNAzyme shows a potent anti‐fibrotic effect, greatly reducing the expression of collagen by 73.12% and restoring liver function nearly to normal. This work proposes a prospective platform enabling ion interference and gene silencing, collectively acting in aHSC for reversal of liver fibrosis.
A New Class of High‐Capacity Fe‐Based Cation‐Disordered Oxide for Li‐Ion Batteries: Li‐Fe‐Ti‐Mo Oxide
Authors: Kim Jieun , Shin Yongho , Kang Byoungwoo
Published: April 2023

Low‐cost Fe can be used for forming cation‐disordered rocksalt Li‐excess (DRX) materials instead of high‐cost d0‐species and then the Fe‐based DRX can be promising electrode materials because they can theoretically achieve high capacity, resulting from additional oxygen redox reaction and stable cation‐disordered structure. However, Fe‐based DRX materials suffer from large voltage hysteresis, low electrochemical activity, and poor cyclability, so it is highly challenging to utilize them as practical electrode materials for a cell. Here, novel high‐capacity Li‐Fe‐Ti‐Mo electrode materials (LFTMO) with high average discharge voltage and reasonable stability are reported. The effect of Ti/Mo on electrochemical reactions in Fe‐based DRX materials (LFTMO) is studied by controlling its composition ratio and using techniques for analyzing the local environment to find the key factors that improve its activity. It is found out that the introduction of appropriate quantity of redox‐active Mo4+/5+ to Fe‐based DRX materials can help stabilize the oxygen redox reaction via changing a local structure and can suppress a Fe redox reaction, which can cause poor performance. The understandings will help develop high capacity and long cyclability Fe‐based DRX electrode materials.
Improper High‐TcPerovskite Ferroelectric with Dielectric Bistability Enables Broadband Ultraviolet‐to‐Infrared Photopyroelectric Effects
Authors: Hua Lina , Wang Jiaqi , Liu Yi , Guo Wuqian , Ma Yu , Xu Haojie , Han Shiguo , Luo Junhua , Sun Zhihua
Published: April 2023

The photopyroelectric effect in ferroelectrics has shown great potential for application in infrared detection and imaging. One particular subclass is broadband with dielectric bistability, which allows for large pyroelectric figures‐of‐merit (FOMs). Herein, an improper high‐Tcperovskite ferroelectric, (IA)2(EA)2Pb3Cl10(1, where IA is isoamylammonium and EA is ethylammonium) is presented, in which spontaneous polarization (Ps) stems from the dynamic ordering of organic cations and the tilting of distorted PbCl6octahedra. Notably,1displays unusual dielectric bistability with small variations in the temperature‐dependent dielectric constants nearTc = 392 K; this bistable attribute endows large pyroelectric FOMs with peak voltage efficiency (FV = 1.7×10−2 cm2µC−1) and sensitivity (FD = 3.9×10−4Pa−1/2). TheseFVandFDparameters, beyond those of their proper counterparts, make1a promising candidate for infrared photodetection. As expected, the broadband photopyroelectric effects observed in1covered the ultraviolet to infrared‐II spectral region (266–1950 nm). SuchPs‐directed photoactivities overcome the optical bandgap limitation and allow for wide‐wave photodetection. As an innovative study on improper ferroelectricity, light is shaded here on the targeted engineering of new electrically ordered candidate materials for smart optoelectronic devices.
Strain Effects in Twisted Spiral Antimonene
Authors: Huang Ding‐Ming , Wu Xu , Chang Kai , Hu Hao , Wang Ye‐Liang , Xu H. Q. , Zhang Jian‐Jun
Published: April 2023

Van der Waals (vdW) layered materials exhibit fruitful novel physical properties. The energy band of such materials depends strongly on their structures, and a tremendous variation in their physical properties can be deduced from a tiny change in inter‐layer spacing, twist angle, or in‐plane strain. In this work, a kind of vdW layered material of spiral antimonene is constructed, and the strain effects in the material are studied. The spiral antimonene is grown on a germanium (Ge) substrate and is induced by a helical dislocation penetrating through few atomic‐layers of antimonene (β‐phase). The as‐grown spiral is intrinsically strained, and the lattice distortion is found to be pinned around the dislocation. Both spontaneous inter‐layer twist and in‐plane anisotropic strain are observed in scanning tunneling microscope (STM) measurements. The strain in the spiral antimonene can be significantly modified by STM tip interaction, leading to a variation in the surface electronic density of states (DOS) and a large modification in the work function of up to a few hundreds of millielectron‐volts (meV). Those strain effects are expected to have potential applications in building up novel piezoelectric devices.
Application of Inorganic Quantum Dots in Advanced Lithium–Sulfur Batteries
Authors: Wang Zhuosen , Che Haiyun , Lu Wenqiang , Chao Yunfeng , Wang Liu , Liang Bingyu , Liu Jun , Xu Qun , Cui Xinwei
Published: April 2023

Lithium–sulfur (Li‐S) batteries have emerged as one of the most attractive alternatives for post‐lithium‐ion battery energy storage systems, owing to their ultrahigh theoretical energy density. However, the large‐scale application of Li–S batteries remains enormously problematic because of the poor cycling life and safety problems, induced by the low conductivity , severe shuttling effect, poor reaction kinetics, and lithium dendrite formation. In recent studies, catalytic techniques are reported to promote the commercial application of Li–S batteries. Compared with the conventional catalytic sites on host materials, quantum dots (QDs) with ultrafine particle size (<10 nm) can provide large accessible surface area and strong polarity to restrict the shuttling effect, excellent catalytic effect to enhance the kinetics of redox reactions, as well as abundant lithiophilic nucleation sites to regulate Li deposition. In this review, the intrinsic hurdles of S conversion and Li stripping/plating reactions are first summarized. More importantly, a comprehensive overview is provided of inorganic QDs, in improving the efficiency and stability of Li–S batteries, with the strategies including composition optimization, defect and morphological engineering, design of heterostructures, and so forth. Finally, the prospects and challenges of QDs in Li–S batteries are discussed.
A Polar Tetragonal Tungsten Bronze with Colossal Second‐Harmonic Generation
Authors: Kuk Yunseung , Bae Seong Bin , Yang Sang Mo , Ok Kang Min
Published: April 2023

A polar tetragonal tungsten bronze, Pb1.91K3.22□0.85Li2.96Nb10O30 (□: vacancies), has been successfully synthesized by a high temperature solid‐state reaction. Single crystal and powder X‐ray diffraction indicate that the structure of Pb1.91K3.22□0.85Li2.96Nb10O30 crystallizing in the noncentrosymmetric (NCS) space group, P4bm, consists of 3D framework with highly distorted NbO6, LiO9, PbO12, and (Pb/K)O15 polyhedra. While NCS Pb1.91K3.22□0.85Li2.96Nb10O30 undergoes a reversible phase transition between polar (P4bm) and nonpolar (P4/mbm) structure at around 460 °C, the material decomposes to centrosymmetric Pb1.45K3.56Li3.54Nb10O30 (P4/mbm) once heated to 1200 °C. Powder second‐harmonic generation (SHG) measurements with 1064 nm radiation indicate that Pb1.91K3.22□0.85Li2.96Nb10O30 exhibits a giant phase‐matchable SHG intensity of ≈71.5 times that of KH2PO4, which is the strongest intensity in the visible range among all nonlinear optical materials reported to date. The observed colossal SHG should be attributable to the synergistic effect of dipole moments from the well‐aligned NbO6 octahedra, the constituting distortive channels with vacancies, and highly polarizable cations.
A Combinatorial Library of Lipid Nanoparticles for Cell Type‐Specific mRNA Delivery
Authors: Naidu Gonna Somu , Yong Seok‐Beom , Ramishetti Srinivas , Rampado Riccardo , Sharma Preeti , Ezra Assaf , Goldsmith Meir , Hazan‐Halevy Inbal , Chatterjee Sushmita , Aitha Anjaiah , Peer Dan
Published: April 2023

Ionizable lipid‐based nanoparticles (LNPs) are the most advanced non‐viral drug delivery systems for RNA therapeutics and vaccines. However, cell type‐specific, extrahepatic mRNA delivery is still a major hurdle, hampering the development of novel therapeutic modalities. Herein, a novel ionizable lipid library is synthesized by modifying hydrophobic tail chains and linkers. Combined with other helper lipids and utilizing a microfluidic mixing approach, stable LNPs are formed. Using Luciferase‐mRNA, mCherry mRNA, and Cre mRNA together with a TdTomato animal model, superior lipids forming LNPs for potent cell‐type specific mRNA delivery are identified. In vitro assays concluded that combining branched ester tail chains with hydroxylamine linker negatively affects mRNA delivery efficiency. In vivo studies identify Lipid 23 as a liver‐trophic, superior mRNA delivery lipid and Lipid 16 as a potent cell type‐specific ionizable lipid for the CD11bhi macrophage population without an additional targeting moiety. Finally, in vivo mRNA delivery efficiency and toxicity of these LNPs are compared with SM‐102‐based LNP (Moderna's LNP formulation) and are shown to be cell‐specific compared to SM‐102‐based LNPs. Overall, this study suggests that a structural combination of tail and linker can drive a novel functionality of LNPs in vivo.
Insights into the Microstructural Engineering of Cobalt‐Free, High‐Nickel Cathodes Based on Surface Energy for Lithium‐Ion Batteries
Authors: Kim Youngjin , Kim Hanseul , Shin Woochul , Jo Eunmi , Manthiram Arumugam
Published: April 2023

In order to reduce cost and increase energy density, it is critical to eliminate cobalt and increase nickel content in practical LiNi1−x−yMnxCoyO2 (NMC) and LiNi1−x−yCoxAlyO2 (NCA) cathodes. However, the implementation of cobalt‐free, high‐nickel layered oxide cathodes in lithium‐ion batteries (LIBs) is hindered by the inherent issue of high surface reactivity with the electrolyte and microcrack formation during cycling. Herein, the origin of key parameters for microstructural engineering in cobalt‐free LiNiO2 (LNO) is comprehensively investigated with two representative dopants, B and Al. A notable difference in the segregation energy between B and Al results in different morphologies of LNO particles. The low solubility of B into the host structure leads to a surface‐confined distribution of B, inhibiting the growth of primary particles, whereas the highly soluble Al facilitates primary particle growth. Recognition of this key parameter can help improve the cycle life of cobalt‐free LIBs via microstructural engineering by increasing the aspect ratio inside the cathode particle. It is demonstrated that boron‐doping in LNO (B‐LNO) is the most effective dopant strategy for microstructural engineering of the primary particles. The B‐LNO exhibits an excellent capacity retention of 81% in full cells after 300 cycles compared to both LNO and Al‐doped LNO (Al‐LNO).
Trace to the Source: Self‐Tuning of MOF Photocatalysts
Authors: Qian Zhiping , Zhang Rui , Xiao Yan , Huang Hongwei , Sun Ying , Chen Yang , Ma Tianyi , Sun Xiaodong
Published: April 2023

Benefitting from ultra‐high porosity, large specific surface area (SSA), and rich active sites, metal–organic frameworks (MOFs) have emerged as a star material in energy and environment related applications, especially in photocatalysis. In comparison with conventional photocatalysts, MOFs can be customized in terms of electronic structure, photo‐responsiveness, and morphological dimensions by rational design, which means that MOFs eliminate the need for other species to achieve enhanced photocatalytic performance, such as metals, compounds, and polymers, which may introduce extra costs, be time‐consuming, be multi‐phase, or have an unclear mechanism. Most previous review works related to MOF photocatalysis have mixed self‐tuning and assisted‐tuning, which often gives an incomplete understanding. In this work, the self‐tunning of MOFs by analyzing component (as clusters, ligands, and inclusions), defect (defect engineering, as linkers, clusters, and oxygen vacancies (OVs), and crystal (as facets, dimensions, and amorphization) is summarized. Then, outstanding examples of these strategies applied to water redox, CO2/N2 reduction, organic conversion, and environmental treatment are discussed. Finally, the opportunities and challenges faced in the self‐tuning of MOFs are analyzed from different perspectives. This paper is a comprehensive and systematic review on the self‐tuning of MOFs to enhance photocatalytic activity.
Fundamentals of Ion‐Exchange Synthesis and Its Implications in Layered Oxide Cathodes: Recent Advances and Perspective
Authors: Luo Yu‐hong , Pan Qing‐lin , Wei Han‐xin , Huang Ying‐de , Tang Lin‐bo , Wang Zhen‐yu , Yan Cheng , Mao Jing , Dai Ke‐hua , Wu Qing , Zhang Xia‐hui , Zheng Jun‐chao
Published: April 2023

Layered oxide cathodes such as Ni‐rich ternary and Li‐rich layered cathode materials have been widely used for lithium‐ion batteries owing to their excellent Li+ transport properties, high energy density, and relatively low cost. However, such layered cathode materials synthesized by high‐temperature sintering face inherent issues such as low structural stability, irreversible migration of transition metal ions, and irreversible redox reactions of oxygen anions. To make a breakthrough from the perspective of material synthesis, a new ion‐exchange synthesis has emerged in recent years, which is a promising strategy for synthesis of Li‐ion cathodes. Herein, the fundamentals of ion‐exchange synthesis and their implications in layered oxide cathodes for lithium‐ion batteries is presented. Specifically, ion‐exchange synthesis and mechanisms of ion exchange are introduced in detail, followed by a discussion of the reduction of synthetic temperature, the synthesis of novel crystal structures, the inhibited migration of transition metal ions, the increased reversibility of anionic redox, and the optimized surface reconstruction. Finally, a summary and outlook is provided for ion‐exchange synthesis of layered oxide cathodes for lithium‐ion batteries. It is anticipated that this ion‐exchange synthesis will facilitate the commercialization of high‐performance cathode materials for next generation Li‐ion batteries.
Graphitic Co‐Products of Clean Hydrogen Production Enabling High‐Rate‐Performance Dual‐Carbon Batteries
Authors: Pan Yuqi , Cao Liuyue , Yao Yuanyuan , Tao Yongwen , Lo Victor , Zheng Zhi , Chivers Benjamin , Prabowo Justin , Liu Fangzhou , Lai Leo , Wei Li , Chen Yuan
Published: April 2023

Methane pyrolysis (CH4 → 2H2 + C) is a promising H2 production process with zero CO2 emissions. Utilizing its solid carbon co‐products can make it economically more competitive. Herein, this work demonstrates that graphitic carbon from methane pyrolysis can work as both cathodes and anodes to enable high‐rate‐performance dual‐carbon batteries (DCBs), outperforming commercial natural and synthetic graphite. The graphite purity can reach 99.32 and 97.59 wt%, respectively, using a standard high‐temperature thermal treatment or a room‐temperature electrochemical method. Compared to graphite, they have smaller crystalline sizes and larger surface areas, enabling faster surface redox reactions and better structural stability upon electrolyte ion intercalation. DCB full cells with LiPF6 ethyl methyl carbonate electrolyte deliver energy storage capacities of 75.1 and 74.7 mAh g−1 at 500 mA g−1 with capacity retentions of 79.2% and 93.4% after the high‐rate charge–discharge over 5000 mA g−1, respectively. They can also be cycled at 500 mA g−1 over 300 cycles without capacity decay, demonstrating excellent cycling stability. They show energy densities of 168.7 and 159.7 Wh kg−1 at power densities of 10.6 and 10.8 kW kg−1, outperforming recently reported DCBs. These findings open a new application of graphite co‐product from the emission‐free H2 production process.
Impact of laparoscopic surgery on short‐term and long‐term outcomes in elderly obese patients with colon cancer
Authors: Hoshino Nobuaki , Hida Koya , Fujita Yusuke , Ohira Masaichi , Ozawa Heita , Bando Hiroyuki , Akagi Tomonori , Kono Yohei , Nakajima Kentaro , Kojima Yutaka , Nakamura Takatoshi , Inomata Masafumi , Yamamoto Seiichiro , Sakai Yoshiharu , Naitoh Takeshi , Watanabe Masahiko , Obama Kazutaka
Published: April 2023

Background

Laparoscopic surgery is reported to be useful in obese or elderly patients with colon cancer, who are at increased risk of postoperative complications because of comorbidities and physical decline. However, its usefulness is less clear in patients who are both elderly and obese and may be at high risk of complications.

Methods

Data for obese patients (body mass index ≥25) who underwent laparoscopic or open surgery for stage II or III colon cancer between January 2009 and December 2013 were collected by the Japan Society of Laparoscopic Colorectal Surgery. Surgical outcomes, postoperative complications, and relapse‐free survival (RFS) were compared between patients who underwent open surgery and those who underwent laparoscopic surgery according to whether they were elderly (≥70 y) or nonelderly (<70 y).

Results

Data of 1549 patients (elderly, n = 598; nonelderly, n = 951) satisfied the selection criteria for analysis. Length of stay was shorter and surgical wound infection was less common in elderly obese patients who underwent laparoscopic surgery than in those underwent open surgery. There were no significant between‐group differences in overall complications, anastomotic leakage, ileus/small bowel obstruction, or RFS. There were also no significant differences in RFS after laparoscopic surgery according to patient age.

Conclusion

Laparoscopic surgery is safe in elderly obese patients with colon cancer and does not worsen their prognosis. There was no significant difference in the effectiveness of laparoscopic surgery between obese patients who were elderly and those who were nonelderly.
Photochromic Polyoxoniobates with Photoinduced “D‐f‐A” Electron Transfer Mechanism
Authors: Yu Hao , Lin Yu‐Diao , Huang Shu‐Lin , Li Xin‐Xiong , Sun Cai , Zheng Shou‐Tian
Published: April 2023

Compounds with redox activities have appealing applications in catalytic, electronic and magnetic properties, but the redox inert of polyoxoniobates (PONbs) significantly limits their applications for a long time. In this work, we are able to integrate organophosphate and lanthanide cluster into PONb to create the first family of inorganic‐organic hybrid organophosphate‐Ln‐PONb composite clusters. These novel species not only present the first family of redox active PONbs that can be reduced to form long‐lived “heteropoly blues” under ambient conditions, but also a new photochromic system. More importantly, the analyses of the electronic configurations and photochromic properties for a series of designed proof‐of‐concept PONbs models allow us to discover a D‐f‐A electron transfer mechanism, that is, photoinduced electron is transferred from a photosensitive organophosphate electron donor (D) to the NbV electron acceptor (A) through the unoccupied 4 f‐orbitals of Ln (f). This work paves the way for developing diverse PONb‐based redox materials and expanding the possibility of the applications of PONbs in the redox chemistry.
A Universal CRISPR/Cas12a‐Assisted Methodology Based on Duplex Switch Structure to Detect Multiple Types of Targets
Authors: Xiao Yao , Li Huan , Tang Yidan , Li Bingling
Published: April 2023

Recent years, molecular detection technology has been playing an unprecedentedly important role in disease prevention and public health. Clustered Regularly Interspaced Short Palindromic Repeat (CRISPR) systems such as CRISPR/Cas12a and CRISPR/Cas13a, have been increasingly used in the detection of nucleic acid molecules because of its collateral cleavage ability in recent years. Herein, we develop a universal CRISPR/Cas12a‐assisted methodology based on a nucleic acid duplex switch structure that can distinguish different categories of targets, such as DNA, RNA and small molecules. It is worth noting that for nucleic acid detection, this method can significantly identify single base substitutions with high specificity, compared with other Cas12a‐assisted biosensing systems. The experimental results suggest that this method has great specificity for different targets, promising to be applied to rapid molecular diagnosis.
3D porous carbon nitride composited oxygen vacancy‐induced indium oxide for high photocatalytic nitrogen fixation on the interfacial surface
Authors: Sun Ting , Gao Ping , Zhang Shixian , Wu Zhiren , Liu Jun , Rong Xinshan
Published: April 2023

Semiconductor photocatalysis can utilize solar energy for clean energy conversion, but the catalytic efficiency is often unsatisfactory due to limited photo response and efficient separation of photogenerated carriers. In this work, 3D porous carbon nitride (3DPCN) composited oxygen vacancy‐induced indium oxide (3DPCN/VO‐In2O3) was successfully prepared and analyzed by some characterization methods. Meanwhile, the performance of photocatalytic nitrogen fixation was further investigated. X‐ray photoelectron spectroscopy and X‐Ray diffraction (XRD) confirmed the successful preparation of the composites and revealed the electron flow direction; scanning electron microscopy (SEM) and transmission electron microscopy showed the surface structure of the composites; diffuse reflectance spectroscopy and temperature programmed desorption (TPD) revealed the energy band position and adsorption mechanism; electron paramagnetic resonance (EPR) characterization confirms the successful construction of oxygen vacancies; and electrochemical impedance spectroscopy, photoluminescence, and other photochemical characterization results showed that 3DPCN/VO‐In2O3 band gap is narrower and more effective in capturing light than other materials, improving the photocatalytic nitrogen fixation ability. The test results show that the nitrogen fixation capacity of 3DPCN/VO‐In2O3 can reach a maximum value of 156 within 2 h. This result demonstrates that the modification of carbon nitride improves its nitrogen fixation effect, and the introduction of oxygen vacancy‐induced In2O3 improves the light absorption performance and is advantageous to the separation of photogenerated charge carriers.
The Natural Sequence in Which Subclinical Inflamed Joint Tissues Subside or Progress to Rheumatoid Arthritis: A Study of Serial MRIs in the TREAT EARLIER Trial
Authors: Krijbolder Doortje I. , Matthijssen Xanthe M. E. , van Dijk Bastiaan T. , van Steenbergen Hanna W. , Boeters Debbie M. , Willemze Annemiek , Schouffoer Anne A. , van der Helm‐van Mil Annette H. M.
Published: April 2023

Objective

The natural trajectory of clinical arthritis progression at the tissue level remains elusive. We hypothesized that subclinical inflammation in different joint tissues (synovitis, tenosynovitis, osteitis) increases in a distinct temporal order in patients with clinically suspect arthralgia (CSA) who develop rheumatoid arthritis (RA) and subsides in a different sequence when CSA spontaneously resolves.

Methods

We studied 185 serial magnetic resonance images (MRIs) from CSA patients with subclinical joint inflammation from the placebo arm of the TREAT EARLIER trial: 52 MRIs from 21 RA progressors (MRIs conducted at 1 year before, at 4 months before, and upon RA development), and 133 MRIs from 35 patients with spontaneous resolution of pain (MRIs conducted at baseline and at 4, 12, and 24 months). MRIs were scored for osteitis, synovitis, and tenosynovitis. We used cross‐lagged models to evaluate 2 types of time patterns between pairs of inflamed tissues: a simultaneous pattern (coinciding changes) and a subsequent pattern (inflammatory changes in 1 tissue preceding changes in another tissue).

Results

In patients who developed RA, synovitis, tenosynovitis, and osteitis increased simultaneously. Increasing osteitis occurred in the final 4 months before RA diagnosis, following incremental tenosynovitis and synovitis changes during the 1 year to 4 months before diagnosis (P < 0.01). In anti–citrullinated protein antibody (ACPA)‐positive and ACPA‐negative patients who progressed to RA, osteitis increased just before RA development. In patients with pain resolution, simultaneous decreases in synovitis, tenosynovitis, and osteitis occurred, with tenosynovitis decreasing in the first 4 months after CSA onset preceding decreasing synovitis and osteitis during 4–12 months (P = 0.02 and P < 0.01).

Conclusion

We identified natural sequences of subclinical inflammation in different joint tissues, which deepens our understanding of clinical arthritis and RA development. During RA progression, increasing osteitis followed previous increases in tenosynovitis and synovitis. During pain resolution, tenosynovitis decreased first, followed by decreasing synovitis and osteitis.
Phenol Hydrogenation to Cyclohexanol Catalysed by Palladium Supported on CuO/CeO2
Authors: Kasabe Mirabai M. , Kotkar Vaibhav R. , Dongare Mohan K. , Umbarkar Shubhangi B.
Published: April 2023

Hydrogenation of phenol to cyclohexanone/cyclohexanol is an important reaction in production of nylon‐6, nylon‐66 and in petroleum industry. Liquid phase phenol hydrogenation over Pd‐CuO/CeO2 was carried out under mild conditions. Palladium impregnated over CuO/CeO2 synthesized by co‐precipitation method showed excellent catalytic activity for phenol hydrogenation (99% conversion with 80% cyclohexanol yield) at 90 °C and 10 bar H2 pressure in water. Commercial 10%Pd/C showed only 8% phenol conversion under identical conditions. The detailed characterization revealed significant improvement in surface area of ceria after addition of CuO and decrease in crystallite size with creation of defects in CeO2 lattice. XPS analysis showed Pd loading on CuO/CeO2 to cause hydrogen spillover on the surface leading to increase in the oxygen vacancies. The interaction of phenol with catalyst surface studied by detailed FTIR analysis, revealed activation of phenol on oxygen vacancy of ceria as phenoxide ion with perpendicular orientation of aromatic ring on catalyst surface.
Weber's syndrome revealing a Percheron artery infarction: A case report
Authors: Mbodji Ahmadou Bamba , Faye Ibrahima , Diop Ndeye Rokhaya , Ndiaye Moustapha
Published: April 2023

Key Clinical Message

Weber's syndrome revealing a Percheron artery infarction is a rare clinical occurrence. Its diagnosis requires careful clinical examination and brain MRI, which is the gold standard for diagnosis. If this is not available, combined cerebral CT scan with a CT angiography of supra‐aortic arteries may be useful for the diagnosis.

Percheron's artery (PA) occlusion is an uncommon type of stroke involving paramedian thalamus and/or midbrain infarction. It accounts for 4%–18% of all thalamic infarcts and 0.1%–2% of all strokes. Its clinical manifestations are variable and its mode of presentation as Weber's syndrome is exceptional due to the unusual clinical presentation.
Wettability‐Regulated Synthesis of Metal–Organic Framework Array with Subnanochannels Enables Efficient Separation of Mono‐/Multivalent Metal Ions
Authors: Wu Zihan , Li Chen , Huang Cheng , Cheng Sha , Ouyang Xiaozhi , Chen Wen , Zhang Pengchao , Jiang Yanan , Jiang Lei
Published: April 2023

Achieving efficient separation of mono‐/multivalent metal ions is essential in various fields, yet it remains a significant challenge. In this work, a metal–organic framework (MOF) array with subnanochannels that exhibit high selectivity and ion permeability in the sieving of mono‐/multivalent metal ion was developed. Specifically, we used confined interfacial reaction at room temperature to synthesis the MOF array inside the micrometer through‐pores of a polyethylene terephthalate (PET) membrane. The location of the oil/water interface was regulated by adjusting the surface wettability of the PET membrane. By taking advantage of size sieving effect of the subnanochannels of MOF crystals, we were able to effectively separate monovalent metal ions from multivalent metal ions with selectivity reaching up to 3930±373 (e.g., Li+/Zr4+). The fluxes of Li+ ions were observed to be as high as 1.97 mol h−1 m−2. The MOF array‐based membrane with subnanochannels that we have developed exhibits great promise for applications in wastewater treatment, lithium extraction from salt‐lake brines, and other related fields.
In situ study of chiral symmetry breaking in sodium chlorate solutions by Mueller matrix polarimetry
Authors: Arteaga Oriol , Arango‐Restrepo Andrés , Barragán Daniel , Ossikovski Razvigor , Rubí Jose Miguel
Published: April 2023

This work presents a novel approach for investigating symmetry‐breaking processes during crystallization using Mueller matrix polarimetry. By applying this method to the cooling process of NaClO3 solutions, we demonstrate its ability to capture not only the initial and final stages of crystallization but also the intermediate steps and dynamics of the process. This technique provides more comprehensive information and insights into the symmetry‐breaking mechanisms involved in crystal formation. Overall, this study highlights the potential of Mueller matrix polarimetry for in situ statistical measurements of the optical rotation and for monitoring the evolution of enantiomeric excesses.
Von Gold‐Clustern zu Gold‐Kolloiden
Authors: Schubert Ulrich
Published: April 2023

In der Strukturchemie von Au(I)‐Komplexen spielen aurophile Wechselwirkungen, also anziehende Kräfte zwischen den Goldatomen, eine wichtige Rolle. Das gilt auch für Gold(I)‐Cluster, in denen deswegen oft keine verbrückenden Gruppen notwendig sind, um den Clusterkern aufzubauen. In „metalloiden“ Clustern, die mehrere Hundert Goldatome enthalten können, hat Gold eine mittlere Oxidationsstufe zwischen Null und Eins. Solche Cluster bestehen aus einem Kern von Ligand‐freien und einer äußeren Schicht von Ligand‐haltigen Metallatomen. Da sie definierte Strukturen haben, sind sie Modellsysteme für Gold‐Kolloide, in denen die Größenverteilung der Metallpartikel mehr oder weniger breit ist. Gold‐Kolloide zeichnen sich durch Farben aus, die von der Partikelgröße abhängig sind. An strukturell definierten metalloiden Clustern lässt sich untersuchen, ab welcher Größe der Übergang von nichtmetallischem zu metallischem Verhalten stattfindet. Dieser beginnt bei ungefähr 150 Goldatomen, und bei ungefähr 250 Atomen sind die Partikel metallisch. Bezüglich Strukturen und Eigenschaften sind die Übergänge von molekularen Koordinationsverbindungen über Cluster und Partikel bis hin zu metallischem Gold fließend.