bluuebunny/crossref_metadata_2025 huggingface dataset:
High‐Performance Tandem Quantum‐Dot Light‐Emitting Diodes Based on Bulk‐Heterojunction‐Like Charge‐Generation Layers
Authors: Zhou Taiying , Wang Ting , Bai Jialin , Liu Shihao , Zhang Hanzhuang , Xie Wenfa , Ji Wenyu
Published: March 2024

In this study, the fundamental but previously overlooked factors of charge generation efficiency and light extraction efficiency (LEE) are explored and collaboratively optimized in tandem quantum‐dot light‐emitting diodes (QLEDs). By spontaneously forming a microstructured interface, a bulk‐heterojunction‐like charge‐generation layer composed of a poly(3,4‐ethylenedioxythiophene):poly(styrene sulfonate)/ZnO bilayer is fabricated and an ideal charge‐generation efficiency surpassing 115% is obtained. The coupling strength of the waveguide mode for the top unit and the plasmon polariton loss for the bottom unit are highly suppressed using precise thickness control, which increases the LEE of the tandem devices. The red tandem QLED achieves an exceptionally low turn‐on voltage for electroluminescence at 4.0 V and outstanding peak external quantum efficiency of 42.9%. The ultralow turn‐on voltage originates from the sequential electroluminescence turn‐on of the two emissive units of the tandem QLED. Benefiting from its unique electroluminescent features, an easily fabricated optical‐electrical dual anti‐counterfeiting display is built by combining a dichromatic tandem QLED with masking technology.
Electromagnetic Waves in Crystals: The Presence of Exceptional Points
Authors: Sturm Chris
Published: March 2024

Although the investigation of the propagation of electromagnetic waves in crystals dates back to the 19th century, the presence of singular optic axes in optically anisotropic materials has not been fully explored until now. Along such an axis, either a left or a right circular polarized wave can propagate without changing its polarization state. More generally, these singular optic axes belong to exceptional points (EPs) in the momentum space and correspond to a simultaneous degeneration of the eigenmodes and their propagation properties. Herein, a comprehensive discussion on EPs in optically anisotropic materials, their occurrence, and properties as well as the properties of the electromagnetic waves propagating along such EPs is presented. The presence of such EPs, their spatial and spectral distribution in bulk, and semi‐infinite and finite crystals are discussed. It is shown that the presence of interfaces has a strong impact on the presence of the EPs and their spatial distribution. At an EP, the propagation of an arbitrarily polarized wave cannot be described by a superposition of two eigenmodes, as typically described in textbooks. This leads to singularities if the reflection and transmission coefficients have to be calculated. Here, two approaches are presented to overcome these limitations.
Silver‐catalyzed Cascade Bis‐heteroannulation Reaction of Enynones and o‐Hydroxyphenyl Enaminones: Access to Highly Functionalized 3‐Furylmethyl Chromones
Authors: Zhang Mingshuai , Liu Meichen , Qiu Yuetong , Peng Menglin , Zhang Zhilai , Song Siyu , Chen Xue‐Bing , Yu Fuchao
Published: March 2024

A synthetic protocol was developed to synthesize highly functionalized 3‐furylmethyl chromones from enynones and o‐hydroxyphenyl enaminones via silver‐catalyzed cascade bis‐heteroannulation reaction. This strategy features broad substrate scope and good functional group tolerance. Furthermore, the 3‐furylmethyl chromone skeleton shows the potential synthetic application value through further gram‐scale synthesis and derivatization.
Catalytic Asymmetric Dearomative Arylation of 2‐Naphthols Enabled by o‐Quinone Diimides
Authors: Li Yuan‐Yang , Yang Fu‐Yuan , Wu Meng‐Yuan , Huang Lihua , Mei Guang‐Jian
Published: March 2024

The catalytic asymmetric dearomative arylation of 2‐naphthols enabled by the unconventional reactivity of o‐quinone diimides, i. e. the 1,4‐conjugate addition on quinone sp2 hybridized carbon, has been established. Under the catalysis of chiral phosphoric acid, various cyclohexaenones bearing an all‐carbon quaternary stereocenter have been prepared with excellent yields and enantioselectivities.
Paintable Decellularized‐ECM Hydrogel for Preventing Cardiac Tissue Damage
Authors: Lee Jaewoo , Lee Seul‐Gi , Kim Beom‐seok , Park Shinhye , Sundaram M. Nivedhitha , Kim Byung‐gee , Kim C‐Yoon , Hwang Nathaniel S.
Published: March 2024

The tissue‐specific heart decellularized extracellular matrix (hdECM) demonstrates a variety of therapeutic advantages, including fibrosis reduction and angiogenesis. Consequently, recent research for myocardial infarction (MI) therapy has utilized hdECM with various delivery techniques, such as injection or patch implantation. In this study, a novel approach for hdECM delivery using a wet adhesive paintable hydrogel is proposed. The hdECM‐containing paintable hydrogel (pdHA_t) is simply applied, with no theoretical limit to the size or shape, making it highly beneficial for scale‐up. Additionally, pdHA_t exhibits robust adhesion to the epicardium, with a minimal swelling ratio and sufficient adhesion strength for MI treatment when applied to the rat MI model. Moreover, the adhesiveness of pdHA_t can be easily washed off to prevent undesired adhesion with nearby organs, such as the rib cages and lungs, which can result in stenosis. During the 28 days of in vivo analysis, the pdHA_t not only facilitates functional regeneration by reducing ventricular wall thinning but also promotes neo‐vascularization in the MI region. In conclusion, the pdHA_t presents a promising strategy for MI treatment and cardiac tissue regeneration, offering the potential for improved patient outcomes and enhanced cardiac function post‐MI.
In Vivo Intelligent Fluorescence Endo‐Microscopy by Varifocal Meta‐Device and Deep Learning
Authors: Chia Yu‐Hsin , Liao Wei‐Hao , Vyas Sunil , Chu Cheng Hung , Yamaguchi Takeshi , Liu Xiaoyuan , Tanaka Takuo , Huang Yi‐You , Chen Mu Ku , Chen Wen‐Shiang , Tsai Din Ping , Luo Yuan
Published: March 2024

Endo‐microscopy is crucial for real‐time 3D visualization of internal tissues and subcellular structures. Conventional methods rely on axial movement of optical components for precise focus adjustment, limiting miniaturization and complicating procedures. Meta‐device, composed of artificial nanostructures, is an emerging optical flat device that can freely manipulate the phase and amplitude of light. Here, an intelligent fluorescence endo‐microscope is developed based on varifocal meta‐lens and deep learning (DL). The breakthrough enables in vivo 3D imaging of mouse brains, where varifocal meta‐lens focal length adjusts through relative rotation angle. The system offers key advantages such as invariant magnification, a large field‐of‐view, and optical sectioning at a maximum focal length tuning range of ≈2 mm with 3 µm lateral resolution. Using a DL network, image acquisition time and system complexity are significantly reduced, and in vivo high‐resolution brain images of detailed vessels and surrounding perivascular space are clearly observed within 0.1 s (≈50 times faster). The approach will benefit various surgical procedures, such as gastrointestinal biopsies, neural imaging, brain surgery, etc.
Enhancing Tumor Immunotherapy by Multivalent Anti‐PD‐L1 Nanobody Assembled via Ferritin Nanocage
Authors: Liu Manman , Jin Duo , Yu Wenxin , Yu Jiaji , Cao Kaiming , Cheng Junjie , Zheng Xiaohu , Wang Andrew , Liu Yangzhong
Published: March 2024

Increasing immunotherapy response rate and durability can lead to significant improvements in cancer care. To address this challenge, a novel multivalent immune checkpoint therapeutic platform is constructed through site‐specific ligation of anti‐PD‐L1 nanobody (Nb) on ferritin (Ftn) nanocage. Nb‐Ftn blocks PD‐1/PD‐L1 interaction and downregulates PD‐L1 levels via endocytosis‐induced degradation. In addition, the cage structure of Ftn allows encapsulation of indocyanine green (ICG), an FDA‐approved dye. Photothermal treatment with Nb‐Ftn@ICG induces immunogenic death of tumor cells, which improves systemic immune response via maturation of dendritic cells and enhanced infiltration of T cells. Moreover, Nb‐Ftn encapsulation significantly enhances cellular uptake, tumor accumulation and retention of ICG. In vivo assays showed that this nanoplatform ablates the primary tumor, suppresses abscopal tumors and inhibits tumor metastasis, leading to a prolonged survival rate. This work presents a novel strategy for improving cancer immunotherapy using multivalent nanobody‐ferritin conjugates as immunological targeting and enhancing carriers.
In Vitro Transcribed mRNA Immunogenicity Induces Chemokine‐Mediated Lymphocyte Recruitment and Can Be Gradually Tailored by Uridine Modification
Authors: Drzeniek Norman M. , Kahwaji Nourhan , Picht Samira , Dimitriou Ioanna Maria , Schlickeiser Stephan , Moradian Hanieh , Geissler Sven , Schmueck‐Henneresse Michael , Gossen Manfred , Volk Hans‐Dieter
Published: March 2024

Beyond SARS‐CoV2 vaccines, mRNA drugs are being explored to overcome today's greatest healthcare burdens, including cancer and cardiovascular disease. Synthetic mRNA triggers immune responses in transfected cells, which can be reduced by chemically modified nucleotides. However, the side effects of mRNA‐triggered immune activation on cell function and how different nucleotides, such as the N1‐methylpseudouridine (m1Ψ) used in SARS‐CoV2 vaccines, can modulate cellular responses is not fully understood. Here, cellular responses toward a library of uridine‐modified mRNAs are investigated in primary human cells. Targeted proteomics analyses reveal that unmodified mRNA induces a pro‐inflammatory paracrine pattern marked by the secretion of chemokines, which recruit T and B lymphocytes toward transfected cells. Importantly, the magnitude of mRNA‐induced changes in cell function varies quantitatively between unmodified, Ψ‐, m1Ψ‐, and 5moU‐modified mRNA and can be gradually tailored, with implications for deliberately exploiting this effect in mRNA drug design. Indeed, both the immunosuppressive effect of stromal cells on T‐cell proliferation, and the anti‐inflammatory effect of IL‐10 mRNA are enhanced by appropriate uridine modification. The results provide new insights into the effects of mRNA drugs on cell function and cell‐cell communication and open new possibilities to tailor mRNA‐triggered immune activation to the desired pro‐ or anti‐inflammatory application.
Defect Engineering of Hexagonal MAB Phase Ti2InB2 as Anode of Lithium‐Ion Battery with Excellent Cycling Stability
Authors: Shen Qing , Shi Yang , He Yibo , Wang Junjie
Published: March 2024

Hexagonal MAB phases （h‐MAB） have attracted attention due to their potential to exfoliate into MBenes, similar to MXenes, which are predicted to be promising for Li‐ion battery applications. However, the high cost of synthesizing MBenes poses challenges for their use in batteries. This study presents a novel approach where a simple ball‐milling treatment is employed to enhance the purity of the h‐MAB phase Ti2InB2 and introduce significant indium defects, resulting in improved conductivity and the creation of abundant active sites. The synthesized Ti2InB2 with indium defects (VIn‐Ti2InB2) exhibits excellent electrochemical properties, particularly exceptional long‐cycle stability at current densities of 5 A g−1 (5000 cycles, average capacity decay of 0.0018%) and 10 A g−1 (15 000 cycles, average capacity decay of 0.093%). The charge storage mechanism of VIn‐Ti2InB2, involving a dual redox reaction, is proposed, where defects promote the In‐Li alloy reaction and a redox reaction with Li in the TiB layer. Finally, a Li‐ion full cell demonstrates cycling stability at 0.5 A g−1 after 350 cycles. This work presents the first accessible and scalable application of VIn‐Ti2InB2 as a Li‐ion anode, unlocking a wealth of possibilities for sustainable electrochemical applications of h‐MAB phases.
An Antibiotic Nanobomb Constructed from pH‐Responsive Chemical Bonds in Metal‐Phenolic Network Nanoparticles for Biofilm Eradication and Corneal Ulcer Healing
Authors: Gao Qiang , Chu Xiaoying , Yang Jie , Guo Yishun , Guo Hanwen , Qian Siyuan , Yang Ying‐Wei , Wang Bailiang
Published: March 2024

In the treatment of refractory corneal ulcers caused by Pseudomonas aeruginosa, antibacterial drugs delivery faces the drawbacks of low permeability and short ocular surface retention time. Hence, novel positively‐charged modular nanoparticles (NPs) are developed to load tobramycin (TOB) through a one‐step self‐assembly method based on metal‐phenolic network and Schiff base reaction using 3,4,5‐trihydroxybenzaldehyde (THBA), ε‐poly‐ʟ‐lysine (EPL), and Cu2+ as matrix components. In vitro antibacterial test demonstrates that THBA‐Cu‐TOB NPs exhibit efficient instantaneous sterilization owing to the rapid pH responsiveness to bacterial infections. Notably, only 2.6 µg mL−1 TOP is needed to eradicate P. aeruginosa biofilm in the nano‐formed THBA‐Cu‐TOB owing to the greatly enhanced penetration, which is only 1.6% the concentration of free TOB (160 µg mL−1). In animal experiments, THBA‐Cu‐TOB NPs show significant advantages in ocular surface retention, corneal permeability, rapid sterilization, and inflammation elimination. Based on molecular biology analysis, the toll‐like receptor 4 and nuclear factor kappa B signaling pathways are greatly downregulated as well as the reduction of inflammatory cytokines secretions. Such a simple and modular strategy in constructing nano‐drug delivery platform offers a new idea for toxicity reduction, physiological barrier penetration, and intelligent drug delivery.
Ru/Ir‐Based Electrocatalysts for Oxygen Evolution Reaction in Acidic Conditions: From Mechanisms, Optimizations to Challenges
Authors: Qin Rong , Chen Guanzhen , Feng Xueting , Weng Jiena , Han Yunhu
Published: March 2024

The generation of green hydrogen by water splitting is identified as a key strategic energy technology, and proton exchange membrane water electrolysis (PEMWE) is one of the desirable technologies for converting renewable energy sources into hydrogen. However, the harsh anode environment of PEMWE and the oxygen evolution reaction (OER) involving four‐electron transfer result in a large overpotential, which limits the overall efficiency of hydrogen production, and thus efficient electrocatalysts are needed to overcome the high overpotential and slow kinetic process. In recent years, noble metal‐based electrocatalysts (e.g., Ru/Ir‐based metal/oxide electrocatalysts) have received much attention due to their unique catalytic properties, and have already become the dominant electrocatalysts for the acidic OER process and are applied in commercial PEMWE devices. However, these noble metal‐based electrocatalysts still face the thorny problem of conflicting performance and cost. In this review, first, noble metal Ru/Ir‐based OER electrocatalysts are briefly classified according to their forms of existence, and the OER catalytic mechanisms are outlined. Then, the focus is on summarizing the improvement strategies of Ru/Ir‐based OER electrocatalysts with respect to their activity and stability over recent years. Finally, the challenges and development prospects of noble metal‐based OER electrocatalysts are discussed.
Highly Sensitive Iontronic Pressure Sensor with Side‐by‐Side Package Based on Alveoli and Arch Structure
Authors: Ding Zhi , Li Weijian , Wang Weidong , Zhao Zhengqian , Zhu Ye , Hou Baoyin , Zhu Lijie , Chen Ming , Che Lufeng
Published: March 2024

Flexible pressure sensors play a significant role in wearable devices and electronic skin. Iontronic pressure sensors with high sensitivity, wide measurement range, and high resolution can meet requirements. Based on the significant deformation characteristics of alveoli to improve compressibility, and the ability of the arch to disperse vertical pressure into horizontal thrust to increase contact area, a graded hollow ball arch (GHBA) microstructure is proposed, greatly improving sensitivity. The fabrication of GHBA ingeniously employs a double‐sided structure. One side uses mold casting to create convex structures, while the other utilizes the evaporation of moisture during the curing process to form concave structures. At the same time, a novel side‐by‐side package structure is proposed, ensuring pressure on flexible substrate is maximally transferred to the GHBA microstructure. Within the range of 0.2 Pa–300 kPa, the iontronic pressure sensor achieves a maximum sensitivity of 10 420.8 kPa−1, pressure resolution of 0.1% under the pressure of 100 kPa, and rapid response/recovery time of 40/35 ms. In wearable devices, it is capable of monitoring dumbbell curl exercises and wirelessly correcting sitting positions. In electronic skin, it can non‐contactly detect the location of the wind source and achieve object classification prediction when combined with the CNN model.
Polyketide Trimming Shapes Dihydroxynaphthalene‐Melanin and Anthraquinone Pigments
Authors: Schmalhofer Maximilian , Vagstad Anna L. , Zhou Qiuqin , Bode Helge B. , Groll Michael
Published: March 2024

Pigments such as anthraquinones (AQs) and melanins are antioxidants, protectants, or virulence factors. AQs from the entomopathogenic bacterium Photorhabdus laumondii are produced by a modular type II polyketide synthase system. A key enzyme involved in AQ biosynthesis is PlAntI, which catalyzes the hydrolysis of the bicyclic‐intermediate‐loaded acyl carrier protein, polyketide trimming, and assembly of the aromatic AQ scaffold. Here, multiple crystal structures of PlAntI in various conformations and with bound substrate surrogates or inhibitors are reported. Structure‐based mutagenesis and activity assays provide experimental insights into the three sequential reaction steps to yield the natural product AQ‐256. For comparison, a series of ligand‐complex structures of two functionally related hydrolases involved in the biosynthesis of 1,8‐dihydroxynaphthalene‐melanin in pathogenic fungi is determined. These data provide fundamental insights into the mechanism of polyketide trimming that shapes pigments in pro‐ and eukaryotes.
Gradient Graphene Spiral Sponges for Efficient Solar Evaporation and Zero Liquid Discharge Desalination with Directional Salt Crystallization
Authors: Zhao Demin , Ding Meichun , Lin Tianhao , Duan Zhenying , Wei Rui , Feng Panpan , Yu Jiahui , Liu Chen‐Yang , Li Chenwei
Published: March 2024

Solar desalination is a promising strategy to utilize solar energy to purify saline water. However, the accumulation of salt on the solar evaporator surface severely reduces light absorption and evaporation performance. Herein, a simple and eco‐friendly method to fabricate a 3D gradient graphene spiral sponge (GGS sponge) is presented that enables high‐rate solar evaporation and zero liquid discharge (ZLD) desalination of high‐salinity brine. The spiral structure of the GGS sponge enhances energy recovery, while the gradient network structures facilitate radial brine transport and directional salt crystallization, which cooperate to endow the sponge with superior solar evaporation (6.5 kg m−2 h−1 for 20 wt.% brine), efficient salt collection (1.5 kg m−2 h−1 for 20 wt.% brine), ZLD desalination, and long‐term durability (continuous 144 h in 20 wt.% brine). Moreover, the GGS sponge shows an ultrahigh freshwater production rate of 3.1 kg m−2 h−1 during the outdoor desalination tests. A continuous desalination–irrigation system based on the GGS sponge for crop growth, which has the potential for self‐sustainable agriculture in remote areas is demonstrated. This work introduces a novel evaporator design and also provides insight into the structural principles for designing next‐generation solar desalination devices that are salt‐tolerant and highly efficient.
Sustainable Recycling of Selenium‐Based Optoelectronic Devices
Authors: Wang Xia , Li Zongbao , Jin Bowen , Lu Wenbo , Feng Mingjie , Dong Binghai , Liu Qingxiang , Yan Hui‐Juan , Wang Shi‐Min , Xue Ding‐Jiang
Published: March 2024

Selenium (Se), the world's oldest optoelectronic material, has been widely applied in various optoelectronic devices such as commercial X‐ray flat‐panel detectors and photovoltaics. However, despite the rare and widely‐dispersed nature of Se element, a sustainable recycling of Se and other valuable materials from spent Se‐based devices has not been developed so far. Here a sustainable strategy is reported that makes use of the significantly higher vapor pressure of volatile Se compared to other functional layers to recycle all of them from end‐of‐life Se‐based devices through a closed‐space evaporation process, utilizing Se photovoltaic devices as a case study. This strategy results in high recycling yields of ≈ 98% for Se and 100% for other functional materials including valuable gold electrodes and glass/FTO/TiO2 substrates. The refabricated photovoltaic devices based on these recycled materials achieve an efficiency of 12.33% under 1000‐lux indoor illumination, comparable to devices fabricated using commercially sourced materials and surpassing the current indoor photovoltaic industry standard of amorphous silicon cells.
Multistrand Twisted Triboelectric Kevlar Yarns for Harvesting High Impact Energy, Body Injury Location and Levels Evaluation
Authors: Xing Fangjing , Gao Xiaobo , Wen Jing , Li Hao , Liu Hui , Wang Zhong Lin , Chen Baodong
Published: March 2024

Developing ultrahigh‐strength fabric‐based triboelectric nanogenerators for harvesting high‐impact energy and sensing biomechanical signals is still a great challenge. Here, the constraints are addressed by design of a multistrand twisted triboelectric Kevlar (MTTK) yarn using conductive and non‐conductive Kevlar fibers. Manufactured using a multistrand twisting process, the MTTK yarn offers superior tensile strength (372 MPa), compared to current triboelectric yarns. In addition, a self‐powered impact sensing fabric patch (SP‐ISFP) comprising signal acquisition, processing, communication circuit, and MTTK yarns is integrated. The SP‐ISFP features withstanding impact (4 GPa) and a sensitivity and response time under the high impact condition (59.68 V GPa−1; 0.4 s). Furthermore, a multi‐channel smart bulletproof vest is developed by the array of 36 SP‐ISFPs, enabling the reconstruction of impact mapping and assessment of body injury location and levels by real‐time data acquisition. Their potential to reduce body injuries, professional security, and construct a multi‐point personal vital signs dynamic monitoring platform holds great promise.
Electrical Properties of Electrochemically Exfoliated 2D Transition Metal Dichalcogenides Transistors for Complementary Metal‐Oxide‐Semiconductor Electronics
Authors: Zou Taoyu , Kim Soonhyo , Reo Youjin , Heo Seongmin , Liu Ao , Noh Yong‐Young
Published: March 2024

The unique semiconducting characteristics of 2D materials, such as transition metal dichalcogenides (TMDs), have drawn significant interest in the field of electronic devices. However, the dependence of the device performance on the electrical properties of electrochemically exfoliated TMD nanoflakes remains unclear. In this study, the intrinsic electrical properties of diverse electrochemically exfoliated TMD nanoflakes are investigated and their applications in fully solution‐processed 2D electronics are explored. The study reveals that MoSe2 and WS2 nanoflakes are suitable candidates with moderate electron concentrations of 5.7 × 1012 and 2.5 × 1012 cm−2, respectively. These moderate electron concentrations enable a low off‐state current and high on‐state current, leading to a large on–off ratio (> 106) for the fabricated transistors. Furthermore, moderate annealing can increase the mobility by one order of magnitude by reducing the contact resistance and improving charge transport. Additionally, the trap density is significantly reduced, leading to an improved stability. Finally, fully solution‐processed 2D complementary inverters with a high voltage gain of 60 are demonstrated. This study contributes to a growing understanding of the properties of 2D materials in terms of transistor performances and promotes the development of solution‐processed devices applicable in next‐generation electronics.
Minutes‐Fast Production of Vacancy‐Enriched MXenes as an Efficient Platform for Single‐Atom Electrocatalysts
Authors: Guo Yu , Zhu Qi , Wang Ziming , Ye Yuxuan , Hu Jiarui , Shang Jiaxiang , Li Bin , Du Zhiguo , Yang Shubin
Published: March 2024

Although MXenes have been synthesized by liquid phase and molten salt etching approaches, it still suffers from sluggish reaction kinetics of removing A species from MAX phases associated with an overlong production time (5–48 h). Here, a minute‐level production approach is developed to produce MXenes (Ti2CClx) by selectively etching MAX phases (Ti2AlC) under metal chloride (ZnCl2) vapor. In this synthetic protocol, metal chloride vapor possesses a very high chemical activity to the interlaminar A metal layers of MAX phases owing to negative Gibbs free energies, accompanied with the fast removal of gaseous A‐containing chlorides in the reaction system. Moreover, some M species can be controllably etched off from the lattice of MX slabs to generate metal vacancies, which have a high reducing ability to implant single‐atom Zn from ZnCl2 vapor. Finally, vacancy‐enriched MXenes are produced after the volatilization of Zn. In this manner, the etching time is less than one‐sixtieth those of liquid phase and molten salt etching approaches. The resultant MXenes can be employed as an efficient platform for implanting single‐atom Pt, showing a low overpotential of 41 mV at a current density of 10 mA cm−2 and a good long‐term stability up to 5000 cycles.
A New Design Strategy Enables High Mn‐Utilization Rate in Aqueous Zinc–Manganese Batteries: Constructing Cathodic Local Mn‐Rich Region
Authors: Liu Yonghang , Ma Yandong , Zhang Yi , Li Yi , Chen Juan , Wang Lei , Bao Shujuan , Qi Yuruo , Chen Hao , Xu Maowen
Published: March 2024

The deposition–dissolution mechanism with a two‐electron transfer reaction endows aqueous Zn–Mn batteries with a desirable theoretical energy density. However, due to the limited solubility of traditional manganese‐based materials and the competitive Mn shuttle behavior, the practical performance is unsatisfactory. Herein, by synergistically incorporating a novel Mn‐rich Mn4N cathode with a plasma functionalized carbon nanotubes film (PCNT) interlayer, an aqueous Zn–Mn battery with a high Mn‐utilization rate and high energy/power density is successfully developed. Specifically, the Mn4N cathode boasts high manganese content and dissolution activity, thereby offering a copious supply of Mn2+ ions for the battery system. The PCNT interlayer, with abundant micropore structures and functional groups, not only restrains the Mn2+ shuttle by entrapping the dissolved Mn2+ but also offers copious reaction sites, ensuring concentrating Mn2+ on the cathodic side and maximizing their contribution to the electrochemical reaction. Consequently, Mn4N‐PCNT exhibits a low polarization voltage and superior Mn‐utilization rate (64.8%). Without the MnSO4 additive, Mn4N‐PCNT achieves an ultra‐high energy density of 821.9 W h kg−1 and remarkable long‐term cycling stability (90% capacity retention over 9000 cycles). The delightful results demonstrate the practical application potential of Mn4N‐PCNT and open up new avenues for the rational design of advanced Zn–Mn batteries.
Clinical characteristics, imaging features, and outcomes of primary hepatic angiosarcoma: A single‐center study and literature review
Authors: Wu Pei‐Jui , Kuo Hsing‐Tao , Sun Chi‐Shu , Feng I‐Che , Li Wan‐Shan , Ho Chung‐Han , Sheu Ming‐Jen
Published: March 2024

Primary hepatic angiosarcoma (PHA) accounts for 0.5% to 2% of all primary hepatic malignancies, and histopathology findings are required to diagnose PHA accurately. This study investigated 12 patients with PHA at a single medical center in southern Taiwan. We analyzed the clinical characteristics, imaging features, histopathology findings, and survival outcomes of patients with PHA. Of the 12 patients, abdominal pain and fullness were the most common symptoms, and their liver biochemistry data and tumor markers were mostly within the normal limits. The liver tumors tended to present as multifocal or diffuse nodules with bilobar involvement. The median overall survival (OS) of the 12 patients after diagnosis was 9 months. Improved OS was observed in the surgery group compared with the nonsurgery group (15 vs. 2 months, p = .003). The median OS of patients in the surgery ± systemic therapy group was superior to that of patients in the systemic therapy group and in the no‐therapy groups (15 vs. 5 vs. 2 months, respectively; p = .012). Complete surgical resection remains the optimal treatment choice, and combined surgery and systemic therapy seem beneficial but require further investigation.
Favorable outcome of non‐myeloablative allogeneic transplantation in adult patients with severe sickle cell disease: A single center experience of 200 patients
Authors: Damlaj Moussab , Alahmari Bader , Alaskar Ahmed , Alhejazi Ayman , Alsadi Husam , Ahmed Mazin , Alanazi Tahani , Ahmed Rasha , Alharbi Amani , Shehabeddine Inaam , Alzaidi Afnan , Alkhuraisat Suha , Mahassnah Isam , Alquraan Hamza , Ballili Maybelle , Alzahrani Mohsen
Published: March 2024

Allogeneic hematopoietic stem cell transplant (HSCT) for adults with severe sickle cell disease (SCD) is potentially curative but not commonly utilized therapy due to complications such as graft failure (GF) and organ toxicity. Herein, we are reporting our long‐term outcome data of non‐myeloablative (NMA) HSCT in adults with severe SCD with emphasis on factors predicting event free survival (EFS). Adults with severe SCD undergoing NMA match‐related donor allogeneic HSCT from 2015 to 2021 with at least 12 months of follow‐up were included. A total of 200 patients were included with a median age of 26 years (14–43) and 56% were male. The median infused CD34 dose was 13.7 (5.07–25.8), respectively. Median absolute neutrophil count engraftment was 19 (13–39) days with 51% of patients receiving GCSF to expedite recovery. A total of 17 patients experienced GF; 3 as primary and 14 as secondary within a median time of 204 days (40–905). A 76% successfully discontinued sirolimus at the last follow‐up. Median follow‐up for the cohort is 29.2 (2.1–71.4) months. Estimated 3‐year EFS and OS were 88.2% (81.9–92.5) and 94.6% (89.2–97.3). At multivariable analysis, minor ABC incompatibility hazard ratio (HR) 4 (1.3–12.1; 0.014) and allo‐antibody against non‐ABO donor antigens HR 4.3 (1.3–14.1; 0.016) were significant for EFS. No clonal evolution or myeloid malignancies were seen. This largest single‐center report of NMA HSCT in adults with severe SCD further delineated its feasibility, potential toxicities, and fertility outcomes. GF remains a major impediment and appears dependent on ABO matching and non‐ABO antibodies.
New insights into patterns of integration in the femur and pelvis among catarrhines
Authors: Cosnefroy Quentin , Berillon Gilles , Gilissen Emmanuel , Brige Pauline , Chaumoître Kathia , Lamberton Franck , Marchal François
Published: March 2024

Objectives

Integration reflects the level of coordinated variation of the phenotype. The integration of postcranial elements can be studied from a functional perspective, especially with regards to locomotion. This study investigates the link between locomotion, femoral structural properties, and femur‐pelvis complex morphology.

Materials and Methods

We measured (1) morphological integration between femoral and pelvic morphologies using geometric morphometrics, and (2) covariation between femoral/pelvic morphologies and femoral diaphyseal cross‐sectional properties, which we defined as morpho‐structural integration. Morphological and morpho‐structural integration patterns were measured among humans (n = 19), chimpanzees and bonobos (n = 16), and baboons (n = 14), whose locomotion are distinct.

Results

Baboons show the highest magnitude of morphological integration and the lowest of morpho‐structural integration. Chimpanzees and bonobos show intermediate magnitude of morphological and morpho‐structural integration. Yet, body size seems to have a considerable influence on both integration patterns, limiting the interpretations. Finally, humans present the lowest morphological integration and the highest morpho‐structural integration between femoral morphology and structural properties but not between pelvic morphology and femur.

Discussion

Morphological and morpho‐structural integration depict distinct strategies among the samples. A strong morphological integration among baboon's femur‐pelvis module might highlight evidence for long‐term adaptation to quadrupedalism. In humans, it is likely that distinct selective pressures associated with the respective function of the pelvis and the femur tend to decrease morphological integration. Conversely, high mechanical loading on the hindlimbs during bipedal locomotion might result in specific combination of structural and morphological features within the femur.
Control of the Hydroquinone/Benzoquinone Redox State in High‐Mobility Semiconducting Conjugated Coordination Polymers
Authors: Huang Xing , Li Yang , Fu Shuai , Ma Chao , Lu Yang , Wang Mingchao , Zhang Peng , Li Ze , He Feng , Huang Chuanhui , Liao Zhongquan , Zou Ye , Zhou Shengqiang , Helm Manfred , Petkov Petko St. , Wang Hai I. , Bonn Mischa , Li Jian , Xu Wei , Dong Renhao , Feng Xinliang
Published: March 2024

Conjugated coordination polymers (c‐CPs) are unique organic–inorganic hybrid semiconductors with intrinsically high electrical conductivity and excellent charge carrier mobility. However, it remains a challenge in tailoring electronic structures, due to the lack of clear guidelines. Here, we develop a strategy wherein controlling the redox state of hydroquinone/benzoquinone (HQ/BQ) ligands allows for the modulation of the electronic structure of c‐CPs while maintaining the structural topology. The redox‐state control is achieved by reacting the ligand TTHQ (TTHQ=1,2,4,5‐tetrathiolhydroquinone) with silver acetate and silver nitrate, yielding Ag4TTHQ and Ag4TTBQ (TTBQ=1,2,4,5‐tetrathiolbenzoquinone), respectively. In spite of sharing the same topology consisting of a two‐dimensional Ag−S network and HQ/BQ layer, they exhibit different band gaps (1.5 eV for Ag4TTHQ and 0.5 eV for Ag4TTBQ) and conductivities (0.4 S/cm for Ag4TTHQ and 10 S/cm for Ag4TTBQ). DFT calculations reveal that these differences arise from the ligand oxidation state inhibiting energy band formation near the Fermi level in Ag4TTHQ. Consequently, Ag4TTHQ displays a high Seebeck coefficient of 330 μV/K and a power factor of 10 μW/m ⋅ K2, surpassing Ag4TTBQ and the other reported silver‐based c‐CPs. Furthermore, terahertz spectroscopy demonstrates high charge mobilities exceeding 130 cm2/V ⋅ s in both Ag4TTHQ and Ag4TTBQ.
Weakly Coordinating Diluent Modulated Solvation Chemistry for High‐Performance Sodium Metal Batteries
Authors: Li Jiaxin , Sui Simi , Zhou Xunzhu , Lei Kaixiang , Yang Qian , Chu Shenxu , Li Lin , Zhao Yuqing , Gu Mengjia , Chou Shulei , Zheng Shijian
Published: March 2024

Diluents have been extensively employed to overcome the disadvantages of high viscosity and sluggish kinetics of high‐concentration electrolytes, but generally do not change the pristine solvation structure. Herein, a weakly coordinating diluent, hexafluoroisopropyl methyl ether (HFME), is applied to regulate the coordination of Na+ with diglyme and anion and form a diluent‐participated solvate. This unique solvation structure promotes the accelerated decomposition of anions and diluents, with the construction of robust inorganic‐rich electrode‐electrolyte interphases. In addition, the introduction of HFME reduces the desolvation energy of Na+, improves ionic conductivity, strengthens the antioxidant, and enhances the safety of the electrolyte. As a result, the assembled Na||Na symmetric cell achieves a stable cycle of over 1800 h. The cell of Na||P’2‐Na0.67MnO2 delivers a high capacity retention of 87.3 % with a high average Coulombic efficiency of 99.7 % after 350 cycles. This work provides valuable insights into solvation chemistry for advanced electrolyte engineering.
Porous Ceramic Metal‐Based Flow Battery Composite Membrane
Authors: Huang Kang , Mu Feiyan , Hou Xiaoxuan , Cao Hongyan , Liu Xin , Chen Ting , Xia Yu , Xu Zhi
Published: March 2024

In metal‐based flow battery, membranes significantly impact energy conversion efficiency and security. Unfortunately, damages to the membrane occur due to gradual accumulation of metal dendrites, causing short circuits and shortening cycle life. Herein, we developed a rigid hierarchical porous ceramic flow battery composite membrane with a sub‐10‐nm‐thick polyelectrolyte coating to achieve high ion selectivity and conductivity, to restrain dendrite, and to realize long cycle life and high areal capacity. An aqueous zinc‐iron flow battery prepared using this membrane achieved an outstanding energy efficiency of >80%, exhibiting excellent long‐term stability (over 1000 h) and extremely high areal capacity (260 mAh cm−2). Low‐field nuclear magnetic resonance (NMR) spectroscopy, small‐angle X‐ray scattering, in situ infrared spectroscopy, solid‐state NMR analysis, and nano‐computed tomography revealed that the rigid hierarchical pore structures and numerous hydrogen bonding networks in the membrane contributed to the stable operation and superior battery performance. This study contributes to the development of next‐generation metal‐based flow battery membranes for energy and power generation.
Vinyl‐Group‐Anchored Covalent Organic Framework for Promoting the Photocatalytic Generation of Hydrogen Peroxide
Authors: Yu Hong , Zhang Fengtao , Chen Qian , Zhou Pan‐Ke , Xing Wandong , Wang Sibo , Zhang Guigang , Jiang Yi , Chen Xiong
Published: March 2024

The artificial photosynthesis of H2O2 from water and oxygen using semiconductor photocatalysts is attracting increasing levels of attention owing to its green, environmentally friendly, and energy‐saving characteristics. Although covalent organic frameworks (COFs) are promising materials for promoting photocatalytic H2O2 production owing to their structural and functional diversity, they typically suffer from low charge‐generation and ‐transfer efficiencies as well as rapid charge recombination, which restricts their use as catalysts for photocatalytic H2O2 production. Herein, we report a strategy for anchoring vinyl moieties to a COF skeleton to facilitate charge separation and migration, thereby promoting photocatalytic H2O2 generation. This vinyl‐group‐bearing COF photocatalyst exhibits a H2O2‐production rate of 84.5 μmol h−1 (per 10 mg), which is ten‐times higher than that of the analog devoid of vinyl functionality and superior to most reported COF photocatalysts. Both experimental and theoretical studies provide deep insight into the origin of the improved photocatalytic performance. These findings are expected to facilitate the rational design and modification of organic semiconductors for use in photocatalytic applications.
Simultane Funktionalisierung von Einwandigen Kohlenstoff‐Nanoröhren von Innen und Außen
Authors: Kraus Jan , Meingast Laura , Hald Janina , Beil Sebastian B. , Biskupek Johannes , Ritterhoff Christian L. , Gsänger Sebastian , Eisenkolb Jasmin , Meyer Bernd , Kaiser Ute , Maultzsch Janina , von Delius Max
Published: March 2024

Die Funktionalisierung einwandiger Kohlenstoff‐Nanoröhren (SWCNTs) auf eine robuste Weise, die das sp2 Kohlenstoffgerüst nicht beeinträchtigt ist in der aktuellen Forschung eine große Herausforderung. Hier beschreiben wir, wie Triiodidsalze von positiv geladenen Makrozyklen verwendet werden können, um SWCNTs nicht nur von außen, sondern auch gleichzeitig von innen zu funktionalisieren. Wir setzten den Disulfidaustausch in wässrigem Lösungsmittel ein, um den solvophoben Effekt zu maximieren und so einen hohen Grad an Makrozyklus Immobilisierung zu erreichen. Die Charakterisierung mittels Raman‐Spektroskopie, EDX‐STEM und HR‐TEM zeigte deutlich, dass dieses nasschemische Funktionalisierungsprotokoll auch zur Verkapselung von Polyiodidketten im Inneren der Nanoröhren führte. Die resultierenden dreischaligen Kompositmaterialien sind redoxaktiv und weisen ein faszinierendes Zusammenspiel von elektrostatischen, solvophoben und mechanischen Effekten auf, was für Anwendungen in der Energiespeicherung von Interesse sein könnte.
Contact‐Electro‐Catalysis for Direct Oxidation of Methane under Ambient Conditions
Authors: Li Weixin , Sun Jikai , Wang Mingda , Xu Jiajia , Wang Yanjie , Yang Li , Yan Ran , He Haoxian , Wang Shuai , Deng Wei‐Qiao , Tian Zhong‐Qun , Fan Feng Ru
Published: March 2024

The conversion of methane under ambient conditions has attracted significant attention. Although advancements have been made using active oxygen species from photo‐ and electro‐ chemical processes, challenges such as complex catalyst design, costly oxidants, and unwanted byproducts remain. This study exploits the concept of contact‐electro‐catalysis, initiating chemical reactions through charge exchange at a solid–liquid interface, to report a novel process for directly converting methane under ambient conditions. Utilizing the electrification of commercially available Fluorinated Ethylene Propylene (FEP) with water under ultrasound, we demonstrate how this interaction promote the activation of methane and oxygen molecules. Our results show that the yield of HCHO and CH3OH can reach 467.5 and 151.2 μmol ⋅ gcat−1, respectively. We utilized electron paramagnetic resonance (EPR) to confirm the evolution of hydroxyl radicals (⋅OH) and superoxide radicals (⋅OOH). Isotope mass spectrometry (MS) was employed to analyze the elemental origin of CH3OH, which can be further oxidized to HCHO. Additionally, we conducted density functional theory (DFT) simulations to assess the reaction energies of FEP with H2O, O2, and CH4under these conditions. The implications of this methodology, with its potential applicability to a wider array of gas‐phase catalytic reactions, underscore a significant advance in catalysis.
Manganese(I)‐Catalyzed Enantioselective C(sp2)−C(sp3) Bond‐Forming for the Synthesis of Skipped Dienes with Synergistic Aminocatalysis
Authors: Zhao Chuan‐Gang , Cai Junzhe , Du Chaoyu , Gao Qi , Han Jie , Xie Jin
Published: March 2024

Mn(I)‐catalyzed enantioselective C−C bond‐forming reactions represent a great challenge in homogeneous catalysis primarily due to a limited understanding of its mechanistic principles. Herein, we have developed an interesting catalytic strategy that leverages a synergistic combination of a dimeric manganese(I) catalyst and a chiral aminocatalyst to address this issue. A range of conjugated dienals and trienals can exclusively proceed 1,4‐hydroalkenylation by using readily available aromatic and aliphatic alkenyl boronic acids as coupling partners, producing a rich library of skipped diene aldehydes in synthetically useful yields and high levels of enantioselectivities. Notably, downstream transformations of these products can not only afford a concise approach to construct enantioenriched skipped trienes but also realize enantioselective total synthesis of analogues to (−)‐Blepharocalyxin D in four steps. DFT calculations suggest the 1,4‐hydroalkenylation is kinetically more favorable than 1,6‐hydroalkenylation.
Elastic Relaxor Ferroelectric by Thiol‐ene Click Reaction
Authors: Li Bowen , Wang Linping , Gao Liang , Xu Tianhua , Zhang Dongyang , Li Fangzhou , Lyu Jike , Zhu Ren , Gao Xin , Zhang Heng , Hu Ben‐Lin , Li Run‐Wei
Published: March 2024

As ferroelectrics hold significance and application prospects in wearable devices, the elastification of ferroelectrics becomes more and more important. Nevertheless, achieving elastic ferroelectrics requires stringent synthesis conditions, while the elastification of relaxor ferroelectric materials remains unexplored, presenting an untapped potential for utilization in energy storage and actuation for wearable electronics. The thiol‐ene click reaction offers a mild and rapid reaction platform to prepare functional polymers. Therefore, we employed this approach to obtain an elastic relaxor ferroelectric by crosslinking an intramolecular carbon‐carbon double bonds (CF=CH) polymer matrix with multiple thiol groups via a thiol‐ene click reaction. The resulting elastic relaxor ferroelectric demonstrates pronounced relaxor‐type ferroelectric behaviour. This material exhibits low modulus, excellent resilience, and fatigue resistance, maintaining a stable ferroelectric response even under strains up to 70 %. This study introduces a straightforward and efficient approach for the construction of elastic relaxor ferroelectrics, thereby expanding the application possibilities in wearable electronics.
N‐Heteroaromatic Fluoroalkylation through Ligand Coupling Reaction of Sulfones
Authors: Liang Huamin , Wang Qian , Zhou Xin , Zhang Rongyi , Zhou Min , Wei Jun , Ni Chuanfa , Hu Jinbo
Published: March 2024

Ligand coupling on hypervalent main group elements has emerged as a pivotal methodology for the synthesis of functionalized N‐heteroaromatic compounds in recent years due to the avoidance of transition metals and the mildness of the reaction conditions. In this direction, the reaction of N‐heteroaryl sulfur(IV) and N‐heteroaryl phosphorus(V) compounds has been well studied. However, the ligand coupling of sulfur(VI) is still underdeveloped and the reaction of alkyl N‐heteroarylsulfones is still elusive, which does not match the high status of sulfones as the chemical chameleons in organic synthesis. Here we present a ligand coupling‐enabled formal SO2 extrusion of fluoroalkyl 2‐azaheteroarylsulfones under the promotion of Grignard reagents, which not only enriches the chemistry of sulfones, but also provides a novel and practical synthetic tool towards N‐heteroaromatic fluoroalkylation.
Water‐Soluble Fluorescent Polymer Dyes with Tunable Emission Spectra for Flow Cytometry Applications
Authors: Berndt Daniel , Glaap Dorina , Jennings Travis , Dose Christian , Werz Daniel B. , Reckert Dirk N. H.
Published: March 2024

The application of spectrally unique, bright, and water‐soluble fluorescent dyes is indispensable for the analysis of biological systems. Multiparameter flow cytometry is a powerful tool for characterization of mixed cell populations. To discriminate the different cell populations, they are typically stained by a set of fluorescent reagents, e.g., antibody‐fluorophore conjugates. The number of parameters which can be studied simultaneously strongly depends on the availability of reagents which can be differentiated by their spectral properties. In this study a series of fluorescent polymer dyes was developed, that can be excited with a single violet laser (405 nm) but distinguished by their unique emission spectra. The polyfluorene‐based polymers can be used on their own, or in combination with covalently bound small‐molecule dyes to generate energy transfer constructs to red‐shift the emission wavelength based on Förster resonance energy transfer (FRET). The polymer dyes were utilized in a biological flow cytometry assay by conjugating several of them to antibodies, demonstrating their effectiveness as reagents. This report represents the first systematic investigation of structure–property relationships for this type of fluorescent dyes.