bluuebunny/crossref_metadata_2025 huggingface dataset:
Process Intensification
Authors: Harmsen Jan
Published: April 2024

Process intensification is a set of radically innovative process design principles that can bring significant benefits in terms of efficiency, cost, product quality, safety, and health, over conventional process designs based on (conventional) unit operations.

The principles are perfect reactions, optimized driving forces, and synergy. The PI unit operations generated by these principles via research can be classified into spatial domain, alternative energy supply, synergy, and dynamic operation.

In addition to these PI unit operations, a PI process concept design method, based on function integration, has also been developed, and finally, there is also a new engineering and construction method with modular design and prefabricated skid‐mounted construction.

Many PI unit operations and PI‐based processes have been implemented at commercial scale. The largest number of unit operation implementations are reactive distillation, dividing wall distillation, and microwave heating. The main benefits are reduced investment cost, reduced energy requirements, and lower diffusive emissions to the environment. Several universities have included PI in their education program as elective courses.
Pentamode Structures Optimized by Machine Learning with Adaptive Sampling
Authors: Bronder Stefan , Jung Anne
Published: April 2024

Pentamode structures, gain increasing interest as insulation or stealth material. The enhancements in computers and clusters make it possible to investigate those structures not only in theory but also with simulations. Their applicability to mechanical wave dampening is the main focus of the present work, which leads to a structure with good damping and enough strength as the goal. Therefore, a parametrized geometry based on the diamond lattice is examined within a design space. A factorial testing plan investigates the boundaries and gives first hints on the structure's behaviour under compressive and oscillatory loading and also reveals the necessity of a multi objective optimization. Feed‐forward neural networks are then trained to predict the material properties action and mass specific stiffness utilizing adaptive sampling in order to save time and computational cost. An optimization procedure to gain the structure with lowest mass, highest stiffness, and best damping capabilities, which means lowest action, is successfully implemented and yields the best compromise solution for an equally balanced optimization. This structure is then investigated by finite element simulations and confirms the optimization as well as the neural network training, thus being the best trade‐off of all optimization targets.
Size‐Dependent Multi‐Electron Donation in Metal‐Complex Quantum Dots Hybrid Catalyst for Photocatalytic Carbon Dioxide Reduction
Authors: Zhao Qian , Abdellah Mohamed , Cao Yuehan , Meng Jie , Zou Xianshao , Ene‐mark‐Rasmussen Kasper , Lin Weihua , Li Yi , Chen Yijiang , Duan Hengli , Pan Qinying , Zhou Ying , Pullerits Tonu , Xu Hong , Canton Sophie E. , Niu Yuran , Zheng Kaibo
Published: April 2024

The effective conversion of carbon dioxide (CO2) into valuable chemical fuels relies significantly on the donation of multiple electrons. Its efficiency  is closely linked to both the density and lifetime of excited charge carriers. In this study, a hybrid catalyst system comprising covalently bonded InP/ZnS quantum dots (QDs) and Re‐complexes is showcased. The electronic band alignment between the QDs and the Re‐complexes is revealed to dominate the multi‐electron transfer process for photocatalytic conversion to methane (CH4). Notably, the size of the QDs is found to be a determining parameter. Among the three QD sizes investigated,  transient absorption spectroscopy studies unveil that rapid multi‐electron transfer from the QDs to the Re‐catalyst occurs in smaller QDs (2.3 nm) due to the substantial driving force. Consequently, the photocatalytic conversion of CO2 to CH4 is significantly enhanced with a turnover number of 6, corresponding to the overall apparent quantum yield of ≈1%. This research underscores the possibilities of engineering multi‐electron transfer by manipulating the electronic band alignment within a catalytic system. This can serve as a guide for optimizing photocatalytic CO2 reduction.
Janus Conductive Mechanism: An Innovative Strategy Enabling Ultra‐Wide Linearity Range Pressure Sensing for Multi‐Scenario Applications
Authors: Lin Xiuzhu , Teng Ye , Xue Hua , Bing Yu , Li Fan , Wang Juan , Li Juan , Zhao Hongran , Zhang Tong
Published: April 2024

The wide range of pressure detection and the exceptional linearity are essential performance parameters for flexible pressure sensors, enabling them to adapt to diverse scenarios and acquire information accurately. However, currently available “ultra‐wide range” piezoresistive sensors lack an optimal solution that effectively balances sensing properties, device thickness, and process cost. This study proposes a distinctive approach by introducing a Janus conductive structure assembled with dual resistive sensitive layers. The design allows for a pressure‐induced staged transformation of the current transport path, effectively mitigating variations and saturation in sensor resistance over a wide pressure range. The resulting piezoresistive sensor demonstrates an unprecedented detection range of 0–3800 kPa, showcasing remarkable sensitivity of 4.11 kPa−1 and outstanding linearity of 99.9% within the range of 0–1000 kPa. Additionally, the sensor boasts a thickness of only ≈200 µm, made possible through the utilization of a cellulose nanofibers material matrix. These performance achievements stand at the forefront when compared to existing reports. This research explores the potential applications of these sensors and extended arrays in the domains of human health and motion monitoring. It investigates their utility in gait analysis for assisted posture correction, as well as in the assessment and rehabilitation of gait instability.
Vacancy‐Assisted Transformation of MoS2 Nanosheets into Defective MoSx Nanoclusters to Regulate Sodium‐Ion Electrode Functionality
Authors: Jin Xiaoyan , Lee Taehun , Soon Aloysius , Hwang Seong‐Ju
Published: April 2024

Defect structure has attracted significant attention because of its importance as design factor for exploring high‐performance functional materials. This study reports a defect‐engineering strategy to optimize the electrode performance of transition metal dichalcogenides and a clear elucidation of the underlying mechanism on the benefit of defect engineering with cycling‐induced transformation into small nanoclusters. The intercalative hybridization of monolayered MoS2 nanosheets with bulky tetraalkylammonium cations is effective for generating abundant crystal vacancies in the MoS2 lattice and improving the sodium‐ion electrode performance, achieving one of the excellent performances among MoS2‐based sodium‐ion anode materials. The improved electrode activity of the tetrapropylammonium−MoS2 nanohybrid is ascribed to the vacancy‐assisted transformation from monolayered MoS2 nanosheets into trimeric/dimeric MoSx nanoclusters during electrochemical cycling. 23Na/1H magic angle spinning‐nuclear magnetic resonance analyses demonstrated that cycling‐induced defective MoSx nanoclusters yields a complex Na environment with high ion mobility and enhanced electrolyte absorptivity, promoting the excellent electrode functionality of tetrapropylammonium‐assembled MoS2 nanosheets.
A Novel Catalase Nanogels for Effective Treatment of Neutrophilic Asthma
Authors: Zuo Xu , Guo Xiaoping , Gu Yinuo , Zhao Dan , Zou Zheng , Shen Yuanyuan , He Chaoliang , Rong Yan , Xu Caina , Wang Fang
Published: April 2024

Neutrophilic asthma, as corticosteroid resistant asthma, is clinically more severe than eosinophilic asthma. Therefore, the treatment of neutrophilic asthma has been a challenging. Reactive oxygen species (ROS) play a key role in the neutrophilic asthma. However, the direct use of antioxidant enzymes, such as catalase (CAT), is challenging due to the poor stability, short plasma half‐life, and the lack of effective drug delivery systems to pulmonary systems. In this work, a novel kind of nanogels for delivering CAT (CAT‐NGs) is synthesized, incorporating CAT with an antibacterial “protective film”, as a modality for the treatment of neutrophilic asthma. Compared with free CAT, CAT‐NGs demonstrated superior enzyme activity and trypsin resistance, and exhibited outstanding anti‐inflammatory and antioxidant activities in vitro. Furthermore, CAT‐NGs showed significant inhibitory effects on nontypeable Haemophilus influenzae (NTHi), Staphylococcus aureus (S. aureus) and Escherichia coli (E. coli). Additionally, nebulized inhalation of CAT‐NGs alleviated pulmonary inflammation in neutrophilic asthma mice. Mechanistically, the alleviation of neutrophilic asthma symptoms by CAT‐NGs is possibly associated with the clearance of ROS in the lung and the inhibition of the NLRP3 and NF‐κB pathways. Hence, the work have demonstrated the therapeutic potential of CAT‐NGs, offering new insights into the clinical treatment of neutrophilic asthma.
Self‐Recoverable, Highly Repeatable, and Thermally Stable Mechanoluminescence for Dual‐Mode Information Storage and Photonic Skin Applications
Authors: Qin Shiye , Wei Wanyuan , Tian Birong , Ma Zhidong , Fang Shaofan , Wang Yongsheng , Zhang Jiachi , Wang Zhaofeng
Published: April 2024

Mechanically driven light generation is an intriguing phenomenon holding great promise in various fields. However, the existing mechanoluminescence (ML) materials always suffer from poor self‐recoverability, low repeatability, and environmental disturbance, severely hindering their practical applications. In this work, a self‐activating ML system based on interfacial triboelectrification is created by compositing the Ca6BaP4O17:0.02Ce3+ powders into a flexible polydimethylsiloxane (PDMS) matrix. With no need for pre‐irradiation, the composite film emits self‐activating and self‐charging ML simultaneously in response to the rubbing or stretching stimuli. Accordingly, the Ca6BaP4O17:0.02Ce3+/PDMS exhibits desirable self‐recovery and repeatable ML performance, which could still be recorded (or observed by naked eyes) even after ca. 1000 stretching cycles with a fast self‐recovery period of < 0.1 s. Furthermore, the Ca6BaP4O17:0.02Ce3+/PDMS possesses good thermal stability in a temperature range from 298 to 473 K. The developed Ca6BaP4O17:0.02Ce3+/PDMS is applicable to various fields, and the dual‐mode information storage and photonic skin devices are created as representatives. Compared to the existing oxide‐based ML materials (the ML signal disappears after only several or tens of rapid mechanics cycles), this work breaks through the bottleneck issues on the self‐recoverability, repeatability, and thermal stability, which significantly advances the ML field.
Burgeoning Silicon/MXene Nanocomposites for Lithium Ion Batteries: A Review
Authors: Zhang Peng , Wang Xindi , Zhang Yifan , Wei Yi , Shen Nan , Chen Shi , Xu Bin
Published: April 2024

Silicon‐based materials are regarded as the most promising negative electrode materials for next‐generation high‐energy lithium ion batteries due to their high theoretical capacity, low lithiation plateau and low cost, but they still suffer from dramatic volume variation during charge/discharge and sluggish kinetics, substantially restricting their practical applications. Recently, 2D MXenes are demonstrated to improve the electrochemical performances of Si‐based materials owing to their metallic conductivity, large surface aspect ratio, rich surface chemistry, good mechanical strength, etc. Serving as conductive host, MXenes can alleviate the volume expansion of Si during lithiation, enhance the electronic conductivity of the composite and facilitate the electron/ion transport, thus making the resultant Si/MXene composites exhibit excellent performance as negative electrodes of secondary batteries. Herein, an overview toward the recent advances of Si/MXene nanocomposites is presented for lithium storage applications. The preparation strategies and structural characteristics of the Si/MXene nanocomposites are introduced. The applications of diverse Si/MXene nanostructures such as powders, 3D architectures, films and fibers, in lithium ion batteries with corresponding structure‐performance relationships are discussed. Finally, the challenges and perspectives for the future research of Si/MXene nanocomposites are highlighted, aiming to provide a fundamental reference in designing advanced Si/MXene nanocomposites for high‐energy lithium ion batteries.
A Stable, Self‐Healable, and Stretchable Dielectric Polymer for Electroluminescent Device Working Underwater
Authors: Liu Yuncong , Sun Lin , Feng Wenwen , Jin Zhekai , Wang Chao
Published: April 2024

Stretchable dielectric polymer with high dielectric constant is a major component for electroluminescent devices. However, the intrinsic instability toward water severely limits their further applications in marine environment. Here, a transparent, underwater stable, and self‐healable dielectric material with high dielectric constant is reported. The electroluminescent device based on this newly designed fluoropolymer can work stably in aqueous conditions. There is no significant attenuation of mechanical and optoelectronic property after immersed in water and salty water for a month. The intrinsic self‐healing ability of the device makes it robust and resilient against unexpected minor or severe damages.
Refined Pore Structure Design and Surface Modification of 3D Porous Copper Achieving Highly Stable Dendrite‐Free Lithium‐Metal Anode
Authors: Guo Gengde , Zhang Kai , Zhu Kaiping , Yang Peng , Shao Zhipeng , Liu Shizhuo , Lin Lin , Zhuang Wubin , Xue Pan , Zhang Qichong , Yao Yagang
Published: April 2024

3D porous copper is anticipated to serve as an ideal current collector for lithium‐metal anodes (LMAs) owing to its excellent conductivity, huge surface area, and cost‐effectiveness. However, most pertinent studies center around commercial copper foams, where their notable large pore size (150–400 µm) is identified as a primary inducement for dendrite formation and ultimate battery failure. Hence, ensuring the appropriate pore structure in 3D porous copper for achieving highly reversible lithium deposition/stripping process plays a pivotal role in stabilizing LMAs. Herein, the hydrogen bubble template method is employed to fabricate five distinct types of 3D porous copper. Among them, the one with an average surface pore diameter of 25.18 µm and the lowest probability of macropores distribution within the pore walls demonstrates optimal electrochemical performance. To further improve the inherent lithiophobicity of copper, Cu2Se/Cu2O heterostructure nanowires are loaded as kinetic enhanced nucleation sites. Benefiting from the synergistic effect of optimized pore structure and heterostructure nanowires, the Cu2Se/Cu2O@3D Cu composite current collector exhibits excellent dendrite‐free characteristics and outstanding electrochemical performance, showcasing an ultra‐long symmetrical‐cell lifespan of 3000 h at 1 mA cm−2 and stability for 300 h even under 20 mA cm−2.
Integrated Microprism and Microelectrode Array for Simultaneous Electrophysiology and Two‐Photon Imaging across All Cortical Layers
Authors: Yang Qianru , Wu Bingchen , Castagnola Elisa , Pwint May Yoon , Williams Nathaniel P. , Vazquez Alberto L. , Cui Xinyan Tracy
Published: April 2024

Cerebral neural electronics play a crucial role in neuroscience research with increasing translational applications such as brain–computer interfaces for sensory input and motor output restoration. While widely utilized for decades, the understanding of the cellular mechanisms underlying this technology remains limited. Although two‐photon microscopy (TPM) has shown great promise in imaging superficial neural electrodes, its application to deep‐penetrating electrodes is technically difficult. Here, a novel device integrating transparent microelectrode arrays with glass microprisms, enabling electrophysiology recording and stimulation alongside TPM imaging across all cortical layers in a vertical plane, is introduced. Tested in Thy1‐GCaMP6 mice for over 4 months, the integrated device demonstrates the capability for multisite electrophysiological recording/stimulation and simultaneous TPM calcium imaging. As a proof of concept, the impact of microstimulation amplitude, frequency, and depth on neural activation patterns is investigated using the setup. With future improvements in material stability and single unit yield, this multimodal tool greatly expands integrated electrophysiology and optical imaging from the superficial brain to the entire cortical column, opening new avenues for neuroscience research and neurotechnology development.
Engineering Nanoplatforms for Theranostics of Atherosclerotic Plaques
Authors: Liu Yuying , Jiang Zeyu , Yang Xiao , Wang Yin , Yang Bin , Fu Qinrui
Published: April 2024

Atherosclerotic plaque formation is considered the primary pathological mechanism underlying atherosclerotic cardiovascular diseases, leading to severe cardiovascular events such as stroke, acute coronary syndromes, and even sudden cardiac death. Early detection and timely intervention of plaques are challenging due to the lack of typical symptoms in the initial stages. Therefore, precise early detection and intervention play a crucial role in risk stratification of atherosclerotic plaques and achieving favorable post‐interventional outcomes. The continuously advancing nanoplatforms have demonstrated numerous advantages including high signal‐to‐noise ratio, enhanced bioavailability, and specific targeting capabilities for imaging agents and therapeutic drugs, enabling effective visualization and management of atherosclerotic plaques. Motivated by these superior properties, various noninvasive imaging modalities for early recognition of plaques in the preliminary stage of atherosclerosis are comprehensively summarized. Additionally, several therapeutic strategies are proposed to enhance the efficacy of treating atherosclerotic plaques. Finally, existing challenges and promising prospects for accelerating clinical translation of nanoplatform‐based molecular imaging and therapy for atherosclerotic plaques are discussed. In conclusion, this review provides an insightful perspective on the diagnosis and therapy of atherosclerotic plaques.
Exploring Mechanisms of Lipid Nanoparticle‐Mucus Interactions in Healthy and Cystic Fibrosis Conditions
Authors: Tafech Belal , Rokhforouz Mohammad‐Reza , Leung Jerry , Sung Molly MH , Lin Paulo JC , Sin Don D , Lauster Daniel , Block Stephan , Quon Bradley S. , Tam Ying , Cullis Pieter , Feng James J , Hedtrich Sarah
Published: April 2024

Mucus forms the first defense line of human lungs, and as such hampers the efficient delivery of therapeutics to the underlying epithelium. This holds particularly true for genetic cargo such as CRISPR‐based gene editing tools which cannot readily surmount the mucosal barrier. While lipid nanoparticles (LNPs) emerge as versatile non‐viral gene delivery systems that can help overcome the delivery challenge, many knowledge gaps remain, especially for diseased states such as cystic fibrosis (CF). This study provides fundamental insights into Cas9 mRNA or ribonucleoprotein‐loaded LNP‐mucus interactions in healthy and diseased states by assessing the impact of the genetic cargo, mucin sialylation, mucin concentration, ionic strength, pH, and polyethylene glycol (PEG) concentration and nature on LNP diffusivity leveraging experimental approaches and Brownian dynamics (BD) simulations. Taken together, this study identifies key mucus and LNP characteristics that are critical to enabling a rational LNP design for transmucosal delivery.
Single Layer Silk and Cotton Woven Fabrics for Acoustic Emission and Active Sound Suppression
Authors: Yang Grace H. , Lin Jinuan , Cheung Henry , Rui Guanchun , Zhao Yongyi , Balachander Latika , Joo Taigyu , Lee Hyunhee , Smith Zachary P. , Zhu Lei , Ma Chu , Fink Yoel
Published: April 2024

Whether intentionally generating acoustic waves or attempting to mitigate unwanted noise, sound control is an area of challenge and opportunity. This study investigates traditional fabrics as emitters and suppressors of sound. When attached to a single strand of a piezoelectric fiber actuator, a silk fabric emits up to 70 dB of sound. Despite the complex fabric structure, vibrometer measurements reveal behavior reminiscent of a classical thin plate. Fabric pore size relative to the viscous boundary layer thickness is found—through comparative fabric analysis—to influence acoustic‐emission efficiency. Sound suppression is demonstrated using two distinct mechanisms. In the first, direct acoustic interference is shown to reduce sound by up to 37 dB. The second relies on pacifying the fabric vibrations by the piezoelectric fiber, reducing the amplitude of vibration waves by 95% and attenuating the transmitted sound by up to 75%. Interestingly, this vibration‐mediated suppression in principle reduces sound in an unlimited volume. It also allows the acoustic reflectivity of the fabric to be dynamically controlled, increasing by up to 68%. The sound emission and suppression efficiency of a 130 µm silk fabric presents opportunities for sound control in a variety of applications ranging from apparel to transportation to architecture.
Pyroelectric Photoconductive Diode for Highly Sensitive and Fast DUV Detection
Authors: Hou Xiaohu , Liu Yan , Bai Shiyu , Yu Shunjie , Huang Hong , Yang Kai , Li Chen , Peng Zhixin , Zhao Xiaolong , Zhou Xuanze , Xu Guangwei , Long Shibing
Published: April 2024

Detecting high‐energy photons from the deep ultraviolet (DUV) to X‐rays is vital in security, medicine, industry, and science. Wide bandgap (WBG) semiconductors exhibit great potential for detecting high‐energy photons. However, the implementation of highly sensitive and high‐speed detectors based on WBG semiconductors has been a huge challenge due to the inevitable deep level traps and the lack of appropriate device structure engineering. Here, a sensitive and fast pyroelectric photoconductive diode (PPD), which couples the interface pyroelectric effect with the photoconductive effect based on tailored polycrystal Ga‐rich GaOx (PGR‐GaOx) Schottky photodiode, is first proposed. The PPD device exhibits ultrahigh detection performance for DUV and X‐ray light. The responsivity for DUV light and sensitivity for X‐ray are up to 104 A W−1 and 105 µC Gyair−1 cm−2, respectively. Especially, the interface pyroelectric effect induced by polar symmetry in the depletion region of the PGR‐GaOx can significantly improve the response speed of the device by 105 times. Furthermore, the potential of the device is demonstrated for imaging enhancement systems with low power consumption and high sensitivity. This work fully excavates the potential of the pyroelectric effect for detectors and provides a novel design strategy to achieve sensitive and high‐speed detectors.
A Solid–Liquid Bicontinuous Fiber with Strain‐Insensitive Ionic Conduction
Authors: Ye Huating , Wu Baohu , Sun Shengtong , Wu Peiyi
Published: April 2024

Stretchable ionic conductors are crucial for enabling advanced iontronic devices to operate under diverse deformation conditions. However, when employed as interconnects, existing ionic conductors struggle to maintain stable ionic conduction under strain, hindering high‐fidelity signal transmission. Here, it is shown that strain‐insensitive ionic conduction can be achieved by creating a solid–liquid bicontinuous microstructure. A bicontinuous fiber from polymerization‐induced phase separation, which contains a solid elastomer phase interpenetrated by a liquid ion‐conducting phase, is fabricated. The spontaneous partitioning of dissolved salts leads to the formation of a robust self‐wrinkled interface, fostering the development of highly tortuous ionic channels. Upon stretch, these meandering ionic channels are straightened, effectively enhancing ionic conductivity to counteract the strain effect. Remarkably, the fiber retains highly stable ionic conduction till fracture, with only 7% resistance increase at 200% strain. This approach presents a promising avenue for designing durable ionic cables capable of signal transmission with minimal strain‐induced distortion.
Molecular Templates on Surfaces by Exploiting Supramolecular Chemistry in Langmuir–Blodgett Monolayers
Authors: Escorihuela Enrique , Concellón Alberto , Cardona Teresa , Zuccheri Giampaolo , Martín Santiago , Serrano José L. , Cea Pilar
Published: April 2024

Attaining precise control over molecular arrangements is of paramount importance for numerous applications in nanotechnology, particularly in constructing molecular templates to accurately immobilize target materials on surfaces. A strategic combination of supramolecular and interfacial chemistry may serve to build a well‐organized molecular network, enabling the subsequent location of target molecules on specific positions of a surface. A supramolecular complex (compound 1) comprised of a melamine unit forming hydrogen bonds with dendritic arms terminated in a coumarin unit is utilized, which readily undergoes photodimerization. The research demonstrates the formation of well‐organized Langmuir films of compound 1 which can be transferred on substrates at low surface pressures adopting a lying‐flat orientation. Upon irradiation of the pristine films at 365 nm the coumarin units undergo photo‐cross linking, leading to the formation of a compact photo‐crosslinked film. Incubation of these photo‐crosslinked films in a solution containing 1‐hexanethiol results in the withdrawal of the melamine and the chemisorption of two thiol molecules per each melamine unit. The nanopores created by the removal of the melamine core are attributed to the disruption of hydrogen bonds in compound 1 by the thiols. This precisely defined molecular network holds significant promise as a template for orchestrating the arrangement of functional materials on surfaces.
A Dual Mode MoTe2/WS2/WSe2 Double Van der Waals Heterojunctions Phototransistor for Optical Imaging and Communication
Authors: Li Zhongming , Zheng Tao , Yang Mengmeng , Sun Yiming , Luo Dongxiang , Gao Wei , Zheng Zhaoqiang , Li Jingbo
Published: April 2024

Van der Waals (vdW) heterostructures, formed by stacking different two‐dimensional (2D) materials, have emerged as a promising platform for next‐generation optoelectronic devices through band engineering. While various all‐2D and mixed‐dimensional heterojunction phototransistors based on p–n junctions or Schottky junctions have been developed, their performance, often constrained by the trade‐off between responsivity (R) and response speed, limits their widespread application. Here, a dual‐mode phototransistor based on a MoTe2/WS2/WSe2 double vdW heterostructure is designed. The bottom WSe2 layer effectively modulates the entire MoTe2/WS2 heterojunction channel, enabling both photoconductive and photovoltaic modes with exceptional optoelectronic properties in a single device. Specifically, the proposed device exhibits a maximum R of 2540 A W−1 and an impressive specific detectivity of 8 × 1012 Jones under the photoconductive mode. Under the photovoltaic mode, it achieves a fast response speed of 35.3/49.1 µs and a high light on/off ratio of 2 × 105. Additionally, the device exhibits latent potential for high‐resolution imaging across various wavelengths and fast optical communication. This work offers a rational alternative for achieving dual‐mode photodetection and highlights its promising application prospects in imaging and optical communication.
In Situ Hydrogel Modulates cDC1‐Based Antigen Presentation and Cancer Stemness to Enhance Cancer Vaccine Efficiency
Authors: Gao Tong , Yuan Shijun , Liang Shuang , Huang Xinyan , Liu Jinhu , Gu Panpan , Fu Shunli , Zhang Na , Liu Yongjun
Published: April 2024

Effective presentation of antigens by dendritic cells (DC) is essential for achieving a robust cytotoxic T lymphocytes (CTLs) response, in which cDC1 is the key DC subtype for high‐performance activation of CTLs. However, low cDC1 proportion, complex process, and high cost severely hindered cDC1 generation and application. Herein, the study proposes an in situ cDC1 recruitment and activation strategy with simultaneous inhibiting cancer stemness for inducing robust CTL responses and enhancing the anti‐tumor effect. Fms‐like tyrosine kinase 3 ligand (FLT3L), Poly I:C, and Nap‐CUM (NCUM), playing the role of cDC1 recruitment, cDC1 activation, inducing antigen release and decreasing tumor cell stemness, respectively, are co‐encapsulated in an in situ hydrogel vaccine (FP/NCUM‐Gel). FP/NCUM‐Gel is gelated in situ after intra‐tumoral injection. With the near‐infrared irradiation, tumor cell immunogenic cell death occurred, tumor antigens and immunogenic signals are released in situ. cDC1 is recruited to tumor tissue and activated for antigen cross‐presentation, followed by migrating to lymph nodes and activating CTLs. Furthermore, tumor cell stemness are inhibited by napabucasin, which can help CTLs to achieve comprehensive tumor killing. Collectively, the proposed strategy of cDC1 in situ recruitment and activation combined with stemness inhibition provides great immune response and anti‐tumor potential, providing new ideas for clinical tumor vaccine design.
Biomimetic Chiral Nanomaterials with Selective Catalysis Activity
Authors: Cao Honghui , Yang En , Kim Yoonseob , Zhao Yuan , Ma Wei
Published: April 2024

Chiral nanomaterials with unique chiral configurations and biocompatible ligands have been booming over the past decade for their interesting chiroptical effect, unique catalytical activity, and related bioapplications. The catalytic activity and selectivity of chiral nanomaterials have emerged as important topics, that can be potentially controlled and optimized by the rational biochemical design of nanomaterials. In this review, chiral nanomaterials synthesis, composition, and catalytic performances of different biohybrid chiral nanomaterials are discussed. The construction of chiral nanomaterials with multiscale chiral geometries along with the underlying principles for enhancing chiroptical responses are highlighted. Various biochemical approaches to regulate the selectivity and catalytic activity of chiral nanomaterials for biocatalysis are also summarized. Furthermore, attention is paid to specific chiral ligands, materials compositions, structure characteristics, and so on for introducing selective catalytic activities of representative chiral nanomaterials, with emphasis on substrates including small molecules, biological macromolecule, and in‐site catalysis in living systems. Promising progress has also been emphasized in chiral nanomaterials featuring structural versatility and improved chiral responses that gave rise to unprecedented chances to utilize light for biocatalytic applications. In summary, the challenges, future trends, and prospects associated with chiral nanomaterials for catalysis are comprehensively proposed.
Autonomously Self‐healing, Adhesive, and Stretchable Triboelectric Nanogenerator Using Multifunctional Hydrogel‐Elastomer Double Layer with a Power Management Circuit
Authors: Oh Jinseok , Kang Minkyong , Park Jae , Kim Tae Young , Park Kijun , Seo Jungmok
Published: April 2024

Triboelectric nanogenerators (TENGs) are promising candidates replacing conventional batteries in wearable devices, owing to their self‐powering properties. Although TENGs can convert mechanical energy into electrical energy, excessive mechanical stresses can degrade their performance. Moreover, conformal adhesion to skin is required to improve its performance in wearable devices. Here, a stretchable, adhesive, and self‐healing single‐electrode TENG with a multifunctional hydrogel‐elastomer double layer is developed. Carbon nanotubes (CNTs)‐doped hydrogel is used as the electrode. Subsequently, the electrode is covered with an Ecoflex elastomer that acted as a triboelectrification layer. The soft tissue‐like properties of the hydrogel allow conformal adhesion to nonplanar skin, whereas the dynamic polymer network of the hydrogel endows toughness and ability to self‐heal (within 5 min) against external damage. The TENG demonstrates an output voltage and current peak at 180 V and 0.8 µA. Moreover, it can generate a maximum power peak at 37.8 mW m−2, which is sufficient to power small electronics like stopwatches and light‐emitting diodes, with a power management circuit. The proposed TENG devices can function as telecommunication touch panels via Morse code. Thus, this study presents a promising approach for advancing the flexible power supplies and self‐powered sensors that can be applied to wearable devices.
Effects of Calcination Conditions on the Structural and Electrochemical Behaviors of High‐Nickel, Cobalt‐Free LiNi0.9Mn0.1O2 Cathode
Authors: Lee Steven , Li Cheng , Manthiram Arumugam
Published: April 2024

Eliminating cobalt from high‐nickel layered oxide cathodes lowers the cost of lithium‐ion batteries for electric vehicles. However, cobalt‐free cathodes with high Mn4+ and Ni2+ contents are prone to Li/Ni mixing after synthesis, potentially compromising battery energy density, rate capability, and cycling stability. Without cobalt facilitating cation ordering in the layered structure, the degree of Li/Ni mixing in cobalt‐free cathodes depends heavily on the calcination conditions. In this study, a systematic exploration of calcination temperatures and LiOH ratio for LiNi0.9Mn0.1O2 (NM‐90) provides detailed insights into the optimal synthesis conditions for high‐capacity cobalt‐free cathodes with extended cycle life. Surprisingly, high Li/Ni mixing does not necessarily lead to poor cycling stability whereas low Li/Ni mixing does not guarantee a long cycle life. More importantly, although excessive calcination temperature can further decrease Li/Ni mixing, it does not necessarily enhance capacity. Instead, the pernicious effects from the H2 → H3 phase transition are amplified due to a pronounced two‐phase reaction. An extensive suite of chemical and structural characterization methods uncovers a correlation between elevated calcination temperature, phase transformation, cation ordering, and capacity fading behavior: “overcooking” high‐nickel, cobalt‐free cathodes induce structural arrangement toward that of LiNiO2, with exacerbated lattice distortion and surface instability accelerating capacity fade.
Working toward reunification in New South Wales: Professional perspectives on navigating complex systems
Authors: Collings Susan , McLaine Meredith , Ciftci Sarah , Luu Betty
Published: April 2024

Achieving timely “permanency” for children after statutory child removal has become a key policy driver internationally. In New South Wales, child protection reforms include prioritising reunification; introducing time frames for resolution of legal proceedings; and outsourcing a substantial proportion of casework to the non‐government sector. In assessing the viability of reunification, courts place responsibility for behaviour change on parents and obscure the role of systems in supporting these changes. Professionals, as actors within a complex system, have an insider perspective on factors that influence reunification. A qualitative study was undertaken to elicit the perspectives of professionals working with parents involved in care proceedings. A total of 29 caseworkers and lawyers took part in focus groups. Complexity theory was used as an interpretive framework, and thematic analysis was completed. Themes about barriers to reunification exposed the unintended consequences of change in a complex adaptive system. Far from making reunification more achievable by streamlining the legal process, changes introduced impediments in the form of role, goal and process confusion and low levels of professional confidence in their capacity to help parents and achieve predictable legal outcomes. These results strengthen calls for a different approach to confront system‐induced barriers. Embedding interagency collaboration, challenging risk narratives about parents and offering them dedicated services are areas that demand urgent attention in order to ensure no child, whose safety and best interests could be met by reunification, remains in care.
Structural white matter properties and cognitive resilience to tau pathology
Authors: Qiu Ting , Liu Zhen‐Qi , Rheault François , Legarreta Jon Haitz , Valcourt Caron Alex , St‐Onge Frédéric , Strikwerda‐Brown Cherie , Metz Amelie , Dadar Mahsa , Soucy Jean‐Paul , Pichet Binette Alexa , Spreng R. Nathan , Descoteaux Maxime , Villeneuve Sylvia ,   for the PREVENT‐AD Research Group
Published: April 2024

INTRODUCTION

We assessed whether macro‐ and/or micro‐structural white matter properties are associated with cognitive resilience to Alzheimer's disease pathology years prior to clinical onset.

METHODS

We examined whether global efficiency, an indicator of communication efficiency in brain networks, and diffusion measurements within the limbic network and default mode network moderate the association between amyloid‐β/tau pathology and cognitive decline. We also investigated whether demographic and health/risk factors are associated with white matter properties.

RESULTS

Higher global efficiency of the limbic network, as well as free‐water corrected diffusion measures within the tracts of both networks, attenuated the impact of tau pathology on memory decline. Education, age, sex, white matter hyperintensities, and vascular risk factors were associated with white matter properties of both networks.

DISCUSSION

White matter can influence cognitive resilience against tau pathology, and promoting education and vascular health may enhance optimal white matter properties.

Highlights

Aβ and tau were associated with longitudinal memory change over ∼7.5 years.

White matter properties attenuated the impact of tau pathology on memory change.

Health/risk factors were associated with white matter properties.
Antidepressant use in relation to dementia risk, cognitive decline, and brain atrophy
Authors: vom Hofe Ilse , Stricker Bruno H. , Vernooij Meike W. , Ikram M. Kamran , Ikram M. Arfan , Wolters Frank J.
Published: April 2024

INTRODUCTION

We aimed to assess the effect of antidepressant use on dementia risk, cognitive decline, and brain atrophy.

METHODS

In this prospective cohort study, we included 5511 dementia‐free participants (Mini‐Mental State Examination [MMSE] > 25) of the Rotterdam study (57.5% women, mean age 70.6 years). Antidepressant use was extracted from pharmacy records from 1991 until baseline (2002–2008). Incident dementia was monitored from baseline until 2018, with repeated cognitive assessment and magnetic resonance imaging (MRI) every 4 years.

RESULTS

Compared to never use, any antidepressant use was not associated with dementia risk (hazard ratio [HR] 1.14, 95% confidence interval [CI] 0.92–1.41), or with accelerated cognitive decline or atrophy of white and gray matter. Compared to never use, dementia risk was somewhat higher with tricyclic antidepressants (HR 1.36, 95% CI 1.01–1.83) than with selective serotonin reuptake inhibitors (HR 1.12, 95% CI 0.81–1.54), but without dose–response relationships, accelerated cognitive decline, or atrophy in either group.

DISCUSSION

Antidepressant medication in adults without indication of cognitive impairment was not consistently associated with long‐term adverse cognitive effects.

Highlights

Antidepressant medications are frequently prescribed, especially among older adults.

In this study, antidepressant use was not associated with long‐term dementia risk.

Antidepressant use was not associated with cognitive decline or brain atrophy.

Our results support safe prescription in an older, cognitively healthy population.
Early‐onset dementia and risk of hip fracture and major osteoporotic fractures
Authors: Matsumoto Shoya , Hosoi Tatsuya , Yakabe Mitsutaka , Fujimori Kenji , Tamaki Junko , Nakatoh Shinichi , Ishii Shigeyuki , Okimoto Nobukazu , Akishita Masahiro , Iki Masayuki , Ogawa Sumito
Published: April 2024

INTRODUCTION

There is limited knowledge about early‐onset dementia (EOD) on fracture risk.

METHODS

Individuals ages 50 to 64 were identified from the National Database of Health Insurance Claims and Specific Health Checkups of Japan (2012 to 2019). The association between EOD and fractures and the association between cholinesterase inhibitors for EOD and fractures were evaluated using logistic regression analyses.

RESULTS

We identified 13,614 EOD patients and 9,144,560 cognitively healthy individuals. The analysis revealed that EOD was associated with an increased risk of hip fractures (adjusted odds ratio, 95% confidence interval: 8.79, 7.37–10.48), vertebral fractures (1.73, 1.48–2.01), and major osteoporotic fractures (2.05, 1.83–2.30) over 3 years. The use of cholinesterase inhibitors was significantly associated with a reduction in hip fractures among EOD patients (0.28, 0.11–0.69).

DISCUSSION

EOD patients have a higher risk of osteoporotic fractures than cognitively healthy individuals. The use of cholinesterase inhibitors may reduce the risk of hip fracture among EOD patients.

Highlights

It is unknown whether early‐onset dementia (EOD) increases the risk of fractures.

We identified 13,614 individuals with EOD using a nationwide administrative database.

Patients with EOD have a higher risk of hip, vertebral, and major osteoporotic fractures.

The use of cholinesterase inhibitors may reduce hip fracture among patients with EOD.
Unlocking the Metalation Applications of TMP‐powered Fe and Co(II) bis(amides): Synthesis, Structure and Mechanistic Insights
Authors: Logallo Alessandra , Maddock Lewis C. H. , Mu Manting , Gravogl Lisa , Jin Na , Peñas‐Defrutos Marconi N. , Meyer Karsten , García‐Melchor Max , Hevia Eva
Published: April 2024

Typified by LiTMP and TMPMgCl.LiCl, (TMP=2,2,6,6‐tetramethylpiperidide), s‐block metal amides have found widespread applications in arene deprotonative metalation. On the contrary, transition metal amides lack sufficient basicity to activate these substrates. Breaking new ground in this field, here we present the synthesis and full characterisation of earth‐abundant transition metals M(TMP)2 (M=Fe, Co). Uncovering a new reactivity profile towards fluoroarenes, these amide complexes can promote direct M−H exchange processes regioselectively using one or two of their basic amide arms. Remarkably, even when using a perfluorinated substrate, selective C‐H metalation occurs leaving C−F bonds intact. Their kinetic basicity can be boosted by LiCl or NBu4Cl additives which enables formation of kinetically activated ate species. Combining spectroscopic and structural studies with DFT calculations, mechanistic insights have been gained on how these low polarity metalation processes take place. M(TMP)2 can also be used to access ferrocene and cobaltocene by direct deprotonation of cyclopentadiene and undergo efficient CO2 insertion of both amide groups under mild reaction conditions.
Distinguish MnO2/Mn2+ Conversion/ Zn2+ Intercalation/ H+ Conversion Chemistries at Different Potentials in Aqueous Zn||MnO2 Batteries
Authors: Li Chuan , Yuan Haonan , Liu Tong , Zhang Rong , Zhu Jiaxiong , Cui Huilin , Wang Yanbo , Cao Duanyun , Wang Donghong , Zhi Chunyi
Published: April 2024

The rechargeable aqueous Zn||MnO2 chemistry has been extensively explored, but its electrochemical reaction mechanisms, especially in the context of MnO2/Mn2+ conversion and Zn2+/H+ intercalation chemistry, remain not fully understood. Here, we designed an amphiphilic hydrogel electrolyte, which distinguished the MnO2/Mn2+ conversion, Zn2+ intercalation, and H+ intercalation and conversion processes at three distinct discharge plateaus of an aqueous Zn||MnO2 battery. The amphiphilic hydrogel electrolyte is featured with an extended electrochemical stability window up to 3.0 V, high ionic conductivity, Zn2+‐selective ion tunnels, and hydrophobic associations with cathode materials. This specifically designed electrolyte allows the MnO2/Mn2+ conversion reaction at a discharge plateau of 1.75 V. More interesting, the discharge plateaus of ~1.33 V, previously assigned as the co‐intercalation of Zn2+ and H+ ions in the MnO2 cathode, are specified as the exclusive intercalation of Zn2+ ions, leading to an ultra‐flat voltage plateau. Furthermore, with a distinct three‐step electrochemical energy storage process, a high areal capacity of 1.8 mAh cm−2 and high specific energy of 0.858 Wh cm−2, even at a low MnO2 loading mass of 0.5 mg cm−2 are achieved. To our knowledge, this is the first report to fully distinguish different mechanisms at different potentials in aqueous Zn||MnO2 batteries.
Recent Advances and Opportunities in Reactivating Inactive Lithium in Batteries
Authors: Li Qianya , Liu Hao , Wu Feng , Li Li , Ye Yusheng , Chen Renjie
Published: April 2024

The loss of active materials is one of the main culprits of the battery failures. As a typical example, the presence of inactive lithium, also known as “dead lithium”, contributes to the rapid capacity deterioration and reduces energy output in lithium batteries. This phenomenon has long been recognized as irreversible. In this Minireview, the first of this kind, we aim to summarize the formation of inactive lithium and reassess its impact on battery performance metrics. Additionally, we explore various strategies that have been devised to rejuvenate inactive lithium. This comprehensive overview of the latest advancements in reactivating inactive lithium not only offers insights into restoring capacity and enhancing battery performance metrics but also provides a foundation for future research in reviving other inactive materials found in next‐generation batteries, such as lithium metal batteries, lithium‐sulfur batteries, other alkali metal batteries, and liquid flow batteries.
Stereodivergent Synthesis of Spiroaminals via Chiral Bifunctional Hydrogen Bonding Organocatalysis
Authors: Gayen Prasenjit , Sar Suman , Ghorai Prasanta
Published: April 2024

Spiroaminals represent novel structural motifs prevalent in diverse natural products and biologically active molecules. Achieving their enantioselective synthesis is a highly desirable and challenging task in synthetic endeavors due to their intricate molecular frameworks. Herein, we accomplished the first stereodivergent construction of spiroaminals using chiral bifunctional organocatalyzed intramolecular 1,2‐addition followed by an oxa‐Michael addition cascade in a high atom and step economical pathway. A proper modulation of the cinchona‐derived squaramide catalysts efficiently provided access to all the possible stereoisomers with high yield, diastereoselectivity, and excellent enantioselectivity while displaying a broad substrate tolerance. Additionally, we validated the scalability of the reaction and demonstrated the synthesis of variable spiroaminal scaffolds, confirming the viability of our protocol.