bluuebunny/crossref_metadata_2025 huggingface dataset:
Van der Waals Multilayered Films: Wafer‐Scale Synthesis and Applications in Electronics and Optoelectronics
Authors: Yun Seok Joon , Ko Hayoung , Park Sunny , Lee Byung Hoon , Kim Nahun , Duong Hai Phuong , Lee Yeojin , Kim Soo Min , Kim Ki Kang
Published: September 2024

2D materials possess significant potential across various applications, with physical and chemical properties that can be effectively modulated by their thickness, enabling tailored optimization for specific uses. For instance, 2D monolayers are ideal for transparent and flexible electronics, while 2D multilayers are more suitable for solar cells and high‐speed devices. Although scalable methods for synthesizing large‐area 2D materials and their applications have been developed, most research has focused on monolayers, with comparatively limited efforts directed toward multilayers. This review provides an overview of the emerging field of 2D multilayers, revisiting the analysis of layer‐dependent properties to determine the optimal material thickness for various applications. It introduces representative techniques for synthesizing 2D multilayer films and presents applications where multilayer structures demonstrate superior performance compared to monolayers, particularly in electronics and optoelectronics. The review advocates for the development of synthesis and integration methods for 2D multilayers, calling for a shift in research focus toward these materials to enhance their technological impact and unlock new industrial applications.
Single‐Atom Ti Decorated Carbon Black and Carbon Nanotubes: Modular Dual‐Carbon Electrode for Optimizing the Charge Transport Kinetics of Perovskite Solar Cells
Authors: Cheng Jiashuo , Ma Hongru , Shi Yanying , Liu Lida , Shang Wenzhe , Liu Wei , Li Siao , Li Wenrui , Wang Yudi , Shi Yantao
Published: September 2024

In the landscape of photovoltaic research, carbon‐based perovskite solar cells (C‐PSCs) have attracted widespread attention due to their outstanding stability. However, compared to metal‐based PSCs, their power conversion efficiency (PCE) lags markedly behind. The key lies in two primary factors: First, the inefficiency of the carbon electrode in transporting and collecting carriers; second, the energy level mismatch with adjacent functional layers. These problems increase both the charge transport resistance and the charge injection barriers, thereby diminishing the overall efficiency of the device. In this study, an effective strategy is presented to tackle this issue by developing modular C‐PSCs that utilize dual carbon electrodes and implement multiscale modulation. This approach specifically focuses on three crucial aspects: establishing a highly conductive network, ensuring sufficient interfacial contact, and achieving well‐matched energy band alignment. By synergistically incorporating 0D carbon black (CB) and 1D carbon nanotube (CNT) into dual carbon electrodes, a resilient conductive network with enhanced interfacial contact is established, creating favorable conditions for efficient carrier transfer. Additionally, the energy level structure of CB is meticulously adjusted at the molecular scale by introducing individually adsorbed titanium (Ti) atoms, effectively addressing the energy level mismatch with the hole transport layer (spiro‐OMeTAD), and notably reducing the charge injection barrier at the interface. Based on the above strategy, the PCE of the C‐PSCs has undergone a remarkable enhancement from 15.27% to 22.45%. Moreover, the device shows excellent stability, with its PCE retaining over 95% of the initial value even after 1000 h of continuous operation under one‐sun intensity.
Wavelength‐Selective Near‐Infrared Organic Upconversion Detectors for Miniaturized Light Detection and Visualization
Authors: Li Ning , Hu Xin , Lu Ying , Li Yiwei , Ren Mingyang , Luo Xi , Ji Yifan , Chen Qian , Sui Xiubao
Published: September 2024

Upconversion detectors monolithically combining a detection unit and a light emitting unit, enables light detection and visualization in a compact structure, promising great advances in miniaturized multifunctional optoelectronics. The detection range of upconversion detectors usually covers a broadband spectrum, limiting their use in spectroscopic fields. This work investigates two wavelength‐selective upconversion detectors made with organic semiconductors to realize narrowband near‐infrared (NIR) light detection and visualization dual function. Two non‐fullerene‐based NIR‐sensitive bulk‐heterojunctions (BHJs) are exploited to make wavelength‐selective upconversion detectors, achieving peak sensitivity at 860 and 890 nm, with full width at half maximum of 125 and 170 nm, respectively. Each NIR‐sensitive BHJ comprises a donor polymer and a non‐fullerene acceptor, both of which are selectively sensitive to NIR light. The cumulative analysis of the optical properties of the absorber and current–voltage characteristics of the device indicates that the wavelength selectivity stems mainly from the wavelength‐dependent absorption. In particular, the upconversion detectors exhibit wavelength‐selective electronic and optical dual‐readouts, which are appealing for miniaturized spectroscopic applications, including health monitoring, optical communication, and microbead imaging, paving the way for practical applications.
Surface Reconstruction of Perovskites with Organosilanes for High Performance and Highly Stable Solar Cells
Authors: Soliman Ahmed I. A. , Zhang Yiqing , Zhang Lin , Wu Haotian , Shan Shiqi , Zhou Yu , Xu Chang , Fu Weifei , Chen Hongzheng
Published: September 2024

Surface or interface engineering is one of the most effective strategies to improve the device performance and stability of perovskite solar cells (PSCs), owing to the fact that the defects are mainly located at the surface. Organosilanes are among the most promising surface modifiers due to their unique cross‐linking ability, which makes a robust layer to further protect the underneath perovskites. However, the influence of tail functional groups of organosilanes on the device performance and stability has never been systematically investigated. Herein, a series of organosilanes with different chain lengths, fluorination, and different interactions toward perovskite are applied to modify the perovskite. Tail functional groups that show passivation ability toward perovskite are demonstrated to effectively reduce trap densities and thus improve the power conversion efficiencies (PCEs), while the fluorinated functional groups are beneficial for high stability. Finally, PSCs based on 3,3,3‐trifluoropropyltrimethoxysilane (FPTMS) modification showed a high PCE of 23.0% with the best operational stability. The encapsulated device maintained 85% of the initial PCE after 1725 h under continuous 1 sun equivalent illumination in air. The work may provide important insights into designing modifiers for high‐performance PSCs with high stability.
Managing Crystallization and Phase Distribution via 2D Perovskite Seed Crystals for 2D‐3D Tin‐based Perovskite Solar Cells
Authors: Du Fenqi , Gu Hao , Jiang Wenye , Yang Wenhan , Lin Yuexin , Zhu Wenjing , Qin Xin , Xie Xianqiang , Bu Laju , Liu Xiaolong , Yang Shengchun , Liang Chao
Published: September 2024

Various popular large organic cations have been extensively used as the essential additives in the perovskite precursor solution due to their satisfactory passivation effect but may produce the low‐n value (n ≤ 2) 2D perovskite phases with undesired distribution. Meanwhile, the remaining easy oxidation of Sn2+ and the p‐type self‐doping in the perovskites are also detrimental to the ultimate photovoltaic properties and stability of tin (Sn)‐based perovskite solar cells (PSCs). Here, 3AMPYSnI4 crystals (3AMPY = 3‐(aminomethyl)pyridinium)) are designed and applied to adjust the crystallization process and the phase distribution of the Sn‐based perovskite. Consequently, the strong coordination interaction between 3AMPY2+ and 3D perovskite components and the introduced nucleation sites by 3AMPYSnI4 crystals not only decreases the low‐n value 2D phase and increases 3D perovskite phase, but also inhibits the oxidation of Sn2+ and the self‐p‐doping in the Sn‐based perovskites, resulting in lower trap density and non‐radiative recombination loss, faster carrier extraction and transfer, and higher stability for 2D‐3D Sn‐based PSCs. As a result, the optimized devices deliver an increased power conversion efficiency from an initial 10.91% to 13.28% and retain 96.0% of their original performance for more than 3000 h in the nitrogen (N2) atmosphere.
Electric Field Regulator Constructed by Magnetron Sputtering for Dendrite‐Free and Stable Zinc Metal Anode
Authors: Sun Mengxuan , Cheng Qi , Ren Xiaohe , Wang Nengze , Hu Lei , Gan Ziwei , Xiang Yong , Yan Zongkai , Jia Chunyang , Li Zhijie
Published: September 2024

Rechargeable aqueous zinc‐ion batteries (AZIBs) are considered to be one of the most promising devices in the next generation of energy storage systems. However, the uncontrolled growth of Zn dendrites during electroplating leads to rapid battery failure, which hinders the wide application of AZIBs. In this work, an Fe metal interface (FMI) with electric field regulation is designed on the Zn metal anode using a magnetron sputtering technology. The FMI layer with nanosheet array not only uniforms the surface electric field, but also adjusts the surface Zn2+ ion distribution to inhibit 2D diffusion. The strong orientation relationships of the FMI layer enhance the reversibility of Zn plating/stripping, improving the structural stability of the interface layer. Consequently, FMI@Zn symmetric cell exhibits ultra‐stable lifespan for over 6000 h (Cumulative plated capacity, CPC = 15 Ah cm−2) with a low voltage hysteresis of 46.4 mV and high Coulombic efficiency of 99.8% at 5 mA cm−2. Even at the large current density of 40 mA cm−2, the CPC reaches 19.7 Ah cm−2. The proposed electric field regulation strategy reveals a promising prospect for designing highly stable Zn anode, which also applies to other metal anodes in energy storage systems.
Tailoring the Gating Effect of Organic Cage via a Porous Liquid Approach
Authors: Li Errui , Ganesan Arvind , Qiu Liqi , Liu Hongjun , Ivanov Alexander S. , He Lilin , Nalaoh Phattananawee , Jenkins David M. , Wang Tao , Kim Ellie , Jiang De‐en , Mahurin Shannon M. , Yang Zhenzhen , Dai Sheng
Published: September 2024

Porous liquids (PLs) represent a new frontier in material design combining the merits of solid porous host and liquid phase in gas separation and catalysis. Herein, the PL construction approach is harnessed to tailor the gating effect of organic cages toward enhanced gas separation. A type‐II fluorinated PL (F‐PL) is developed via liquifying a fluorinated organic cage (F‐cage) by a fluorinated ionic liquid (F‐IL). The F‐cage is featured by a small window size (≈5.1 Å), high surface area, good stability under highly ionic conditions, and abundant fluorine moieties. The F‐IL possesses high steric hindrance (bulky cation) and structure similarity with the F‐cage (fluorinated alkyl chain in the anion). The existing status structure integrity of F‐cage in F‐IL upon F‐PL formation is illustrated via spectroscopy and X‐ray‐based techniques. The existence of rigid voids in F‐PL is illustrated by positron annihilation lifetime spectroscopy (PALS) and the improved gas uptake capacity than F‐IL via pressure‐swing CO2 uptake isotherms (0−40) bar. The comparison of the gas uptake behavior (CO2, N2, CH4, and Xe) of F‐PL and F‐cage, combining the computational simulation, highlights that the PL construction can be leveraged to tune the window size of porous scaffolds, leading to enhanced gas selectivity.
Nanomaterials: Recent Advances in Knee Osteoarthritis Treatment
Authors: Peng Yufeng , Wang Ying , Bai Ru , Shi Kejian , Zhou Huige , Chen Chunying
Published: September 2024

Osteoarthritis (OA) of the knee is the most prevalent degenerative joint condition that places a substantial financial and medical burden on society. However, due to drawbacks such as inefficiency, adverse effects, and brief duration of action, the clinical efficacy of the current major therapies for knee OA is largely restricted. Therefore, novel medication development is highly required to address these issues. Numerous studies in recent years have established that nanomaterials can be a potential and highly effective way to overcome these challenges. In this review, the anatomical distinctions between healthy and OA knee joints, as well as novel advances in the field of nanomaterials for the treatment of knee OA are summarized. The limits of the present therapeutic strategies for treating knee OA are also highlighted, as well as the potential prospects of nanomaterials in the future.
Ions‐induced Assembly of Perovskite Nanocomposites for Highly Efficient Light‐Emitting Diodes with EQE Exceeding 30%
Authors: Xing Zhaohui , Jin Guangrong , Du Qing , Pang Peiyuan , Liu Tanghao , Shen Yang , Zhang Dengliang , Yu Bufan , Liang Yue , Yang Dezhi , Tang Jianxin , Wang Lei , Xing Guichuan , Chen Jiangshan , Ma Dongge
Published: September 2024

Metal halide perovskites, a cost‐effective class of semiconductos, hold great promise for display technologies that demand high‐efficiency, color‐pure light‐emitting diodes (LEDs). Early research on three‐dimensional (3D) perovskites showed low radiative efficiencies due to modest exciton binding energies. To inprove luminescence, reducing dimensionality or grain size has been a common approach. However, dividing the perovskite lattice into smaller units may hinder carrier transport, compromising electrical performance. Moreover, the increased surface area introduce additional surface trap states, leading to greater non‐radiative recombination. Here, an ions‐induced growth method is employed to assembe lattice‐anchored perovskite nanocomposites for efficient LEDs with high color purity. This approach enables the nanocomposite thin films, composed of 3D CsPbBr3 and its variant of zero‐dimensional (0D) Cs4PbBr6, to feature significant low trap‐assisted nonradiative recombination, enhanced light out‐coupling with a corrugated surface, and well‐balanced charge carrier transport. Based on the resultant 3D/0D perovskite nanocomposites, the perovskite LEDs (PeLEDs) achieving an remarkable external quantum efficiency of 31.0% at the emission peak of 521 nm with a narrow full width at half‐maximum of only 18 nm. This sets a new benchmark for color purity in high performance PeLED research, highlighting the significant advantage of this approach.
Flexible Neural Interface From Non‐Transient Silk Fibroin With Outstanding Conformality, Biocompatibility, and Bioelectric Conductivity
Authors: Hu Zhanao , Liang Yuqing , Fan Suna , Niu Qianqian , Geng Jingjing , Huang Qimei , Hsiao Benjamin S. , Chen Hao , Yao Xiang , Zhang Yaopeng
Published: September 2024

Silk fibroin (SF) with good biocompatibility can enable an efficient and safe implementation of neural interfaces. However, it has been difficult to achieve a robust integration of patterned conducting materials (multichannel electrodes) on flexible SF film substrates due to the absence of some enduring interactions. In this study, a thermo‐assisted pattern‐transfer technique is demonstrated that can facilely transfer a layer of pre‐set poly(3,4‐ethylenedioxythiophene) (PEDOT) onto the flexible SF substrate through an interpenetrating network of 2 polymer chains, achieving a desired substrate/conductor intertwined interface with good flexibility (≈33 MPa), conductivity (386 S cm−1) and stability in liquid state over 4 months simultaneously. Importantly, this technique can be combined with ink‐jet printing to prepare a multichannel SF‐based neural interface for the electrocorticogram (ECoG) recording and inflammation remission in rat models. The SF‐based neural interface with satisfied tissue conformability, biocompatibility, and bioelectric conductivity is a promising ECoG acquisition tool, where the demonstrated approach can also be useful to develop other SF‐based flexible bioelectronics.
Programming Hydrogen Bonds for Reversible Elastic‐Plastic Phase Transition in a Conductive Stretchable Hydrogel Actuator with Rapid Ultra‐High‐Density Energy Conversion and Multiple Sensory Properties
Authors: Guo Ping , Zhang Zhaoxin , Qian Chengnan , Wang Ruofei , Cheng Lin , Tian Ye , Wu Huaping , Zhu Shuze , Liu Aiping
Published: September 2024

Smart hydrogels have recently garnered significant attention in the fields of actuators, human‐machine interaction, and soft robotics. However, when constructing large‐scale actuated systems, they usually exhibit limited actuation forces (≈2 kPa) and actuation speeds. Drawing inspiration from hairspring energy conversion mechanism, an elasticity‐plasticity‐controllable composite hydrogel (PCTA) with robust contraction capabilities is developed. By precisely manipulating intermolecular and intramolecular hydrogen‐bonding interactions, the material's elasticity and plasticity can be programmed to facilitate efficient energy storage and release. The proposed mechanism enables rapid generation of high contraction forces (900 kPa) at ultra‐high working densities (0.96 MJ m−3). Molecular dynamics simulations reveal that modifications in the number and nature of hydrogen bonds lead to a distinct elastic‐plastic transition in hydrogels. Furthermore, the conductive PCTA hydrogel exhibits multimodal sensing capabilities including stretchable strain sensing with a wide sensing range (1–200%), fast response time (180 ms), and excellent linearity of the output signal. Moreover, it demonstrates exceptional temperature and humidity sensing capabilities with high detection accuracy. The strong actuation power and real‐time sensory feedback from the composite hydrogels are expected to inspire novel flexible driving materials and intelligent sensing systems.
Spatial Control of Nickel Vacancies in Colloidal NiMgO Nanocrystals for Efficient and Stable All‐inorganic Quantum Dot Light‐Emitting Diodes
Authors: Jung Woon Ho , Kim Byong Jae , Choi Mahnmin , Lee Hyeonjun , Cho Hyunjin , Kwon Yong Woo , Choi Yeongho , Lee Hyo Geun , Yoon Jinha , Lee Keeyong , Oh Sang Ho , Cho Seong‐Yong , Lee Doh C. , Jeong Sohee , Lim Jaehoon
Published: September 2024

Colloidal quantum dot (QD)–based light‐emitting diodes (QD‐LEDs) have reached the pinnacle of quantum efficiency and are now being actively developed for next‐generation displays and brighter light sources. Previous research has suggested utilizing inorganic hole‐transport layers (HTLs) to explore brighter and more stable QD‐LEDs. However, the performance metrics of such QD‐LEDs with inorganic HTLs generally lag behind those of organic‐inorganic hybrid QD‐LEDs employing organic HTLs. In this study, colloidal NiMgO nanocrystals (NCs) with spatially controlled Mg are introduced as HTLs for realizing efficient and stable all‐inorganic QD‐LEDs. During the co‐condensation of Ni and Mg precursors to produce valence band‐lowered NiMgO NCs, incorporating ≈2% Mg into the NiO lattice creates additional Ni vacancies (VNi) within and on the NCs, influencing the hole concentration and mobility of the NiMgO NC films. Passivating the VNi exposed on the surface with magnesium hydroxide allows for tuning the electrical properties of the NiMgO NCs relative to those of an electron transport layer, allowing for a balanced charge supply and suppressed negative charging of the QDs. Optimized all‐inorganic QD‐LEDs employing NiMgO NCs achieved a peak external quantum efficiency of 16.4%, peak luminance of 269 455 cd m⁻2, and a half‐life of 462 690 h at 100 nit.
Single Atom Engineered Antibiotics Overcome Bacterial Resistance
Authors: Panáček David , Belza Jan , Hochvaldová Lucie , Baďura Zdeněk , Zoppellaro Giorgio , Šrejber Martin , Malina Tomáš , Šedajová Veronika , Paloncýová Markéta , Langer Rostislav , Zdražil Lukáš , Zeng Jianrong , Li Lina , Zhao En , Chen Zupeng , Xiong Zhiqiang , Li Ruibin , Panáček Aleš , Večeřová Renata , Kučová Pavla , Kolář Milan , Otyepka Michal , Bakandritsos Aristides , Zbořil Radek
Published: September 2024

The outbreak of antibiotic‐resistant bacteria, or “superbugs”, poses a global public health hazard due to their resilience against the most effective last‐line antibiotics. Identifying potent antibacterial agents capable of evading bacterial resistance mechanisms represents the ultimate defense strategy. This study shows that –the otherwise essential micronutrient– manganese turns into a broad‐spectrum potent antibiotic when coordinated with a carboxylated nitrogen‐doped graphene. This antibiotic material (termed NGA‐Mn) not only inhibits the growth of a wide spectrum of multidrug‐resistant bacteria but also heals wounds infected by bacteria in vivo and, most importantly, effectively evades bacterial resistance development. NGA‐Mn exhibits up to 25‐fold higher cytocompatibility to human cells than its minimum bacterial inhibitory concentration, demonstrating its potential as a next‐generation antibacterial agent. Experimental findings suggest that NGA‐Mn acts on the outer side of the bacterial cell membrane via a multimolecular collective binding, blocking vital functions in both Gram‐positive and Gram‐negative bacteria. The results underscore the potential of single‐atom engineering toward potent antibiotics, offering simultaneously a long‐sought solution for evading drug resistance development while being cytocompatible to human cells.
Routes to Bidirectional Cathodes for Reversible Aprotic Alkali Metal–CO2 Batteries
Authors: Cheng Yihao , Wang Yuxuan , Chen Biao , Han Xiaopeng , He Fang , He Chunnian , Hu Wenbin , Zhou Guangmin , Zhao Naiqin
Published: September 2024

Aprotic alkali metal–CO2 batteries (AAMCBs) have garnered significant interest owing to fixing CO2 and providing large energy storage capacity. The practical implementation of AAMCBs is constrained by the sluggish kinetics of the CO2 reduction reaction (CO2RR) and the CO2 evolution reaction (CO2ER). Because the CO2ER and CO2RR take place on the cathode, which connects the internal catalyst with the external environment. Building a bidirectional cathode with excellent CO2ER and CO2RR kinetics by optimizing the cathode's internal catalyst and environment has attracted most of the attention to improving the electrochemical performance of AAMCBs. However, there remains a lack of comprehensive understanding. This review aims to give a route to bidirectional cathodes for reversible AAMCBs, by systematically discussing engineering strategies of both the internal catalyst (atomic, nanoscopic, and macroscopic levels) and the external environment (photo, photo‐thermal, and force field). The CO2ER and CO2RR mechanisms and the “engineering strategies from internal catalyst to the external environment–cathode properties–CO2RR and CO2ER kinetics and mechanisms–batteries performance” relationship are elucidated by combining computational and experimental approaches. This review establishes a fundamental understanding for designing bidirectional cathodes and gives a route for developing reversible AAMCBs and similar metal–gas battery systems.
On‐Chip Synthesis of Quasi‐2D Semimetals from Multi‐Layer Chalcogenides
Authors: Cai Jun , Zhang Huairuo , Tan Yuanqiu , Sun Zheng , Wu Peng , Tripathi Rahul , Krylyuk Sergiy , Suhy Caleb , Kong Jing , Davydov Albert V. , Chen Zhihong , Appenzeller Joerg
Published: September 2024

Reducing the dimensions of materials from three to two, or quasi‐two, provides a fertile platform for exploring emergent quantum phenomena and developing next‐generation electronic devices. However, growing high‐quality, ultrathin, quasi2D materials in a templated fashion on an arbitrary substrate is challenging. Here, the study demonstrates a simple and reproducible on‐chip approach for synthesizing non‐layered, nanometer‐thick, quasi‐2D semimetals. In one implementation, this method starts with thin semiconducting InSe flakes of below 20 nm in thickness with nickel deposited on top, followed by a low‐temperature annealing step that results in a controlled transformation of the layered InSe to a non‐layered, crystalline semimetal via reaction with the laterally diffusing nickel. Atomic resolution microscopy reveals the transformed semimetal to be Ni3In2Se2 with a Kagome‐lattice structure. Moreover, it is demonstrated that this synthesis method is generalizable by transforming 2D layered chalcogenides such as SnS and SnSe employing Ni and Co to non‐layered semimetals, paving the way for engineering novel types of devices.
Unlocking Enhanced Light Harvesting in Perovskites: A Light‐Mediated Ligand Management Approach
Authors: Singh Siddharth , Ganguly Debarjya , Aggarwal Pooja , Govind Rao Vishal
Published: September 2024

Interfaces between nanocrystals and their stabilizing ligands in light‐harvesting devices are crucial for mediating energy transfer, essential for efficient solar energy conversion. In metal halide perovskites, a promising material for these devices, Förster resonance energy transfer (FRET) within perovskite/acceptor‐molecule complexes offers a pathway for optimized energy transfer. However, traditional methods for optimizing FRET in perovskite‐chromophore hybrids are based on static modifications. This study presents an innovative approach for light‐driven dynamic control of FRET, achieving an ≈14% enhancement in efficiency between CsPbBr3 nanocrystals (CPB NCs) and rhodamine B isothiocyanate (RITC) dye. UV light is utilized to reversibly regulate NC‐ligand binding and thus control the coupling between CPB NCs and RITC at their interface. This approach critically relies on strong NC–ligand interactions, such as the Pb─S bond between CPB NCs and RITC. Light exposure weakens the binding of surface ligands, allowing RITC, with its strong bond, to attach more effectively and promote enhanced energy transfer. This light‐activated control is absent with Rhodamine B (RhB) lacking ─NCS group, a strong binding motif. The findings reveal the importance of NC–ligand interactions in dynamically manipulating FRET with light. This pioneering method for nanoscale FRET control paves the way for more efficient light‐harvesting devices.
Ag‐Catalyzed Asymmetric 1,3‐Dipolar Cycloaddition of N‐2,2,2‐Trifluoroethylisatin Ketimines with Conjugated Exocyclic Double Bonds: Access to Pyrrolidines with Four Consecutive Stereocenters Including Two Adjacent Spiro‐Quaternary Centers
Authors: Liu Ji‐Hong , Zhang Yan‐Ping , Wang Zhen‐Hua , Lu Ji‐Hong , Yang Lei , You Yong , Zhao Jian‐Qiang , Zhou Ming‐Qiang , Yuan Wei‐Cheng
Published: September 2024

Ag‐catalyzed enantioselective 1,3‐dipolar cycloaddition of N‐2,2,2‐trifluoroethylisatin ketimines with conjugated exocyclic double bonds including α‐alkylidene succinimides and aurone derivatives was developed for the first time. Using a catalyst system consisting of a ferrocenyl P,N‐ligand and AgNO2, the reaction provides a facile method for the construction of chiral pyrrolidines bearing four consecutive stereocenters and two adjacent spiro‐quaternary chiral centers, as well as offers a direct route to structurally diverse enantioenriched CF3‐containing 3,2′‐pyrrolidinyl spirooxindole derivatives.
Spatiotemporal Analysis of Mesenchymal Stem Cells Fate Determination by Inflammatory Niche Following Soft Tissue Injury at a Single‐Cell Level
Authors: Kan Chen , Tan Zhenya , Wang Haitao , Wang Wei , Yang Jiazhao , Zhang Ya , Lu Xiaoling , Cheng Qirong , Chai Lanyi , Peng Chao , Zhu Jicheng , Zhu Chenghang , Wang Hailin , Zhan Li , Lin Keqiong , Liu Yakun , Zhang Lingqiang , Fan Haitao , Zheng Hong
Published: September 2024

Heterotopic ossification (HO), often arising in response to traumatic challenges, results from the aberrant osteochondral differentiation of mesenchymal stem cells (MSCs). Nevertheless, the impact of trauma‐induced inflammatory exposure on MSC fate determination remains ambiguous. In this study, the cellular diversity within inflammatory lesions is elucidated, comprising MSCs and several innate and adaptive immune cells. It is observed that quiescent MSCs transition into cycling MSCs, subsequently giving rise to chondrogenic (cMSC) and/or osteogenic (oMSC) lineages within the inflammatory microenvironment following muscle or tendon injuries, as revealed through single‐cell RNA sequencing (scRNA‐seq), spatial transcriptome and lineage tracing analysis. Moreover, these investigations demonstrate that neutrophils and natural killer (NK) cells enhance transition of quiescent MSCs into cycling MSCs, which is also controlled by M1 macrophages, a subpopulation of macrophages can also stimulate cMSC and oMSC production from cycling MSCs. Additionally, M2 macrophages, CD4+ and CD8+ T lymphocytes are found to promote chondrogenesis. Further analysis demonstrates that immune cells promotes the activation of signaling transducers and activators of transcription (STAT) pathway and phosphoinositide 3 (PI3K)/protein kinase B (AKT) pathway in MSC proliferation and osteochondral progenitors’ production, respectively. These findings highlight the dynamics of MSC fate within the inflammatory lesion and unveil the molecular landscape of osteoimmunological interactions, which holds promise for advancing HO treatment.
A ROS‐Responsive Lipid Nanoparticles Release Multifunctional Hydrogel Based on Microenvironment Regulation Promotes Infected Diabetic Wound Healing
Authors: Yang Hao , Lv Dongming , Qu Shanqiang , Xu Hailin , Li Shuting , Wang Zhiyong , Cao Xiaoling , Rong Yanchao , Li Xiaohui , Wu Honglin , Chen Yongfei , Zhu Jiayuan , Tang Bing , Hu Zhicheng
Published: September 2024

The continuous imbalance of the diabetic wound microenvironment is an important cause of chronic nonhealing, which manifests as a vicious cycle between excessive accumulation of reactive oxygen species (ROS) and abnormal healing. Regulating the microenvironment by suppressing wound inflammation, oxidative stress, and bacterial infection is a key challenge in treating diabetic wounds. In this study, ROS‐responsive hydrogels are developed composed of silk fibroin methacrylated (SFMA), modified collagen type III (rCol3MA), and lipid nanoparticles (LNPs). The newly designed hydrogel system demonstrated stable physicochemical properties and excellent biocompatibility. Moreover, the release of antimicrobial peptide (AMP) and puerarin (PUE) demonstrated remarkable efficacy in eradicating bacteria, regulating inflammatory responses, and modulating vascular functions. This multifunctional hydrogel is a simple and efficient approach for the treatment of chronic diabetic infected wounds and holds tremendous potential for future clinical applications.
Evolution and Domestication of a Novel Biosynthetic Gene Cluster Contributing to the Flavonoid Metabolism and High‐Altitude Adaptability of Plants in the Fagopyrum Genus
Authors: Huang Xu , He Yuqi , Zhang Kaixuan , Shi Yaliang , Zhao Hui , Lai Dili , Lin Hao , Wang Xiangru , Yang Zhimin , Xiao Yawen , Li Wei , Ouyang Yinan , Woo Sun Hee , Quinet Muriel , Georgiev Milen I. , Fernie Alisdair R. , Liu Xu , Zhou Meiliang
Published: September 2024

The diversity of secondary metabolites is an important means for plants to cope with the complex and ever‐changing terrestrial environment. Plant biosynthetic gene clusters (BGCs) are crucial for the biosynthesis of secondary metabolites. The domestication and evolution of BGCs and how they affect plant secondary metabolites biosynthesis and environmental adaptation are still not fully understood. Buckwheat exhibits strong resistance and abundant secondary metabolites, especially flavonoids, allowing it to thrive in harsh environments. A non‐canonical BGC named UFGT3 cluster is identified, which comprises a phosphorylase kinase (PAK), two transcription factors (MADS1/2), and a glycosyltransferase (UFGT3), forming a complete molecular regulatory module involved in flavonoid biosynthesis. This cluster is selected during Tartary buckwheat domestication and is widely present in species of the Fagopyrum genus. In wild relatives of cultivated buckwheat, a gene encoding anthocyanin glycosyltransferase (AGT), which glycosylates pelargonidin into pelargonidin‐3‐O‐glucoside, is found inserted into this cluster. The pelargonidin‐3‐O‐glucoside can help plants resist UV stress, endowing wild relatives with stronger high‐altitude adaptability. This study provides a new research paradigm for the evolutionary dynamics of plant BGCs, and offers new perspectives for exploring the mechanism of plant ecological adaptability driven by environmental stress through the synthesis of secondary metabolites.
Multi‐Zone Visco‐Node‐Pore Sensing: A Microfluidic Platform for Multi‐Frequency Viscoelastic Phenotyping of Single Cells
Authors: Lai Andre , Hinz Stefan , Dong Alan , Lustig Michael , LaBarge Mark A. , Sohn Lydia L.
Published: September 2024

This study introduces multi‐zone visco‐Node‐Pore Sensing (mz‐visco‐NPS), an electronic‐based microfluidic platform for single‐cell viscoelastic phenotyping. mz‐visco‐NPS implements a series of sinusoidal‐shaped contraction zones that periodically deform a cell at specific strain frequencies, leading to changes in resistance across the zones that correspond to the cell's frequency‐dependent elastic G′ and viscous G″ moduli. mz‐visco‐NPS is validated by measuring the viscoelastic changes of MCF‐7 cells when their cytoskeleton is disrupted. mz‐visco‐NPS is also employed to measure the viscoelastic properties of human mammary epithelial cells across the entire continuum of epithelial transformation states, from average‐ and high‐risk primary epithelial cells, to immortal non‐malignant (MCF‐10A), malignant (MCF‐7), and metastatic (MDA‐MB‐231) cell lines. With a throughput of 600 cells per hour and demonstrated ease‐of‐use, mz‐visco‐NPS reveals a remarkable level of single‐cell heterogeneity that would otherwise be masked by ensemble averaging.
Nucleic Acid Amplification Circuit‐Based Hydrogel (NACH) Assay for One‐Step Detection of Metastatic Gastric Cancer‐Derived Exosomal miRNA
Authors: Seo Seung Beom , Lim Jaewoo , Kim Kyujung , Maeng Inhee , Rho Hyun Wook , Son Hye Young , Kim Eunjung , Jang Eunji , Kang Taejoon , Jung Juyeon , Oh Seung Jae , Huh Yong‐Min , Lim Eun‐Kyung
Published: September 2024

Gastric cancer (GC) is recognized as the fifth most prevalent malignant tumor worldwide. It is characterized by diverse clinical symptoms, treatment responses, and prognoses. In GC prognosis, the promotion of epithelial–mesenchymal transition (EMT) fosters cancer cell invasion and metastasis, thereby triggering the dissemination of tumor cells. This study proposes a nucleic acid amplification circuit‐based hydrogel (NACH) assay for identifying exosomal miRNA derived from metastatic GC. The NACH assay employs the rolling circle amplification method and targets miRNA‐21, a tumor‐related oncogene, and miRNA‐99a, which promotes EMT. Specific amplification probes for each target are immobilized within the hydrogel, enabling a streamlined, one‐step amplification reaction. The NACH assay exhibits a detection limit of 1 fm for miRNA‐21 and miRNA‐99a, thereby enabling rapid and highly sensitive on‐site detection. Performance evaluation using exosomal miRNA extracted from cell culture media, mouse plasma, and human plasma revealed fluorescence intensity patterns similar to those obtained in qRT‐PCR. Furthermore, deploying a custom‐developed portable fluorometer for the NACH assay allows for diagnostic performance assessment and point‐of‐care testing using clinical samples from GC patients. These findings emphasize the potential of the NACH assay to be used as a robust tool for the genetic diagnosis of GC based on exosome detection.
A Three–Dimensional Nanoscale View of Electrocatalyst Degradation in Hydrogen Fuel Cells
Authors: Amichi Lynda , Yu Haoran , Ziabari Amirkoushyar , Rahman Obaidullah , Arregui‐Mena David , Hu Leiming , Neyerlin K. C. , Cullen David A.
Published: September 2024

The loss of platinum (Pt) electrochemically active surface area (ECSA) is a critical degradation mode that often becomes a limiting factor for heavy‐duty proton exchange membrane fuel cell vehicles. High surface area carbon supports have been shown to improve Pt dispersion and limit detrimental ionomer‐electrocatalyst interactions due to their large interior pore volume. In this work, using automated scanning transmission electron tomography, the degradation of nanoparticles located on the interior versus exterior surfaces of the carbon support is compared following a catalyst‐specific accelerated stress test (AST) of 90,000 voltage cycles between 0.6 V to 0.95 V. The results reveal a notable increase in median particle size for both interior and exterior Pt catalyst particles, with a slightly higher increase in particle size distribution and loss of specific surface area for the particles located on the exterior carbon surface. The fraction of Pt nanoparticles that reside within the interior of the carbon support also increased following the AST test, accompanied by evidence of an increase in average carbon mesopore size. The results shed light on the degradation mechanisms affecting electrochemical properties and the enhanced particle accessibility at lower relative humidity.
Molecular layer deposition of polyhydroquinone thin films for Li‐ion battery applications
Authors: Paranamana Nikhila C. , Datta Amit K. , Wyatt Quinton K. , Gettler Ryan C. , Werbrouck Andreas , Young Matthias J.
Published: September 2024

Many next‐generation materials for Li‐ion batteries are limited by material instabilities. To stabilize these materials, ultrathin, protective coatings are needed that conduct both lithium ions and electrons. Here, we demonstrate a hybrid chemistry combining molecular layer deposition (MLD) of trimethylaluminum (TMA) and p‐hydroquinone (HQ) with oxidative molecular layer deposition (oMLD) of molybdenum pentachloride (MoCl5) and HQ to enable vapor‐phase molecular layer growth of poly(p‐hydroquinone) (PHQ)—a mixed electron and lithium ion conducting polymer. We employ quartz crystal microbalance (QCM) studies to understand the chemical mechanism and demonstrate controlled linear growth with a 0.5 nm/cycle growth rate. Spectroscopic characterization indicates that this hybrid MLD/oMLD chemistry polymerizes surface HQ monomers from the TMA‐HQ chemistry to produce PHQ. The polymerization to PHQ improves air stability over MLD TMA‐HQ films without crosslinking. Electrochemical measurements on hybrid MLD/oMLD films indicate electronic conductivity of ~10−9 S/cm and a Li‐ion conductivity of ~10−4 S/cm. While these coatings show promise for Li‐ion battery applications, this work focuses on establishing the coating chemistry and future studies are needed to examine the stability, structure, and cycling performance of these coatings in full Li‐ion cells.
Cracking the physical insight of power law models: Bridging the gap between macroscopic kinetics and surface coverages
Authors: Vega‐Ramon Fernando , Rogers Alexander W. , Hardacre Christopher , Zhang Dongda
Published: September 2024

We propose a methodological framework to quantify the relative abundance of key surface intermediates via analysis of the macroscopic intrinsic kinetic characteristics of gas‐phase data. At the core of this approach is the development of analytical expressions, which link reaction orders and activation energies in macroscopic power law models to the fractional coverage of the non‐observable intermediates. Through the design of an advanced parameter estimation methodology, these relationships were further exploited to develop thermodynamically consistent and mechanistic‐based power law models which could capture the evolution of surface occupancy profiles along the reactor length. The developed framework was tested through in‐silico water gas shift reaction case‐studies; the results indicate the robustness of the approach and the mechanistic insight that can be gained from its application. The methodology proposed in this study could thus be of general value to assist in reaction mechanism analysis, identification of key surface intermediates, and reactor optimization.
Howler Monkey Die‐Off in Southern Mexico
Authors: Pozo‐Montuy Gilberto , Aguilar‐Cucurachi María del Socorro , Aureli Filippo , Briseño‐Jaramillo Margarita , Canales‐Espinosa Domingo , Cárdenas‐Navarrete Anaid , Cortés‐Ortiz Liliana , Coyohua‐Fuentes Alejandro , Espinosa‐Gómez Fabiola Carolina , Franquesa‐Soler Montserrat , García‐Duran Candelaria , García‐Ojeda Yuliana , González‐Acosta Mónica Rosario , Hermida‐Lagunes Javier , Hernández‐Salazar Laura Teresa , Jasso‐del‐Toro Cristina , Lizama‐Hernández José Alberto , Martínez‐Ramos Ileana Zorhaya , Montejo‐Zetina Edgar J. , Núñez‐Martínez Guadalupe , Nuñez‐Ramírez Paulina Y. , Pareja‐Badillo Pedro Shautamai , Pinacho‐Guendulain Braulio , Ramos‐Fernández Gabriel , Rangel‐Negrín Ariadna , Rivera‐Sánchez Alix Fernanda , Sánchez‐Domínguez Elizabeth , Serio‐Silva Juan Carlos , Smith‐Aguilar Sandra E. , Solórzano‐García Brenda , Spaan Denise , Van Belle Sarie , Dias Pedro A. D.
Published: September 2024

In May and June 2024, a die‐off of Mexican mantled howler monkeys (Alouatta palliata mexicana) occurred in southern Mexico. This commentary documents the event, attributing it to extreme heatwaves, drought, wildfires, and habitat impoverishment. Despite their reported resilience to habitat disturbances, mantled howler monkey mortality rate in some areas reached 31%. Key evidence points to heatstroke as the primary cause of death, exacerbated by limited hydration and reduced dietary diversity in disturbed habitats. Immediate responses included community‐led rescues (e.g., hydrating the monkeys), coordination of rescue activities by nongovernmental organizations (NGOs) (e.g., managing donations), involvement of scientists (e.g., monitoring of primate populations), and assistance from government officials (e.g., providing legal support for animal management). This event underscores the urgency of developing action plans to prevent and attend future crises. Among other actions, we highlight (i) establishing primate care infrastructure with medical and rehabilitation centers; (ii) developing protocols and training programs to ensure rapid crisis response; (iii) fostering collaboration among government, NGOs, and academic institutions for effective crisis management; and (iv) developing targeted research on climate change impacts, predictive models, and long‐term health monitoring. We emphasize the critical need for coordinated conservation efforts to protect wild primates and maintain natural ecosystem resilience in the face of escalating climate challenges.
Loss of TREM2 diminishes CAA despite an overall increase of amyloid load in Tg‐SwDI mice
Authors: Zhong Rui , Xu Yingzheng , Williams Jesse W. , Li Ling
Published: September 2024

INTRODUCTION

The microglial receptor triggering receptor expressed on myeloid cells 2 (TREM2) is a major risk factor for Alzheimer's disease (AD). Experimentally, Trem2 deficiency affects parenchymal amyloid beta (Aβ) deposition. However, the role of TREM2 in cerebrovascular amyloidosis, especially cerebral amyloid angiopathy (CAA), remains unexplored.

METHODS

Tg‐SwDI (SwDI) mice, a CAA‐prone model of AD, and Trem2 knockout mice were crossed to generate SwDI/TWT, SwDI/THet, and SwDI/TKO mice, followed by pathological and biochemical analyses at 16 months of age.

RESULTS

Loss of Trem2 led to a dramatic decrease in CAA and microglial association, despite a marked increase in overall brain Aβ load. Single nucleus RNA sequencing analysis revealed that in the absence of Trem2, microglia were activated but trapped in transition to the fully reactive state, with distinct responses of vascular cells.

DISCUSSION

Our study provides the first evidence that TREM2 differentially modulates parenchymal and vascular Aβ pathologies, offering significant implications for both TREM2‐ and Aβ‐targeting therapies for AD.

Highlights

Triggering receptor expressed on myeloid cells 2 (TREM2) differentially modulates brain parenchymal and vascular amyloidosis.

Loss of Trem2 markedly reduces cerebral amyloid angiopathy despite an overall increase of amyloid beta load in Tg‐SwDI mice.

Microglia are trapped in transition to the fully reactive state without Trem2.

Perivascular macrophages and other vascular cells have distinct responses to Trem2 deficiency.

Balanced TREM2‐targeting therapies may be required for optimal outcomes.
Self‐ and study partner–reported cognitive decline in older adults without dementia: The role of α‐synuclein and amyloid biomarkers in the Alzheimer's Disease Neuroimaging Initiative
Authors: Thomas Kelsey R. , Bangen Katherine J. , Rotblatt Lindsay J. , Weigand Alexandra J. , Edwards Lauren , Tosun Duygu , Galasko Douglas ,   for the Alzheimer's Disease Neuroimaging Initiative
Published: September 2024

INTRODUCTION

Subjective cognitive decline (SCD) may be an early marker of Alzheimer's disease (AD) pathology. Until recently, it was impossible to measure biomarkers specific for α‐synuclein pathology; therefore, its association with subjective reports of cognitive decline is unknown.

METHODS

Alzheimer's Disease Neuroimaging Initiative participants without dementia (n = 918) were classified as positive or negative for amyloid beta (Aβ+ or Aβ−) and α‐synuclein (α‐syn+ or α‐syn−) biomarkers. Self‐ and study partner–reported cognitive decline was measured with the Everyday Cognition (ECog) questionnaire.

RESULTS

Per self‐report, Aβ+/α‐syn+ had the greatest cognitive decline. Aβ−/α‐syn+ did not differ from Aβ−/α‐syn− across ECog scores. Study partner–reported results had a similar pattern, but Aβ+/α‐syn− and Aβ+/α‐syn+ did not differ across ECog scores. Mild cognitive impairment classification moderated the study partner–reported memory score.

DISCUSSION

While α‐syn+ alone did not increase subjective reports of cognitive decline, Aβ+/α‐syn+ had the most self‐ and study partner–rated cognitive decline. Therefore, the presence of multiple pathologies was associated with greater SCD.

Highlights

Cerebrospinal fluid α‐synuclein (α‐syn) seed amplification assay was used to determine α‐syn positivity.

Amyloid beta (Aβ)−/α‐syn−, Aβ−/α‐syn+, Aβ+/α‐syn−, and Aβ+/α‐syn+ biomarker groups were created.

Aβ+/α‐syn+ had greater subjective cognitive decline (SCD) than the other biomarker groups.

Aβ−/α‐syn+ did not differ from Aβ−/α‐syn− across self‐ or study–partner reported SCD scores.

Study partner–reported subjective memory results were largely driven by participants with mild cognitive impairment.
Atmosphere Induces Tunable Oxygen Vacancies to Stabilize Single‐Atom Copper in Ceria for Robust Electrocatalytic CO2 Reduction to CH4
Authors: Huang Fang , Chen Xiangyu , Sun Huanhuan , Zeng Qingduo , Ma Junjie , Wei Dong , Zhu Jinliang , Chen Zhengjun , Liang Taoyuan , Yin Xucai , Liu Xijun , Xu Jing , He Huibing
Published: September 2024

Electrochemical carbon dioxide reduction (ECO2RR) shows great potential to create high‐value carbon‐based chemicals, while designing advanced catalysts at the atomic level remains challenging. The ECO2RR performance is largely dependent on the catalyst microelectronic structure that can be effectively modulated through surface defect engineering. Here, we provide an atmosphere‐assisted low‐temperature calcination strategy to prepare a series of single‐atomic Cu/ceria catalysts with varied oxygen vacancy concentrations for robust electrolytic reduction of CO2 to methane. The obtained Cu/ceria catalyst under H2 environment (Cu/ceria‐H2) exhibits a methane Faraday efficiency (FECH4) of 70.03 % with a turnover frequency (TOFCH4) of 9946.7 h−1 at an industrial‐scale current density of 150 mA cm−2 in a flow cell. Detailed studies indicate the copious oxygen vacancies in the Cu/ceria‐H2 are conducive to regulating the surface microelectronic structure with stabilized Cu+ active center. Furthermore, density functional theory calculations and operando ATR‐SEIRAS demonstrate that the Cu/ceria‐H2 can markedly enhance the activation of CO2, facilitate the adsorption of pivotal intermediates *COOH and *CO, thus ultimately enabling the high selectivity for CH4 production. This study presents deep insights into designing effective electrocatalysts for CO2 to CH4 conversion by controlling the surface microstructure via the reaction atmosphere.