bluuebunny/crossref_metadata_2025_split huggingface dataset:
Dual‐Shelled Hollow Leafy Carbon Support with Atomically Dispersed (N,S)‐Bridged Hydroxy‐Coordinated Asymmetric Fe Sites for Oxygen Reduction
Authors: Yuan Min , Liu Yang , Du Yunmei , Xiao Zhenyu , Li Hongdong , Liu Kang , Wang Lei 
Published: April 2024

AbstractSingle‐atom catalysts (SACs) are widely studied in various chemical transformations due to their high catalytic activity and atom utilization. However, modulating the catalytic performance of catalysts by adjusting the microenvironment remains a great challenge. In this paper, a novel master‐double guest vulcanization‐assisted strategy is reported for synthesizing Fe single‐atom catalysts on N,S codoped porous hollow leaf carbon (FeSA/N,S‐PHLC) with highly exposed FeN3SOH sites. Fe(mIm) (guest I) is loaded on the surface of ZIF‐L (host) and then trithiocyanuric acid (TCA, guest II) is bonded with Fe(mIm), and the resulting ZIF‐L@Fe(mIm)@TCA precursors can be converted to FeSA/N,S‐PHLC with controllable structures. In addition, XPS analysis yield an increase in pyridine N content in FeSA/N,S‐PHLC compared to FeSA/N‐PHLC. It can be demonstrated by theoretical calculations that the N,S‐coordinated axially hydroxy‐coordinated asymmetric Fe centers synergistically with the abundance of pyridinic nitrogen facilitate the adsorption and desorption of oxygen intermediates, and the 3d orbitals of the Fe active centers can be optimized. The prepared FeSA/N,S‐PHLC catalyst has a half‐wave potential (E1/2) of 0.91 V under alkaline conditions, and E1/2 = 0.75 V under acidic conditions. It shows excellent cycle stability (882 h) and power density (217 mW cm−2) in the assembly of zinc–air battery (ZABs) devices.
Artificial Muscles Based on Coiled Conductive Polymer Yarns
Authors: Hu Hongwei , Zhang Shengtao , Zhang Mengyang , Xu Jiawei , Salim Teddy , Li Yan , Hu Xinghao , Zhang Zhongqiang , Cheng Guanggui , Yuan Ningyi , Lam Yeng Ming , Ding Jianning 
Published: April 2024

AbstractLightweight artificial muscles with large strain and large stress output have great application prospects in robotics, rehabilitation, prosthetic, and exoskeletons. Despite the excellent performance of carbon nanotube‐based artificial muscles in recent years, their widespread use is hindered by the high manufacturing costs associated with carbon nanotubes. In this paper, the study introduces a novel approach by developing artificial muscles based on pure conductive polymer coiled yarns. This achievement is facilitated by the successful fabrication of high‐strength conductive polymer microfibers. Furthermore, the study elucidates the molecular structural changes occurring during electrochemical processes that induce a substantial radial volume expansion in the microfibers. The resultant anisotropic volume change is magnified by the coiled yarn, yielding a remarkable contractile strain exceeding 11% at a high stress of 5 MPa, equivalent to lifting loads more than 4000 times their own masses, all achieved with a low input voltage of 1 V. Additionally, these conductive polymer‐based artificial muscles exhibit hydration‐induced contraction up to 33%, with swift recovery through electrical heating, leveraging their intrinsic high conductivity. This breakthrough positions high‐performance conductive polymer microfibers as a promising cost‐effective alternative to carbon nanotubes, establishing them at the forefront of lightweight artificial muscles.
Hydrogen Bond Network Regulation in Electrolyte Structure for Zn‐based Aqueous Batteries
Authors: Sheng Dawei , Liu Xiaoxu , Yang Zhuo , Zhang Man , Li Yang , Ren Peipei , Yan Xueru , Shen Ze Xiang , Chao Dongliang 
Published: April 2024

AbstractElectrolyte regulation in Zn‐based aqueous batteries (ZABs) has been extensively reported, and a broad range of strategies has been proposed. However, there is currently a lack of systematic summaries and a comprehensive understanding of the impact of hydrogen bond (H‐bond) networks on electrolyte performance. This work presents the electrolyte structure model, encompassing solvation structure, electrolyte/Zn anode interface, and H‐bond network. Through emphasizing and summarizing the reconstruction, strengthening, and breaking of the H‐bond network within the electrolyte structure, various specific regulation strategies are identified, such as high Gutmann donor number solvent, organic co‐solvent, molecular crowding additives, structure‐breaking ions, and solid‐state design. A critical appraisal is then provided on the key performance metrics influenced by these regulation methods, including Coulomb efficiency, voltage hysteresis, freezing point, and lifespan. This work is expected to illustrate electrolyte structure design to improve the comprehensive performance of ZABs. Last, a data‐driven summary and outlook on hydrogen bond network regulation in electrolyte structure is provided, to objectively evaluate the overall performances of ZABs.
Impact of Amorphous LiF Coating Layers on Cathode‐Electrolyte Interfaces in Solid‐State Batteries
Authors: Hu Taiping , Xu Linhan , Dai Fuzhi , Zhou Guobing , Fu Fangjia , Wang Xiaoxu , Li Linsen , Ai Xinping , Xu Shenzhen 
Published: April 2024

AbstractHigh interfacial resistance between electrodes and solid‐state electrolyte is the major cause for the failure of all‐solid‐state Li‐ion batteries. Spontaneous (electro)chemical reactions and poor Li‐ion diffusion at the interfaces are closely related to this increased impedance. Although introducing a coating layer can mitigate interfacial reactions and structural reconstruction, it may also lead to poor Li‐ion diffusion. Balancing this trade‐off therefore is crucial for the design of coating layer materials. In this study, the impact of the amorphous LiF (a‐LiF) coating layer on interfacial structural reconstruction and Li‐ion diffusion at the LiCoO2/Li6PS5Cl solid‐state interface is explicitly elucidated via machine‐learning‐assisted molecular dynamics (MD) simulations. It is found that the a‐LiF can effectively protect the P‐S tetrahedron local structures in Li6PS5Cl but cannot suppress the formation of side product S2 dimers. It is further discovered that once the a‐LiF coating exceeds a certain critical thickness, emergence of ordered local structures will inhibit Li‐ion diffusion. The simulations propose that the optimal thickness of the coating layer is around 1 nm. Overall, the work provides a microscopic understanding for effects of the a‐LiF coating layer on the structural and kinetic properties of cathode‐solid electrolyte interfaces and can guide the design of interfacial coating materials for solid‐state batteries.
Macrophage‐Derived Nanosponges Adsorb Cytokines and Modulate Macrophage Polarization for Renal Cell Carcinoma Immunotherapy
Authors: Jiang Yao , Nie Disen , Hu Zhihao , Zhang Chao , Chang Lingdi , Li Yu , Li Zhengxuan , Hu Wei , Li Hongji , Li Sikai , Xu Chao , Liu Shaojie , Yang Fa , Wen Weihong , Han Donghui , Zhang Keying , Qin Weijun 
Published: April 2024

AbstractRenal cell carcinoma (RCC) is a hot tumor infiltrated by large numbers of CD8+ T cells and is highly sensitive to immunotherapy. However, tumor‐associated macrophages (TAMs), mainly M2 macrophages, tend to undermine the efficacy of immunotherapy and promote the progression of RCC. Here, macrophage‐derived nanosponges are fabricated by M2 macrophage membrane‐coated poly（lactic‐co‐glycolic acid）（PLGA）, which could chemotaxis to the CXC and CC chemokine subfamily‐enriched RCC microenvironment via corresponding membrane chemokine receptors. Subsequently, the nanosponges act like cytokine decoys to adsorb and neutralize broad‐spectrum immunosuppressive cytokines such as colony stimulating factor‐1(CSF‐1), transforming growth factor‐β（TGF‐β）, and Lnterleukin‐10（IL‐10）, thereby reversing the polarization of M2‐TAMs toward the pro‐inflammatory M1 phenotype, and enhancing the anti‐tumor effect of CD8+ T cells. To further enhance the polarization reprogramming efficiency of TAMs, DSPE‐PEG‐M2pep is conjugated on the surface of macrophage‐derived nanosponges for specific recognition of M2‐TAMs, and the toll like receptors 7/8（TLR7/8） agonist, R848, is encapsulated in these nanosponges to induce M1 polarization, which result in significant efficacy against RCC. In addition, these nanosponges exhibit undetectable biotoxicity, making them suitable for clinical applications. In summary, a promising and facile strategy is provided for immunomodulatory therapies, which are expected to be used in the treatment of tumors, autoimmune diseases, and inflammatory diseases.
Injectable Inflammation‐Responsive Hydrogels for Microenvironmental Regulation of Intervertebral Disc Degeneration
Authors: Liu Lei , Wang Wantao , Huang Lin , Xian Yiwen , Ma Wenzheng , Zhao Lei , Li Yixi , Zheng Zhaomin , Liu Hongmei , Wu Decheng 
Published: April 2024

AbstractChronic local inflammation and excessive cell apoptosis in nucleus pulposus (NP) tissue are the main causes of intervertebral disc degeneration (IDD). Stimuli‐responsive hydrogels have great potential in the treatment of IDD by facilitating localized and controlled drug delivery. Herein, an injectable drug‐loaded dual stimuli‐responsive adhesive hydrogel for microenvironmental regulation of IDD, is developed. The gelatin methacryloyl is functionalized with phenylboronic acid groups to enhance drug loading capacity and enable dual stimuli‐responsive behavior, while the incorporation of oxidized hyaluronic acid further improves the adhesive properties. The prepared hydrogel exhibits an enhanced drug loading capacity for diol‐containing drugs, pH‐ and reactive oxygen species (ROS)‐responsive behaviors, excellent radical scavenging efficiency, potent antibacterial activity, and favorable biocompatibility. Furthermore, the hydrogel shows a beneficial protective efficacy on NP cells within an in vitro oxidative stress microenvironment. The in vivo results demonstrate the hydrogel's excellent therapeutic effect on treating IDD by maintaining water retention, restoring disc height, and promoting NP regeneration, indicating that this hydrogel holds great potential as a promising therapeutic approach for regulating the microenvironment and alleviating the progression of IDD.
Hydrogen Bonds Induced Ultralong Stability of Conductive π–d Conjugated FeCo3(DDA)2 with High OER Activity
Authors: Lin Lingtong , Zhang Caiyun , Liang Congcong , Zhang Honggang , Wang Zeyan , Wang Peng , Zheng Zhaoke , Cheng Hefeng , Xing Danning , Dai Ying , Huang Baibiao , Liu Yuanyuan 
Published: April 2024

AbstractConductive π–d conjugated metal–organic frameworks (MOFs) have attracted wide concerns in electrocatalysis due to their intrinsic high conductivity. However, the poor electrocatalytic stability is still a major problem that hinders the practical application of MOFs. Herein, a novel approach to enhancing the stability of MOF‐based electrocatalyst, namely, the introduction of hydrogen bonds (H‐bonds), is reported. Impressively, the π–d conjugated MOF FeCo3(DDA)2 (DDA = 1,5‐diamino‐4,8‐dihydroxy‐9,10‐anthraceneedione) exhibits ultrahigh oxygen evolution reaction (OER) stability (up to 2000 h). The experimental studies demonstrate that the presence of H‐bonds in FeCo3(DDA)2 is responsible for its ultrahigh OER stability. Besides that, FeCo3(DDA)2 also displays a prominent OER activity (an overpotential of 260 mV vs reversible hydrogen electrode (RHE) at a current density of 10 mA cm−2 and a Tafel slope of 46.86 mV dec−1). Density functional theory (DFT) calculations further indicate that the synergistic effect of the Fe and Co sites in FeCo3(DDA)2 contributes to its prominent OER performance. This work provides a new avenue of boosting the electrocatalytic stability of conductive π–d conjugated MOFs.
Topological Defect‐Regulated Porous Carbon Anodes with Fast Interfacial and Bulk Kinetics for High‐Rate and High‐Energy‐Density Potassium‐Ion Batteries
Authors: Huang Junlong , Chen Yongqi , Cen Zongheng , Yi Tan , Liang Min , Zhu Youlong , Liu Ruliang , Fu Ruowen , Liu Shaohong , Wu Dingcai 
Published: April 2024

AbstractCarbonaceous materials are regarded as one of the most promising anodes for potassium‐ion batteries (PIBs), but their rate capabilities are largely limited by the slow solid‐state potassium diffusion kinetics inside anode and sluggish interfacial potassium ion transfer process. Herein, high‐rate and high‐capacity PIBs are demonstrated by facile topological defect‐regulation of the microstructure of carbon anodes. The carbon lattice of the as‐obtained porous carbon nanosheets (CNSs) with abundant topological defects (TDPCNSs) holds relatively high potassium adsorption energy yet low potassium migration barrier, thereby enabling efficient storage and diffusion of potassium inside graphitic layers. Moreover, the topological defects can induce preferential decomposition of anions, leading to the formation of high potassium ion conductive solid electrolyte interphase (SEI) film with decreased potassium ion de‐solvation and transfer barrier. Additionally, the dominant sp2‐hybridized carbon conjugated skeleton of TDPCNSs enables high electrical conductivity (39.4 S cm−1) and relatively low potassium storage potential. As a result, the as‐constructed TDPCNSs anode demonstrates high potassium storage capacity (504 mA h g−1 at 0.1 A g−1), remarkable rate capability (118 mA h g−1 at 40 A g−1), as well as long‐term cycling stability.
Unravelling the Ageing Effects of PDMS‐Based Triboelectric Nanogenerators
Authors: Xu Tianhuai , Ye Jiahao , Tan Jin‐Chong 
Published: April 2024

AbstractAgeing of elastomeric materials in triboelectric nanogenerators (TENGs) often leads to compromised electrical performance and can greatly affect their real‐world application as next‐generation energy harvesters and self‐powered sensors. Herein, the ageing behavior of PDMS‐based TENGs is investigated by probing the dielectric and mechanical properties of the membrane materials. Over time, ageing of PDMS after 17 months is evinced by a decline by 71%, 68% and 52% in open‐circuit voltage, short‐circuit current and charge transfer, respectively, and an increase by 6.8 times in surface charge decay rate. The reduced electrical performance can be attributed to a decrease in work function, dielectric constant, surface adhesion and heterogeneity in stiffness, as well as an increase in loss tangent. The effect of chemical chain scission on the PDMS surface is confirmed through nearfield infrared nanospectroscopy. This study gives insights into the underlying mechanism behind the ageing of PDMS‐based TENGs, paving the way to future work for ameliorating these ageing‐related issues with the aim to ensure long‐term stability of practical triboelectric devices.
R‐Vine Copulas for Data‐Driven Quantification of Descriptor Relationships in Porous Materials
Authors: Neumann Matthias , Gräfensteiner Phillip , Machado Charry Eduardo , Hirn Ulrich , Hilger André , Manke Ingo , Schennach Robert , Schmidt Volker , Zojer Karin 
Published: April 2024

AbstractLocal variations in the 3D microstructure can control the macroscopic behavior of heterogeneous porous materials. For example, the permittivity through porous sheets or membranes is governed by local high‐volume pathways or bottlenecks. Due to local variations, unfeasibly large amounts of microstructure data may be needed to reliably predict such material properties directly from image data. Here it is demonstrated that a vine copula approach provides parametric models for local microstructure descriptors that compactly capture the 3D microstructure including its local variations and efficiently probe it with respect to selected, measurable properties. In contrast to common methods of complexity reduction, the proposed approach creates parametric models for the multivariate probability distribution of high‐dimensional descriptor vectors that inherently contain the complex, nonlinear dependencies between these descriptors. Therein, material properties are offered in physically motivated distributions of microstructure descriptors rather than as normally distributed data. Applied to porous fiber networks (paper) before and after unidirectional compression, it is shown that the copula‐based models reveal material‐characteristic relationships between two or more microstructure descriptors. In this way, the presented modeling approach can provide deeper insight into the microscopic origin of effective macroscopic properties of heterogeneous porous materials.
Magnetic Nanoparticle‐Assisted Non‐Viral CRISPR‐Cas9 for Enhanced Genome Editing to Treat Rett Syndrome
Authors: Cho Hyeon‐Yeol , Yoo Myungsik , Pongkulapa Thanapat , Rabie Hudifah , Muotri Alysson R. , Yin Perry T. , Choi Jeong‐Woo , Lee Ki‐Bum 
Published: April 2024

AbstractThe CRISPR‐Cas9 technology has the potential to revolutionize the treatment of various diseases, including Rett syndrome, by enabling the correction of genes or mutations in human patient cells. However, several challenges need to be addressed before its widespread clinical application. These challenges include the low delivery efficiencies to target cells, the actual efficiency of the genome‐editing process, and the precision with which the CRISPR‐Cas system operates. Herein, the study presents a Magnetic Nanoparticle‐Assisted Genome Editing (MAGE) platform, which significantly improves the transfection efficiency, biocompatibility, and genome‐editing accuracy of CRISPR‐Cas9 technology. To demonstrate the feasibility of the developed technology, MAGE is applied to correct the mutated MeCP2 gene in induced pluripotent stem cell‐derived neural progenitor cells (iPSC‐NPCs) from a Rett syndrome patient. By combining magnetofection and magnetic‐activated cell sorting, MAGE achieves higher multi‐plasmid delivery (99.3%) and repairing efficiencies (42.95%) with significantly shorter incubation times than conventional transfection agents without size limitations on plasmids. The repaired iPSC‐NPCs showed similar characteristics as wild‐type neurons when they differentiated into neurons, further validating MAGE and its potential for future clinical applications. In short, the developed nanobio‐combined CRISPR‐Cas9 technology offers the potential for various clinical applications, particularly in stem cell therapies targeting different genetic diseases.
Cascade Reactions Catalyzed by Gold Hybrid Nanoparticles Generate CO Gas Against Periodontitis in Diabetes
Authors: Wang Yi , Chu Tengda , Jin Ting , Xu Shengming , Zheng Cheng , Huang Jianmin , Li Sisi , Wu Lixia , Shen Jianliang , Cai Xiaojun , Deng Hui 
Published: April 2024

AbstractThe treatment of diabetic periodontitis poses a significant challenge due to the presence of local inflammation characterized by excessive glucose concentration, bacterial infection, and high oxidative stress. Herein, mesoporous silica nanoparticles (MSN) are embellished with gold nanoparticles (Au NPs) and loaded with manganese carbonyl to prepare a carbon monoxide (CO) enhanced multienzyme cooperative hybrid nanoplatform (MSN‐Au@CO). The Glucose‐like oxidase activity of Au NPs catalyzes the oxidation of glucose to hydrogen peroxide (H2O2) and gluconic acid，and then converts H2O2 to hydroxyl radicals (•OH) by peroxidase‐like activity to destroy bacteria. Moreover, CO production in response to H2O2, together with Au NPs exhibited a synergistic anti‐inflammatory effect in macrophages challenged by lipopolysaccharides. The underlying mechanism can be the induction of nuclear factor erythroid 2‐related factor 2 to reduce reactive oxygen species, and inhibition of nuclear factor kappa‐B signaling to diminish inflammatory response. Importantly, the antibacterial and anti‐inflammation effects of MSN‐Au@CO are validated in diabetic rats with ligature‐induced periodontitis by showing decreased periodontal bone loss with good biocompatibility. To summarize, MSN‐Au@CO is fabricate to utilize glucose‐activated cascade reaction to eliminate bacteria, and synergize with gas therapy to regulate the immune microenvironment, offering a potential direction for the treatment of diabetic periodontitis.
Reaction Mechanism and Performance of Innovative 2D Germanane‐Silicane Alloys: SixGe1−xH Electrodes in Lithium‐Ion Batteries
Authors: Wei Shuangying , Hartman Tomáš , Mourdikoudis Stefanos , Liu Xueting , Wang Gang , Kovalska Evgeniya , Wu Bing , Azadmanjiri Jalal , Yu Ruizhi , Chacko Levna , Dekanovsky Lukas , Oliveira Filipa M. , Li Min , Luxa Jan , Jamali Ashtiani Saeed , Su Jincang , Sofer Zdeněk 
Published: April 2024

AbstractThe adjustable structures and remarkable physicochemical properties of 2D monoelemental materials, such as silicene and germanene, have attracted significant attention in recent years. They can be transformed into silicane (SiH) and germanane (GeH) through covalent functionalization via hydrogen atom termination. However, synthesizing these materials with a scalable and low‐cost fabrication process to achieve high‐quality 2D SiH and GeH poses challenges. Herein, groundbreaking 2D SiH and GeH materials with varying compositions, specifically Si0.25Ge0.75H, Si0.50Ge0.50H, and Si0.75Ge0.25H, are prepared through a simple and efficient chemical exfoliation of their Zintl phases. These 2D materials offer significant advantages, including their large surface area, high mechanical flexibility, rapid electron mobility, and defect‐rich loose‐layered structures. Among these compositions, the Si0.50Ge0.50H electrode demonstrates the highest discharge capacity, reaching up to 1059 mAh g−1 after 60 cycles at a current density of 75 mA g−1. A comprehensive ex‐situ electrochemical analysis is conducted to investigate the reaction mechanisms of lithiation/delithiation in Si0.50Ge0.50H. Subsequently, an initial assessment of the c‐Li15(SixGe1‐x)4 phase after lithiation and the a‐Si0.50Ge0.50 phase after delithiation is presented. Hence, this study contributes crucial insights into the (de)lithiation reaction mechanisms within germanane‐silicane alloys. Such understanding is pivotal for mastering promising materials that amalgamate the finest properties of silicon and germanium.
Alleviating Recombinant Tissue Plasminogen Activator‐induced Hemorrhagic Transformation in Ischemic Stroke via Targeted Delivery of a Ferroptosis Inhibitor
Authors: Geng Yan‐Qin , Qiu Li‐Na , Cheng Yuan‐Qiu , Li Juan‐Juan , Ma Yi‐Lin , Zhao Cheng‐Cheng , Cai Ying , Zhang Xue‐Bin , Chen Jieli , Pan Yu‐Chen , Wang Ke‐Rang , Yao Xiu‐Hua , Guo Dong‐Sheng , Wu Jia‐Ling 
Published: April 2024

AbstractIntravenous thrombolysis with recombinant tissue plasminogen activator (rtPA) is the primary treatment for ischemic stroke. However, rtPA treatment can substantially increase blood‐brain barrier (BBB) permeability and susceptibility to hemorrhagic transformation. Herein, the mechanism underlying the side effects of rtPA treatment is investigated and demonstrated that ferroptosis plays an important role. The ferroptosis inhibitor, liproxstatin‐1 (Lip) is proposed to alleviate the side effects. A well‐designed macrocyclic carrier, glucose‐modified azocalix[4]arene (GluAC4A), is prepared to deliver Lip to the ischemic site. GluAC4A bound tightly to Lip and markedly improved its solubility. Glucose, modified at the upper rim of GluAC4A, imparts BBB targeting to the drug delivery system owing to the presence of glucose transporter 1 on the BBB surface. The responsiveness of GluAC4A to hypoxia due to the presence of azo groups enabled the targeted release of Lip at the ischemic site. GluAC4A successfully improved drug accumulation in the brain, and Lip@GluAC4A significantly reduced ferroptosis, BBB leakage, and neurological deficits induced by rtPA in vivo. These findings deepen the understanding of the side effects of rtPA treatment and provide a novel strategy for their effective mitigation, which is of great significance for the treatment and prognosis of patients with ischemic stroke.