bluuebunny/crossref_metadata_2025_split huggingface dataset:
Combining Hard Shell with Soft Core to Enhance Enzyme Activity and Resist External Disturbances
Authors: Wang Yiwen , Tong Hongfei , Ni Shulan , Huo Kaiyuan , Liu Wenjie , Zan Xingjie , Yuan Xiaodie , Wang Shuangshuang 
Published: January 2025

AbstractImmobilizing enzymes onto solid supports having enhanced catalytic activity and resistance to harsh external conditions is considered as a promising and critical method of broadening enzymatic applications in biosensing, biocatalysis, and biomedical devices; however, it is considerably hampered by limited strategies. Here, a core–shell strategy involving a soft‐core hexahistidine metal assembly (HmA) is innovatively developed and characterized with encapsulated enzymes (catalase (CAT), horseradish peroxidase, glucose oxidase (GOx), and cascade enzymes (CAT+GOx)) and hard porous shells (zeolitic imidazolate framework (ZIF), ZIF‐8, ZIF‐67, ZIF‐90, calcium carbonate, and hydroxyapatite). The enzyme‐friendly environment provided by the embedded HmA proves beneficial for enhanced catalytic activity, which is particularly effective in preserving fragile enzymes that will have been deactivated without the HmA core during the mineralization of porous shells. The enzyme encapsulated within a core–shell particle exhibits noteworthy resilience against harsh external conditions, including heat, organic solvents, and proteinase K. Additionally, no significant alteration in the catalytic behavior of the enzyme is observed after multiple cycles of usage. This study offers a novel approach for immobilizing enzymes and rendering them resistant to harsh external conditions, with potential applications in diverse fields, including biocatalysis, bioremediation, and biomedical engineering.
Phase Transition Process of Graphite to Diamond Induced by Monodispersed Tantalum Atoms at Ordinary Pressure
Authors: Zhu Zhiguang , Chen Chengke , Lu Shaohua , Li Xiao , Hu Xiaojun 
Published: January 2025

AbstractThe transformation of graphite into diamond (2–10 nm) at ordinary pressure by monodispersed Ta atoms was recently reported, while the effects of Ta concentration on the transition process remain obscure. Here, by regulating the Ta wire treatment time, as well as the annealing time and temperature, larger diamond grians (5–20 nm) are successfully synthesized, and the transition process of graphite to diamond is revealed to vary with Ta concentration. Specifically, short Ta wire treatments (5–10 min) induce graphite to form a “circle” structure and transforms into diamond directly after annealing. Long Ta wire treatments (15–25 min) produce larger and more “circle” structures, containing an increased number of graphite layers. After annealing at 1100 °C for 30–120 min, graphite first transforms into amorphous carbon, then to i‐Carbon and n‐Diamond, and finally to diamond. Notably, a large amount of n‐Diamond and diamond are formed after 120 min annealing. By modulating the annealing temperature from 500 to 1200 °C for 30 min, diamond is already obtained at 500 °C, and hexagonal diamond up to 20 nm in size at 1200 °C. This provides a fresh insight into the graphite/diamond transition process and an approach for diamond synthesis.
ZnFe Layered Double Hydroxide Nanosheets Loaded with Cu Single‐Atom Nanozymes with Multi‐Enzyme‐Like Catalytic Activities as an Effective Treatment for Bacterial Keratitis
Authors: Wang Keke , Yuan Mao‐sen , Dai Pengxiu , Li Jing , Tao Anju , Zhang Xinke , Wang Jinyi , Tu Qin 
Published: January 2025

AbstractBacterial keratitis (BK) is a type of corneal inflammation resulting from bacterial infection in the eye. Although nanozymes have been explored as promising materials in corneal wound healing, currently available nanozymes lack sufficient catalytic activity and the ability to penetrate bacterial biofilms, limiting their efficacy against the treatment of BK. To remedy this, ZnFe layered double hydroxide (ZnFe‐LDH) nanosheets are loaded with Cu single‐atom nanozymes (Cu‐SAzymes) and aminated dextran (Dex‐NH2), resulting in the formation of the nanozyme DT‐ZnFe‐LDH@Cu, which possesses peroxidase (POD)‐, oxidase (OXD)‐, and catalase (CAT)‐like catalytic activities. This enables the nanozyme to generate reactive oxygen species (ROS), such as hydroxyl radicals (•OH), superoxide anion radical (O2•−), and singlet oxygen (1O2) from hydrogen peroxide (H2O2), thereby killing the bacteria causing the infections. The surface Dex‐NH2 enabled the DT‐ZnFe‐LDH@Cu to penetrate the biofilm and adsorb onto extracellular polymeric substances (EPS) produced by bacteria in the biofilm. Additionally, the DT‐ZnFe‐LDH@Cu successfully repaired P. aeruginosa‐infected corneal injury in a BK rabbit model more effectively than commercially available tobramycin eye drops. This was enabled, in part, by the ability of DT‐ZnFe‐LDH@Cu to reduce inflammation by promoting the polarization of pro‐inflammatory macrophages (M1) to anti‐inflammatory macrophages (M2) and decrease the expression of α‐smooth muscle actin (α‐SMA) to promote wound healing without scar formation. This study provides an innovative concept for the treatment of BK and holds great scientific value and clinical application potential.
Omnidirectional 3D Printing of PEDOT: PSS Aerogels with Tunable Electromechanical Performance: A Playground for Unconventional Stretchable Interconnects and Thermoelectrics
Authors: Baysal Hasan Emre , Yu Tzu‐Yi , Naenen Viktor , De Smedt Stijn , Hiz Defne , Zhang Bokai , Xia Heyi , Florenciano Isidro , Rosenthal Martin , Cardinaels Ruth , Molina‐Lopez Francisco 
Published: January 2025

AbstractThe next generation of soft electronics will expand to the third dimension. This will require the integration of mechanically compliant 3D functional structures with stretchable materials. Here, omnidirectional direct ink writing (DIW) of poly(3,4‐ethylenedioxythiophene): polystyrene sulfonate (PEDOT:PSS) aerogels with tunable electrical and mechanical performance is demonstrated, which can be integrated with soft substrates. Several PEDOT:PSS hydrogels are formulated for DIW and freeze‐dried directly on stretchable substrates to form integrated aerogels displaying high shape fidelity and minimal shrinkage. This technology demonstrates 3D‐structured stretchable interconnects, planar thermoelectric generators for skin electronics, and vertically printed high aspect ratio thermoelectric pillars with ultralow thermal conductivity of 0.065 W m−1 K−1. The aerogel pillars outpower their dense counterparts in realistic energy harvesting scenarios, where contact resistances cannot be ignored and produced up to 26 nW cm−2 (corresponding to a gravimetric power density of 0.76 mW kg−1) for a difference of temperature of 15 K. Here, promising advancements in soft and energy‐efficiency electronic systems relevant to soft robotics and wearables are suggested.
Advanced Morphological and Material Engineering for High‐Performance Interfacial Iontronic Pressure Sensors
Authors: Zhuo Fengling , Ding Zhi , Yang Xi , Chu Fengjian , Liu Yulu , Gao Zhuoqing , Jin Hao , Dong Shurong , Wang Xiaozhi , Luo Jikui 
Published: January 2025

AbstractHigh‐performance flexible pressure sensors are crucial for applications such as wearable electronics, interactive systems, and healthcare technologies. Among these, iontronic pressure sensors have garnered particular attention due to their superior sensitivity, enabled by the giant capacitance variation of the electric double layer (EDL) at the ionic‐electronic interface under deformation. Key advancements, such as incorporating microstructures into ionic layers and employing diverse materials, have significantly improved sensor properties like sensitivity, accuracy, stability, and response time. This review highlights advancements in flexible EDL pressure sensors, focusing on structural designs and material engineering. These strategies are tailored to optimize key metrics such as sensitivity, detection limit, linearity, stability, response speed, hysteresis, transparency, wearability, selectivity, and multifunctionality. Key fabrication techniques, including micropatterning and externally assisted methods, are reviewed, along with strategies for sensor comparison and guidelines for selecting appropriate sensors. Emerging applications in healthcare, environmental and aerodynamic sensing, human–machine interaction, robotics, and machine learning‐assisted intelligent sensing are explored. Finally, this review discusses the challenges and future directions for advancing EDL‐based pressure sensors.
Ferroelectric and Optoelectronic Coupling Effects in Layered Ferroelectric Semiconductor‐Based FETs for Visual Simulation
Authors: Zhao Can , Gao Zhaotan , Hong Zian , Guo Hongzhi , Cheng Zhili , Li Yawei , Shang Liyan , Zhu Liangqing , Zhang Jinzhong , Hu Zhigao 
Published: January 2025

AbstractControlling polarization states of ferroelectrics can enrich optoelectronic properties and functions, offering a new avenue for designing advanced electronic and optoelectronic devices. Here, ferroelectric semiconductor‐based field‐effect transistors (FeSFETs) are fabricated, where the channel is a ferroelectric semiconductor (e.g., α‐In2Se3). Multiple conductance states are achieved in α‐In2Se3‐based FeSFETs by controlling the ferroelectric polarization. The on/off current ratio (Ion/Ioff) is ≈105 with a dark current of ≈10−11 A by applying a single positive gate voltage pulse. Moreover, the device shows excellent endurance and retention performance. In a further step, the carrier transports and corresponding physics mechanism in various polarization states are studied by using Kelvin probe force microscopy (KPFM) and optoelectronic measurements. Finally, the α‐In2Se3‐based FETs can be trained. It can recognize handwritten digit images from MNIST dataset with a successful recognition accuracy of ≈95.5%. This work provides a new design idea and theoretical support for advanced optoelectronic devices in the field of in‐memory sensing and computing.
Significant Efficiency Enhancements in Non‐Y Series Acceptors by the Addition of Outer Side Chains
Authors: He Qiao , Hadmojo Wisnu Tantyo , Hu Xiantao , Mukherjee Subhrangsu , Alqurashi Maryam , Althobaiti Wejdan , De Castro Catherine S. P. , Lee Byongkyu , Ding Bowen , Luke Joel , Kafourou Panagiota , Fei Zhuping , White Andrew J. P. , Gorenflot Julien , Glöcklhofer Florian , Laquai Frédéric , Ade Harald , Anthopoulos Thomas D. , Heeney Martin 
Published: January 2025

AbstractMost current highly efficient organic solar cells utilize small molecules like Y6 and its derivatives as electron acceptors in the photoactive layer. In this work, a small molecule acceptor, SC8‐IT4F, is developed through outer side chain engineering on the terminal thiophene of a conjugated 6,12‐dihydro‐dithienoindeno[2,3‐d:2′,3′‐d′]‐s‐indaceno[1,2‐b:5,6‐b′]dithiophene (IDTT) central core. Compared to the reference molecule C8‐IT4F, which lacks outer side chains, SC8‐IT4F displays notable differences in molecule geometry (as shown by simulations), thermal behavior, single‐crystal packing, and film morphology. Blend films of SC8‐IT4F and the polymer donor PM6 exhibit larger carrier mobilities, longer carrier lifetimes, and reduced recombination compared to C8‐IT4F, resulting in improved device performance. Binary photovoltaic devices based on the PM6:SC8‐IT4F films reveal an optimal efficiency over 15%, which is one of the best values for non‐Y type small molecule acceptors (SMAs). The resultant devices also show better thermal and operational stability than the control PM6:L8‐BO devices. SC8‐IT4F and its blend exhibit a higher relative degree of crystallinity and π coherence length, compared to C8‐IT4F samples, beneficial for charge transport and device performance. The results indicate that outer side chain engineering on existing small electron acceptors can be a promising molecular design strategy for further pursuing high‐performance organic solar cells.
Efficient Carbon‐Based Optoelectronic Synapses for Dynamic Visual Recognition
Authors: Liu Wenhao , Wang Jihong , Guo Jiahao , Wang Lin , Gu Zhen , Wang Huifeng , Fang Haiping 
Published: January 2025

AbstractThe human visual nervous system excels at recognizing and processing external stimuli, essential for various physiological functions. Biomimetic visual systems leverage biological synapse properties to improve memory encoding and perception. Optoelectronic devices mimicking these synapses can enhance wearable electronics, with layered heterojunction materials being ideal materials for optoelectronic synapses due to their tunable properties and biocompatibility. However, conventional synthesis methods are complex and environmentally harmful, leading to issues such as poor stability and low charge transfer efficiency. Therefore, it is imperative to develop a more efficient, convenient, and eco‐friendly method for preparing layered heterojunction materials. Here, a one‐step ultrasonic method is employed to mix fullerene (C60) with graphene oxide (GO), yielding a homogeneous layered heterojunction composite film via self‐assembly. The biomimetic optoelectronic synapse based on this film achieves 97.3% accuracy in dynamic visual recognition tasks and exhibits capabilities such as synaptic plasticity. Experiments utilizing X‐ray photoelectron spectroscopy (XPS), X‐ray diffraction spectroscopy (XRD), Fourier–transform infrared spectroscopy (FTIR), ultraviolet‐visible spectroscopy (UV‐vis), scanning electron microscopy (SEM), and transmission electron microscopy (TEM) confirms stable π‐π interactions between GO and C60, facilitating electron transfer and prolonging carrier recombination times. The novel approach leveraging high‐density π electron materials advances artificial intelligence and neuromorphic systems.
Ischemic Area‐Targeting and Self‐Monitoring Nanoprobes Ameliorate Myocardial Ischemia/Reperfusion Injury by Scavenging ROS and Counteracting Cardiac Inflammation
Authors: Ma Xiaobin , Fan Zhijin , Peng Jingyan , Nie Liming 
Published: January 2025

AbstractPrecise and effective management of myocardial ischemia/reperfusion injury (MIRI) is still a formidable challenge in clinical practice. Additionally, real‐time monitoring of drug aggregation in the MIRI region remains an open question. Herein, a drug delivery system, hesperadin and ICG assembled in PLGA‐Se‐Se‐PEG‐IMTP (HI@PSeP‐IMTP), is designed to deliver hesperadin and ICG to the MIRI region for in vivo optical imaging tracking and to ameliorate MIRI. The peak aggregation of nanoprobes in the MIRI region is monitored by near‐infrared fluorescence and photoacoustic imaging. The maximal fluorescence and photoacoustic signals of the HI@PSeP‐IMTP group in the MIRI region rise ≈32% and 40% respectively compared with that of HI@PSeP group. Moreover, HI@PSeP‐IMTP effectively mitigates MIRI due to a synergistic integration of diselenide bonds and hesperadin, which can eliminate ROS and suppress cardiac inflammation. Specifically, the expression levels of p‐CaMKII, p‐IκBα, and p65 in the MIRI region in the HI@PSeP‐IMTP group demonstrate a reduction of 30%, 46%, and 42% respectively compared to that of the PBS group. Collectively, HI@PSeP‐IMTP provides new insights into the development of drugs integrating diagnosis and treatment for MIRI.
Hinged Carboxylate in the Artificial Distal Pocket of an Iron Porphyrin Enhances CO2 Electroreduction at Low Overpotential
Authors: Smith Adrien , Gotico Philipp , Guillot Régis , Le Gac Stéphane , Leibl Winfried , Aukauloo Ally , Boitrel Bernard , Sircoglou Marie , Halime Zakaria 
Published: January 2025

AbstractTo efficiently capture, activate, and transform small molecules, metalloenzymes have evolved to integrate a well‐organized pocket around the active metal center. Within this cavity, second coordination sphere functionalities are precisely positioned to optimize the rate, selectivity, and energy cost of catalytic reactions. Inspired by this strategy, an artificial distal pocket defined by a preorganized 3D strap is introduced on an iron‐porphyrin catalyst (sc‐Fe) for the CO2‐to‐CO electrocatalytic reduction. Combined electrochemical, kinetic, and computational studies demonstrate that the adequate positioning of a carboxylate/carboxylic group acting in synergy with a trapped water molecule within this distal pocket remarkably enhances the reaction turnover frequency (TOF) by four orders of magnitude compared to the perfluorinated iron‐tetraphenylporphyrin catalyst (F20Fe) operating at a similar low overpotential. A proton‐coupled electron transfer (PCET) is found to be the key process responsible for the unexpected protonation of the coordinating carboxylate, which, upon CO2 insertion, shifts from the first to the second coordination sphere to play a possible secondary role as a proton relay.
Supramolecular Complexes of Ultrashort Cationic Lipopeptides with Cyclodextrins: Improved Selectivity and Therapeutic Potential
Authors: Bellini Chiara , Atxabal Unai , Bősze Szilvia , Dobay Orsolya , Horváth Andrea , Szigyártó Imola Cs. , Beke‐Somfai Tamás , Jiménez‐Barbero Jesús , Puskás István , Horváti Kata 
Published: January 2025

ABSTRACTIn the last decade, the rise of antibiotic resistance has heightened interest in antimicrobial peptides and lipopeptides as promising alternatives to conventional antibiotics because of their lower propensity to develop resistance. However, lipopeptides often show undesired cytotoxicity due to their non‐selective membrane disruptive effect, and their limited aqueous solubility represents a matter of concern from a pharmaceutical point of view. This study demonstrates a panel of ultrashort cationic lipopeptides (USCLs) consisting of a tetrapeptide (L1), originated from buforin II, coupled with saturated fatty acids of different lengths. Our results highlight that the 16‐carbon fatty acid lipopeptide (Pal‐L1) exhibits relevant antibacterial activity against multiresistant Staphylococcus aureus strain. However, the formation of heterogenic aggregates in cell culture medium and toxic effects on human cells were also observed. Pal‐L1 formulation with the randomly methylated α‐cyclodextrin (RAMEA) and the sulfobutylether‐β‐cyclodextrin (SBECD) has resulted in a production of ultralow‐sized molecular dispersion systems and reduced lipopeptide toxicity without compromising its antimicrobial activity. With titration 1H‐NMR, 2D NMR experiments, together with molecular dynamics simulations, we described the size, structure, stoichiometry, and dissociation constant of the supramolecular complexes. Interactions of neutral and negatively charged model liposomes with Pal‐L1 lipopeptide in the presence or absence of cyclodextrins serve an explanation for the membrane selectivity, and based on the results, we proposed a potential mechanism of action for the Pal‐L1+cyclodextrin complexes on different biological membranes. Overall, our model characterization points out that cyclodextrin formulation improves the therapeutical applicability of lipopeptides.
RYR3 Variants Are Potentially Associated With Idiopathic (Non‐Lesional) Partial Epilepsy/Susceptibility of Seizures, Toward Understanding the Gene‐Disease Association by Genetic Dependent Nature
Authors: Tian Yang , Hou Yun‐Qi , Zhai Qiong‐Xiang , Song Xing‐Wang , Li Bing‐Mei , Wang Jie , Ji Jing‐Jing , Liao Yin‐Ting , Chen Wen‐Xiong , Li Bin , Liao Wei‐Ping 
Published: January 2025

ABSTRACTThe RYR3 gene encodes a brain‐type ryanodine receptor that functions to release calcium from intracellular storage and plays an essential role in calcium signaling. The associations between RYR3 variants and brain disorders remain unknown. We performed whole‐exome sequencing in patients with idiopathic (non‐lesional) partial epilepsy of unknown etiology. One de novo missense and six biallelic missense RYR3 variants were identified in seven unrelated cases. These variants had no or extremely low allele frequencies in the general population and were predicted to alter hydrogen bonds/decrease protein stability. Patients presented with partial seizures or secondarily generalized tonic–clonic seizures. All patients were seizure‐free with/without anti‐seizure treatment. Four showed antecedent febrile seizures, a typical susceptibility disorder that is related to the precipitating factor of fever. The genetic dependence nature (GDN) of RYR3, which is defined as the distinct impact of the absence of a gene on normal life, is “obligatory” (causing disease phenotypes). Complete abolishing of RYR3 results in abnormal phenotypes instead of lethality, whereas partial/mild impairment (usually more common) is associated with mild disease or increased susceptibility to disease, consistent with our findings. RYR3 is therefore potentially a candidate disease gene or susceptibility gene for idiopathic partial epilepsy.
Contrasting Mechanochromic Luminescence of Enantiopure and Racemic Pyrenylprolinamides: Elucidating Solid‐State Excimer Orientation by Circularly Polarized Luminescence
Authors: Ito Suguru , Wakiyama Shin , Chen Hao , Abekura Masato , Uekusa Hidehiro , Ikemura Ryoya , Imai Yoshitane 
Published: January 2025

AbstractCircularly polarized luminescence (CPL) and mechanochromic luminescence (MCL) have independently made substantial progress in recent years. However, the exploration of MCL in solid‐state CPL materials, which holds practical significance, is still in its infancy. Herein, we report the MCL properties of readily accessible chiral pyrenylprolinamides bearing tert‐butoxycarbonyl (Boc) or 2,2,2‐trichloroethoxycarbonyl (Troc) groups. Enantiopure crystals of the Boc derivative display a greater MCL wavelength shift than racemic crystals, while the Troc derivative exhibit the opposite trend. Most notably, the enantiopure crystals show mechanochromic CPL. Unlike in previous examples, where CPL is quenched upon amorphization, robust CPL spectra were observed even in the amorphous states. By applying the excimer chirality rule, we have, for the first time, acquired insights into the excited‐state structures within mechanically generated amorphous states. These findings offer a novel design strategy for developing mechanochromic CPL materials, paving the way for the future advancements in this emerging field.
Catalytic Hydrogenation of CO2 by Direct Air Capture to Valuable C1 Products Using Homogenous Catalysts
Authors: Bhardwaj Ritu , Choudhury Joyanta 
Published: January 2025

AbstractGrowing atmospheric CO2 concentrations are a global concern and a primary factor contributing to global warming. Development of integrated CO2 capture and conversion protocols is necessary to mitigate this alarming challenge. Though CO2 hydrogenation to produce formic acid and methanol has seen many strides in the past decades, most studies utilize pure CO2 for this transformation. The CO2 concentration in the atmosphere stands at 400 ppm and reports that utilize direct air capture as the strategy to capture CO2 and utilize it for production of formic acid and methanol have only been reported in the past few years. This perspective summarizes such reports with a focus on the CO2‐capturing additive, reaction solvent, and the molecular catalyst used to affect the transformation.