bluuebunny/crossref_metadata_2025_split huggingface dataset:
Exploring and Understanding the Multiscale Mechanical Degradation in Graphene Assemblies via Practical Microstructure Guided Modeling
Authors: Qin Huasong , Tong Wenhao , Pei Qing‐Xiang , Wang Ziqiu , Zhang Guoqiang , Chen Yan , Li Peng , Liu Jingran , Xu Zhen , Liu Yilun 
Published: June 2023

AbstractExploring and understanding the structure‐mechanical property relations in hierarchical graphene assemblies is crucial for optimizing their mechanical properties and developing new functionalities, as the tensile strength is two orders of magnitude degradation from pristine graphene to graphene assemblies. Yet, quantifying the strength degradation across multiscale is a challenge due to the complex hierarchical structures. Thus, key structures and dominated factors at different lengthscales that affect the mechanical properties of graphene assemblies should be extracted for the reasonable unveiling of this problem. In this study, the multiscale mechanical degradation of graphene assemblies through practical microstructure‐guided multiscale modeling is characterized. Combining with experimental observations, three representative models are developed to study the mechanical behaviors of graphene assemblies at different lengthscales. Then, the dominated factors affecting the strength at these lengthscales are identified, that is the defects in monolayer graphene, tension‐shear load transfer for stacked graphene, and uniformity of graphene assemblies. Based on the simulation results, the structure‐strength relation of graphene assemblies is given, and practical strategies are proposed followed by experimental realization, to significantly improve the mechanical properties of graphene‐based nanocomposites.
H2S‐Activated Ion‐Interference Therapy: A Novel Tumor Targeted Therapy Based on Copper‐Overload‐Mediated Cuproptosis and Pyroptosis
Authors: Zhao Fan , Liang Liying , Wang Heng , Wang Chen , Su Dan , Ying Yao , Li Wangchang , Li Juan , Zheng Jingwu , Qiao Liang , Mou Xiaozhou , Che Shenglei , Yu Jing 
Published: June 2023

AbstractCopper overload is a novel way to achieve copper‐ion‐interference therapy by disrupting copper homeostasis and treating diseases through multiple cell death pathways. However, it is difficult to reach copper overload since excess intracellular copper ions will be pumped out. Herein, copper overload is achieved by both raising cellular uptake and reducing the efflux of copper ions using hydrogen sulfide (H2S)‐responsive copper hydroxyphosphate nanoparticles (Cu2(PO4)(OH) NPs). After immersion in an H2S‐enriched colon cancer microenvironment, Cu2(PO4)(OH) NPs can transform into copper sulfide NPs with reduced size for higher cell entering, resulting in improved Fenton activity as well as copper ion dissociation. Reactive oxygen species generated by the Fenton reaction not only activate inflammasomes and Caspase‐1 proteins, cause the cleavage of gasdermin D to induce pyroptosis, but also affect mitochondrial function and down‐regulate copper exporter ATP7A to further reduce the copper excretion. The combination of higher endocytosis and lower exportation leads to maximized copper overload. Together with the efficient copper ions release, mitochondrial tricarboxylic acid cycle can be disrupted and iron‐sulfur cluster proteins are downregulated, ultimately triggering cuproptosis. As both pyroptosis and cuproptosis are efficient ways to induce cell death, this study provides a novel way to realize effective tumor‐targeted therapy based on H2S‐activated copper overload with simple Cu2(PO4)(OH) NPs.
Relaxation‐Induced Significant Room‐Temperature Dielectric Pulsing Effects
Authors: Li Zhenzhen , Gong Yutie , Xu Aihua , Zhao Jiayu , Li Qiong , Dong Lijie , Xiong Chuanxi , Jiang Ming 
Published: June 2023

AbstractThermo‐responsive dielectric materials are in urgent demand owing to the rapid development of smart electronic/electrical systems. Although different types and structures of thermally responsive dielectric materials have been continuously reported, their dielectric response behaviors all originate from thermodynamic phase transitions. Herein, it is demonstrated that structural relaxation in poly(vinylidene fluoride) (PVDF), a non‐thermodynamic phase transition, can induce a significant thermal dielectric pulse at room temperature. The dielectric pulse strength of up to 6.3 × 105 at 20 Hz, with a dielectric pulsing temperature of 24 °C, is achieved from polyethylene glycol (PEG)‐PVDF coaxial nanofibrous films (PVDF@PEG), fabricated via a continuous blow spinning method. Moreover, the films exhibit excellent flexibility, adjustable strength and toughness, switchable hydrophilicity/hydrophobicity, and effective thermal management capability. The relaxation‐induced dielectric pulsing effect, outstanding multifunctionality, and simple preparation combine to promote further scalability and prospects of PVDF@PEG. In particular, the work contributes to the discovery of the relaxation‐induced dielectric response mechanism, which provides a new strategy for the generation of thermo‐responsive dielectric materials.
A Hierarchical 3D Graft Printed with Nanoink for Functional Craniofacial Bone Restoration
Authors: Shi Yang , Shi Jue , Sun Yuan , Liu Qiqi , Zhang Chun , Shao Changyu , Yu Kang , Ge Mingjie , Mi Rui , Gu Jingyi , Wu Wenzhi , Lu Weiying , Chen Zhuo , He Yong , Tang Ruikang , Xie Zhijian 
Published: June 2023

AbstractAn ideal craniofacial bone repair graft shall not only focus on the repair ability but also the regeneration of natural architecture with occlusal loads‐related function restoration. However, such functional bone tissue engineering scaffold has rarely been reported. Herein, a hierarchical 3D graft is proposed for rebuilding craniofacial bone with both natural structure and healthy biofunction reconstruction. Inspired by the bone healing process, an organic–inorganic nanoink with ultrasmall calcium phosphate oligomers and bone morphogenetic protein‐2 incorporated is developed for spatiotemporal guidance of new bone. Based on such homogeneous nanoink, a biomimetic graft, including a cortical layer containing Haversian system, and a cancellous layer featured with triply periodic minimum surface macrostructures, is fabricated via projection‐based 3D printing method, and the layers are loaded with distinct concentrations of bioactive factors for regenerating new bone with gradient density. The graft exhibits excellent osteogenic and angiogenic potential in vitro, and accelerates revascularization and reconstructs neo‐bone with original morphology in vivo. Benefiting from such natural architecture, loading force is widely transferred with reduced stress concentration around the inserted dental implant. Taken from native physiochemical and structural cues, this wstudy provides a novel strategy for functional tissue engineering through designing function‐oriented biomaterials.
MXenes and Their Derivatives for Advanced Solid‐State Energy Storage Devices
Authors: Man Quanyan , An Yongling , Shen Hengtao , Wei Chuanliang , Zhang Xinlu , Wang Zhengran , Xiong Shenglin , Feng Jinkui 
Published: June 2023

AbstractSolid‐state energy storage devices (SSESDs) are believed to significantly improve safety, long‐term electrochemical/thermal stability, and energy/power density as well as reduce packaging demands, showing the huge application potential in large‐scale energy storage. Nevertheless, some key issues like low ionic conductivities, poor interface contact, and dendrites growth limit the practical application of SSESDs. In recent years, MXenes for SSESDs have received reassuring advances on account of unique parameters. Nevertheless, overall reviews about the subject are seldom. In this review, current advances of MXenes and their derivatives in solid‐state Li–metal, Li‐ion, Li–I/S, Na‐ion, Zn–air, Zn–metal batteries, and supercapacitors in cathode/anode optimization, interface medication, and electrolyte fillers, etc., are comprehensively reviewed. First of all, essential principles of MXenes are shown, such as precursors, etching/delamination strategies, as well as superior properties for energy storage systems. Meanwhile, the classification and evaluation parameters of solid‐state electrolytes are summarized. Subsequently, the application, modification mechanism, and design strategy of MXenes for boosting electrochemical behaviors of SSESDs are systematically reviewed and discussed. At last, perspectives and challenges about the future construction strategies of MXenes for SSESDs are recommended. This review shall assist scientists design and build advanced SSESDs with superior energy density along with safety.
Biomimetic Alveoli System with Vivid Mechanical Response and Cell–Cell Interface
Authors: Niu Mengying , Zhu Yujuan , Ding Xiaoya , Zu Yan , Zhao Yuanjin , Wang Yongan 
Published: June 2023

AbstractAlveolar microenvironmental models are important for studying the basic biology of the alveolus, therapeutic trials, and drug testing. However, a few systems can fully reproduce the in vivo alveolar microenvironment including dynamic stretching and the cell–cell interface. Here, a novel biomimetic alveolus‐on‐a‐chip microsystem is presented suitable for visualizing physiological breathing for simulating the 3D architecture and function of human pulmonary alveoli. This biomimetic microsystem contains an inverse opal structured polyurethane membrane that achieves real‐time observation of mechanical stretching. In this microsystem, the alveolar‐capillary barrier is created by alveolar type 2 (ATII) cells cocultured with vascular endothelial cells (ECs) on this membrane. Based on this microsystem, the phenomena of flattening and the tendency of differentiation in ATII cells are observed. The synergistic effects of mechanical stretching and ECs on the proliferation of ATII cells are also observed during the repair process following lung injury. These features indicate the potential of this novel biomimetic microsystem for exploring the mechanisms of lung diseases, which can provide future guidance concerning drug targets for clinical therapies.
Stimuli‐Responsive Polymer Nanoprobes Intended for Fluorescence‐Guided Surgery of Malignant Head‐and‐Neck Tumors and Metastases
Authors: Pola Robert , Grosmanová Eliška , Pechar Michal , Horák Dominik , Krunclová Tereza , Pankrác Jan , Henry Maxime , Kaňa Martin , Bouček Jan , Šefc Luděk , Coll Jean‐Luc , Etrych Tomáš 
Published: June 2023

AbstractNano‐sized carriers are widely studied as suitable candidates for the advanced delivery of various bioactive molecules such as drugs and diagnostics. Herein, the development of long‐circulating stimuli‐responsive polymer nanoprobes tailored for the fluorescently‐guided surgery of solid tumors is reported. Nanoprobes are designed as long‐circulating nanosystems preferably accumulated in solid tumors due to the Enhanced permeability and retention effect, so they act as a tumor microenvironment‐sensitive activatable diagnostic. This study designs polymer probes differing in the structure of the spacer between the polymer carrier and Cy7 by employing pH‐sensitive spacers, oligopeptide spacers susceptible to cathepsin B‐catalyzed enzymatic hydrolysis, and non‐degradable control spacer. Increased accumulation of the nanoprobes in the tumor tissue coupled with stimuli‐sensitive release behavior and subsequent activation of the fluorescent signal upon dye release facilitated favorable tumor‐to‐background ratio, a key feature for fluorescence‐guided surgery. The probes show excellent diagnostic potential for the surgical removal of intraperitoneal metastasis and orthotopic head and neck tumors with very high efficacy and accuracy. In addition, the combination of macroscopic resection followed by fluorescence‐guided surgery using developed probes enable the identification and resection of most of the CAL33 intraperitoneal metastases with total tumor burden reduced to 97.2%.
Molecular One‐ and Two‐Qubit Systems with Very Long Coherence Times
Authors: Schäfter Dennis , Wischnat Jonathan , Tesi Lorenzo , De Sousa J. Alejandro , Little Edmund , McGuire Jake , Mas‐Torrent Marta , Rovira Concepció , Veciana Jaume , Tuna Floriana , Crivillers Núria , van Slageren Joris 
Published: June 2023

AbstractGeneral‐purpose quantum computation and quantum simulation require multi‐qubit architectures with precisely defined, robust interqubit interactions, coupled with local addressability. This is an unsolved challenge, primarily due to scalability issues. These issues often derive from poor control over interqubit interactions. Molecular systems are promising materials for the realization of large‐scale quantum architectures, due to their high degree of positionability and the possibility to precisely tailor interqubit interactions. The simplest quantum architecture is the two‐qubit system, with which quantum gate operations can be implemented. To be viable, a two‐qubit system must possess long coherence times, the interqubit interaction must be well defined and the two qubits must also be addressable individually within the same quantum manipulation sequence. Here results are presented on the investigation of the spin dynamics of chlorinated triphenylmethyl organic radicals, in particular the perchlorotriphenylmethyl (PTM) radical, a mono‐functionalized PTM, and a biradical PTM dimer. Extraordinarily long ensemble coherence times up to 148 µs are found at all temperatures below 100 K. Two‐qubit and, importantly, individual qubit addressability in the biradical system are demonstrated. These results underline the potential of molecular materials for the development of quantum architectures.
One‐Pot Synthesis and Excited‐State Dynamics of Null Exciton‐Coupled Diketopyrrolopyrroles Oligo‐Grids
Authors: Bo Yifan , Hou Pengfei , Wan Jun , Cao Hongtao , Liu Yuyu , Xie Linghai , Guldi Dirk M. 
Published: June 2023

AbstractExciton coupling in molecular aggregates plays a vital role in impacting and fine‐tuning optoelectronic materials and their efficiencies in devices. A versatile platform to decipher aggregation‐property relationships is built around multichromophoric architectures. Here, a series of cyclic diketopyrrolopyrrole (DPP) oligomers featuring nanoscale gridarene structures and rigid bifluorenyl spacers are designed and synthesized via one‐pot Friedel–Crafts reaction. DPP dimer [2]Grid and trimer [3]Grid, which are cyclic rigid nanoarchitectures of rather different sizes, are further characterized via steady‐state and time‐resolved absorption and fluorescence spectroscopies. They exhibit monomer‐like spectroscopic signatures in the steady‐state measurements, from which null exciton couplings are derived. Moreover, in an apolar solvent, high fluorescence quantum yields and excited‐state dynamics that resembled DPP monomer are gathered. In a polar solvent, the localized singlet excited state on a single DPP dissociates into the adjacent null coupling DPP with charge transfer characteristics. This pathway facilitates the evolution of the symmetry‐broken charge‐separated state (SB‐CS). Notable is the fact that the SB‐CS of [2]Grid is, on one hand, in equilibrium with the singlet excited state and promotes, on the other hand, the formation of the triplet excited state with a yield of 32% via charge recombination.
Aerosol‐Jet‐Printable Covalent Organic Framework Colloidal Inks and Temperature‐Sensitive Nanocomposite Films
Authors: Bradshaw Nathan P. , Hirani Zoheb , Kuo Lidia , Li Siyang , Williams Nicholas X. , Sangwan Vinod K. , Chaney Lindsay E. , Evans Austin M. , Dichtel William R. , Hersam Mark C. 
Published: June 2023

AbstractWith molecularly well‐defined and tailorable 2D structures, covalent organic frameworks (COFs) have emerged as leading material candidates for chemical sensing, storage, separation, and catalysis. In these contexts, the ability to directly and deterministically print COFs into arbitrary geometries will enable rapid optimization and deployment. However, previous attempts to print COFs have been restricted by low spatial resolution and/or post‐deposition polymerization that limits the range of compatible COFs. Here, these limitations are overcome with a pre‐synthesized, solution‐processable colloidal ink that enables aerosol jet printing of COFs with micron‐scale resolution. The ink formulation utilizes the low‐volatility solvent benzonitrile, which is critical to obtaining homogeneous printed COF film morphologies. This ink formulation is also compatible with other colloidal nanomaterials, thus facilitating the integration of COFs into printable nanocomposite films. As a proof‐of‐concept, boronate‐ester COFs are integrated with carbon nanotubes (CNTs) to form printable COF‐CNT nanocomposite films, in which the CNTs enhance charge transport and temperature sensing performance, ultimately resulting in high‐sensitivity temperature sensors that show electrical conductivity variation by 4 orders of magnitude between room temperature and 300 °C. Overall, this work establishes a flexible platform for COF additive manufacturing that will accelerate the incorporation of COFs into technologically significant applications.
Non‐Planar Multiprocess Additive Manufacturing of Multifunctional Composites
Authors: Chauvette Jean‐François , Hia Iee Lee , Pierre Juliette , Chenier Gabriel , Farahani Rouhollah D. , Piccirelli Nicola , Therriault Daniel 
Published: June 2023

AbstractMultiprocess additive manufacturing (AM) consists of integrating different 3D printing techniques to enable the fabrication of multifunctional parts, based on their geometry and material properties. The combination of fused filament fabrication (FFF) and direct ink writing (DIW) techniques, respectively involving thermoplastics and thermosetting polymers (or composites), often focuses on planar and small‐scale applications (i.e., few cm), with limited nozzle orientation freedom for the fabrication of complex parts. Many industries, such as the aerospace sector, could benefit from the AM of lightweight multifunctional parts. For instance, one of the key aircraft components, the abradable seal coating, is applied on gas turbine engines casing to increase engine efficiency and is mechanically abraded by the rotor blades during engine startup. Abradable coatings made of thermosetting polymer could be 3D‐printed using a multiprocess to obtain more functionalities. In this work, a non‐planar multiprocess AM approach involving FFF of a complex large sandwich panel structure with low material density and large‐scale DIW of an abradable thermosetting coating with controlled porosity for sound absorption potential, and better mechanical abradability than a commercial product, is presented. This multiprocess AM approach can be used to manufacture lightweight multifunctional structural parts for the automotive or aerospace industries.
Vertical Photodetectors Based on In Situ Aligned Single‐crystalline PbS Nanocuboids Sandwiched between Graphene Electrodes
Authors: Fu Jintao , Yang Chan , Nie Changbin , Sun Feiying , Li Genglin , Feng Shuanglong , Wei Xingzhan 
Published: June 2023

AbstractLead sulfide (PbS), a classical narrow‐bandgap material, has manifested itself as a reliable choice for short‐wave infrared (SWIR) detection with high sensitivity. The primary efforts of optimizing PbS‐based photodetectors rely on discovering new low‐dimensional morphology and designing delicate device architecture, which may raise problems in the synergistic improvement of response speed, sensitivity, and response region. Herein, a graphene‐PbS nanocuboids‐graphene vertical photodetector is reported, fabricated by in situ electrochemical growth of monocrystalline PbS nanocuboids on graphene using an electrochemical technique. Under illumination, the surface states of PbS nanocuboids trap photogenerated holes and form a photovoltage, which widens the conductive region in the channel. This photogating effect contributes to the photocurrent and renders the device with high responsivity. Moreover, the highly crystalline PbS nanocuboids serve as excellent vertical channels, allowing a fast speed to be achieved. At room temperature, the device shows a responsivity of ≈130 A W−1 at 2700 nm, an external quantum efficiency of ≈6000%, a detectivity of 3 × 109 cm Hz1/2 W−1 (@1 kHz), and response/recovery speeds of 15/42 ms. This vertically integrated device, composed of PbS nanocuboids and graphene, offers a promising approach to complementary metal oxide semiconductor (CMOS)‐compatible SWIR detection, thus opening up an avenue to tailor device performance by exploiting the anisotropic morphology of nanomaterials.
Controllable Photocurrent Generation in Lateral Bilayer MoS2–WS2 Heterostructure
Authors: Zhao Dongyang , Jiao Hanxue , chen Chao , Chen Yan , Wang Shuang , Cao Hechun , Wang Xudong , Yu Guanghui , Bai Wei , Tang Xiaodong , Wang Jianlu , Chu Junhao 
Published: June 2023

AbstractLaterally epitaxial two‐dimensional (2D) transition metal dichalcogenides (TMDs) heterojunctions are of considerable interest in recent years due to atomically sharp interfaces and tunable band alignment, which have potential applications in novel functional electronics and optoelectronics. However, the studies of 2D lateral heterostructures have mainly focused on the synthesis methods and pristine performance of the fabricated heterojunctions. Herein, the controllable photocurrent generation and enhanced performances of the lateral bilayer (LBL) MoS2–WS2 heterojunctions are reported. A tunable and abrupt built‐in field forms at the interface, and the gate‐tunable rectifying behavior and photovoltaic effect are realized. It is demonstrated that the generation of the photocurrent in the device can be highly controlled to realize ultrahigh responsivity of 1.06 × 104 A W−1 and detectivity of 1.14 × 1013 Jones at a 638 nm incident light. The lateral TMDs heterostructures are expected to constitute the ultimate functional elements of novel electronics and optoelectronics.
Experimental Demonstration of Low‐Energy First‐Order Hybridized Plasmon Resonances in Origami Metashells
Authors: Tao Jie , Tang Peng , He Shuchang , Yang Haochen , Li Yuanzhen , Jing Liqiao , Gao Fei , Song Jizhou , Chen Hongsheng , Wang Zuojia 
Published: June 2023

AbstractMetallic nanoshells have emerged as promising optical cavities to steer hybridized plasmonic resonances that show the high spectral tunability and a large surface area of localized fields. Despite various optical and photochemical applications, plasmonic resonances in shells have rarely been explored at low frequencies due to a nonlinear increase in particle size and a rapid degeneration in field localization. Here, this work reports the experimental realization of hybridized plasmon resonances in origami metashells that can be excited by low‐energy photons ≈7 GHz, corresponding to a level below 10−4 eV. Metasurfaces built of interconnected meshes act as thin Drude metallic films that support symmetric spoof surface plasmons. Rigid folding of the metasurface leads to diverse 3D hollow cavities that exhibit strong plasmonic responses, large surface areas, and low relative densities. Experimental measurements demonstrate three typical behaviors in Drude metallic shells: shielding to quasi‐static fields, strong scattering at first‐order hybridized plasmon resonances, and transparency to high frequency radiation. The relative density is remarkably reduced owing to the void cavity enabled by 3D folding, and an extra degree of freedom in anisotropic load capacity is provided by customizing crease patterns. These results open a door for extremely low‐energy plasmons with low‐density mechanics.