bluuebunny/crossref_metadata_2025 huggingface dataset:
Freestanding Serpentine Silicon Strips with Ultrahigh Stretchability over 300% for Wearable Electronics
Authors: Shi Yihao , Zhao Jianzhong , Zhang Bingchang , Qin Jiahao , Hu Xinyue , Cheng Yuan , Yu Jia , Jie Jiansheng , Zhang Xiaohong
Published: March 2024

Well‐functionalized electronic materials, such as silicon, in a stretchable format are desirable for high‐performance wearable electronics. However, obtaining Si materials that meet the required stretchability of over 100% for wearable applications remains a significant challenge. Herein, a rational design strategy is proposed to achieve freestanding serpentine Si strips (FS‐Si strips) with ultrahigh stretchability, fulfilling wearable requirements. The self‐supporting feature makes the strips get rid of excessive constraints from substrates and enables them to deform with the minimum strain energy. Micrometer‐scale thicknesses enhance robustness, and large diameter‐to‐width ratios effectively reduce strain concentration. Consequently, the FS‐Si strips with the optimum design could withstand 300% stretch, bending, and torsion without fracturing, even under rough manual operation. They also exhibit excellent stability and durability over 50,000 cycles of 100% stretching cycles. For wearable applications, the FS‐Si strips can maintain conformal contact with the skin and have a maximum stretchability of 120%. Moreover, they are electrically insensitive to large deformations, which ensure signal stability during their daily use. Combined with mature processing techniques and the excellent semiconductor properties of Si, FS‐Si strips are promising core stretchable electronic materials for wearable electronics.
Single Atom Catalysts Remodel Tumor Microenvironment for Augmented Sonodynamic Immunotherapy
Authors: Geng Bijiang , Hu Jinyan , He Xialing , Zhang Zhenlin , Cai Jinming , Pan Dengyu , Shen Longxiang
Published: March 2024

The immunosuppressive tumor microenvironment (TME) is a huge hurdle in immunotherapy. Sono‐immunotherapy is a new treatment modality that can reverse immunosuppressive TME, but the sonodynamic effects are compromised by overexpressed glutathione (GSH) and hypoxia in the TME. Herein, this work reports a new sono‐immunotherapy strategy using Pdδ+ single atom catalysts to enhance positive sonodynamic responses to the immunosuppressive and sono‐suppressive TME. To demonstrate this technique, this work employs rich and reductive Ti vacancies in Ti3‐xC2Ty nanosheets to construct the atomically dispersed Pd‐C3 single atom catalysts (SAC) with Pd content up to 2.5 wt% (PdSA/Ti3‐xC2Ty). Compared with Pd nanoparticle loaded Ti3‐xC2Ty, PdSA/Ti3‐xC2Ty single‐atom enzyme showed augmented sonodynamic effects that are ascribed to SAC facilitated electron–hole separation, rapid depletion of overexpressed GSH by ultrasound (US) excited holes, and catalytic decomposition of endogenous H2O2 for relieving hypoxia. Importantly, the sono‐immunotherapy strategy can boost abscopal antitumor immune responses by driving maturation of dendritic cells and polarization of tumor‐associated macrophages into the antitumoral M1 phenotype. Bilateral tumor models demonstrate the complete eradication of localized tumors and enhance metastatic regression. Th strategy highlights the potential of single‐atom catalysts for robust sono‐immunotherapy by remodeling the tumor microenvironment.
Building‐Envelope‐Inspired, Thermomechanically Robust All‐Fiber Ceramic Meta‐Aerogel for Temperature‐Controlled Dominant Infrared Camouflage
Authors: Liu Hualei , Zhang Xinxin , Liao Yalong , Yu Jianyong , Liu Yi‐Tao , Ding Bin
Published: March 2024

The unsatisfactory properties of ceramic aerogels when subjected to thermal shock, such as strength degradation and structural collapse, render them unsuitable for use at large thermal gradients or prolonged exposure to extreme temperatures. Here, a building‐envelope‐inspired design for fabricating a thermomechanically robust all‐fiber ceramic meta‐aerogel with interlocked fibrous interfaces and an interwoven cellular structure in the orthogonal directions is presented, which is achieved through a two‐stage physical and chemical process. Inspired by the reinforced concrete building envelope, a solid foundation composed of fibrous frames is constructed and enhanced through supramolecular in situ self‐assembly to achieve high compressibility, retaining over 90% of maximum stress under a considerable compressive strain of 50% for 10 000 cycles, and showing temperature‐invariance when compressed at 60% strain within the range of −100 to 500 °C. As a result of its distinct response to oscillation tolerance coupled with elastic recovery, the all‐fiber ceramic meta‐aerogel exhibits exceptional suitability for thermal shock resistance and infrared camouflage performance in cold (−196 °C) and hot (1300 °C) fields. This study provides an opportunity for developing ceramic aerogels for effective thermal management under extreme conditions.
On‐Demand Crack Formation on DNA Film via Organic Solvent‐Induced Dehydration
Authors: Lee Soeun , Moon Hyeonbin , Kim Juri , Ryu Seunghwa , Park Soon Mo , Yoon Dong Ki
Published: March 2024

Crack is found on the soil when severe drought comes, which inspires the idea to rationalize patterning applications using dried deoxyribonucleic acid (DNA) film. DNA is one of the massively produced biomaterials in nature, showing the lyotropic liquid crystal (LC) phase in highly concentrated conditions. DNA nanostructures in the hydrated condition can be orientation controlled, which can be extended to make dryinginduced cracks. The controlled crack generation in oriented DNA films by inducing mechanical fracture through organic solvent‐induced dehydration (OSID) using tetrahydrofuran (THF) is explored. The corresponding simulations show a strong correlation between the long axis of DNA due to the shrinkage during the dehydration and in the direction of crack propagation. The cracks are controlled by simple brushing and a 3D printing method. This facile way of aligning cracks will be used in potential patterning applications.
Observation of Ultrahigh Photoconductivity in DNA‐MoS2 Nano‐Biocomposite
Authors: Kokkiligadda Samanth , Mondal Ashok , Um Soong Ho , Park Sung Ha , Biswas Chandan
Published: March 2024

A nano‐biocomposite film with ultrahigh photoconductivity remains elusive and critical for bio‐optoelectronic applications. A uniform, well‐connected, high‐concentration nanomaterial network in the biological matrix remains challenging to achieve high photoconductivity. Wafer‐scale continuous nano‐biocomposite film without surface deformations and cracks plays another major obstacle. Here ultrahigh photoconductivity is observed in deoxyribonucleic acid‐molybdenum disulfide (DNA‐MoS2) nano‐biocomposite film by incorporating a high‐concentration, well‐percolated, and uniform MoS2 network in the ss‐DNA matrix. This is achieved by utilizing DNA‐MoS2 hydrogel formation, which results in crack‐free, wafer‐scale DNA‐MoS2 nano‐biocomposite films. Ultra‐high photocurrent (5.5 mA at 1 V) with a record‐high on/off ratio (1.3 × 106) is observed, five orders of magnitude higher than conventional biomaterials (≈101) reported so far. The incorporation of the Wely semimetal (Bismuth) as an electrical contact exhibits ultrahigh photoresponsivity (2.6 × 105 A W−1). Such high photoconductivity in DNA‐MoS2 nano‐biocomposite could bridge the gap between biology, electronics, and optics for innovative biomedicine, bioengineering, and neuroscience applications.
Framework Nucleic Acids Combined with 3D Hybridization Chain Reaction Amplifiers for Monitoring Multiple Human Tear Cytokines
Authors: Lu Xing , Zhou Xujiao , Song Bin , Zhang Hong , Cheng Mingrui , Zhu Xingyu , Wu Yuqi , Shi Haoliang , Chu Binbin , He Yao , Wang Houyu , Hong Jiaxu
Published: March 2024

Existing tear sensors are difficult to perform multiplexed assays due to the minute amounts of biomolecules in tears and the tiny volume of tears. Herein, the authors leverage DNA tetrahedral frameworks (DTFs) modified on the wireless portable electrodes to effectively capture 3D hybridization chain reaction (HCR) amplifiers for automatic and sensitive monitoring of multiple cytokines in human tears. The developed sensors allow the sensitive determination of various dry eye syndrome (DES)‐associated cytokines in human tears with the limit of detection down to 0.1 pg mL−1, consuming as little as 3 mL of tear fluid. Double‐blind testing of clinical DES samples using the developed sensor and commercial ELISA shows no significant difference between them. Compared with single‐biomarker diagnosis, the diagnostic accuracy of this sensor based on multiple biomarkers has improved by ≈16%. The developed system offers the potential for tear sensors to enable personalized and accurate diagnosis of various ocular diseases.
Hydrogen Bond‐Mediated Strong Plasticization for High‐Performance Alginate Plastics
Authors: Yan Hao , Wang Junsheng , Du Cong , Li Zheng , Yuan Hua , Xu Zhen , Tan Yeqiang
Published: March 2024

The increasingly severe plastic pollution has urged an inevitable trend to develop biodegradable plastic products that can take over synthetic plastics. As one of the most abundant natural polymers, polysaccharides are an ideal candidate to substitute synthetic plastics. The rigidity of polysaccharide chains principally allows for high strength and stiffness of their materials, however, challenges the facile orientation in material processing. Here, a general hydrogen bond‐mediated plasticization strategy to regulate isotropic sodium alginate (SA) chains to a highly ordered state is developed, and alginate plastics with high performances are fabricated. It is revealed that hydroxyl groups in glycerol modulate the viscoelasticity of SA solids by forming strong hydrogen bonds with SA chains, achieving a large stretchability at a high solid content. Highly orientated alginate films exhibit a superior tensile strength of 575 MPa and toughness of 60.7 MJ m−3, outperforming most regenerated biomass films. The high solid content and large stretchability mediated by strong hydrogen bonding ensure plastic molding of solid‐like SA with high fidelity. This hydrogen bond‐mediated plasticity provides a facile but effective method to justify the high performances of polysaccharide‐based plastics.
Tunnel‐Oriented VO2 (B) Cathode for High‐Rate Aqueous Zinc‐Ion Batteries
Authors: He Qian , Hu Tao , Wu Qiang , Wang Cheng , Han Xuran , Chen Zibo , Zhu Yuwei , Chen Jianyu , Zhang Yu , Shi Li , Wang Xuebin , Ma Yanwen , Zhao Jin
Published: March 2024

Tunnel‐type vanadium oxides are promising cathodes for aqueous zinc ion batteries. However, unlike layer‐type cathodes with adjustable layer distances, enhancing ion‐transport kinetics in tunnels characterized by fixed sizes poses a considerable challenge. This study highlights that the macroscopic arrangement of the electrode crucially determines tunnel orientation, thereby influencing ion transport. By changing the material morphology, the tunnel orientation can be optimized to facilitate rapid ion diffusion. In a proof‐of‐concept demonstration, it is revealed that (00l) facets‐dominated VO2 (B) nanobelts with dispersive morphology (VO2‐D) tend to adopt a stacking pattern with directional ion transport along the c‐axis on the electrode and guarantee fast ion diffusion. Compared with the aggregated sample (VO2‐A) that tends to random arrangement on the electrode with isotropic and slow ion transfer behavior, the electrode featuring dispersive (00l) facets‐dominated VO2 (B) nanobelts displays directional and fast ion diffusion behavior, thus exhibits an ultrahigh‐rate performance (420.8 and 344.8 mAh g−1 at 0.1 and 10 A g−1, respectively) and long cycling stability (84.3% capacity retention under 5000 cycles at 10 A g−1). The results suggest that simultaneous manipulation of exposed crystal facet and morphology‐related electrode arrangement should be promising for boosting the ion‐transport kinetics in tunnel‐type vanadium oxide cathodes.
Bioorthogonal In Situ Polymerization of Dendritic Agents for Hijacking Lysosomes and Enhancing Antigen Presentation in Cancer Cells
Authors: Zhong Dan , Hou Xingyu , Pan Dayi , Li Zhiqian , Gong Qiyong , Luo Kui
Published: March 2024

A low‐generation lysine dendrimer, SPr‐G2, responds to intracellular glutathione to initiate bioorthogonal in situ polymerization, resulting in the formation of large assemblies in mouse breast cancer cells. The intracellular large assemblies of SPr‐G2 can interact with lysosomes to induce lysosome expansion and enhance lysosomal membrane permeabilization, leading to major histocompatibility complex class I upregulation on tumor cell surfaces and ultimately tumor cell death. Moreover, the use of the SPr‐G2 dendrimer to conjugate the chemotherapeutic drug, camptothecin (CPT), can boost the therapeutic potency of CPT. Excellent antitumor effects in vitro and in vivo are obtained from the combinational treatment of the SPr‐G2 dendrimer and CPT. This combinational effect also enhances antitumor immunity through promoting activation of cytotoxic T cells in tumor tissues and maturation of dendritic cells. This study can shed new light on the development of peptide dendritic agents for cancer therapy.
Hydrogel Ink for 3D Printing with High and Widely Tunable Mechanical Properties via the Salting‐Out Effect
Authors: Ko Kun Woo , Lee Taehoon , Jeong Jae‐Hak , Lee Yeonteak , Kim Ikjin , Seo Jungmok , Park Yong‐Hwa , Kim Jin‐Oh , Park Steve
Published: March 2024

Due to the difficulty of simultaneously ensuring printability and controlling their mechanical properties, 3D printed hydrogels thus far have low modulus, far less than that of many biological tissues and organs. Therefore, their feasibility toward various biomimetic applications is currently limited. Herein, Direct‐Ink‐Writing (DIW) based 3D printable hydrogel ink with broadly adjustable mechanical properties is introduced. The salting‐out effect is utilized to effectively lower the gelation temperature of hydrogel inks with a wide range of modulus (0.193–1.072 MPa), making them all 3D printable. As a proof of concept, multi‐layered synthetic blood vessels that mimic the mechanical properties of biological blood vessels are printed, and their practicability toward surgical training is demonstrated. The versatility and simplicity of this technique make it highly promising for use in various 3D‐printed hydrogel biomaterials applications.
Cancer‐on‐Chip and Integrative Tumor Microenvironment Sensor Technologies for Progressing Precision Radiotherapy
Authors: Dey Shuvashis , Kinoshita Masaki , Puttick Simon , Rose Stephen , Trau Matt , Roberts Matthew J. , Koo Kevin M.
Published: March 2024

Precision radiotherapy, such as targeted radioligand therapy, accentuates the precise delivery of radiation to tumor cells while limiting radiation damage to surrounding normal cells. Although recent clinical trial data has shown targeted radioligand therapy to have significant patient survival benefit, it is still unavoidable that the cancer cells will eventually adapt and develop radioresistance. Thus, the study of radiotherapy‐induced changes in the tumor microenvironment (TME) is crucial for developing strategies to best overcome radioresistance. To this end, organ‐on‐chip (OOC) systems with integrative sensors represent cutting‐edge pre‐clinical models for miniaturized 3D modelling and profiling of the TME. This Review features OOC systems which have demonstrated feasibility for radiation‐associated studies, as well as showcased the progress of different OOC systems for profiling core components of the TME. Furthermore, this Review discusses the knowledge gap in cancer‐on‐chip systems with integrative TME sensors for precision radiotherapy applications. It is anticipated that this Review can kickstart the propagation of new concepts and approaches to drive a new era of miniaturized sensors on OOC systems for precision radiotherapy.
Direct Fabrication of Electronic Circuits on Wooden Surfaces
Authors: Egger Florian , Schiller David , Stockinger Thomas , Pretschuh Claudia , Müller Uwe , Kaltenbrunner Martin
Published: March 2024

Equipping otherwise passive surfaces with electronic functionality enables advanced interactive robotics, consumer products, sensor skins, and structural health monitoring. Concurrently, the rapidly growing number of electronic devices fuels the search for sustainable materials and processes that aid in reducing electronic waste. Wood is CO2‐neutral, omnipresent in the construction industry, in furniture, musical instruments, or packaging, yet so far, its potential for direct integration with electronics remains largely unexplored. Complications arise as traditional methods of equipping wood with electronics often compromise structural integrity and thus limit applications requiring load‐bearing capabilities. Here, seamless fabrication methods that allow the direct enhancement of wooden surfaces with electrically conducting structures, sensors, and microelectronic components based on screen printing of conducting inks or physical vapor deposition of thin metal films in conjunction with laser engraving are presented. Such electronic circuits imperceptibly operate on the surface of structural elements or as parts of decorative wooden furniture. These types of electronic wooden surfaces enable touch‐sensing applications, monitoring temperature, or the curing of varnishes without compromising functionality and mechanical stability. This multidisciplinary approach opens up new avenues for the development of smart wooden structures with embedded electronics, revolutionizing the way it is monitored, controlled, and interacted with wood‐based constructions.
Avocado Pruning Residues for the Formulation of Bio‐Based Polyethylene/Fiber‐Based Biocomposites for Sustainable Food Packaging
Authors: Morcillo‐Martín Ramón , Tarrés Quim , Aguado Roberto J. , Espinosa Eduardo , Delgado‐Aguilar Marc , Rodríguez Alejandro
Published: March 2024

The extensive use of non‐biodegradable bioplastics and fossil‐based plastics in food packaging presents a significant environmental challenge. Consequently, there has been a growing interest in exploring agricultural biomass as a potential source for formulating biocomposites for packaging due to the substantial amount of lignocellulosic residue generated. This study explores the utilization of avocado pruning residue (APR) for isolating lignocellulose fibers and their application as replacement and reinforcement material for bio‐based polyethylene (BioPE) composites. The results obtained reveal that a concentration of 9% (w/w) of maleic anhydride‐grafted‐polyethylene (MAPE) shows the most effective fiber–polymer interaction, resulting in a significant improvement of 25.47% in the mechanical properties. Biocomposites with varying fiber concentrations, ranging from 10% to 40% (w/w), are prepared and assessed for their macro‐ and micromechanical properties. The results demonstrate a substantial 49% increase in tensile strength and a remarkable 325% enhancement in Young's modulus for biocomposites containing 40% (w/w) fiber content. Furthermore, micromechanical analysis provides insights into the intrinsic strength and modulus of avocado fibers, with values of ≈437 MPa and 33 GPa, respectively. This research contributes to the development of sustainable and eco‐friendly alternatives for food packaging, reducing the reliance on fossil‐based plastics, and promoting the utilization of agricultural waste.
Navigating Pubertal Goldilocks: The Optimal Pace for Hierarchical Brain Organization
Authors: Szakács Hanna , Mutlu Murat Can , Balestrieri Giulio , Gombos Ferenc , Braun Jochen , Kringelbach Morten L. , Deco Gustavo , Kovács Ilona
Published: March 2024

Adolescence is a timed process with an onset, tempo, and duration. Nevertheless, the temporal dimension, especially the pace of maturation, remains an insufficiently studied aspect of developmental progression. The primary objective is to estimate the precise influence of pubertal maturational tempo on the configuration of associative brain regions. To this end, the connection between maturational stages and the level of hierarchical organization of large‐scale brain networks in 12‐13‐year‐old females is analyzed. Skeletal maturity is used as a proxy for pubertal progress. The degree of maturity is defined by the difference between bone age and chronological age. To assess the level of hierarchical organization in the brain, the temporal dynamic of closed eye resting state high‐density electroencephalography (EEG) in the alpha frequency range is analyzed. Different levels of hierarchical order are captured by the measured asymmetry in the directionality of information flow between different regions. The calculated EEG‐based entropy production of participant groups is then compared with accelerated, average, and decelerated maturity. Results indicate that an average maturational trajectory optimally aligns with cerebral hierarchical order, and both accelerated and decelerated timelines result in diminished cortical organization. This suggests that a “Goldilocks rule” of brain development is favoring a particular maturational tempo.
Synergistically Modulating Conductive Filaments in Ion‐Based Memristors for Enhanced Analog In‐Memory Computing
Authors: Wang Jinyong , Ren Yujing , Yang Ze , Lv Qiaoya , Zhang Yu , Zhang Mingyue , Zhao Tiancheng , Gu Deen , Liu Fucai , Tang Baoshan , Yang Weifeng , Lin Zhiqun
Published: March 2024

Memristors offer a promising solution to address the performance and energy challenges faced by conventional von Neumann computer systems. Yet, stochastic ion migration in conductive filament often leads to an undesired performance tradeoff between memory window, retention, and endurance. Herein, a robust memristor based on oxygen‐rich SnO2 nanoflowers switching medium, enabled by seed‐mediated wet chemistry, to overcome the ion migration issue for enhanced analog in‐memory computing is reported. Notably, the interplay between the oxygen vacancy (Vo) and Ag ions (Ag+) in the Ag/SnO2/p++‐Si memristor can efficiently modulate the formation and abruption of conductive filaments, thereby resulting in a high on/off ratio (>106), long memory retention (10‐year extrapolation), and low switching variability (SV = 6.85%). Multiple synaptic functions, such as paired‐pulse facilitation, long‐term potentiation/depression, and spike‐time dependent plasticity, are demonstrated. Finally, facilitated by the symmetric analog weight updating and multiple conductance states, a high image recognition accuracy of ≥ 91.39% is achieved, substantiating its feasibility for analog in‐memory computing. This study highlights the significance of synergistically modulating conductive filaments in optimizing performance trade‐offs, balancing memory window, retention, and endurance, which demonstrates techniques for regulating ion migration, rendering them a promising approach for enabling cutting‐edge neuromorphic applications.
2D Ferromagnetic M3GeTe2 (M = Ni/Fe) for Boosting Intermediates Adsorption toward Faster Water Oxidation
Authors: Bo Guyue , Li Peng , Fan Yameng , Zheng Xiaobo , Zhao Mengting , Zhu Qiang , Fu Yang , Li Yitong , Pang Wei Kong , Lai Wei Hong , Johannessen Bernt , Thomsen Lars , Cowie Bruce , Ma Tianyi , Wang Cheng , Yeoh Guan Heng , Du Yi , Dou Shi Xue , Xu Xun
Published: March 2024

In this work, 2D ferromagnetic M3GeTe2 (MGT, M = Ni/Fe) nanosheets with rich atomic Te vacancies (2D‐MGTv) are demonstrated as efficient OER electrocatalyst via a general mechanical exfoliation strategy. X‐ray absorption spectra (XAS) and scanning transmission electron microscope (STEM) results validate the dominant presence of metal‐O moieties and rich Te vacancies, respectively. The formed Te vacancies are active for the adsorption of OH* and O* species while the metal‐O moieties promote the O* and OOH* adsorption, contributing synergistically to the faster oxygen evolution kinetics. Consequently, 2D‐Ni3GeTe2v exhibits superior OER activity with only 370 mV overpotential to reach the current density of 100 mA cm−2 and turnover frequency (TOF) value of 101.6 s−1 at the overpotential of 200 mV in alkaline media. Furthermore, a 2D‐Ni3GeTe2v‐based anion‐exchange membrane (AEM) water electrolysis cell (1 cm2) delivers a current density of 1.02 and 1.32 A cm−2 at the voltage of 3 V feeding with 0.1 and 1 m KOH solution, respectively. The demonstrated metal‐O coordination with abundant atomic vacancies for ferromagnetic M3GeTe2 and the easily extended preparation strategy would enlighten the rational design and fabrication of other ferromagnetic materials for wider electrocatalytic applications.
Asymmetrical Interactions between Ni Single Atomic Sites and Ni Clusters in a 3D Porous Organic Framework for Enhanced CO2 Photoreduction
Authors: Yan Fang‐Qin , Dong Xiao‐Yu , Wang Yi‐Man , Wang Qian‐You , Wang Shan , Zang Shuang‐Quan
Published: March 2024

3D porous organic frameworks, which possess the advantages of high surface area and abundant exposed active sites, are considered ideal platforms to accommodate single atoms (SAs) and metal nanoclusters (NCs) in high‐performance catalysts; however, very little research has been conducted in this field. In the present work, a 3D porous organic framework containing Ni1 SAs and Nin NCs is prepared through the metal‐assisted one‐pot polycondensation of tetraaldehyde and hexaaminotriptycene. The single metal sites and metal clusters confined in the 3D space created a favorable micro‐environment that facilitated the activation of chemically inert CO2 molecules, thus promoting the overall photoconversion efficiency and selectivity of CO2 reduction. The 3D‐NiSAs/NiNCs‐POPs, as a CO2 photoreduction catalyst, demonstrated an exceptional CO production rate of 6.24 mmol g−1 h−1, high selectivity of 98%, and excellent stability. The theoretical calculations uncovered that asymmetrical interaction between Ni1 SAs and Nin NCs not only favored the bending of CO2 molecules and reducing the CO2 reduction energy, but also regulated the electronic structure of the catalyst leading to the optimal binding strength of intermediates.
Boosting Energy Deprivation by Synchronous Interventions of Glycolysis and Oxidative Phosphorylation for Bioenergetic Therapy Synergetic with Chemodynamic/Photothermal Therapy
Authors: Wei Xiangjun , Han Renlu , Gao Yun , Song Pengxin , Guo Zhen , Hou Yafei , Yu Jiancheng , Tang Keqi
Published: March 2024

Bioenergetic therapy is emerging as a promising therapeutic approach. However, its therapeutic effectiveness is restricted by metabolic plasticity, as tumor cells switch metabolic phenotypes between glycolysis and oxidative phosphorylation (OXPHOS) to compensate for energy. Herein, Metformin (MET) and BAY‐876 (BAY) co‐loaded CuFe2O4 (CF) nanoplatform (CFMB) is developed to boost energy deprivation by synchronous interventions of glycolysis and OXPHOS for bioenergetic therapy synergetic with chemodynamic/photothermal therapy (CDT/PTT). The MET can simultaneously restrain glycolysis and OXPHOS by inhibiting hexokinase 2 (HK2) activity and damaging mitochondrial function to deprive energy, respectively. Besides, BAY blocks glucose uptake by inhibiting glucose transporter 1 (GLUT1) expression, further potentiating the glycolysis repression and thus achieving much more depletion of tumorigenic energy sources. Interestingly, the upregulated antioxidant glutathione (GSH) in cancer cells triggers CFMB degradation to release Cu+/Fe2+ catalyzing tumor‐overexpressed H2O2 to hydroxyl radical (∙OH), both impairing OXPHOS and achieving GSH‐depletion amplified CDT. Furthermore, upon near‐infrared (NIR) light irradiation, CFMB has a photothermal conversion capacity to kill cancer cells for PTT and improve ∙OH production for enhanced CDT. In vivo experiments have manifested that CFMB remarkably suppressed tumor growth in mice without systemic toxicity. This study provides a new therapeutic modality paradigm to boost bioenergetic‐related therapies.
Phonon‐Bottleneck Enhanced Exciton Emission in 2D Perovskites
Authors: Thompson Joshua J. P. , Dyksik Mateusz , Peksa Paulina , Posmyk Katarzyna , Joki Ambjörn , Perea‐Causin Raul , Erhart Paul , Baranowski Michał , Loi Maria Antonietta , Plochocka Paulina , Malic Ermin
Published: March 2024

Layered halide perovskites exhibit remarkable optoelectronic properties and technological promise, driven by strongly bound excitons. The interplay of spin‐orbit and exchange coupling creates a rich excitonic landscape, determining their optical signatures and exciton dynamics. Despite the dark excitonic ground state, surprisingly efficient emission from higher‐energy bright states has puzzled the scientific community, sparking debates on relaxation mechanisms. Combining low‐temperature magneto‐optical measurements with sophisticated many‐particle theory, the origin of the bright exciton emission in perovskites is elucidated by tracking the thermalization of dark and bright excitons under a magnetic field. The unexpectedly high emission is clearly attributed to a pronounced phonon‐bottleneck effect, considerably slowing down the relaxation toward the energetically lowest dark states. It is demonstrated that this bottleneck can be tuned by manipulating the bright‐dark energy splitting and optical phonon energies, offering valuable insights and strategies for controlling exciton emission in layered perovskite materials that is crucial for optoelectronics applications.
Upgrading Lignin into Graphene‐Based Materials: State of the Art and Perspectives
Authors: Zhang Hanwen , Yan Qiangu , Peng Yucheng , Cai Zhiyong , Wan Caixia
Published: March 2024

Lignin is a promising precursor to produce graphene materials due to its high carbon and aromatic contents. Upgrading lignin into graphene materials has gained significant interests as it offers a cost‐effective and sustainable route to produce high‐performance carbon materials. This review provides a comprehensive overview of the state‐of‐the‐art technologies on lignin to graphene materials with a focus on thermal catalytic and photothermal upgrading. The applications of lignin‐derived graphene materials and the perspectives for mass production of such graphene materials are also discussed.
Impact of malnutrition and nutritional support after gastrectomy in patients with gastric cancer
Authors: Kang Min Kyu , Lee Hyuk‐Joon
Published: March 2024

Malnutrition, characterized by altered body composition and impaired function, is particularly prevalent among gastric cancer patients, affecting up to 60% of them. Malnutrition in these patients can manifest both before and after surgery, due to factors such as gastric outlet obstruction, cancer cachexia, and anatomical changes. Notably, total gastrectomy (TG) presents the most significant nutritional challenges. However, function‐preserving gastrectomy, such as pylorus‐preserving gastrectomy (PPG) and proximal gastrectomy (PG), have shown promise in improving nutritional outcomes. Effective nutritional risk screening and assessment are vital for identifying patients at risk. Nutritional support not only improves nutritional parameters but also reduces complications, enhances quality of life (QoL) and survival rates. Those unable to maintain more than 50% of the recommended intake for over 7 days are recommended for nutritional support. Common methods of nutritional support include oral nutrition supplements (ONS), enteral nutrition (EN), or parenteral nutrition (PN) depending on the patient's status. Effect of perioperative nutritional support remains controversial. Preoperative interventions including ONS and PN have shown mixed results, with selective benefits in patients with sarcopenia or hypoalbuminaemia, while impact of EN in gastric outlet obstruction patients have been positive. In contrast postoperative support appears to be consistent. Tube feeding after TG has shown improvements, and ONS have been effective in reducing weight loss and improving nutritional biomarkers. PN was also associated with benefits such as weight maintenance and QoL. This review explores the mechanisms, assessment, and clinical impact of malnutrition, emphasizing the importance of nutritional support in gastric cancer patients undergoing gastrectomy.
Short‐acting opioid prescriptions and Workers' Compensation using the National Ambulatory Medical Care Survey
Authors: Thompson Hannah M. , Govindarajulu Usha , Doucette John , Nabeel Ismail
Published: March 2024

Background

Short‐acting opioids have been utilized for pain management with little known about their use in patients on Workers' Compensation (WC) insurance. Our goal was to investigate this association in the ambulatory care setting.

Methods

Using the National Ambulatory Medical Care Survey, visits from patients aged 18–64 during the years 2010 until 2018 were evaluated (excluding 2017 due to data availability). Demographic and co‐morbidity data from each visit was obtained along with the visit year. The first short‐acting opioid medication prescribed in the database was considered. Survey‐weighted frequencies were evaluated. Logistic regression estimated the crude and adjusted odds ratios (OR) with 95% confidence intervals for the use of short‐acting opioid prescription.

Results

There were 155,947 included visits with 62.5% for female patients. Most patients were White with 11.7% identifying as Black, and 6% identifying as another race. Over 13% of the sample was of Hispanic descent. WC was the identified insurance type in 1.6% of the sample population. Of these patients, 25.6% were prescribed a short‐acting opioid, compared with 10.1% of those with another identified insurance. On multivariable regression, Black patients had increased odds of being prescribed a short‐acting opioid compared to white patients (OR: 1.22, 95% CI: 1.11–1.34). Those on WC had 1.7‐fold higher odds of being prescribed short‐acting opioids (95% CI: 1.46–2.06).

Conclusion

Certain patient characteristics, including having WC insurance, increased the odds of a short‐acting opioid prescription. Further work is needed to identify prescribing patterns in specific high‐risk occupational groups, as well as to elicit potential associated health outcomes.
Effects of the active amyloid beta immunotherapy CAD106 on PET measurements of amyloid plaque deposition in cognitively unimpaired APOE ε4 homozygotes
Authors: Riviere Marie‐Emmanuelle , Langbaum Jessica B. , Turner R. Scott , Rinne Juha O. , Sui Yihan , Cazorla Pilar , Ricart Javier , Meneses Kathleen , Caputo Angelika , Tariot Pierre N. , Reiman Eric M. , Graf Ana
Published: March 2024

INTRODUCTION

Alzheimer's Prevention Initiative Generation Study 1 evaluated amyloid beta (Aβ) active immunotherapy (vaccine) CAD106 and BACE‐1 inhibitor umibecestat in cognitively unimpaired 60‐ to 75‐year‐old participants at genetic risk for Alzheimer's disease (AD). The study was reduced in size and terminated early. Results from the CAD106 cohort are presented.

METHODS

Sixty‐five apolipoprotein E ε4 homozygotes with/without amyloid deposition received intramuscular CAD106 450 μg (n = 42) or placebo (n = 23) at baseline; Weeks 1, 7, 13; and quarterly; 51 of them had follow‐up Aβ positron emission tomography (PET) scans at 18 to 24 months.

RESULTS

CAD106 induced measurable serum Aβ immunoglobulin G titers in 41/42 participants, slower rates of Aβ plaque accumulation (mean [standard deviation] annualized change from baseline in amyloid PET Centiloid: −0.91[5.65] for CAD106 versus 8.36 [6.68] for placebo; P < 0.001), and three amyloid‐related imaging abnormality cases (one symptomatic).

DISCUSSION

Despite early termination, these findings support the potential value of conducting larger prevention trials of Aβ active immunotherapies in individuals at risk for AD.

Highlights

This was the first amyloid‐lowering prevention trial in persons at genetic risk of late‐onset Alzheimer's disease (AD).

Active immunotherapy targeting amyloid (CAD106) was tested in this prevention trial.

CAD106 significantly slowed down amyloid plaque deposition in apolipoprotein E homozygotes.

CAD106 was generally safe and well tolerated, with only three amyloid‐related imaging abnormality cases (one symptomatic).

Such an approach deserves further evaluation in larger AD prevention trials.
Carrier Protein Interaction with Competing Adenylation and Epimerization Domains in a Nonribosomal Peptide Synthetase Analyzed by FRET
Authors: Feldberg Anna‐Lena , Mayerthaler Florian , Rüschenbaum Jennifer , Kröger Jonas , Mootz Henning D.
Published: March 2024

In multi‐domain nonribosomal peptide synthetases (NRPSs) the order of domains and their catalytic specificities dictate the structure of the peptide product. Peptidyl‐carrier proteins (PCPs) bind activated amino acids and channel elongating peptidyl intermediates along the protein template. To this end, fine‐tuned interactions with the catalytic domains and large‐scale PCP translocations are necessary. Despite crystal structure snapshots of several PCP‐domain interactions, the conformational dynamics under catalytic conditions in solution remain poorly understood. We report a FRET reporter of gramicidin S synthetase 1 (GrsA; with A‐PCP‐E domains) to study for the first time the interaction between PCP and adenylation (A) domain in the presence of an epimerization (E) domain, a competing downstream partner for the PCP. Bulk FRET measurements showed that upon PCP aminoacylation a conformational shift towards PCP binding to the A domain occurs, indicating the E domain acts on its PCP substrate out of a disfavored conformational equilibrium. Furthermore, the A domain was found to preferably bind the D‐Phe‐S‐Ppant‐PCP stereoisomer, suggesting it helps in establishing the stereoisomeric mixture in favor of the D‐aminoacyl moiety. These observations surprisingly show that the conformational logic can deviate from the order of domains and thus reveal new principles in the multi‐domain interplay of NRPSs.
The Transfer Dehydrogenation Method Enables a Family of High Crystalline Benzimidazole‐linked Cu (II)‐phthalocyanine‐based Covalent Organic Frameworks Films
Authors: Zhang Qingsong , Zhu Zhiheng , Liu Liping , Huang Haojie , Chen Xianjie , Bian Yangshuang , Shao Mingchao , Wei Xiaofang , Wang Chengyu , Wang Dong , Dong Jichen , Guo Yunlong , Zhu Yongfa , Liu Yunqi
Published: March 2024

Heterocycle‐linked phthalocyanine‐based COFs with close‐packed π–π conjugated structures are a kind of material with intrinsic electrical conductivity, and they are considered to be candidates for photoelectrical devices. Previous studies have revealed their applications for energy storage, gas sensors, and field‐effect transistors. However, their potential application in photodetector is still not fully studied. The main difficulty is preparing high‐quality films. In our study, we found that our newly designed benzimidazole‐linked Cu (II)‐phthalocyanine‐based COFs (BICuPc‐COFs) film can hardly formed with a regular aerobic oxidation method. Therefore, we developed a transfer dehydrogenation method with N‐benzylideneaniline (BA) as a mild reagent. With this in hand, we successfully prepared a family of high crystalline BICuPc‐COFs powders and films. Furthermore, both of these new BICuPc‐COFs films showed high electrical conductivity (0.022–0.218 S/m), higher than most of the reported COFs materials. Due to the broad absorption and high conductivity of BICuPc‐COFs, synaptic devices with small source‐drain voltage (VDS=1 V) were fabricated with response light from visible to near‐infrared. Based on these findings, we expect this study will provide a new perspective for the application of conducting heterocycle‐linked COFs in synaptic devices.
Rocking‐Chair Aqueous Fluoride‐Ion Batteries Enabled by Hydrogen Bonding Competition
Authors: Wang Huijian , Lei Chengjun , Liu Tingting , Xu Chen , He Xin , Liang Xiao
Published: March 2024

Aqueous fluoride ion batteries (FIBs) have garnered attention for their high theoretical energy density, yet they are challenged by sluggish fluorination kinetics, active material dissolution, and electrolyte instability. Here, we present a room temperature rocking‐chair aqueous FIBs featuring KOAc‐KF binary salt electrolytes, enabling concurrent fluorination and defluorination reactions at both cathode and anode electrodes. Experimental and theoretical results reveal that acetate ions in the electrolyte compete with fluoride ions in hydrogen bonding formation, weakening the excessively strong solvation between H2O and F− ions. This results in the suppression of detrimental HF formation and a reduced desolvation energy of F− ions, enhancing the electrochemical reaction kinetics. The bismuth‐based cathode exhibits direct conversion in the optimized electrolyte, effectively suppressing the detrimental disproportionation reactions from Bi2+ intermediates. Additionally, zinc anode undergoes a typical fluorination process, forming solid KZnF3 as the electrode product, minimizing the risks of hydrogen evolution. The proposed aqueous FIBs with the optimized electrolyte demonstrate high discharge capacity, long‐term cycling stability and excellent rate capabilities.
Interfacial Engineering for Oriented Crystal Growth toward Dendrite‐Free Zn Anode for Aqueous Zinc Metal Battery
Authors: Zhou Xunzhu , Wen Bo , Cai Yichao , Chen Xiaomin , Li Lin , Zhao Qing , Chou Shu‐Lei , Li Fujun
Published: March 2024

Zn deposition with a surface‐preferred (002) crystal plane has attracted extensive attention due to its inhibited dendrite growth and side reactions. However, the nucleation and growth of the Zn(002) crystal plane are closely related to the interfacial properties. Herein, oriented growth of Zn(002) crystal plane is realized on Ag‐modified surface that is directly visualized by in situ atomic force microscopy. A solid solution HCP‐Zn (~1.10 at. % solubility of Ag, 30 °C) is formed on the Ag coated Zn foil (Zn@Ag) and possesses the same crystal structure as Zn to reduce its nucleation barrier caused by their lattice mismatch. It merits oriented Zn deposition and corrosion‐resistant surface, and presents long cycling stability in symmetric cells and full cells coupled with V2O5 cathode. This work provides insights into interfacial regulation of Zn anodes for high‐performance aqueous zinc metal batteries.
Copper Nanodrugs by Atom Transfer Radical Polymerization
Authors: Chen Peng , Song Ziyan , Yao Xuxia , Wang Weibin , Teng Lisong , Matyjaszewski Krzysztof , Zhu Weipu
Published: March 2024

In this study, some copper catalysts used for atom transfer radical polymerization (ATRP) were explored as efficient anti‐tumor agents. The aqueous solution of copper‐containing nanoparticles with uniform spheric morphology was in situ prepared through a copper‐catalyzed activator generated by electron transfer (AGET) ATRP in water. Nanoparticles were then directly injected into tumor‐bearing mice for antitumor chemotherapy. The copper nanodrugs had prolonged blood circulation time and enhanced accumulation at tumor sites, thus showing potent antitumor activity. This work provides a novel strategy for precise and large‐scale preparation of copper nanodrugs with high antitumor activity.
Selective Peptide Cysteine Manipulation on Demand and Difficult Protein Chemical Synthesis Enabled by Controllable Acidolysis of N,S‐Benzylidene Thioacetals
Authors: Wu Hongxiang , Sun Zhenquan , Li Xuechen
Published: March 2024

Although solid‐phase peptide synthesis combining with chemical ligation provides a way to build up customized polypeptides in general, many targets are still presenting challenges for the conventional synthetic process, such as hydrophobic proteins. New methods and strategies are still required to overcome these obstacles. In this study, kinetic studies of Cys/Pen ligation and its acidolysis were performed, from which the fast acidolysis of substituted N,S‐benzylidene thioacetals (NBTs) was discovered. The study demonstrates the potential of NBTs as a promising Cys switchable protection, facilitating the chemical synthesis of peptides and proteins by efficiently disrupting peptide aggregation. The compatibility of NBTs with other commonly adopted Cys protecting groups and their applications in sequential disulfide bond formation were also investigated. The first chemical synthesis of the native human programmed death ligand 1 immunoglobulin V‐like (PD‐L1 IgV) domain was achieved using the NBT strategy, showcasing its potential in difficult protein synthesis.
Abiotic Methane Production Driven by Ubiquitous Non‐Fenton‐Type Reactive Oxygen Species
Authors: Ye Jie , Hu Andong , Gao Chao , Li Fengqi , Li Lei , Guo Yulin , Ren Guoping , Li Bing , Rensing Christopher , Nealson Kenneth H. , Zhou Shungui , Xiong Yujie
Published: March 2024

Abiotic CH4 production driven by Fenton‐type reactive oxygen species (ROS) has been confirmed to be an indispensable component of the atmospheric CH4 budget. While the chemical reactions independent of Fenton chemistry to ROS are ubiquitous in nature, it remains unknown whether the produced ROS can drive abiotic CH4 production. Here, we first demonstrated the abiotic CH4 production at the soil‐water interface under illumination. Leveraging this finding, polymeric carbon nitrides (CNx) as a typical analogue of natural geobattery material and dimethyl sulfoxide (DMSO) as a natural methyl donor were used to unravel the underlying mechanisms. We revealed that the ROS, photocatalytically produced by CNx, can oxidize DMSO into CH4 with a high selectivity of 91.5 %. Such an abiotic CH4 production process was further expanded to various non‐Fenton‐type reaction systems, such as electrocatalysis, pyrocatalysis and sonocatalysis. This work provides insights into the geochemical cycle of abiotic CH4, and offers a new route to CH4 production via integrated energy development.
Catalyst‐Free α‐Acetyl Cinnamate/Acetoacetate Exchange to Enable High Creep‐Resistant Vitrimers
Authors: Feng Hongzhi , Wang Sheng , Lim Jason Y. C. , Li Bofan , Rusli Wendy , Liu Feng , Hadjichristidis Nikos , Li Zibiao , Zhu Jin
Published: March 2024

Vitrimers represent an emerging class of polymeric materials that combine the desirable characteristics of both thermoplastics and thermosets achieved through the design of dynamic covalent bonds within the polymer networks. However, these materials are prone to creep due to the inherent instability of dynamic covalent bonds. Consequently, there are pressing demands for the development of robust and stable dynamic covalent chemistries. Here, we report a catalyst‐free α‐acetyl cinnamate/acetoacetate (α‐AC/A) exchange reaction to develop vitrimers with remarkable creep resistance. Small‐molecule model studies revealed that the α‐AC/A exchange occurred at temperatures above 140 °C in bulk, whereas at 120 °C, this reaction was absent. For demonstration in the case of polymers, copolymers derived from common vinyl monomers were crosslinked with terephthalaldehyde to produce α‐AC/A vitrimers with tunable thermal and mechanical performance. All resulting α‐AC/A vitrimers exhibited high stability, especially in terms of creep resistance at 120 °C, while retaining commendable reprocessability when subjected to high temperatures. This work showcases the α‐AC/A exchange reaction as a novel and robust dynamic covalent chemistry capable of imparting both reprocessability and high stability to cross‐linked networks.