bluuebunny/crossref_metadata_2025_split huggingface dataset:
Stretchable and Biodegradable Batteries with High Energy and Power Density
Authors: Karami‐Mosammam Mahya , Danninger Doris , Schiller David , Kaltenbrunner Martin 
Published: June 2022

AbstractRealizing a sustainable, technologically advanced future will necessitate solving the electronic waste problem. Biodegradable forms of electronics offer a viable path through their environmental benignity. With both the sheer number of devices produced every day as well as their areas of application ever increasing, new concepts of degradable batteries able to sustain the high power demands of modern electronics must be developed. Simultaneously, integration of electronics in close interaction with its user or powering soft robotic devices necessitates high degrees of compliance, rendering stretchable batteries indispensable. Here, a concept for merging intrinsically stretchable materials with engineered stretchability by kirigami‐patterning on a component level is shown to yield high‐power biodegradable batteries with reversible elasticity up to 35% when stretched uniaxially and 20% for biaxial extension. Using a combination of molybdenum metal foils, a molybdenum trioxide paste, and magnesium metal foils as electrode materials, a peak power output of 196 µW cm–2 and an energy density of 1.72 mWh cm–2 is achieved. The biodegradable batteries are used to power an on‐skin biomedical sensor patch, enabling monitoring of sodium concentration in sweat. This concept provides a versatile route for high‐power biodegradable batteries, enabling untethered soft electronic devices in a sustainable future.
The Structure of Water in Silica Mesopores – Influence of the Pore Wall Polarity
Authors: Weinberger Christian , Zysk Frederik , Hartmann Marc , Kaliannan Naveen K. , Keil Waldemar , Kühne Thomas D. , Tiemann Michael 
Published: June 2022

AbstractIn the spatial confinement of cylindrical mesopores with diameters of a few nanometers, water molecules experience restrictions in hydrogen bonding. This leads to a different behavior regarding the molecular orientational freedom (‘structure of water') compared to the bulk liquid state. In addition to the pore size, the behavior is also strongly affected by the strength of the pore wall‐to‐water interactions, that is, the pore wall polarity. In this work, this is studied both experimentally and theoretically. The surface polarity of mesoporous silica (SiO2) is modified by functionalization with trimethylsilyl moieties, resulting in a change from a hydrophilic (pristine) to a hydrophobic pore wall. The mesopore surface is characterized by N2 and H2O sorption experiments. Those results are combined with IR spectroscopy to investigate pore wall‐to‐water interactions leading to different structures of water in the mesopore. Furthermore, the water's structure is studied theoretically to gain deeper insight into the interfacial interactions. For this purpose, the structure of water is analyzed by pairing densities, coordination, and angular distributions with a novel adaptation of surface‐specific sum‐frequency generation calculation for pore environments.
Air–Water Interfacial Directed Self‐Assembly of Block Copolymer Nanostrand Array
Authors: Kim Dong Hyup , Kim So Youn 
Published: June 2022

AbstractInterfacial self‐assembly (ISA) of block copolymers (BCPs) creates various periodic 2D nanostructures at the air–water interface, such as dot, strand, and planar morphologies, which are widely used in various applications. Here, a directed self‐assembly strategy to control the pattern direction of ISA of strand morphology, so‐called nanostrands, in a large area using a gradual morphology transition is introduced. ISA of BCPs in a lens‐shaped droplet of a concentrated BCP solution at the air–water interface shows the gradual morphology transition from the edge to the center of the droplet. The gradual morphology transition is explained by the spreading area‐dependent dewetting mechanism. Furthermore, a dense nanostrand array in a large area which is highly aligned normal to the radial direction of the droplet at an intermediate transition regime is found. In addition, a density‐doubled metal nanowire fabrication and a hierarchical BCP nanopatterning by using the highly aligned nanostrand array as a template are demonstrated.
Importance of Monitoring the Synthesis of Light‐Interacting Nanoparticles – A Review on In Situ, Ex Situ, and Online Time‐Resolved Studies
Authors: Pinho Bruno , Zhang Kaiwen , Hoye Robert L. Z. , Torrente‐Murciano Laura 
Published: June 2022

AbstractThis review paper analyzes the importance of monitoring the synthesis of plasmonic and optoelectronic materials to provide a mechanistic understanding of their nucleatiçon and growth, as well as crucial kinetic insights to enable their future development. Light‐interacting nanoparticles present strong size–property relationships, such that size control is at the core of any synthetic development. However, conventional ex situ characterization of these materials has heavily limited their development to simple trial‐and‐error approaches. Over the last decade, the development of in situ and online characterization capabilities has transformed the understanding of mechanistic models. In addition, time‐resolved data are able to reveal the step rate, even for phenomena taking place in the microsecond timescale (i.e., nucleation), thanks to the use of micro‐flow‐reactors. However, the literature contains a few disagreements and inaccuracies, which are considered to be due to the general lack of attention and control on mixing (relevant when mixing time is comparable to the reaction time), and the presence of additives during synthesis (e.g., stabilizers). Finally, it is believed that recent in situ monitoring development coupled with reactor design brings unique opportunities to not only synthesize nanoparticles in a reproducible and controllable manner, but also gives data‐rich approaches for self‐regulated and automated systems.
Inhaled Gold Nano‐Star Carriers for Targeted Delivery of Triple Suicide Gene Therapy and Therapeutic MicroRNAs to Lung Metastases: Development and Validation in a Small Animal Model
Authors: Liu Yi , Sukumar Uday Kumar , Jugniot Natacha , Seetharam Sumanth Mosale , Rengaramachandran Adith , Sadeghipour Negar , Mukherjee Pinaki , Krishnan Anandi , Massoud Tarik F. , Paulmurugan Ramasamy 
Published: June 2022

AbstractPulmonary metastases pose treatment challenges for many cancers, including triple‐negative breast cancer (TNBC). A novel suicide gene and therapeutic microRNAs (miRs) combination therapy against lung metastases in vivo is tested in mouse models after intranasal delivery using nontoxic gold nanoparticles (AuNPs) formulated to carry these molecular therapeutics. AuNPs coated with chitosan‐β‐cyclodextrin (CS‐CD) are used and functionalized with a urokinase plasminogen activator (uPA) peptide to carry triple cancer suicide genes (thymidine kinase‐p53‐nitroreductase: TK‐p53‐NTR) plus therapeutic miRNAs (antimiR‐21, antimiR‐10b and miR‐100). Three AuNPs are synthesized: 20 nm gold nanodots (AuND), and 20 nm or 50 nm nanostars (AuNS), all surface coated with CS‐CD using a microfluidic‐optimized method. These positively charged AuNP‐CS‐CD cores are sequentially coated with synthetic miRNAs followed by TK‐p53‐NTR via electrostatic interactions, and uPA peptide is added through CD‐adamantane hostguest chemistry. Transfection efficiency comparisons for different AuNPs shows 50 nm AuNS allows ≈4.16‐fold higher gene transfection than other AuNPs. Intranasal delivery of uPA‐AuNS‐TK‐p53‐NTR‐microRNAs NPs (pAuNS@TK‐p53‐NTR‐miRs) in mice predominantly accumulates in lungs and facilitates ganciclovir and CB1954 prodrug‐mediated gene therapy against TNBC lung metastases. This new nanosystem can serve as an adaptable‐across‐cancer‐type, facile, and clinically scalable platform to allow future inhalational suicide gene‐miR combination therapy for patients harboring pulmonary metastases.
Atomic Layer Deposition of Metal Oxides and Chalcogenides for High Performance Transistors
Authors: Shen Chengxu , Yin Zhigang , Collins Fionn , Pinna Nicola 
Published: June 2022

AbstractAtomic layer deposition (ALD) is a deposition technique well‐suited to produce high‐quality thin film materials at the nanoscale for applications in transistors. This review comprehensively describes the latest developments in ALD of metal oxides (MOs) and chalcogenides with tunable bandgaps, compositions, and nanostructures for the fabrication of high‐performance field‐effect transistors. By ALD various n‐type and p‐type MOs, including binary and multinary semiconductors, can be deposited and applied as channel materials, transparent electrodes, or electrode interlayers for improving charge‐transport and switching properties of transistors. On the other hand, MO insulators by ALD are applied as dielectrics or protecting/encapsulating layers for enhancing device performance and stability. Metal chalcogenide semiconductors and their heterostructures made by ALD have shown great promise as novel building blocks to fabricate single channel or heterojunction materials in transistors. By correlating the device performance to the structural and chemical properties of the ALD materials, clear structure–property relations can be proposed, which can help to design better‐performing transistors. Finally, a brief concluding remark on these ALD materials and devices is presented, with insights into upcoming opportunities and challenges for future electronics and integrated applications.
Lorentz‐Boost‐Driven Magneto‐Optics in a Dirac Nodal‐Line Semimetal
Authors: Wyzula Jan , Lu Xin , Santos‐Cottin David , Mukherjee Dibya Kanti , Mohelský Ivan , Le Mardelé Florian , Novák Jiří , Novak Mario , Sankar Raman , Krupko Yuriy , Piot Benjamin A. , Lee Wei‐Li , Akrap Ana , Potemski Marek , Goerbig Mark O. , Orlita Milan 
Published: June 2022

AbstractOptical response of crystalline solids is to a large extent driven by excitations that promote electrons among individual bands. This allows one to apply optical and magneto‐optical methods to determine experimentally the energy band gap —a fundamental property crucial to our understanding of any solid—with a great precision. Here it is shown that such conventional methods, applied with great success to many materials in the past, do not work in topological Dirac semimetals with a dispersive nodal line. There, the optically deduced band gap depends on how the magnetic field is oriented with respect to the crystal axes. Such highly unusual behavior is explained in terms of band‐gap renormalization driven by Lorentz boosts which results from the Lorentz‐covariant form of the Dirac Hamiltonian relevant for the nodal line at low energies.
Self‐Induced Phase Locking of Terahertz Frequency Combs in a Phase‐Sensitive Hyperspectral Near‐Field Nanoscope
Authors: Pistore Valentino , Pogna Eva Arianna Aurelia , Viti Leonardo , Li Lianhe , Davies A. Giles , Linfield Edmund H. , Vitiello Miriam Serena 
Published: June 2022

AbstractChip‐scale, electrically‐pumped terahertz (THz) frequency‐combs (FCs) rely on nonlinear four‐wave‐mixing processes, and have a nontrivial phase relationship between the evenly spaced set of emitted modes. Simultaneous monitoring and manipulation of the intermode phase coherence, without any external seeding or active modulation, is a very demanding task for which there has hitherto been no technological solution. Here, a self‐mixing intermode‐beatnote spectroscopy system is demonstrated, based on THz quantum cascade laser FCs, in which light is back‐scattered from the tip of a scanning near‐field optical‐microscope (SNOM) and the intracavity reinjection monitored. This enables to exploit the sensitivity of FC phase‐coherence to optical feedback and, for the first time, manipulate the amplitude, linewidth and frequency of the intermode THz FC beatnote using the feedback itself. Stable phase‐locked regimes are used to construct a FC‐based hyperspectral, THz s‐SNOM nanoscope. This nanoscope provides 160 nm spatial resolution, coherent detection of multiple phase‐locked modes, and mapping of the THz optical response of nanoscale materials up to 3.5 THz, with noise‐equivalent‐power (NEP) ≈400 pW √Hz−1. This technique can be applied to the entire infrared range, opening up a new approach to hyper‐spectral near‐field imaging with wide‐scale applications in the study of plasmonics and quantum science, inter alia.
Chemical Factory‐Guaranteed Enhanced Chemodynamic Therapy for Orthotopic Liver Cancer
Authors: Tang Zhongmin , Wu Shiman , Zhao Peiran , Wang Han , Ni Dalong , Li Huiyan , Jiang Xingwu , Wu Yelin , Meng Yun , Yao Zhenwei , Cai Weibo , Bu Wenbo 
Published: June 2022

AbstractIn the field of nanomedicine, there is a tendency of matching designed nanomaterials with a suitable type of orthotopic cancer model, not just a casual subcutaneous one. Under this condition, knowing the specific features of the chosen cancer model is the priority, then introducing a proper therapy strategy using designed nanomaterials. Here, the Fenton chemistry is combined with zinc peroxide nanoparticles in the treatment of orthotopic liver cancer which has a “chemical factory” including that liver is the main place for iron storage, metabolism, and also the main metabolic sites for the majority of ingested substances, guaranteeing customized and enhanced chemodynamic therapy and normal liver cells protection as well. The good results in vitro and in vivo can set an inspiring example for exploring and utilizing suitable nanomaterials in corresponding cancer models, ensuring well‐fitness of nanomaterials for disease and satisfactory therapeutic effect.
The Nucleus Bypasses Obstacles by Deforming Like a Drop with Surface Tension Mediated by Lamin A/C
Authors: Katiyar Aditya , Zhang Jian , Antani Jyot D. , Yu Yifan , Scott Kelsey L. , Lele Pushkar P. , Reinhart‐King Cynthia A. , Sniadecki Nathan J. , Roux Kyle J. , Dickinson Richard B. , Lele Tanmay P. 
Published: June 2022

AbstractMigrating cells must deform their stiff cell nucleus to move through pores and fibers in tissue. Lamin A/C is known to hinder cell migration by limiting nuclear deformation and passage through confining channels, but its role in nuclear deformation and passage through fibrous environments is less clear. Cell and nuclear migration through discrete, closely spaced, slender obstacles which mimic the mechanical properties of collagen fibers are studied. Nuclei bypass slender obstacles while preserving their overall morphology by deforming around them with deep local invaginations of little resisting force. The obstacles do not impede the nuclear trajectory and do not cause rupture of the nuclear envelope. Nuclei likewise deform around single collagen fibers in cells migrating in 3D collagen gels. In contrast to its limiting role in nuclear passage through confining channels, lamin A/C facilitates nuclear deformation and passage through fibrous environments; nuclei in lamin‐null (Lmna−/−) cells lose their overall morphology and become entangled on the obstacles. Analogous to surface tension‐mediated deformation of a liquid drop, lamin A/C imparts a surface tension on the nucleus that allows nuclear invaginations with little mechanical resistance, preventing nuclear entanglement and allowing nuclear passage through fibrous environments.
An Injectable Epigenetic Autophagic Modulatory Hydrogel for Boosting Umbilical Cord Blood NK Cell Therapy Prevents Postsurgical Relapse of Triple‐Negative Breast Cancer
Authors: Gong Yihang , Chen Wenjie , Chen Xiuxing , He Yizhan , Jiang Hua , Zhang Xijian , Pan Lijie , Ni Beibei , Yang Fan , Xu Yan , Zhang Qi , Zhou Lei , Cheng Yusheng 
Published: June 2022

AbstractTriple‐negative breast cancer (TNBC) exhibits resistance to conventional treatments due to the presence of cancer stem cells (CSCs), causing postsurgical relapse and a dismal prognosis. Umbilical cord blood natural killer (UCB‐NK) cell‐based immunotherapy represents a promising strategy for cancer treatment. However, its therapeutic efficacy is greatly restrained by downregulation of the NK cell activation ligand MHC class I‐related chain A/B (MICA/B) and autophagy‐mediated degradation of NK cell‐derived granzyme B (GZMB) in CSCs. Herein, it is demonstrated that suberoylanilide hydroxamic acid (SAHA) epigenetically downregulates let‐7e‐5p and miR‐615‐3p to increase MICA/B expression and that 3‐methyl adenine (3MA) inhibits autophagy‐mediated GZMB degradation, thereby sensitizing breast CSCs to UCB‐NK cells. Then, an injectable hydrogel is designed to codeliver SAHA and 3MA to enhance UCB‐NK cell infusion efficacy in TNBC. The hydrogel precursors can be smoothly injected into the tumor resection bed and form a stable gel in situ, allowing for a pH‐sensitive sustained release of SAHA and 3MA. Moreover, UCB‐NK cell infusion in combination with the hydrogel efficiently controls postsurgical relapse of TNBC. In addition, the hydrogel exhibits good hemostasis and wound‐healing functions. Therefore, the work provides proof of concept that an injectable epigenetic autophagic modulatory hydrogel augments UCB‐NK cell therapy to combat postsurgical relapse of TNBC.
Highly Efficient Electrocatalytic Uranium Extraction from Seawater over an Amidoxime‐Functionalized In–N–C Catalyst
Authors: Liu Xiaolu , Xie Yinghui , Hao Mengjie , Chen Zhongshan , Yang Hui , Waterhouse Geoffrey I. N. , Ma Shengqian , Wang Xiangke 
Published: June 2022

AbstractSeawater contains uranium at a concentration of ≈3.3 ppb, thus representing a rich and sustainable nuclear fuel source. Herein, an adsorption–electrocatalytic platform is developed for uranium extraction from seawater, comprising atomically dispersed indium anchored on hollow nitrogen‐doped carbon capsules functionalized with flexible amidoxime moieties (In–Nx–C–R, where R denotes amidoxime groups). In–Nx–C–R exhibits excellent uranyl capture properties, enabling a uranium removal rate of 6.35 mg g−1 in 24 h, representing one of the best uranium extractants reported to date. Importantly, In–Nx–C–R demonstrates exceptional selectivity for uranium extraction relative to vanadium in seawater (8.75 times more selective for the former). X‐ray absorption spectroscopy (XAS) reveals that the amidoxime groups serve as uranyl chelating sites, thus allowing selective adsorption over other ions. XAS and in situ Raman results directly indicate that the absorbed uranyl can be electrocatalytically reduced to an unstable U(V) intermediate, then re‐oxidizes to U(VI) in the form of insoluble Na2O(UO3·H2O)x for collection, through reversible single electron transfer processes involving InNx sites. These results provide detailed mechanistic understanding of the uranium extraction process at a molecular level. This work provides a roadmap for the adsorption–electrocatalytic extraction of uranium from seawater, adding to the growing suite of technologies for harvesting valuable metals from the earth's oceans.
Selective Nitridation Crafted a High‐Density, Carbon‐Free Heterostructure Host with Built‐In Electric Field for Enhanced Energy Density Li–S Batteries
Authors: Wang Hongmei , Wei Yunhong , Wang Guochuan , Pu Yiran , Yuan Li , Liu Can , Wang Qian , Zhang Yun , Wu Hao 
Published: June 2022

AbstractTo achieve both high gravimetric and volumetric energy densities of lithium–sulfur (Li–S) batteries, it is essential yet challenging to develop low‐porosity dense electrodes along with diminishment of the electrolyte and other lightweight inactive components. Herein, a compact TiO2@VN heterostructure with high true density (5.01 g cm–3) is proposed crafted by ingenious selective nitridation, serving as carbon‐free dual‐capable hosts for both sulfur and lithium. As a heavy S host, the interface‐engineered heterostructure integrates adsorptive TiO2 with high conductive VN and concurrently yields a built‐in electric field for charge‐redistribution at the TiO2/VN interfaces with enlarged active locations for trapping‐migration‐conversion of polysulfides. Thus‐fabricated TiO2@VN–S composite harnessing high tap‐density favors constructing dense cathodes (≈1.7 g cm–3) with low porosity (<30 vol%), exhibiting dual‐boosted cathode‐level peak volumetric‐/gravimetric‐energy‐densities nearly 1700 Wh L−1cathode/1000 Wh kg−1cathode at sulfur loading of 4.2 mg cm−2 and prominent areal capacity (6.7 mAh cm−2) at 7.6 mg cm−2 with reduced electrolyte (<10 µL mg−1sulfur). Particular lithiophilicity of the TiO2@VN is demonstrated as Li host to uniformly tune Li nucleation with restrained dendrite growth, consequently bestowing the assembled full‐cell with high electrode‐level volumetric/gravimetric‐energy‐density beyond 950 Wh L−1cathode+anode/560 Wh kg−1cathode+anode at 3.6 mg cm−2 sulfur loading alongside limited lithium excess (≈50%).
Exciton Transfer at Heterointerfaces of MoS2 Monolayers and Fluorescent Molecular Aggregates
Authors: Kwon Soyeong , Jeong Dong Yeun , Hong Chengyun , Oh Saejin , Song Jungeun , Choi Soo Ho , Kim Ki Kang , Yoon Seokhyun , Choi Taeyoung , Yee Ki‐Ju , Kim Ji‐Hee , You Youngmin , Kim Dong‐Wook 
Published: June 2022

AbstractIntegration of distinct materials to form heterostructures enables the proposal of new functional devices based on emergent physical phenomena beyond the properties of the constituent materials. The optical responses and electrical transport characteristics of heterostructures depend on the charge and exciton transfer (CT and ET) at the interfaces, determined by the interfacial energy level alignment. In this work, heterostructures consisting of aggregates of fluorescent molecules (DY1) and 2D semiconductor MoS2 monolayers are fabricated. Photoluminescence spectra of DY1/MoS2 show quenching of the DY1 emission and enhancement of the MoS2 emission, indicating a strong electronic interaction between these two materials. Nanoscopic mappings of the light‐induced contact potential difference changes rule out the CT process at the interface. Using femtosecond transient absorption spectroscopy, the rapid interfacial ET process from DY1 aggregates to MoS2 and a fourfold extension of the exciton lifetime in MoS2 are elucidated. These results suggest that the integration of 2D inorganic semiconductors with fluorescent molecules can provide versatile approaches to engineer the physical characteristics of materials for both fundamental studies and novel optoelectronic device applications.
Conformationally Confined Emissive Cationic Macrocycle with Photocontrolled Organelle‐Specific Translocation
Authors: Dong Xiaoyun , Dai Xianyin , Li Guorong , Zhang Ying‐Ming , Xu Xiufang , Liu Yu 
Published: June 2022

AbstractThe optimization of molecular conformation and aggregation modes is of great significance in creation of new luminescent materials for biochemical research and medical diagnostics. Herein, a highly emissive macrocycle (1) is reported, which is constructed by the cyclization reaction of triphenylamine with benzyl bromide and exhibits very distinctive photophysical performance both in aqueous solution and the solid state. Structural analysis reveals that the 1 can form self‐interpenetrated complex and emit bright yellow fluorescence in the crystal lattice. The distorted yet symmetrical structure can endow 1 with unique two‐photon absorption property upon excitation by near‐infrared light. Also, 1 can be utilized as an efficient photosensitizer to produce singlet oxygen (1O2) both in inanimate milieu and under cellular environment. More intriguingly, due to the strong association of 1 with negatively charged biomacromolecules, organelle‐specific migration is achieved from lysosome to nucleus during the 1O2‐induced cell apoptosis process. To be envisaged, this conformationally confined cationic macrocycle with photocontrolled lysosome‐to‐nucleus translocation may provide a feasible approach for in situ identifying different biospecies and monitoring physiological events at subcellular level.