bluuebunny/crossref_metadata_2025_split huggingface dataset:
Multicomponent Molecular Assembly of Fluorescent Organic Semiconductors Beyond Three Compounds
Authors: Zhao Panpan , Zhang Lulu , Meng Zhengong , Lei Yilong 
Published: June 2022

AbstractIn contrast to unary assemblies comprising π‐conjugated organic species, elaborate modulation of dimensions, polymorphisms, and compositions of multicomponent assembled architectures with two or more constituent materials has not yet been systematically studied. Herein, a combinatorial library of organic microcrystals made of four components via a solution‐phase assembly route is reported. With the involvement of growth kinetics, four organic species with slight structural modifications can assemble into five unary assemblies, which may endow binary combinations with highly and partially structural miscibility. Consequently, a variety of binary alloyed assemblies and microscale heterostructures with tailorable dimensions, polymorphisms, and emission colors are realized by rational compositional and growth control. The effects of structural relations of binary combinations on their miscibility are systematically uncovered, that gives rise to these intricate microscale architectures as well as diverse energy transfer (ET) efficiencies. Highly efficient ET process in binary alloyed assemblies can be beneficial to steady‐state photoluminescence anisotropy amplification. Benefiting from the information of binary combinations, white‐light‐emitting ternary microsheets can be modulated in a predictable manner. The present work uncovers the rational control of multicomponent microcrystals, which further stretches the boundaries of molecular self‐assembly and may be used to achieve integrated optoelectronic properties, such as multicolor lasers and p–n junctions.
Fabrication and Functionality Integration Technologies for Small‐Scale Soft Robots
Authors: Zhang Shuo , Ke Xingxing , Jiang Qin , Chai Zhiping , Wu Zhigang , Ding Han 
Published: June 2022

AbstractSmall‐scale soft robots are attracting increasing interest for visible and potential applications owing to their safety and tolerance resulting from their intrinsic soft bodies or compliant structures. However, it is not sufficient that the soft bodies merely provide support or system protection. More importantly, to meet the increasing demands of controllable operation and real‐time feedback in unstructured/complicated scenarios, these robots are required to perform simplex and multimodal functionalities for sensing, communicating, and interacting with external environments during large or dynamic deformation with the risk of mismatch or delamination. Challenges are encountered during fabrication and integration, including the selection and fabrication of composite/materials and structures, integration of active/passive functional modules with robust interfaces, particularly with highly deformable soft/stretchable bodies. Here, methods and strategies of fabricating structural soft bodies and integrating them with functional modules for developing small‐scale soft robots are investigated. Utilizing templating, 3D printing, transfer printing, and swelling, small‐scale soft robots can be endowed with several perceptual capabilities corresponding to diverse stimulus, such as light, heat, magnetism, and force. The integration of sensing and functionalities effectively enhances the agility, adaptability, and universality of soft robots when applied in various fields, including smart manufacturing, medical surgery, biomimetics, and other interdisciplinary sciences.
An Encapsulation‐Based Sodium Storage via Zn‐Single‐Atom Implanted Carbon Nanotubes
Authors: Li Xin , Ye Weibin , Xu Pan , Huang Haihong , Fan Jingmin , Yuan Ruming , Zheng Ming‐Sen , Wang Ming‐Sheng , Dong Quanfeng 
Published: June 2022

AbstractThe properties of high theoretical capacity, low cost, and large potential of metallic sodium (Na) has strongly promoted the development of rechargeable sodium‐based batteries. However, the issues of infinite volume variation, unstable solid electrolyte interphase (SEI), and dendritic sodium causes a rapid decline in performance and notorious safety hazards. Herein, a highly reversible encapsulation‐based sodium storage by designing a functional hollow carbon nanotube with Zn single atom sites embedded in the carbon shell (ZnSA‐HCNT) is achieved. The appropriate tube space can encapsulate bulk sodium inside; the inner enriched ZnSA sites provide abundant sodiophilic sites, which can evidently reduce the nucleation barrier of Na deposition. Moreover, the carbon shell derived from ZIF‐8 provides geometric constraints and excellent ion/electron transport channels for the rapid transfer of Na+ due to its pore‐rich shell, which can be revealed by in situ transmission electron microscopy (TEM). As expected, Na@ZnSA‐HCNT anodes present steady long‐term performance in symmetrical battery (>900 h at 10 mA cm−2). Moreover, superior electrochemical performance of Na@ZnSA‐HCNT||PB full cells can be delivered. This work develops a new strategy based on carbon nanotube encapsulation of metallic sodium, which improves the safety and cycling performance of sodium metal anode.
Bioinspired Stretchable Transducer for Wearable Continuous Monitoring of Respiratory Patterns in Humans and Animals
Authors: Cotur Yasin , Olenik Selin , Asfour Tarek , Bruyns‐Haylett Michael , Kasimatis Michael , Tanriverdi Ugur , Gonzalez‐Macia Laura , Lee Hong Seok , Kozlov Andrei S. , Güder Firat 
Published: June 2022

AbstractA bio‐inspired continuous wearable respiration sensor modeled after the lateral line system of fish is reported which is used for detecting mechanical disturbances in the water. Despite the clinical importance of monitoring respiratory activity in humans and animals, continuous measurements of breathing patterns and rates are rarely performed in or outside of clinics. This is largely because conventional sensors are too inconvenient or expensive for wearable sensing for most individuals and animals. The bio‐inspired air‐silicone composite transducer (ASiT) is placed on the chest and measures respiratory activity by continuously measuring the force applied to an air channel embedded inside a silicone‐based elastomeric material. The force applied on the surface of the transducer during breathing changes the air pressure inside the channel, which is measured using a commercial pressure sensor and mixed‐signal wireless electronics. The transducer produced in this work are extensively characterized and tested with humans, dogs, and laboratory rats. The bio‐inspired ASiT may enable the early detection of a range of disorders that result in altered patterns of respiration. The technology reported can also be combined with artificial intelligence and cloud computing to algorithmically detect illness in humans and animals remotely, reducing unnecessary visits to clinics.
Light‐Based Printing of Leachable Salt Molds for Facile Shaping of Complex Structures
Authors: Kleger Nicole , Fehlmann Simona , Lee Seunghun S. , Dénéréaz Cyril , Cihova Martina , Paunović Nevena , Bao Yinyin , Leroux Jean‐Christophe , Ferguson Stephen J. , Masania Kunal , Studart André R. 
Published: June 2022

Abstract3D printing is a powerful manufacturing technology for shaping materials into complex structures. While the palette of printable materials continues to expand, the rheological and chemical requisites for printing are not always easy to fulfill. Here, a universal manufacturing platform is reported for shaping materials into intricate geometries without the need for their printability, but instead using light‐based printed salt structures as leachable molds. The salt structures are printed using photocurable resins loaded with NaCl particles. The printing, debinding, and sintering steps involved in the process are systematically investigated to identify ink formulations enabling the preparation of crack‐free salt templates. The experiments reveal that the formation of a load‐bearing network of salt particles is essential to prevent cracking of the mold during the process. By infiltrating the sintered salt molds and leaching the template in water, complex‐shaped architectures are created from diverse compositions such as biomedical silicone, chocolate, light metals, degradable elastomers, and fiber composites, thus demonstrating the universal, cost‐effective, and sustainable nature of this new manufacturing platform.
Tracking Exciton Diffusion and Exciton Annihilation in Single Nanoparticles of Conjugated Polymers by Photon Correlation Spectroscopy
Authors: Schedlbauer Jakob , Streicher Sabrina , Forster Michael , Scherf Ullrich , Vogelsang Jan , Lupton John M. 
Published: June 2022

AbstractA fundamental question relating to the nature of light emission and absorption in organic semiconductors is the dimension of the domain within a bulk material responsible for the interaction of light and matter. How large can a nanoparticle become to retain the quantized nature of light emission? Excitons are only a few nanometers in size, but because they diffuse in space, they probe a much larger volume than the single molecule. When excitons meet, they may decay non‐radiatively by singlet–singlet or singlet–triplet annihilation (SSA or STA). Fluorescence photon statistics reveal whether single photons are emitted (photon antibunching) or arrive in randomly spaced packets (photon bunching), offering direct insight into excitonic mobility. Single multichain nanoparticles of ladder‐type poly(para‐phenylene) (LPPP) are examined. The effect of SSA and STA is seen in the photon antibunching and bunching, respectively, which both decrease in fidelity as the size of the nanoparticle increases. Time resolving the photon correlation measurement yields microscopic annihilation rates for SSA and STA in agreement with values obtained from bulk LPPP films. Even though triplets in LPPP are known to be highly mobile, the results show that, on the timescale of the singlet exciton lifetime, triplet diffusion is not of significance in the STA process.
Integrated Environmental and Exergoeconomic Analysis of Biomass‐Derived Maleic Anhydride
Authors: Blanco Jorge , Linares Maria , López Granados Manuel , Agirre Ion , Gandarias Iñaki , Arias Pedro Luis , Iglesias Jose , Moreno Jovita , García Alicia 
Published: June 2022

AbstractLife cycle analysis and exergy analysis are applied to compare the production of maleic anhydride from different feedstock, both biomass‐ and petrochemical‐derived raw materials, in order to evaluate the sustainability of alternative biorefinery processes to conventional routes. The considered processes involve two options: gas and aqueous phase furfural oxidation with oxygen (air) and hydrogen peroxide as oxidants, respectively, considered as sustainable technologies because of the use of renewable feedstock. Conventional routes, used as benchmarks, include the current production processes using benzene or butane as raw materials. The results show that the aqueous phase process is far from being viable from an energy and environmental point of view due to the high exergy destruction and the use of H2O2 as oxidant (whose production entails important environmental drawbacks). On the contrary, the gas phase oxidation of furfural shows competitive results with petrochemical technologies. Nevertheless, the major environmental drawback of the new furfural‐to‐maleic anhydride production processes is detected on the environmental profile of the starting raw material. The results suggest that a better environmental footprint for maleic anhydride production in gas phase can be obtained if environmentally friendly furfural production technologies are used at the commercial scale.
The impact of the Meals‐to‐You program on food insecurity
Authors: Anderson Theresa , Waxman Elaine , Gundersen Craig 
Published: June 2022

AbstractFood insecurity among children in the United States remains a serious problem, especially during summer months. While there are summer meal programs such as the Summer Food Service Program (SFSP), participation rates are low. In response, in 2019, Meals‐to‐You (MTY) was piloted by the U.S. Department of Agriculture through the Baylor Collaborative on Hunger and Poverty where food boxes were delivered to households with a focus on rural areas. This was expanded during COVID to an Emergency Meals‐to‐You component. We find that among participating households, those receiving more boxes had larger declines in food insecurity, especially in more remote rural areas.
Contributors to SerumNfLLevels in People without Neurologic Disease
Authors: Fitzgerald Kathryn C. , Sotirchos Elias S. , Smith Matthew D. , Lord Hannah‐Noelle , DuVal Anna , Mowry Ellen M. , Calabresi Peter A. 
Published: June 2022

ObjectiveTo assess the effects of demographics, lifestyle factors, and comorbidities on serum neurofilament light chain (sNfL) levels in people without neurologic disease and establish demographic‐specific reference ranges of sNfL.MethodsThe National Health and Nutrition Examination Survey (NHANES) is a representative sample of the US population in which detailed information on demographic, lifestyle, routine laboratory tests, and overall health status are systematically collected. From stored serum samples, we measured sNfL levels using a novel high‐throughput immunoassay (Siemens Healthineers). We evaluated the predictive capacity of 52 demographic, lifestyle, comorbidity, anthropometric, or laboratory characteristics in explaining variability in sNfL levels. Predictive performance was assessed using cross‐validatedR2(R2cv) and forward selection was used to obtain a set of best predictors of sNfL levels. Adjusted reference ranges were derived incorporating characteristics using generalized additive models for location, scale, and shape.ResultsWe included 1,706 NHANES participants (average age: 43.6 ± 14.8 y; 50.6% male, 35% non‐white) without neurological disorders. In univariate models, age explained the most variability in sNfL (R2cv = 26.8%). Multivariable prediction models for sNfL contained three covariates (in order of their selection): age, creatinine, and glycosylated hemoglobin (HbA1c) (standardized β—age: 0.46, 95% confidence interval [CI]: 0.43, 0.50; creatinine: 0.18, 95% CI: 0.13, 0.22; HbA1c: 0.09, 95% CI: 0.06, 0.11). Adjusted centile curves were derived incorporating identified predictors. We provide an interactive R Shiny application to translate our findings and allow other investigators to use the derived centile curves.InterpretationResults will help to guide interpretation of sNfL levels as they relate to neurologic conditions. ANN NEUROL 2022;92:688–698
Ein Kupfer‐Käfig‐Komplex als Nachahmung der pMMO CuC‐Seite
Authors: Bete Sarah C. , May Leander K. , Woite Philipp , Roemelt Michael , Otte Matthias 
Published: June 2022

AbstractDas aktive Zentrum der partikulären Methan‐Monooxygenase (pMMO) und ihr Wirkungsmechanismus sind nicht bekannt. In den letzten Jahren trat die CuC‐Seite als potentielles aktives Zentrum auf, jedoch fehlt es bisher an biomimetischen Studien zu dieser vom Enzym bereitgestellten Koordinationssphäre. Hier wird über die Synthese eines Käfigliganden berichtet, welcher solch eine Koordinationssphäre bereitstellt. Die Koordination an Kupfer erfolgt durch die beiden Imidazol‐ und eine Carboxylatgruppe des Liganden. Abhängig von der Oxidationsstufe kann der Ligand unterschiedliche Koordinationsmodi annehmen, was durch Festkörperstrukturen und computerchemische Untersuchungen belegt wurde. Der Kupfer(I)‐Komplex reagiert leicht mit Sauerstoff und geht dadurch eine CH‐Aktivierung ein. Darüber hinaus wird die katalytische aerobe Oxidation von Hydrochinonen als Ubichinol‐Nachahmungen gezeigt. Eine saubere Ein‐Elektronen‐Oxidation findet unter milden Bedingungen statt. Die EPR‐Analyse des Kupfer(II)‐Komplexes zeigt in Gegenwart von Wasser bemerkenswerte Ähnlichkeiten zu Daten, welche von pMMO erhalten wurden.
Upconversion Luminescence‐Boosted Escape of DNAzyme from Endosomes for Enhanced Gene‐Silencing Efficacy
Authors: Chen Yaoxuan , Zhao Rupeng , Li Lele , Zhao Yuliang 
Published: June 2022

AbstractDespite the enormous potential of DNAzyme for gene therapy, its efficacy is hampered by the limited endosomal escape capability. Here, we develop a near‐infrared (NIR) light‐controlled DNAzyme delivery platform to achieve enhanced gene‐silencing efficacy. The nanoplatform is composed of therapeutic DNAzyme, photosensitizers (PSs) and upconversion nanoparticles (UCNPs) that can convert NIR light to visible light. The system allows NIR light‐activatable generation of cytotoxic reactive oxygen species due to the energy transfer from the UCNPs to PSs, which boosts the endosomal escape of DNAzyme for an improved gene‐silencing efficacy. We demonstrate that the nanocomposites represent a promising platform to integrate DNAzyme‐based gene therapy with NIR light‐triggered photodynamic therapy for combinational tumor treatment. This work highlights a robust approach to combat the current limitations of DNAzyme delivery systems.
Efficient Broadband Near‐Infrared Emission from Lead‐Free Halide Double Perovskite Single Crystal
Authors: Zhang Gangyi , Wang Deyin , Lou Bibo , Ma Chong‐Geng , Meijerink Andries , Wang Yuhua 
Published: June 2022

AbstractUltra‐broadband near‐infrared (NIR) luminescent materials are the most important component of NIR light‐emitting devices (LED) and are crucial for their performance in sensing applications. A major challenge is to design novel NIR luminescent materials to replace the traditional Cr3+‐doped systems. We report an all‐inorganic bismuth halide perovskite Cs2AgBiCl6 single crystal that achieves efficient broadband NIR emission by introducing Na ions. Experiments and density functional theory (DFT) calculations show that the NIR emission originates from self‐trapped excitons (STE) emission, which can be enhanced by weakening the strong coupling between electrons and phonons. The high photoluminescence quantum efficiency (PLQY) of 51 %, the extensive full width at half maximum (FWHM) of 270 nm and the stability provide advantages as a NIR luminescent material. The single‐crystal‐based NIR LED demonstrated its potential applications in NIR spectral detection as well as night vision.
Photostability and Dynamic Helical Behavior in Chiral Poly(phenylacetylene)s with a Preferred Screw‐Sense
Authors: Rey‐Tarrío Francisco , Guisán‐Ceinos Santiago , Cuerva Juan M. , Miguel Delia , Ribagorda Maria , Quiñoá Emilio , Freire Félix 
Published: June 2022

AbstractHelical polymers such as poly(phenylacetylene)s (PPAs) are interesting materials due to the possibility of tuning their helical scaffold (sense and elongation) once they have been prepared and by the presence of external stimuli. The main limitation in the application of PPAs is their poor photostability. These polymers degrade under visible light exposure through a photochemical electrocyclization process. In this work, it was demonstrated, through a selected example, how the photochemical degradation in PPAs is directly related to their dynamic helical behavior. Thus, while PPAs with dynamic helical structures show poor photostability under UV/Vis light exposure, poly‐(R)‐1, bearing an enantiopure sulfoxide group as pendant group and designed to have a quasi‐static helical behavior, shows a large photostability due to the restricted conformational composition at the polyene backbone, needed to orient the conjugated double bonds prior to the photochemical electrocyclization process and the subsequent degradation of the material.
Simulating the Structure of Carbon Dots via Crystalline π‐Aggregated Organic Nanodots Prepared by Kinetically Trapped Self‐Assembly
Authors: Yang Jianye , Guo Like , Yong Xue , Zhang Tongjin , Wang Boyang , Song Haoqiang , Zhao Yong Sheng , Hou Hongwei , Yang Bai , Ding Jie , Lu Siyu 
Published: June 2022

AbstractThis work reports the successful preparation of a new type of crystalline luminescent organic nanodot (<3.5 nm) by kinetically trapped self‐assembly, which is then used as a simplified π‐packing model to simulate the structure of CDs. The precise structure and J‐aggregation‐induced photoluminescence (PL) of the nanodots are revealed by investigating the structural relationship between the nanodots and the corresponding single crystals and their properties. Compared with the single crystals, crystalline organic nanodots show longer PL lifetime, higher PL quantum yield, and narrower PL peak, indicating that they are potential organic quantum nanodots. In addition, the efficient π‐stacking environment in the corresponding single crystals can promote π‐aggregation‐induced PL anisotropy. This work indicates crystalline organic nanodots with precise structures to be potentially useful for understanding the structures of CDs and to be attractive potential luminescent materials.
PEG‐Functionalized Hollow Multishelled Structures with On‐Off Switch and Rate‐Regulation for Controllable Antimicrobial Release
Authors: Zhao Decai , Wei Yanze , Jin Quan , Yang Nailiang , Yang Yang , Wang Dan 
Published: June 2022

AbstractThe construction of responsive antimicrobial carriers with multifunctional and controllable release is an attractive but challenging proposition. Recently developed hollow multishelled structures (HoMSs) offers structural advantages, such as easily modifiable surfaces and mutually influenced shells. Herein, we report a novel pH‐responsive antimicrobial carrier having hierarchical shells as multilevel responsive bodies using polyethylene glycol (PEG) as a gated regulator. The interaction between PEG‐functionalized shells endows them with a pH‐responsive switch and rate‐regulator capability. These features are present in the form of rapid release of molecules wrapped in the outer shell, and controlled diffusion of antimicrobials stored in the inner shell by electrostatic interaction, resulting in a long‐lasting mildew resistance for up to 71 days. The versatility of the hierarchical interactions of HoMSs will inspire the design of promising smart drug carriers.
Porous carbon‐supported CoPd nanoparticles: High‐performance reduction reaction of nitrophenol
Authors: Buğday Nesrin , Altin Serdar , Yaşar Sedat 
Published: June 2022

AbstractMagnetic porous carbon composite was synthesized from zeolitic imidazolate framework (ZIF‐12) and used as a support material to fabricate CoPd nanoparticles decorated NPC@ZIF‐12 nanocatalyst. The structure of CoPd@NPC@ZIF‐12 has been characterized by scanning electron microscopy (SEM), transmission electron microscopy (TEM), X‐ray diffraction (XRD), Raman, Brunauer–Emmett–Teller (BET), X‐ray photoelectron spectroscopy (XPS), Fourier transform infrared spectroscopy (FTIR), and inductively coupled plasma mass spectrometry (ICP‐MS) techniques. The catalytic reduction reaction of nitrophenols (NP) to aminophenols (AP) was successfully achieved by CoPd@NPC@ZIF‐12 nanocatalyst. When the catalytic performance of the catalyst was compared with other reported catalysts, the performance of the catalyst and reusability was found much better. This better catalytic activity of the CoPd@NPC@ZIF‐12 nanocatalyst may be attributed to facilitating the mass transfer of the nitro compound and the wettability of catalyst caused by the high nitrogen content of the carbon matrix and to the synergistic effect of Co and Pd nanoparticles. The CoPd@NPC@ZIF‐12 nanocatalyst showed perfect catalytic activity in the reduction of 4‐nitrophenol (4‐NP), 3‐nitrophenol (3‐NP), and 2,4‐nitrophenol (2,4‐DNP) reactions with high turnover frequency (TOF) values of 1679, 2687, and 1014 h−1, respectively. The reusability experiments of the CoPd@NPC@ZIF‐12 nanocatalyst showed that the catalytic activity of the CoPd@NPC@ZIF‐12 nanocatalyst was almost retained after 10 consecutive reaction runs. The SEM, XRD, and FTIR analyses of the 10 times used CoPd@NPC@ZIF‐12 nanocatalyst showed that there were limited changes in the structure of the CoPd@NPC@ZIF‐12 nanocatalyst. This highly active, magnetically separable, and recyclable CoPd@NPC@ZIF‐12 catalyst exhibits better catalytic activity than commercial Pd/C catalysts.