bluuebunny/crossref_metadata_2025_split huggingface dataset:
Engineering Next Generation Cyclized Peptide Ligands for Light‐Controlled Capture and Release of Therapeutic Proteins
Authors: Prodromou Raphael , Day Kevin N. , Saberi‐Bosari Sahand , Schneible John D. , Mabe Matthew D. , San Miguel Adriana , Daniele Michael A. , Pozdin Vladimir , Menegatti Stefano 
Published: May 2021

AbstractPhoto‐affinity adsorbents (i.e., translucent matrices functionalized with ligands featuring light‐controlled biorecognition) represent a futuristic technology for purifying labile biologics. In this study, a framework for prototyping photo‐affinity adsorbents comprising azobenzene‐cyclized peptides (ACPs) conjugated to translucent porous beads (ChemMatrix) is presented. This approach combines computational and experimental tools for designing ACPs and investigating their light‐controlled isomerization kinetics and protein biorecognition. First, a modular design for tailoring ACP's conformation, facilitating sequencing, and streamlining the in silico modeling of cis/trans isomers and their differential protein binding is introduced. Then, a spectroscopic system for measuring the photo‐isomerization kinetics of ACPs on ChemMatrix beads is reported; using this device, it is demonstrated that the isomerization at different light intensities is correlated to the cyclization geometry, specifically the energy difference of trans versus cis isomers as calculated in silico. Also, a microfluidic device for sorting ACP‐ChemMatrix beads to select and validate photo‐affinity ligands using Vascular Cell Adhesion Molecule 1 (VCAM‐1) as target protein and cycloAZOB[GVHAKQHRN‐K*]‐G‐ChemMatrix as model photo‐affinity adsorbent is presented. The proposed ACPs exhibit rapid and defined light‐controlled isomerization and biorecognition. Controlling the adsorption and release of VCAM‐1 using light demonstrates the potential of photo‐affinity adsorbents for targets whose biochemical liability poses challenges to its purification.
Rechargeable Potassium–Selenium Batteries
Authors: Huang Xiang Long , Guo Zaiping , Dou Shi Xue , Wang Zhiming M. 
Published: May 2021

AbstractRechargeable potassium–selenium (K–Se) batteries, as an emerging electrochemical energy storage system, has recently captured intensive attention due to the desirable natural abundance and low redox potential of elemental potassium as well as the relatively high electronic conductivity and impressive theoretical volumetric capacity of elemental selenium. Although great progress on cathode materials design and electrochemical performance improvement has been made, K–Se batteries are still confronted with a series of key challenges, including low reactive activity, shuttle effect, volume expansion, potassium dendrite growth, and high chemical activity of potassium metal. The recent advances in rechargeable K–Se batteries are comprehensively summarized with an emphasis on discussing the electrochemical mechanisms and central challenges, presenting the synthesis, properties, and electrochemical performance of selenium‐based cathode materials, and extending potential tactics for tackling the key issues and developmental directions for future research.
Unravelling Magnetic Nanochain Formation in Dispersion for In Vivo Applications
Authors: Nandakumaran Nileena , Barnsley Lester , Feoktystov Artem , Ivanov Sergei A. , Huber Dale L. , Fruhner Lisa S. , Leffler Vanessa , Ehlert Sascha , Kentzinger Emmanuel , Qdemat Asma , Bhatnagar‐Schöffmann Tanvi , Rücker Ulrich , Wharmby Michael T. , Cervellino Antonio , Dunin‐Borkowski Rafal E. , Brückel Thomas , Feygenson Mikhail 
Published: May 2021

AbstractSelf‐assembly of iron oxide nanoparticles (IONPs) into 1D chains is appealing, because of their biocompatibility and higher mobility compared to 2D/3D assemblies while traversing the circulatory passages and blood vessels for in vivo biomedical applications. In this work, parameters such as size, concentration, composition, and magnetic field, responsible for chain formation of IONPs in a dispersion as opposed to spatially confining substrates, are examined. In particular, the monodisperse 27 nm IONPs synthesized by an extended LaMer mechanism are shown to form chains at 4 mT, which are lengthened with applied field reaching 270 nm at 2.2 T. The chain lengths are completely reversible in field. Using a combination of scattering methods and reverse Monte Carlo simulations the formation of chains is directly visualized. The visualization of real‐space IONPs assemblies formed in dispersions presents a novel tool for biomedical researchers. This allows for rapid exploration of the behavior of IONPs in solution in a broad parameter space and unambiguous extraction of ​the parameters of the equilibrium structures. Additionally, it can be extended to study novel assemblies formed by more complex geometries of IONPs.
Ultrathin‐Walled 3D Inorganic Nanostructured Networks Templated from Cross‐Linked Cellulose Nanocrystal Aerogels
Authors: Hiltunen Arto , Or Tyler , Lahtonen Kimmo , Ali‐Löytty Harri , Tkachenko Nikolai , Valden Mika , Sarlin Essi , Cranston Emily D. , Moran‐Mirabal Jose M. , Vapaavuori Jaana 
Published: May 2021

AbstractA key challenge in the development of materials for applications in the fields of opto‐ and nanoelectronics, catalysis, separation, and energy conversion is the ability to fabricate 3D inorganic semiconductive nanostructures in a precisely‐controlled and cost‐effective manner. This work describes the fabrication of 3D nanostructured TiO2 monoliths by coating ultraporous cross‐linked cellulose nanocrystal (CNC) aerogel templates with TiO2 layers of controlled thickness via atomic layer deposition (ALD). Following calcination, the resulting hollow inorganic ultraporous 3D networks form the thinnest self‐supporting semiconductive structure (7 nm) fabricated directly on a conductive substrate. The CNC‐templated ALD–TiO2 electrodes are applied toward photoelectrochemical water splitting. The results show that a TiO2 coating as thin as 15 nm produces a maximum water splitting efficiency, resulting in materials savings and reduced fabrication time.
Control of Stepwise Hg2+ Reduction on Gold to Selectively Tune its Peroxidase and Catalase‐Like Activities and the Mechanism
Authors: Chen Yao , Shen Xiaomei , Carmona Unai , Yang Fan , Gao Xingfa , Knez Mato , Zhang Lianbing , Qin Yong 
Published: May 2021

AbstractThe flexible regulation of enzyme‐like activities of nanozyme is of great importance in biomedical applications. However, the current modulation strategies usually lack activity specificity to reveal precise tuning of the desired activity. In this work, it is demonstrated for the first time that the Hg2+ on surfaces of Au film can be reduced in a chemical path of Hg(II) → Hg(I) → Hg(0) via anti‐Galvanic reaction. Furthermore, it is amazing that the generated Hg0 via Hg(NO3)2 treatment contributes to greatly boosted peroxidase and catalase activities of Au films due to the formation of Au@Hg amalgam, while the main Hg+ species on Au formed by HgCl2 modification results in only catalase‐like activity acceleration. Based on this, the peroxidase‐ and catalase‐like activities of gold can be selectively modulated by controlling the stepwise reduction of Hg2+. Further density functionality theory (DFT) calculations reveal that it is the significantly lowered activation energy by Au@Hg amalgam that accounts for the acceleration of both peroxidase and catalase reaction. These results demonstrate a novel avenue to specifically modulate the enzyme‐mimicking activities of Au, which not only facilitates the design of nanozymes with specific activity, but also broadens their biological usage.
Layer‐by‐Layer 2D Ultrathin Conductive Cu3(HHTP)2 Film for High‐Performance Flexible Transparent Supercapacitors
Authors: Zhao Weiwei , Chen Tiantian , Wang Weikang , Bi Shuaihang , Jiang Mengyue , Zhang Kenneth Yin , Liu Shujuan , Huang Wei , Zhao Qiang 
Published: May 2021

Abstract2D conductive metal–organic frameworks (2D c‐MOFs) naturally possess high active sites, large specific surface areas, and fast ion transport for energy‐storage devices. However, the intelligent exploration of 2D c‐MOFs for the emerging flexible transparent supercapacitors (FTSCs) with excellent photoelectric property and electrochemical activity is rarely implemented. Herein, 2D conductive ultrathin Cu3(HHTP)2 (HHTP = 2,3,6,7,10,11‐hexahydroxytriphenylene) film is synthesized on the indium tin oxide/polyethylene terephthalate (ITO/PET) substrate for flexible transparent conductive electrodes (FTCEs) through the layer‐by‐layer assembly method. The interconnected conductive frameworks possess the cooperative superiority of low internal resistance, fast electrolyte ion diffusion, and quick electron transfer. Cu3(HHTP)2‐15/ITO/PET FTCEs show high photoelectric property of T550 nm = 82.2% and Rs = 49.1 Ω sq−1, and high areal capacitance (CA) of 1700 µF cm−2. The corresponding symmetrical FTSCs (T550 nm = 62.1%) exhibit excellent CA of 939.2 µF cm−2 at the current density of 7 µA cm−2, superior rate capability (63.9% at 150 µA cm−2), long‐term cycling stability (85% after 3000 cycles), and mechanical flexibility under different bending angles. This work provides key insights into the design and synthesis of 2D c‐MOF films for flexible transparent energy‐storage devices.
High‐Linearity, Response‐Range Adjustable Force Sensors Based on a Yarn/Film/Spacer Triboelectric Device Design
Authors: Cao Yuying , Shao Hao , Wang Hongxia , Yang Xiao , Gao Qi , Cheng Tinghai , Fang Jian , Lin Tong 
Published: May 2021

AbstractIn this study, a novel triboelectric device is developed that consists of a silicone‐coated conductive yarn and a PET film as active substances, and an elastic spacer as a force controller. The silicone‐coated yarn is prepared by applying a thermally curable silicone to conductive yarns using a simple but continuous method. The device made of 20 cm long yarn can generate peak voltage as high as 225 V and current outputs of 2.4 µA. The elastic spacer functions to maintain the yarn and PET film in a separate state when no force is loaded and to adjust the response threshold and detection range by changing the spacer area. In comparison to the triboelectric force‐sensors reported previously, this yarn/film device shows a much larger detection range (24–380 N) and higher flexibility in tuning the detection range. The output voltage‐input force curves of the devices have an R2 value above 0.91, indicating the good linearity between the input force and voltage output. Moreover, a theoretical model is developed to elucidate the influence of the spacer area on the detection range and sensitivity. Such a yarn/film/spacer sensor design may be useful for the development of low‐cost force sensors for various applications.
Synthesis of Pyrazolo[1,2‐a]cinnolines via Rhodium(III)‐Catalyzed [4+2] Annulation Reactions of Pyrazolidinones with Sulfoxonium Ylides
Authors: Hu Shulei , Han Xu , Xie Xiong , Fang Feifei , Wang Yong , Saidahmatov Abdusaid , Liu Hong , Wang Jiang 
Published: May 2021

AbstractA method to synthesize pyrazolo[1,2‐a]cinnolines via rhodium(III)‐catalyzed C−H activation of pyrazolidinones and subsequent [4+2] annulation of sulfoxonium ylides was developed. 5‐Substituted or 5,10‐disubstituted pyrazolo[1,2‐a]cinnolines could be obtained by slightly adjusting the reaction conditions. Gram‐scale synthesis and practical transformations proved the practicability of this method. The mechanism of this method was proposed in the article on the basis of preliminary mechanistic results and previous reports. This method features simplified operation, metal‐oxidant free, and readily available reactants.magnified image
Antisolvent‐ and Annealing‐Free Deposition for Highly Stable Efficient Perovskite Solar Cells via Modified ZnO
Authors: Wang Ziyu , Zhu Xuejie , Feng Jiangshan , Wang Chenyu , Zhang Cong , Ren Xiaodong , Priya Shashank , Liu Shengzhong (Frank) , Yang Dong 
Published: May 2021

AbstractEven though ZnO is commonly used as the ETL in the perovskite solar cell (PSC), the reactivity of perovskite deposited thereupon limits its performance. Herein, an ethylene diamine tetraacetic acid‐complexed ZnO (E‐ZnO) is successfully developed as a significantly improved electron selective layer (ESLs) in perovskite device. It is found that E‐ZnO exhibits higher electron mobility and better matched energy level with perovskite compared to ZnO. In addition, in order to eliminate the proton transfer reaction at the ZnO/perovskite interface, a high quality perovskite film fabrication process that requires neither annealing nor antisolvent is developed. By taking advantages of both E‐ZnO and the new process, the highest efficiency of 20.39% is obtained for PSCs based on E‐ZnO. Moreover, the efficiency of unencapsulated PSCs with E‐ZnO retains 95% of its initial value exposed in an ambient atmosphere after 3604 h. This work provides a feasible path toward high performance of PSCs, and it is believed that the present work will facilitate transition of perovskite photovoltaics in flexible and tandem devices since the annealing‐ and antisolvent‐free technology.
Negative Photoconductance Effect: An Extension Function of the TiOx‐Based Memristor
Authors: Zhou Guangdong , Sun Bai , Hu Xiaofang , Sun Linfeng , Zou Zhuo , Xiao Bo , Qiu Wuke , Wu Bo , Li Jie , Han Juanjuan , Liao Liping , Xu Cunyun , Xiao Gang , Xiao Lihua , Cheng Jianbo , Zheng Shaohui , Wang Lidan , Song Qunliang , Duan Shukai 
Published: May 2021

AbstractThe negative photoconductance (NPC) effect, defined as an increase in resistance upon exposure to illumination, holds great potential for application in photoelectric devices. A prepared memristor with the structure of Ag|graphene quantum dots (GQDs)|TiOx|F‐doped SnO2 exhibits typical bipolar resistive switching (RS) memory behavior. The NPC effect is impressively observed in the high resistance state branch of the RS memory, enabling the memristor function to be extended to both memory logic display and multistate data storage. The observed NPC effect is attributed to the excitation, migration, and compensation of oxygen vacancy at the GQDs/TiOx interface, at which the electron transportation is efficiently restricted because of the variation in the charge distribution and electrostatic potential under illumination. Experiments, theoretical calculations, and physical models are used to provide engineer the interface with the aim of building the NPC effect in the memristive device. These results unveil a new horizon on extending the functionality of the memristor.
Dissolving Candlelit Microneedle for Chronic Inflammatory Skin Diseases
Authors: Ohn Jungyoon , Jang Mingyu , Kang Bo Mi , Yang Huisuk , Hong Jin Tae , Kim Kyu Han , Kwon Ohsang , Jung Hyungil 
Published: May 2021

AbstractChronic inflammatory skin diseases (CISDs) negatively impact a large number of patients. Injection of triamcinolone acetonide (TA), an anti‐inflammatory steroid drug, directly into the dermis of diseased skin using needle‐syringe systems is a long‐established procedure for treating recalcitrant lichenified lesions of CISDs, referred to as TA intralesional injection (TAILI). However, TAILI causes severe pain, causing patients to be stressed and reluctant to undergo treatment. Furthermore, the practitioner dependency on the amount and depth of the injected TA makes it difficult to predict the prognosis. Here, candle flame (“candlelit”)‐shaped TA‐loaded dissolving microneedles (Candlelit‐DMN) are designed and fabricated out of biocompatible and biodegradable molecules. Candlelit‐DMN distributes TA evenly across human skin tissue. Conjoined with the applicator, Candlelit‐DMN is efficiently inserted into human skin in a standardized manner, enabling TA to be delivered within the target layer. In an in vivo skin inflammation mouse model, Candlelit‐DMN inserted with the applicator effectively alleviates inflammation by suppressing inflammatory cell infiltration and cytokine gene expression, to the same extent as TAILI. This Candlelit‐DMN with the applicator arouses the interest of dermatologists, who prefer it to the current TAILI procedure.
A Noninvasive Multianalytical Approach for Lung Cancer Diagnosis of Patients with Pulmonary Nodules
Authors: Liu Quan‐Xing , Zhou Dong , Han Tian‐Cheng , Lu Xiao , Hou Bing , Li Man‐Yuan , Yang Gui‐Xue , Li Qing‐Yuan , Pei Zhi‐Hua , Hong Yuan‐Yuan , Zhang Ya‐Xi , Chen Wei‐Zhi , Zheng Hong , He Ji , Dai Ji‐Gang 
Published: May 2021

AbstractAddressing the high false‐positive rate of conventional low‐dose computed tomography (LDCT) for lung cancer diagnosis, the efficacy of incorporating blood‐based noninvasive testing for assisting practicing clinician's decision making in diagnosis of pulmonary nodules (PNs) is investigated. In this prospective observative study, next generation sequencing‐ (NGS‐) based cell‐free DNA (cfDNA) mutation profiling, NGS‐based cfDNA methylation profiling, and blood‐based protein cancer biomarker testing are performed for patients with PNs, who are diagnosed as high‐risk patients through LDCT and subsequently undergo surgical resections, with tissue sections pathologically examined and classified. Using pathological classification as the gold standard, statistical and machine learning methods are used to select molecular markers associated with tissue's malignant classification based on a 98‐patient discovery cohort (28 benign and 70 malignant), and to construct an integrative multianalytical model for tissue malignancy prediction. Predictive models based on individual testing platforms have shown varying levels of performance, while their final integrative model produces an area under the receiver operating characteristic curve (AUC) of 0.85. The model's performance is further confirmed on a 29‐patient independent validation cohort (14 benign and 15 malignant, with power > 0.90), reproducing AUC of 0.86, which translates to an overall sensitivity of 80% and specificity of 85.7%.
Emergent Magnetic Phenomenon with Unconventional Structure in Epitaxial Manganate Thin Films
Authors: Yang Mingwei , Jin Kuijuan , Yao Hongbao , Zhang Qinghua , Ji Yiru , Gu Lin , Ren Wenning , Zhao Jiali , Wang Jiaou , Guo Er‐Jia , Ge Chen , Wang Can , Xu Xiulai , Wu Qiong , Yang Guozhen 
Published: May 2021

AbstractA variety of emergent phenomena are enabled by interface engineering in the complex oxides heterostructures. While extensive attention is attracted to LaMnO3 (LMO) thin films for observing the control of functionalities at its interface with substrate, the nature of the magnetic phases in the thin film is, however, controversial. Here, it is reported that the ferromagnetism in two and five unit cells thick LMO films epitaxially deposited on (001)‐SrTiO3 substrates, a ferromagnetic/ferromagnetic coupling in eight and ten unit cells ones, and a striking ferromagnetic/antiferromagnetic pinning effect with apparent positive exchange bias in 15 and 20 unit cells ones are observed. This novel phenomenon in both 15 and 20 unit cells films indicates a coexistence of three magnetic orderings in a single LMO film. The high‐resolution scanning transmission electron microscopy suggests a P21/n to Pbnm symmetry transition from interface to surface, with the spatial stratification of MnO6 octahedral morphology, corresponding to different magnetic orderings. These results can shed some new lights on manipulating the functionality of oxides by interface engineering.
Mitigating the Undesirable Chemical Reaction between Organic Molecules for Highly Efficient Flexible Organic Photovoltaics
Authors: Prasetio Adi , Jahandar Muhammad , Kim Soyeon , Heo Jinhee , Kim Yong Hyun , Lim Dong Chan 
Published: May 2021

AbstractOrganic photovoltaics (OPVs) with nonfullerene acceptors (NFAs) feature excellent device performance and device stability. However, they are facing problems when the amine‐rich polyelectrolytes are used as cathode interfacial layers. In this work, a small molecule, ethanedithiol (EDT) at the polyethyleneimine ethoxylated (PEIE)/active layer interface is inserted for mitigating the undesirable reaction between amine‐rich groups and electron‐acceptor moieties in NFA. The main role of EDT is to passivate the PEIE surface and prevent electron flow to NFA and the unwanted reaction can be mitigated. It improves the performance of OPV devices by reducing the work function, decreasing trap‐assisted recombination, and improving electron‐mobility. As a result, the flexible device with the PEIE interfacial layer with a power conversion efficiency (PCE) of 7.20% can be improved to 10.11% after the inclusion of EDT. Moreover, EDT‐modified device can retain 98.18% after it is bent for 200 cycles and can maintain 80.83% of its initial PCE under continuous light illuminated in ambient conditions without any encapsulation. Based on these findings, the proposed strategy constitutes a crucial step toward highly efficient flexible OPVs.
Influence of Crystallinity of Lithium Thiophosphate Solid Electrolytes on the Performance of Solid‐State Batteries
Authors: Wang Shuo , Zhang Wenbo , Chen Xiang , Das Dyuman , Ruess Raffael , Gautam Ajay , Walther Felix , Ohno Saneyuki , Koerver Raimund , Zhang Qiang , Zeier Wolfgang G. , Richter Felix H. , Nan Ce‐Wen , Janek Jürgen 
Published: May 2021

AbstractSolid electrolytes (SEs) largely define the properties of all‐solid‐state batteries (ASSBs) and are expected to improve their safety, stability, and performance. Their ionic conductivity has much improved in recent years, enabling higher power and energy density. However, more subtle parameters, such as crystallinity, may also influence the electrochemical performance of cells. In this work, the correlation between the performance of ASSBs and thiophosphate SEs having the same stoichiometry, but different crystallinity is investigated. In In/InLi | SE | LiCoO2@ LiNb0.5Ta0.5O3 model cells, better cycling and rate performance is achieved when using glass/glass‐ceramic SEs (e.g., 75Li2S·25P2S5 glass, 70Li2S·30P2S5 glass, and Li6PS5Cl glass‐ceramic). This can be mostly attributed to the mitigation of contact loss by the glass/glass‐ceramic SEs compared to their crystalline SE counterparts. Furthermore, the SE decomposition at typical cathode potentials is investigated by using SE and carbon composites as cathodes. Larger volume changes and more severe decomposition are observed with crystalline SEs in the SE/carbon composite cathode after cycling. The crystalline SEs show higher electronic partial conductivity which results in more degradation in the composite cathode. This work sheds light on optimized composite cathode design for ASSB by carefully choosing solid electrolytes with appropriate mechanical and (electro‐)chemical properties.