bluuebunny/crossref_metadata_2025_split huggingface dataset:
Circularly Polarized Luminescence based on 0D Lead‐Free Antimony (III) Halide Hybrids
Authors: Xuan Hong‐Li , Li Jin‐Long , Xu Liang‐Jin , Zheng Da‐Sheng , Chen Zhong‐Ning 
Published: June 2022

AbstractChiral materials with circularly polarized luminescence (CPL) are currently attracting great attention for their wide applications in bioresponsive imaging, 3D displays, and storage of information. Herein, CPL‐active enantiomorphic hybrids (R)‐ and (S)‐C6H15Cl2NO⋅SbCl5are obtained by self‐assembling chiral R/S‐(3‐chloro‐2‐hydroxypropyl)trimethylammonium chloride with antimony(III) chloride, giving a 0D structure with SbCl5pyramids isolated by (3‐chloro‐2‐hydroxypropyl)trimethylammonium chloride cations. The formed enantiomers exhibit brilliant orange emission peaked at 604 nm with photoluminescence quantum yield as high as 71.2%, originating from the self‐trapped exciton emission demonstrated by photophysical characterization. Due to the existence of chiral organic cations, the enantiomers exhibit strong chiral‐optical properties with mirror‐image circular dichroism signals in ground state and obvious CPL activity with the dissymmetry factorglumof 2.5 × 10−4and −1.6 × 10−4for R‐type and S‐type, respectively. It should be mentioned that these are the first reported 0D hybrids with CPL‐activity. This work paves an avenue for developing eco‐friendly CPL materials with highly ‐efficient luminescence.
Modulating the Band Structure of Metal Coordinated Salen COFs and an In Situ Constructed Charge Transfer Heterostructure for Electrocatalysis Hydrogen Evolution
Authors: Zhang Boying , Chen Liling , Zhang Zhenni , Li Qing , Khangale Phathutshedzo , Hildebrandt Diane , Liu Xinying , Feng Qingliang , Qiao Shanlin 
Published: June 2022

AbstractA series of crystalline, stable Metal (Metal = Zn, Cu, Ni, Co, Fe, and Mn)‐Salen covalent organic framework (COF)EDA complex are prepared to continuously tune the band structure of Metal‐Salen COFEDA, with the purpose of optimizing the free energy intermediate species during the hydrogen evolution reaction (HER) process. The conductive macromolecular poly(3,4‐ethylenedioxythiophene) (PEDOT) is subsequently integrated into the one‐dimensional (1D) channel arrays of Metal‐Salen COFEDA to form heterostructure PEDOT@Metal‐Salen COFEDA via the in situ solid‐state polymerization method. Among the Metal‐Salen COFEDA and PEDOT@Metal‐Salen COFEDA complexes, the optimized PEDOT@Mn‐Salen COFEDA displays prominent electrochemical activity with an overpotential of 150 mV and a Tafel slope of 43 mV dec−1. The experimental results and density of states data show that the continuous energy band structure modulation in Metal‐Salen COFEDA has the ability to make the metal d‐orbital interact better with the s‐orbital of H, which is conducive to electron transport in the HER process. Moreover, the calculated charge density difference indicates that the heterostructures composed of PEDOT and Metal‐Salen COFEDA induce an intramolecular charge transfer and construct highly active interfacial sites.
Shielding Surfaces from Viruses and Bacteria with a Multiscale Coating
Authors: Ashok Deepu , Taheri Mahdiar , Garg Puneet , Webb Daryl , Parajuli Pawan , Wang Yi , Funnell Bronte , Taylor Bradley , Tscharke David C. , Tsuzuki Takuya , Verma Naresh K. , Tricoli Antonio , Nisbet David R. 
Published: June 2022

AbstractThe spread of viral and bacterial pathogens mediated by contact with surfaces is a leading cause of infection worldwide. COVID‐19 and the continuous rise of deaths associated with antibiotic‐resistant bacteria highlight the need to impede surface‐mediated transmission. A sprayable coating with an intrinsic ability to resist the uptake of bacteria and viruses from surfaces and droplets, such as those generated by sneezing or coughing, is reported. The coating also provides an effective microbicidal functionality against bacteria, providing a dual barrier against pathogen uptake and transmission. This antimicrobial functionality is fully preserved following scratching and other induced damage to its surface or 9 days of submersion in a highly concentrated suspension of bacteria. The coatings also register an 11‐fold decrease in viral contamination compared to the noncoated surfaces.
Small Molecule NIR‐II Dyes for Switchable Photoluminescence via Host –Guest Complexation and Supramolecular Assembly with Carbon Dots
Authors: Sar Dinabandhu , Ostadhossein Fatemeh , Moitra Parikshit , Alafeef Maha , Pan Dipanjan 
Published: June 2022

AbstractSmall molecular NIR‐II dyes are highly desirable for various biomedical applications. However, NIR‐II probes are still limited due to the complex synthetic processes and inadequate availability of fluorescent core. Herein, the design and synthesis of three small molecular NIR‐II dyes are reported. These dyes can be excited at 850–915 nm and emitted at 1280–1290 nm with a large stokes shift (≈375 nm). Experimental and computational results indicate a 2:1 preferable host–guest assembly between the cucurbit[8]uril (CB) and dye molecules. Interestingly, the dyes when self‐assembled in presence of CB leads to the formation of nanocubes (≈200 nm) and exhibits marked enhancement in fluorescence emission intensity (Switch‐On). However, the addition of red carbon dots (rCDots, ≈10 nm) quenches the fluorescence of these host–guest complexes (Switch‐Off) providing flexibility in the user‐defined tuning of photoluminescence. The turn‐ON complex found to have comparable quantum yield to the commercially available near‐infrared fluorophore, IR‐26. The aqueous dispersibility, cellular and blood compatibility, and NIR‐II bioimaging capability of the inclusion complexes is also explored. Thus, a switchable fluorescence behavior, driven by host–guest complexation and supramolecular self‐assembly, is demonstrated here for three new NIR‐II dyes.
Regulating *OCHO Intermediate as Rate‐Determining Step of Defective Oxynitride Nanosheets Enabling Robust CO2 Electroreduction
Authors: Zhang Bo , Chang Yuan , Wu Yunzhen , Fan Zhaozhong , Zhai Panlong , Wang Chen , Gao Junfeng , Sun Licheng , Hou Jungang 
Published: June 2022

AbstractThe electrochemical conversion of CO2 into hydrocarbons is an important approach to store sustainable energy and address climate concerns. However, it is a huge challenge to unearth a promising model for elucidating the role of dopants and vacancies on catalysts upon CO2 electroreduction. Herein, porous indium oxynitride nanosheets with simultaneous incorporation of nitrogen dopant and oxygen vacancy (Vo‐N‐InON) are reported for achieving efficient CO2 conversion to formic acid (HCOOH). As a result, the catalyst exhibits an extremely high formate selectivity of 95.1% at a low potential of −0.8 V versus reversible hydrogen electrode (RHE) compared with pristine In2O3, Vo‐In2O3, and InN, delivering a large partial current density of 121.1 mA cm–2 for formate production at −1.13 V versus RHE in the flow cell. Density functional theory calculations reveal that the generation of *OCHO intermediate is the rate‐determining step. The synergistic effect between nitrogen dopants and oxygen vacancies contributes to the activation of CO2, facilitates the charge transfer, and reduces the reaction free energy of *OCHO protonation. This work not only discloses a fundamental understanding of synergistic effects between nitrogen dopants and oxygen vacancies to improve catalytic performance, but also provides an effective platform toward CO2 conversion.
Study of hydrodynamics and flow characteristics in a twin‐blade planetary mixer with non‐Newtonian fluids
Authors: Long Jiecai , Zhan Xiaobin , Guo Fang , Sun Zhibin , Shen Baojun , He Yu , Li Xiwen 
Published: June 2022

AbstractThis study aims to characterize the hydrodynamics and flow characteristics in a twin‐blade planetary mixer with non‐Newtonian fluids by using CFD modeling technique. The kneading pressure was recorded using an experimental setup, and a CFD model was verified. The flow characteristics and hydrodynamics in the mixing vessel containing the power‐law fluids were analyzed quantitatively, particularly the influence of the flow behavior index n. Results revealed that as n increased from 0.25 to 1.75, the maximum shear rate decreased from 733 to 120 s−1 and the local apparent viscosity in the kneading regions increased significantly. The maximum kneading pressure and power consumption increased almost exponentially with increasing n. The correlation for the kneading pressure and the correlation for the power consumption were established by introducing the pressure‐oriented effective viscosity μe‐p, the pressure‐oriented effective shear rate , the improved effective viscosity μei and the improved effective shear rate .
Evolution and Single‐Droplet Analysis of Fuel‐Driven Compartments by Droplet‐Based Microfluidics
Authors: Bergmann Alexander M. , Donau Carsten , Späth Fabian , Jahnke Kevin , Göpfrich Kerstin , Boekhoven Job 
Published: June 2022

AbstractActive droplets are a great model for membraneless organelles. However, the analysis of these systems remains challenging and is often limited due to the short timescales of their kinetics. We used droplet‐based microfluidics to encapsulate a fuel‐driven cycle that drives phase separation into coacervate‐based droplets to overcome this challenge. This approach enables the analysis of every coacervate‐based droplet in the reaction container throughout its lifetime. We discovered that the fuel concentration dictates the formation of the coacervate‐based droplets and their properties. We observed that coacervate‐based droplets grow through fusion, decay simultaneously independent of their volume, and shrinkage rate scales with their initial volume. This method helps to further understand the regulation of membraneless organelles, and we believe the analysis of individual coacervate‐based droplets enables future selection‐ or evolution‐based studies.
An Oxazine‐Based Fluorogenic Probe with Changeable π‐Conjugation to Eliminate False‐Positive Interference of Albumin and Its Application to Sensing Aminopeptidase N
Authors: Shang Jizhen , Zhang Xiaofan , He Zixu , Shen Shili , Liu Diankai , Shi Wen , Ma Huimin 
Published: June 2022

AbstractMany fluorophores/probes suffer from the interference of albumin in biosystems. Herein, we propose an effective strategy to overcome this interference by virtue of both an albumin‐insensitive fluorophore and its changeable π‐conjugation, and demonstrate the strategy by designing an oxazine‐based fluorogenic probe for aminopeptidase N (APN). The modification on the N atom in the oxazine fluorophore with alanine through a cleavable linker locks the resulting probe in a non‐conjugated, colorless and non‐fluorescent state, so the non‐specific interaction of albumin produces no spectroscopic response. APN can selectively cleave the alanine moiety, restoring the large π‐conjugation and strong fluorescence. The capability of the probe to eliminate the albumin influence has been demonstrated by imaging APN in different cell lines, and by quantitatively determining APN in human serum and mouse urine. The present strategy may be useful for developing more specific fluorogenic probes for other enzymes.
Straightforward Access to Multifunctional π‐Conjugated P‐Heterocycles Featuring an Internal Ylidic Bond**
Authors: Delouche Thomas , Caytan Elsa , Cordier Marie , Roisnel Thierry , Taupier Grégory , Molard Yann , Vanthuyne Nicolas , Le Guennic Boris , Hissler Muriel , Jacquemin Denis , Bouit Pierre‐Antoine 
Published: June 2022

AbstractWe report the straightforward one‐pot synthesis of novel 5‐ or 6‐membered P‐heterocycles featuring an internal ylidic bond: P‐containing acenaphthylenes and phenanthrenes. The stability of the compounds tolerates post‐functionalization through direct arylation to introduce electron‐rich/poor substituents and the synthetic strategy is also compatible with the preparation of more elaborate polyaromatic scaffolds such as acenes and helicenes. Using a joint experimental (X‐ray analysis, optical and redox properties) and theoretical approach, we perform a full structure–property relationships study on these new platforms. In particular, we show that molecular engineering allows not only tuning their absorption/emission across the entire visible range but also endowing them with chiroptical or non‐linear optical properties, making them valuable dyes for a large panel of photonic or opto‐electronic applications.
Embedding Multiphoton Active Units within Metal–Organic Frameworks for Turning on High‐Order Multiphoton Excited Fluorescence for Bioimaging
Authors: Li Bo , Lu Xin , Tian Yupeng , Li Dandan 
Published: June 2022

AbstractThe fabrication of high‐order multiphoton excited fluorescent materials for second near‐infrared (NIR‐II, 1000–1700 nm) light‐induced fluorescence imaging has always been an intractable challenge. In this study, a reasonable strategy guided by theoretical calculations was employed to fabricate a novel high‐order multiphoton excited fluorescence (H‐MPEF)‐responsive UiO‐type metal–organic framework (MOF, ZrTc). Strategically, the functionalization of the photonic‐responsive thiazolothiazole‐based organic ligand gave rise to amplified H‐MPEF (four‐photon activity) performance and prolonged excitation wavelength (1550 nm) of ZrTcI. The results reveal that the extended π‐electron system, enhanced charge transfer, improved dipole moment, and weakened π‐π stacking interactions within the MOFs endow them with excellent H‐MPEF performance for NIR‐II light‐induced fluorescence imaging. It is an extremely rare report on H‐MPEF bioimaging using MOFs and provide a universal strategy for the fabrication of H‐MPEF‐responsive materials.
Tuning Interphase Chemistry to Stabilize High‐Voltage LiCoO2Cathode Material via Spinel Coating
Authors: Liu Junxiang , Wang Jiaqi , Ni Youxuan , Liu Jiuding , Zhang Yudong , Lu Yong , Yan Zhenhua , Zhang Kai , Zhao Qing , Cheng Fangyi , Chen Jun 
Published: June 2022

AbstractCathode electrolyte interphases (CEIs) are critical to the cycling stability of high‐voltage cathodes for batteries, yet their formation mechanism and properties remain elusive. Here we report that the compositions of CEIs are largely controlled by abundant species in the inner Helmholtz layer (IHL) and can be tuned from material aspects. The IHL of LiCoO2(LCO) was found to alter after charging, with a solvent‐rich environment that results in fragile organic‐rich CEIs. By passivated spinel Li4Mn5O12coating, we achieve an anion‐rich IHL after charging, thus enabling robust LiF‐rich CEIs. In situ microscopy reveals that LiF‐rich CEIs maintain mechanical integrity at 500 °C, in sharp contrast to organic‐rich CEIs which undergo severe expansion and subsequent voids/cracks in the cathode. As a result, the spinel‐coated LCO exhibits a high specific capacity of 194 mAh g−1at 0.05 C and a capacity retention of 83 % after 300 cycles at 0.5 C. Our work sheds new light on modulating CEIs for advanced lithium‐ion batteries.
Discovery and Genetic Code Expansion of a Polyethylene Terephthalate (PET) Hydrolase from the Human Saliva Metagenome for the Degradation and Bio‐Functionalization of PET
Authors: Eiamthong Bhumrapee , Meesawat Piyachat , Wongsatit Thanakrit , Jitdee Jariya , Sangsri Raweewan , Patchsung Maturada , Aphicho Kanokpol , Suraritdechachai Surased , Huguenin‐Dezot Nicolas , Tang Shan , Suginta Wipa , Paosawatyanyong Boonchoat , Babu M. Madan , Chin Jason W. , Pakotiprapha Danaya , Bhanthumnavin Worawan , Uttamapinant Chayasith 
Published: June 2022

AbstractWe report a bioinformatic workflow and subsequent discovery of a new polyethylene terephthalate (PET) hydrolase, which we named MG8, from the human saliva metagenome. MG8 has robust PET plastic degradation activities under different temperature and salinity conditions, outperforming several naturally occurring and engineered hydrolases in degrading PET. Moreover, we genetically encoded 2,3‐diaminopropionic acid (DAP) in place of the catalytic serine residue of MG8, thereby converting a PET hydrolase into a covalent binder for bio‐functionalization of PET. We show that MG8(DAP), in conjunction with a split green fluorescent protein system, can be used to attach protein cargos to PET as well as other polyester plastics. The discovery of a highly active PET hydrolase from the human metagenome—currently an underexplored resource for industrial enzyme discovery—as well as the repurposing of such an enzyme into a plastic functionalization tool, should facilitate ongoing efforts to degrade and maximize reusability of PET.
Self‐Assembly of 2D Hybrid Double Perovskites on 3D Cs2AgBiBr6 Crystals towards Ultrasensitive Detection of Weak Polarized Light
Authors: Zhang Xinyuan , Yao Yunpeng , Liang Lishan , Niu Xinyi , Wu Jianbo , Luo Junhua 
Published: June 2022

AbstractWe report the self‐assembly of 2D double perovskite (BLA)2CsAgBiBr7 (BLA=benzylammonium) on 3D Cs2AgBiBr6 crystals, providing the first demonstration of polarization‐sensitive photodetection using lead‐free double perovskite heterocrystals (HCs). The (BLA)2CsAgBiBr7/Cs2AgBiBr6 HC successfully combines the anisotropy of 2D double perovskites with the well‐defined interface provided by heterogeneous integration. Driven by the built‐in electric field in junction, photodetectors of HCs exhibit unique polarization dependence of zero‐bias photocurrent with a large anisotropy ratio up to 9, which is 6 times amplified as compared to the pristine 2D (BLA)2CsAgBiBr7. More importantly, the present devices can remain polarization‐sensitive with incident light intensity down to the nW cm−2 level. Our study on lead‐free hybrid perovskite HCs marks a step toward establishing robust material foundations for fundamental scientific investigations and the development of optoelectronic devices.
Nitric‐Oxide‐Releasing aza‐BODIPY: A New Near‐Infrared J‐Aggregate with Multiple Antibacterial Modalities
Authors: Bao Xinyao , Zheng Shaoqiu , Zhang Lei , Shen Aizong , Zhang Guoying , Liu Shiyong , Hu Jinming 
Published: June 2022

AbstractThe development of near‐infrared (NIR) J‐aggregates has received increasing attention due to their broad applications. Here, we report the nitrosation of an amine‐containing aza‐BODIPY precursor (BDP‐NH2), affording the first nitric oxide (NO)‐releasing NIR J‐aggregate (BDP‐NO). The introduction of N‐nitrosamine moieties efficiently inhibits the aromatic interactions of BDP‐NH2, which instead promotes the formation of J‐aggregates within micellar nanoparticles with a remarkable bathochromic shift of ≈109 nm to the NIR window (820 nm). Interestingly, the NO release and photothermal conversion efficiency (PTCE) can be delicately tuned by the loading contents of BDP‐NO within micellar nanoparticles, thereby enabling multiple antibacterial modalities by exploring either NO release, photothermal therapy (PTT), or both. We demonstrate the combination of NO and PTT can elevate antibacterial activity while attenuating PTT‐associated inflammation for the in vivo treatment of MRSA infection.
Self‐assembled graphene oxide microcapsules in Pickering emulsions for photo‐responsive self‐healing epoxy coatings
Authors: Yu Fei , Feng Hengyu , Leng Jinpeng , Xue Hongying , Zhong Ziyi , Yan Zhen , Liu Xudong , Liu Yu , Xiao Linghan 
Published: June 2022

AbstractIn regard to the nonfatal harm self‐healing of natural species, microcapsule‐based polymeric materials for self‐healing have been considered to be highly desirable in light of their ability to heal cracks in significant volumes, leaving the original chemical structures of polymers unchanged. Accordingly, this study sought to design a one‐component photo‐responsive self‐healing polymer composite based on Bisphenol A epoxy acrylate resin @graphene oxide microcapsules (BAEA@GOMCs) that are capable of photo‐absorption in order to reduce difficulties of processing and inhomogeneous distributions of the two components. Embedding of BAEA@GOMCs were carried out in waterborne epoxy matrix, and self‐healing composite coatings were generated onto surfaces of hot‐dip steel via galvanization. Upon incurring mechanical damage, solidification of the agents of photo‐responsive healing and the flowing the cracks were achieved as the agents were exposed to light to achieve self‐healing. In addition, the solidification within the unbroken microcapsules was maintained, and there were continuous no reactions. Given the simplicity of the proposed preparation, incorporating light‐absorbing particles into the microcapsule shell can further broaden the application range of the aforementioned common materials.
Anti‐migration performance of EPDM composite improved by octadecylamine‐functionalized graphene oxide
Authors: Lu Zhehong , Hu Yubing , Zhang Bohan , Zhang Guangpu , Guo Fan , Jiang Wei 
Published: June 2022

AbstractIn this paper, the ethylene propylene diene monomer (EPDM) was used as a composite matrix and octadecylamine‐functionalized graphene oxide (GA) was applied as insulation nanofiller to prevent plasticizer migration. To study the anti‐migration behavior of EPDM under plasticizer environment and different temperatures, we investigated the diffusion of dioctyl phthalate (DOP) in EPDM and its composites. The migration kinetics of DOP into EPDM composites with respect to filler and temperature were observed by the immersion absorption method. The process is dynamic and conforms to Fick's law. The composite show a 90% increase in tensile strength and 151% improvement in elongation at break by the addition of 5 phr filler of GA. Meanwhile, the EPDM/GA composite show an obviously improved anti‐migration performance, compared to pure EPDM at different temperatures, the composite show a 22.68%, 17.35%, 14.95%, 7.63% increase. Well layer‐structure of graphene offers a chance to improve the anti‐migration performance of insulation.
Hybrid imidazo[1,2‐a]pyridine analogs as potent ATX inhibitors with concrete in vivo antifibrosis effect
Authors: Li Tong , Lei Hongrui , Yang Juanjuan , Cao Zhi , Yang Yu , Liu Zimeng , Sun Ruonan , Yang Xinlian , Zhai Xin 
Published: June 2022

AbstractIn recent years, small‐molecule inhibitors targeting the autotaxin (ATX)/lysophosphatidic acid axis gradually brought excellent disease management benefits. Herein, a series of imidazo[1,2‐a]pyridine compounds (1–11) were designed as ATX inhibitors through a hybrid strategy by combining the imidazo[1,2‐a]pyridine skeleton in GLPG1690 and the benzyl carbamate moiety in PF‐8380. As indicated by FS‐3‐based enzymatic assay, the carbamate derivatives revealed moderate to satisfying ATX inhibitory potency (IC50 = 23–343 nM). Subsequently, the carbamate linker was altered to a urea moiety (12–19) with the aim of retaining ATX inhibition and improving the druglikeness profile. The binding mode analysis all over the modification process well rationalized the leading activity of urea derivatives in an enzymatic assay. Following further structural optimization, the diethanolamine derivative 19 exerted an amazing inhibitory activity (IC50 = 3.98 nM) similar to the positive control GLPG1690 (IC50 = 3.72 nM) and PF‐8380 (IC50 = 4.23 nM). Accordingly, 19 was tested directly for in vivo antifibrotic effects through a bleomycin model (H&E staining), in which 19 effectively alleviated lung structural damage and fibrosis at an oral dose of 20 and 60 mg/kg. Collectively, 19 qualified as a promising ATX inhibitor for potential application in fibrosis‐relevant disease treatment.