bluuebunny/crossref_metadata_2025_split huggingface dataset:
Bioinspired MXene‐Based Piezoresistive Sensor with Two‐stage Enhancement for Motion Capture
Authors: Wang Shenglong , Deng Weili , Yang Tao , Ao Yong , Zhang Hongrui , Tian Guo , Deng Lin , Huang Haichao , Huang Junfeng , Lan Boling , Yang Weiqing 
Published: February 2023

AbstractStructured piezoresistive membranes are compelling building blocks for wearable bioelectronics. However, the poor structural compressibility of conventional microstructures leads to rapid saturation of detection range and low sensitivity of piezoresistive devices, limiting their commercial applications. Herein, a bioinspired MXene‐based piezoresistive device is reported, which can effectively boost the sensitivity while broadening the response range by architecting intermittent villus‐like microstructures. Benefitting from the two‐stage amplification effect of this intermittent architecture, the developed MXene‐based piezoresistive bioelectronics exhibit a high sensitivity of 461 kPa−1 and a broad pressure detection range of up to 311 kPa, which are about 20 and 5 times higher than that of the homogeneous microstructures, respectively. Cooperating with the deep‐learning algorithm, the designed bioelectronics can effectively capture complex human movements and precisely identify human motion with a high recognition accuracy of 99%. Evidently, this intermittent architecture of biomimetic strategy may pave a promising avenue to overcome the limitation of rapid saturation and low sensitivity in piezoresistive bioelectronics, and provide a general way to promote its large‐scale applications.
Biosafe Saccharomyces Cerevisiae Immobilized Nanofibrous Aerogels for Integrated Lead Removal in Human Body
Authors: Cao Shiyi , Wu Shuangquan , Dong Xiangyang , Long Min , Lin Heng , Liu Fangtian , Wu Yang , Zhao Ze , Chen Chaoji , Deng Hongbing 
Published: February 2023

AbstractEmerging adsorption technology shows great potential for Pb2+ removal in the human body because of its high adsorption efficiency and easy operation. However, biosafety concerns in the human body limit the development of adsorbents in integrated lead removal for acute poisoning in humans from the gastrointestinal tract and even the blood. In this work, highly bio‐safe and natural saccharomyces cerevisiae cells are immobilized on the interworking natural regenerated cellulose nanofibers network for integrated lead removal in the human body. High intrinsic biosafety of the aerogel is guaranteed due to the biocompatibility of aerogel composition and the absence of cross‐linking substances. Attributing to the porous structure of cellulose nanofibrous scaffolds, saccharomyces cerevisiae cells are protected from shedding, and considerable loading sites for saccharomyces cerevisiae cells are ensured. Simultaneously, abundant functional groups on the saccharomyces cerevisiae cells exhibit superior adsorption ability with a saturated adsorption capacity of lead ions as high as 107 mg g−1 in the aquatic environment. After adsorption, Pb2+ concentration decreases from 879.70 to 248.53 µg L−1 in the intestinal phase and from 400 to 186.29 µg L−1 (within a safe level) in blood, providing an attractive strategy for detoxification of integrated lead in the human body.
Electric Control of 2D Van Hove Singularity in Oxide Ultra‐Thin Films
Authors: Kim Donghan , Kim Younsik , Sohn Byungmin , Kim Minsoo , Kim Bongju , Noh Tae Won , Kim Changyoung 
Published: February 2023

AbstractDivergent density of states (DOS) can induce extraordinary phenomena such as significant enhancement of superconductivity and unexpected phase transitions. Moreover, van Hove singularities (VHSs) lead to divergent DOS in 2D systems. Despite recent interest in VHSs, only a few controllable cases have been reported to date. In this work, by utilizing an atomically ultra‐thin SrRuO3 film, the electronic structure of a 2D VHS is investigated with angle‐resolved photoemission spectroscopy and transport properties are controlled. By applying electric fields with alkali metal deposition and ionic‐liquid gating methods, the 2D VHS and the sign of the charge carrier are precisely controlled. Use of a tunable 2D VHS in an atomically flat oxide film could serve as a new strategy to realize infinite DOS near the Fermi level, thereby allowing efficient tuning of electric properties.
Sub‐Nanosecond 2D Perovskite Scintillators by Dielectric Engineering
Authors: Xia Mengling , Xie Zuoxiang , Wang Hanqi , Jin Tong , Liu Linyue , Kang Jun , Sang Ziru , Yan Xianchang , Wu Boning , Hu Hao , Tang Jiang , Niu Guangda 
Published: February 2023

AbstractPerovskite materials have demonstrated great potential for ultrafast scintillators with high light yield. However, the decay time of perovskite still cannot be further minimized into sub‐nanosecond region, while sub‐nanosecond scintillators are highly demanded in various radiation detection, including high speed X‐ray imaging, time‐of‐flight based tomography or particle discrimination, and timing resolution measurement in synchrotron radiation facilities, etc. Here, a rational design strategy is showed to shorten the scintillation decay time, by maximizing the dielectric difference between organic amines and Pb‐Br octahedral emitters in 2D organic‐inorganic hybrid perovskites (OIHP). Benzimidazole (BM) with low dielectric constant inserted between [PbBr6]2− layers, resulting in a surprisingly large exciton binding energy (360.3 ± 4.8 meV) of 2D OIHP BM2PbBr4. The emitting decay time is shortened as 0.97 ns, which is smallest among all the perovskite materials. Moreover, the light yield is 3190 photons MeV−1, which is greatly higher than conventional ultrafast scintillator BaF2 (1500 photons MeV−1). The rare combination of ultrafast decay time and considerable light yield renders BM2PbBr4 excellent performance in γ‐ray, neutron, α‐particle detection, and the best theoretical coincidence time resolution of 65.1 ps, which is only half of the reference sample LYSO (141.3 ps).
Unveiling the Morphological and Physical Mechanism of Burn‐in Loss Alleviation by Ternary Matrix Toward Stable and Efficient All‐Polymer Solar Cells
Authors: Ma Ruijie , Fan Qunping , Dela Peña Top Archie , Wu Baohua , Liu Heng , Wu Qiang , Wei Qi , Wu Jiaying , Lu Xinhui , Li Mingjie , Ma Wei , Li Gang 
Published: February 2023

AbstractAll‐polymer solar cells (All‐PSCs) are considered the most promising candidate in achieving both efficient and stable organic photovoltaic devices, yet the field has rarely presented an in‐depth understanding of corresponding device stability while efficiency is continuously boosted via the innovation of polymer acceptors. Herein, a ternary matrix is built for all‐PSCs with optimized morphology, improved film ductility and importantly, boosted efficiency and better operational stability than its parental binary counterparts, as a platform to study the underlying mechanism. The target system PQM‐Cl:PTQ10:PY‐IT (0.8:0.2:1.2) exhibits an alleviated burn‐in loss of morphology and efficiency under light soaking, which supports its promoted device lifetime. The comprehensive characterizations of fresh and light‐soaked active layers lead to a clear illustration of opposite morphological and physical degradation direction of PQM‐Cl and PTQ10, thus resulting in a delicate balance at the optimal ternary system. Specifically, the enlarging tendency of PQM‐Cl and shrinking preference of PTQ10 in terms of phase separation leads to a stable morphology in their mixing phase; the hole transfer kinetics of PQM‐Cl:PY‐IT host is stabilized by incorporating PTQ10. This work succeeds in reaching a deep insight into all‐PSC's stability promotion by a rational ternary design, which booms the prospect of gaining high‐performance all‐PSCs.
High‐Performance Hydrogel SERS Chips with Tunable Localized Surface Plasmon Resonance for Coordinated Electromagnetic Enhancement with Chemical Enhancement
Authors: Chen Mingming , Liu Zhihong , Su Bihang , Hu Rongjing , Fu Fengfu , Jiang Xiancai , Lin Zhenyu , Dong Yongqiang 
Published: February 2023

AbstractHydrogel surface‐enhanced Raman scattering (SERS) chips with tunable localized surface plasmon resonance (LSPR) wavelength are prepared to coordinate the chemical enhancement (CM) and electromagnetic enhancement (EM) effects for molecules. When detecting different molecules, a laser with matched energy is selected according to energy intervals between the molecular energy levels and the Fermi level of Ag nanoparticles to obtain the strongest CM effect. Meanwhile, a hydrogel SERS chip with the LSPR wavelength matching with the laser is selected to gain the strongest EM effect. As a result, the constructed hydrogel SERS chips show outstanding activity to many molecules. Amoxicillin, pymetrozine, and chlorpyrifos are used as the model molecules to demonstrate the great importance of CM effect and the working principle of the obtained hydrogel SERS chips. Besides the ultrahigh activity, the obtained hydrogel SERS chips also show high uniformity, long‐term stability, and strong anti‐interference to the sample matrix, and thereby are highly practical. This work not only provides an efficient strategy for building high‐performance SERS substrates, but also sheds the light on the mechanism of wave selection of SERS.
Promoting Reversibility of Co‐Free Layered Cathodes by Al and Cation Vacancy
Authors: Wang Tongshuai , Yang Jia , Wang Hailong , Ma Wei , He Miao , He Yufang , He Xiangming 
Published: February 2023

AbstractLi‐ion batteries adopting layered cathodes can effectively alleviate the range limitations of electric vehicles. Unfortunately the scarcity of Co inhibits massive deployment of layered cathodes. Eliminating Co from layered cathodes is necessary to make a breakthrough in global application of electric vehicles. However, Co‐free layered cathodes face challenges in delithiation/lithiation reversibility since Co plays a pivotal role in suppressing Li/Ni mixing. Many metals have been proposed to replace Co in layered cathodes, and sophisticated compositional designs always consider suppressing Li/Ni mixing as the top priority. Here, the authors show that Li/Ni mixing can be suppressed by Al and cation vacancies in different manners; however, irreversible capacities are prominently different given similar Li/Ni mixing. In‐situ X‐ray diffraction monitored potentiostatic‐intermittent‐titration measurements reveal that Al decreases the lattice strain between H2 and H3 phase by 13.6%, but Al has an adverse impact on structure reversibility. While Al and cation vacancies together not only significantly reduce the H2/H3 lattice strain by 78% but also greatly enhance structure reversibility. Furthermore, the first‐principles calculation shows that cation vacancies can remarkably reduce the Li migration energy barrier by an order of magnitude. Reversibility of the newly designed Co‐free cathode is significantly enhanced through the synergic effect of Al and cation vacancies.
Mechanism of Cations Suppressing Proton Diffusion Kinetics for Electrocatalysis
Authors: Li Xiao‐Yu , Wang Tao , Cai Yu‐Chen , Meng Zhao‐Dong , Nan Jing‐Wen , Ye Jin‐Yu , Yi Jun , Zhan Dong‐Ping , Tian Na , Zhou Zhi‐You , Sun Shi‐Gang 
Published: February 2023

AbstractProton transfer is crucial for electrocatalysis. Accumulating cations at electrochemical interfaces can alter the proton transfer rate and then tune electrocatalytic performance. However, the mechanism for regulating proton transfer remains ambiguous. Here, we quantify the cation effect on proton diffusion in solution by hydrogen evolution on microelectrodes, revealing the rate can be suppressed by more than 10 times. Different from the prevalent opinions that proton transport is slowed down by modified electric field, we found water structure imposes a more evident effect on kinetics. FTIR test and path integral molecular dynamics simulation indicate that proton prefers to wander within the hydration shell of cations rather than to hop rapidly along water wires. Low connectivity of water networks disrupted by cations corrupts the fast‐moving path in bulk water. This study highlights the promising way for regulating proton kinetics via a modified water structure.
Copper‐Catalysed Rearrangement of Cyclic Ethynylethylene Carbonates: Synthetic Applications and Mechanistic Studies
Authors: Xu Chao , Zhang Hao , Lan Shouang , Liu Jinggong , Yang Shuang , Zhang Qi , Fang Xinqiang 
Published: February 2023

AbstractTransition‐metal‐catalysed reactions of cyclic ethynylethylene carbonates have been intensively studied because of their robustness in new bond formation and diversified molecule construction. Known reaction modes usually involve a substitution step occurring at either the propargylic or terminal alkyne positions. Here, we report an unprecedented reaction pattern in which cyclic ethynylethylene carbonates first undergo a rearrangement to release allenal intermediates, which subsequently react with diverse nucleophiles to furnish synthetically useful allylic and propargylic allenols, phosphorus ylides, and cyclopropylidene ketones through an addition process rather than a substitution pathway. The products enable various further transformations, and mechanistic studies and theoretical calculations reveal that the reaction does not proceed via a semipinacol type [1,2]‐hydride shift, but through base‐mediated deprotonation as the key step to induce the rearrangement.
Catalytic Asymmetric Synthesis of Axially Chiral Diaryl Ethers through Enantioselective Desymmetrization
Authors: Bao Hanyang , Chen Yunrong , Yang Xiaoyu 
Published: February 2023

AbstractAxially chiral diaryl ethers are a type of unique atropisomers bearing two potential axes, which have potential applications in a variety of research fields. However, the catalytic enantioselective synthesis of these diaryl ether atropisomers is largely underexplored when compared to the catalytic asymmetric synthesis of biaryl or other types of atropisomers. Herein, we report a highly efficient catalytic asymmetric synthesis of diaryl ether atropisomers through an organocatalyzed enantioselective desymmetrization protocol. The chiral phosphoric acid‐catalyzed asymmetric electrophilic aromatic aminations of the symmetrical 1,3‐benzenediamine type substrates afforded a series of diaryl ether atropisomers in excellent yields and enantioselectivities. The facile construction of heterocycles by the utilizations of the 1,2‐benzenediamine moiety in the products provided access to a variety of structurally diverse and novel azaarene‐containing diaryl ether atropisomers.
Single‐Molecule Two‐Color Coincidence Detection of Unlabeled alpha‐Synuclein Aggregates
Authors: Chappard Alexandre , Leighton Craig , Saleeb Rebecca S. , Jeacock Kiani , Ball Sarah R. , Morris Katie , Kantelberg Owen , Lee Ji‐Eun , Zacco Elsa , Pastore Annalisa , Sunde Margaret , Clarke David J. , Downey Patrick , Kunath Tilo , Horrocks Mathew H. 
Published: February 2023

AbstractProtein misfolding and aggregation into oligomeric and fibrillar structures is a common feature of many neurogenerative disorders. Single‐molecule techniques have enabled characterization of these lowly abundant, highly heterogeneous protein aggregates, previously inaccessible using ensemble averaging techniques. However, they usually rely on the use of recombinantly‐expressed labeled protein, or on the addition of amyloid stains that are not protein‐specific. To circumvent these challenges, we have made use of a high affinity antibody labeled with orthogonal fluorophores combined with fast‐flow microfluidics and single‐molecule confocal microscopy to specifically detect α‐synuclein, the protein associated with Parkinson's disease. We used this approach to determine the number and size of α‐synuclein aggregates down to picomolar concentrations in biologically relevant samples.
Crystallization‐driven Nanoparticle Crystalsomes
Authors: Gao Lingfeng , Mei Shan , Qian Qian , Yu Shichen , Zhao Bin , Tu Yingfeng , Li Christopher Y. 
Published: February 2023

AbstractNanoparticle (NP) assembly has been extensively studied, and a library of NP superstructures has been synthesized. These intricate structures show unique collective optical, electronic, and magnetic properties. In this work, we report a bottom‐up approach for fabricating spherical gold nanoparticle (AuNP) assemblies that mimic colloidosomes. Co‐crystallization of lipoic acid‐end‐functionalized poly(ethylene oxide) (PEO) and AuNPs in solution via a self‐seeding method led to the formation of hollow spherical NP assemblies named nanoparticle crystalsomes (NPCs). Due to the spherical shape, the translational symmetry of PEO crystals is broken in NPCs, which can be attributed to the competition between NP close packing and polymer crystallization. This was confirmed by tuning the NPC morphology via varying the self‐seeding temperature, crystallization temperature, and PEO molecular weight. We envisage that this strategy paves the way to attaining exquisite morphological control of NP assemblies with broken translational symmetry.
Orthogonal Trichromatic Upconversion with High Color Purity in Core‐Shell Nanoparticles for a Full‐Color Display
Authors: Huang Kaofeng , Qiu Haiyi , Zhang Xintong , Luo Wang , Chen Ying , Zhang Jiacheng , Chen Yihang , Wang Guannan , Zheng Kezhi 
Published: February 2023

AbstractMaterials with tunable emission colors has attracted increasing interest in both fundamental research and applications. As a key member of light‐emitting materials family, lanthanide doped upconversion nanoparticles (UCNPs) have been intensively demonstrated to emit light in any color upon near‐infrared excitation. However, realizing the trichromatic emission in UCNPs with a fixed composition remains a great challenge. Here, without excitation pulsed modulation and three different near‐infrared pumping, we report an experimental design to fine‐control emission in the full color gamut from core–shell‐structured UCNPs by manipulating the energy migration through dual‐channel pump scheme. We also demonstrate their potential application in full‐color display. These findings may benefit the future development of convenient and versatile optical methos for multicolor tuning and open up the possibility of constructing full‐color volumetric display systems with high spatiotemporal resolution.
Total Syntheses of Kopsaporine, Kopsinol and Kopsiloscine A
Authors: Tian Hongchang , Wu Yinxia , Li Xiujuan , Hao Zhen , He Wenyan , Huang Xiangdi , Chen Wen , Zhang Hongbin 
Published: February 2023

AbstractKopsiaalkaloids represent a complex class of natural products bearing a polycyclic ring system with two or three consecutive quaternary carbon centers. In this article, we report the first total synthesis of Kopsaporine related alkaloids. Features of our structure‐unit‐based strategy are an intramolecular Pummerer rearrangement induced nucleophilic cyclization/aza‐Prins cyclization to construct the highly functional hexahydrocarbazole skeleton, an olefin migration vinylogous alkylation to establish the C20 all‐carbon quaternary center, an iridium complex mediated radical addition to fuse the aspidofractine framework, an unprecedented IBX oxidation to introduce the α‐hydroxyketone moiety, and a bioinspired retro‐Aldol/Aldol reaction to convert kopsaporine to kopsiloscine A.
Simple Ether‐Directed Enantioselective C(sp3)−H Borylation of Cyclopropanes Enabled by Iridium Catalysis
Authors: Xie Tian , Chen Lili , Shen Zhenlu , Xu Senmiao 
Published: February 2023

AbstractReported here is an efficient and simple ether‐directed iridium‐catalyzed enantioselective C(sp3)−H borylation of cyclopropanes. Various functional groups were well‐tolerated, affording a vast array of chiral cyclopropanes with high enantioselectivities. We also demonstrated that the turnover numbers of the current reaction could be up to 335.
Structural and Mechanistic Studies on Substrate and Stereoselectivity of the Indole Monooxygenase VpIndA1: New Avenues for Biocatalytic Epoxidations and Sulfoxidations
Authors: Kratky Julia , Eggerichs Daniel , Heine Thomas , Hofmann Sarah , Sowa Philipp , Weiße Renato H. , Tischler Dirk , Sträter Norbert 
Published: February 2023

AbstractFlavoprotein monooxygenases are a versatile group of enzymes for biocatalytic transformations. Among these, group E monooxygenases (GEMs) catalyze enantioselective epoxidation and sulfoxidation reactions. Here, we describe the crystal structure of an indole monooxygenase from the bacterium Variovorax paradoxus EPS, a GEM designated as VpIndA1. Complex structures with substrates reveal productive binding modes that, in conjunction with force‐field calculations and rapid mixing kinetics, reveal the structural basis of substrate and stereoselectivity. Structure‐based redesign of the substrate cavity yielded variants with new substrate selectivity (for sulfoxidation of benzyl phenyl sulfide) or with greatly enhanced stereoselectivity (from 35.1 % to 99.8 % ee for production of (1S,2R)‐indene oxide). This first determination of the substrate binding mode of GEMs combined with structure‐function relationships opens the door for structure‐based design of these powerful biocatalysts.
Convective flow of ethylene glycol‐silver Jeffery nanofluid in a Hele‐Shaw cell with an influence of external magnetic field
Authors: Yadav Dhananjay , Al‐Balushi Sara , Awasthi Mukesh Kumar , Al‐Hadi Taif , Al‐Abri Raya , Al‐Wahaibi Jawhara , Al‐Nasseri Fatan , Al‐Siyabi Sara , Ragoju Ravi , Bhattacharyya Krishnendu 
Published: February 2023

AbstractThis effort investigates the arrival of magnetothermal convection of ethylene glycol‐silver Jeffrey nanofluid in a Hele‐Shaw cell utilizing the linear stability concept. The model practiced for the Jeffrey nanofluid includes the impacts of Brownian movement and thermophoresis. The norms for both marginal and overstable modes of convections are developed analytically. The impact of magnetic Chandrasekhar number
, magnetic Prandtl number
, Jeffrey parameter
, Hele‐Shaw number
, and a variety of nanofluid parameters such as the volumetric fraction of nanoparticles
, nanoparticle Rayleigh number
, adjusted diffusive ratio
, and Lewis number
on the beginning of convective motion are investigated, and results are illustrated graphically. It is observed that the overstable approach of convection is probable below the certain threshold estimate of the magnetic Prandtl number
. This threshold estimate of the magnetic Prandtl number
upturns with a rise in the rate of
,
, and
, while it drops with a surge in the nanofluid parameters. The system was found to be more stable by decreasing the Hele‐Shaw number
, the Jeffery parameter
, and nanofluid parameters, while it was unstable by decreasing the magnetic Chandrasekhar number
and the magnetic Prandtl number
.