bluuebunny/crossref_metadata_2025_split huggingface dataset:
Lifelong deep learning‐based control of robot manipulators
Authors: Ganie Irfan , Sarangapani Jagannathan 
Published: September 2023

SummaryThis study proposes a lifelong deep learning control scheme for robotic manipulators with bounded disturbances. This scheme involves the use of an online tunable deep neural network (DNN) to approximate the unknown nonlinear dynamics of the robot. The control scheme is developed by using a singular value decomposition‐based direct tracking error‐driven approach, which is utilized to derive the weight update laws for the DNN. To avoid catastrophic forgetting in multi‐task scenarios and to ensure lifelong learning (LL), a novel online LL scheme based on elastic weight consolidation is included in the DNN weight‐tuning laws. Our results demonstrate that the resulting closed‐loop system is uniformly ultimately bounded while the forgetting is reduced. To demonstrate the effectiveness of our approach, we provide simulation results comparing it with the conventional single‐layer NN approach and confirm its theoretical claims. The cumulative effect of the error and control input in the multitasking system shows a 43% improvement in performance by using the proposed LL‐based DNN control over recent literature.
High‐Speed Deposition of Large‐Area Narrow‐Bandgap Perovskite Films for All‐Perovskite Tandem Solar Mini‐Modules
Authors: Shi Yang , Sun Jinglin , Zhou Jie , Wen Tianyu , Zou Can , Liu Da , Liu Feng , Yang Shuang , Deng Yehao , Yang Zhibin 
Published: September 2023

AbstractDeveloping all‐perovskite tandem solar cells is an effective approach to extend the limit of power conversion efficiency. However, fast preparation of large‐area and high‐quality narrow‐bandgap Sn‐based perovskite films still remains a major challenge in fabricating all‐perovskite tandem modules. Here high‐crystalline and compact narrow‐bandgap perovskite films with an area over 100 cm2 are well prepared by combining compositional, solvent and additive engineering. The use of 2‐methoxyethanol as a solvent enables the fast deposition of narrow‐bandgap perovskite films. Adding proper amounts of dimethyl sulfoxide and surfactant L‐α‐phosphatidylcholine into the narrow‐bandgap perovskite precursor effectively enhances the crystallinity and coverage of the resulting perovskite films, respectively. Based on these studies, narrow‐bandgap perovskite and all‐perovskite tandem mini‐modules with an aperture area of 10.4 cm2 are constructed and exhibit high efficiencies of 13.2% and 16.4%, respectively. This study provides an option for fast deposition of high‐quality narrow‐bandgap perovskite films, which is beneficial for the scalable production of all‐perovskite tandem solar modules.
Non‐Linear Optics at Twist Interfaces in h‐BN/SiC Heterostructures
Authors: Biswas Abhijit , Xu Rui , Alvarez Gustavo A. , Zhang Jin , Christiansen‐Salameh Joyce , Puthirath Anand B. , Burns Kory , Hachtel Jordan A. , Li Tao , Iyengar Sathvik Ajay , Gray Tia , Li Chenxi , Zhang Xiang , Kannan Harikishan , Elkins Jacob , Pieshkov Tymofii S. , Vajtai Robert , Birdwell A. Glen , Neupane Mahesh R. , Garratt Elias J. , Ivanov Tony G. , Pate Bradford B. , Zhao Yuji , Zhu Hanyu , Tian Zhiting , Rubio Angel , Ajayan Pulickel M. 
Published: September 2023

AbstractUnderstanding the emergent electronic structure in twisted atomically thin layers has led to the exciting field of twistronics. However, practical applications of such systems are challenging since the specific angular correlations between the layers must be precisely controlled and the layers have to be single crystalline with uniform atomic ordering. Here, an alternative, simple, and scalable approach is suggested, where nanocrystallinetwo‐dimensional (2D) film on 3D substrates yields twisted‐interface‐dependent properties. Ultrawide‐bandgap hexagonal boron nitride (h‐BN) thin films are directly grown on high in‐plane lattice mismatched wide‐bandgap silicon carbide (4H‐SiC) substrates to explore the twist‐dependent structure‐property correlations. Concurrently, nanocrystalline h‐BN thin film shows strong non‐linear second‐harmonic generation and ultra‐low cross‐plane thermal conductivity at room temperature, which are attributed to the twisted domain edges between van der Waals stacked nanocrystals with random in‐plane orientations. First‐principles calculations based on time‐dependent density functional theory manifest strong even‐order optical nonlinearity in twisted h‐BN layers. This work unveils that directly deposited 2D nanocrystalline thin film on 3D substrates could provide easily accessible twist‐interfaces, therefore enabling a simple and scalable approach to utilize the 2D‐twistronics integrated in 3D material devices for next‐generation nanotechnology.
Defect‐Engineering‐Mediated Long‐Lived Charge‐Transfer Excited‐State in Fe–Gallate Complex Improves Iron Cycle and Enables Sustainable Fenton‐Like Reaction
Authors: Shi Yanfeng , Zhang Gong , Xiang Chao , Liu Chengzhen , Hu Jun , Wang Junhu , Ge Rile , Ma Haixia , Niu Yusheng , Xu Yuanhong 
Published: September 2023

AbstractFenton reactions are inefficient because the Fe(II) catalyst cannot be recycled in time due to the lack of a rapid electron transport pathway. This results in huge H2O2 wastage in industrial applications. Here, it is shown that a sustainable heterogeneous Fenton system is attainable by enhancing the ligand‐to‐metal charge‐transfer (LMCT) excited‐state lifetime in Fe–gallate complex. By engineering oxygen defects in the complex, the lifetime is improved from 10–90 ps. The lengthened lifetime ensures sufficient concentrations of excited‐states for an efficient Fe cycle, realizing previously unattainable H2O2 activation kinetics and hydroxyl radical (•OH) productivity. Spectroscopic and electrochemical studies show the cyclic reaction mechanism involves in situ Fe(II) regeneration and synchronous supply of oxygen atoms from water to recover dissociated Fe─O bonds. Trace amounts of this catalyst effectively destroy two drug‐resistant bacteria even after eight reaction cycles. This work reveals the link among LMCT excited‐state lifetime, Fe cycle, and catalytic activity and stability, with implications for de novo design of efficient and sustainable Fenton‐like processes.
Selective Surface Treatment Using Atmospheric Ar Plasma Jet for Aluminum‐doped Zinc Oxide Based Transparent and Flexible Electronics
Authors: Lee Haechang , Seo Yong Hyeok , Kwon Sang Jik , Jeon Yongmin , Cho Eou‐Sik 
Published: September 2023

AbstractTransparent and flexible electronics are emerging technologies with the potential to enable new applications. However, to ensure high‐performance transparent electronics, post‐processing such as thermal annealing and vacuum plasma treatment is necessary, which are difficult to apply to polymer‐based flexible substrates. This study analyzed the feasibility of applying selective Ar plasma jet treatment at atmospheric pressure to transparent flexible electronics. When atmospheric Ar plasma treatment is applied to transparent flexible aluminum‐doped zinc oxide (AZO), it showed a maximum 83.1% improvement in sheet resistance while maintaining a high transmittance performance, of over 70%. To verify the mechanism behind the surface treatment effect using atmospheric Ar plasma, comprehensive analyses are performed using atomic force microscopy, X‐ray diffraction, and X‐ray photoelectron spectroscopy, which confirmed that the effect is due to oxygen vacancy formation caused by ion bombardment and thermal diffusion. The application of atmospheric plasma treatment to a patterned transparent flexible AZO device resulted in a reduction in contact resistance, and it is confirmed that the performance improvement effects can be retained for >500 h by applying additional passivation.
Cone‐Shaped Electrodes for Capacitive Tactile Sensors with High Sensitivity and Broad Linearity Range
Authors: Chen Liting , Zheng Bingying , Ye Jinhua , Wu Haibin 
Published: September 2023

Flexible tactile sensors with high sensitivity typically suffer from a dramatically reduces pressure resolution with increasing pressure, resulting in narrow linear ranges and limited application scenarios. Herein, a capacitive tactile sensor based on cone‐shaped electrodes (CSE) that can maintain high sensitivity over a broad linearity range is proposed. The linear response comes from the novel sensing mechanism based on the change in the facing electrode area and the rational design of the conical architecture. Finite element analysis (FEA) confirms that the interfacial contact area between the elastic electrodes and the dielectric layer can respond linearly to pressure over a broad spectrum. Based on this strategy, the fabricated sensors perform a high sensitivity (0.23 kPa−1) and superior linearity (R2 = 0.999) across a wide pressure range of up to 130 kPa. The sensors demonstrate several key features, such as good repeatability, fast response speed, low detection limit, and high durability. These attributes enable the successful use of the sensors for monitoring artery pulses and providing weighting capabilities to robots, showing promising potential for applications in daily health monitoring and human‐machine interaction.
Synthesis of Furfural Sulfides and 4‐Alkylthiopyridines via Heterocyclization of α‐Acyl Ketene Dithioacetals
Authors: Zhang Xiaoxuan , Chang Jian , Chen Chong , Zhai Qianqian , Li Shengnan , Song Xiaoning 
Published: September 2023

AbstractHerein, we devised a synthetic approach for skeletally diversified furfuryl sulfides and 4‐alkylthiopyridines involving the heterocyclization of flexible α‐acyl ketene dithioacetals, enabled by cooperative Pd/Cu catalysis. The overall transformation was initiated by acyl‐directed desulfurative Sonogashira coupling, which was proposed as the key step in surmounting the competitive carbothiolation pathway. This step was followed by 1,6‐addition of either a S‐ or N‐nucleophile and intramolecular cyclization. Notably, the two different annulation reactions featured readily accessible starting materials, selective cleavage and reassembly of multiple chemical bonds, broad functional group tolerance, pharmacologically significant heterocyclic products with high regio‐ and chemoselectivities, and high atom economy.
Photocatalytic N‐Alkylation of NH‐Sulfoximines via Anti‐Markovnikov Hydroamination of Alkenes
Authors: Wang Cong , Jia Tiezheng 
Published: September 2023

AbstractSulfoximines, the isoelectronic with sulfones, represent a class of alternative and intriguing motifs in both discovery program and agrochemistry. N‐Alkylation on imines could significantly improve their bioactivities, but the lack of general method has hindered their further uptake by medicinal chemistry and drug development. Herein, we present a mild photocatalytic anti‐Markovnikov hydroamination of alkenes to construct N‐alkylated sulfoximines with broad substrate tolerance on primary, secondary and tertiary alkyl substituents as well as a diverse range of sulfoximines. The mechanistic studies support the photocatalytic pathway, and demonstrate that the alkene radical cation rather than the iminium radical serves as the key intermediate in the transformation.
Photoredox‐Catalyzed Trifunctionalization of 5‐Heteroaryl‐Substituted 1‐Hexenes or 5‐hexenenitriles via Remote Heteroaryl or Cyano Group Migration
Authors: Guo Kang 
Published: September 2023

AbstractA photoredox‐catalyzed trifunctionalization of 5‐heteroaryl‐substituted 1‐hexenes via remote heteroaryl migration and a photoredox‐catalyzed trifunctionalization of 5‐hexenenitriles via cyano migration are reported. This protocol provides access to a broad scope of CFnR‐containing ketones with high molecular complexity and functional group diversity. The reaction features mild conditions and high chemo‐ and regioselectivities. The success of gram‐scale reactions and the versatility of products in derivative synthesis illustrated the potential value of this transformation in synthetic chemistry.
Giant Piezoelectric Output and Stability Enhancement in Piezopolymer Composites with Liquid Metal Nanofillers
Authors: Liu Jingyan , Zeng Shi , Zhang Mingrui , Xiong Juan , Gu Haoshuang , Wang Zhao , Hu Yongming , Zhang Xianghui , Du Yi , Ren Long 
Published: September 2023

AbstractIntegrating nanomaterials into the polymer matrix is an effective strategy to optimize the performance of polymer‐based piezoelectric devices. Nevertheless, the trade‐off between the output enhancement and stability maintenance of piezoelectric composites usually leads to an unsatisfied overall performance for the high‐strength operation of devices. Here, by setting liquid metal (LM) nanodroplets as the nanofillers in a poly(vinylidene difluoride) (PVDF) matrix, the as‐formed liquid‐solid/conductive‐dielectric interfaces significantly promote the piezoelectric output and the reliability of this piezoelectric composite. A giant performance improvement featured is obtained with, nearly 1000% boosting on the output voltage (as high as 212 V), 270% increment on the piezoelectric coefficient (d33∼51.1 pC N−1) and long‐term reliability on both structure and output (over 36 000 cycles). The design of a novel heterogenous interface with both mechanical matching and electric coupling can be the new orientation for developing high performance piezoelectric composite‐based devices.
High‐Performance Binary All‐Polymer Solar Cells with Efficiency Over 18.3% Enabled by Tuning Phase Transition Kinetics
Authors: Bi Pengqing , Zhang Tao , Cui Yong , Wang Jianqiu , Qiao Jiawei , Xian Kaihu , Chua Xian Wei , Chen Zhihao , Goh Wei Peng , Ye Long , Hao Xiaotao , Hou Jianhui , Yang Le 
Published: September 2023

AbstractAll‐polymer solar cells (All‐PSCs) are considered to be the most promising candidates for realizing efficient and stable organic solar cells (OSCs). However, the challenge of controlling morphology has hindered the performance of All‐PSCs. Compared to small molecule acceptors, polymer acceptors play a more crucial role in obtaining an ideal morphology for All‐PSCs. The molecular weight of polymer acceptors is one of the key factors determining the morphological and mechanical properties as well as the interactions with donors. Herein, by using a monomer of PYIT (PYIT1) and PYITs with low (PYIT2) and high (PYIT3) molecular weights, the impact of molecular weight of the polymer acceptor is systematically investigated on the phase transition process, morphological, and photovoltaic properties. It is found that tuning the molecular weight effectively regulates the phase transition process of the polymer acceptor and its interaction with the polymer donor. This induces significant effects on the aggregation behaviors of the polymers. Appropriate molecular weight polymer acceptors can facilitate favorable phase separation morphology. With PBQx‐Cl as the donor and PYIT2 as acceptor, a high‐performance binary All‐PSC is achieved with an efficiency of 18.39%. This study provides deep insights into the performance enhancement of All‐PSCs through rational polymer acceptor design.
Boosting Active Species Ru‐O‐Zr/Ce Construction at the Interface of Phase‐Transformed Zirconia‐Ceria Isomerism toward Advanced Catalytic Cathodes for Li‐CO2 Batteries
Authors: Deng Qinghua , Yang Yong , Yin Kai , Yi Jiachen , Zhou Yuming , Zhang Yiwei 
Published: September 2023

AbstractOptimized structural support widely affects the improvement of interface structure, promoting the quantity and quality of active species simultaneously for Lithium battery cathodes. Herein, a highly dispersed and anchored active species at the interface of the Zr/CeO2(111) are achieved and are used for advanced Li‐CO2 batteries cathodes. Benefiting from the abundant Ru‐O‐Zr/Ce site, the CO2 adsorption and reduction is enhanced by the migration of the electron density in the C═O of CO2 to Ru. The established Li‐CO2 batteries exhibit excellent activity of 21 075 mAh g−1 and outstanding durability of over 167 cycles as well as low overpotential with 1.03 V at a discharge/recharge rate of 100 mA g−1. The executed experiments combined with DFT calculations unveil that the cubic bimetallic oxide supported Ru exhibits optimized electronic structure at the interface compared to the monoclinic or tetragonal monometallic oxide support, promoting the increase of discharge voltage (from ≈2.5 to 2.73 V). Fundamentally, the redistribution of electron density on the active species Ru‐O‐Zr/Ce are intrinsic to above positive change, which are promoted by the synergistic interaction of Zr and Ce. This investigation provides an approach for the advancement of Li‐CO2 batteries catalytic cathodes and for the promotion of “carbon neutral” goals.
Composite Lithium Metal Structure to Mitigate Pulverization and Enable Long‐Life Batteries
Authors: Yu Sicen , Wang Shen , Miao Qiushi , Hui Zeyu , Hyun Gayea , Holoubek John , Yu Xiaolu , Gao Junwei , Liu Ping 
Published: September 2023

AbstractIn lithium metal batteries, non‐uniform stripping of lithium results in pit formation, which promotes subsequent non‐uniform, dendritic deposition. This viscous cycle leads to pulverization of lithium which promotes cell shorting or capacity degradation, symptoms further exaggerated by high electrode areal loading and lean electrolytes. To address this challenge, a composite lithium metal anode is engineered that contains uniformly distributed, nanometer‐sized carbon particles. This composite lithium is shown to strip more uniformly since the growth of non‐uniform pits is intercepted by the carbon particles. This mechanism is corroborated by a continuum electrochemical model. Subsequent lithium deposition on carbon particles is also found to be more uniform than on the surface with irregular pits. Notably, the pulverization rate of composite lithium is 26 times slower than that of commercial lithium. Moreover, in a Li‐S battery with sulfurized polyacrylonitrile cathode, the use of the composite anode extends the cycle life by three times when the areal capacity is 8 mAh cm−2. The approach of using an engineered lithium composite structure to address challenges during both stripping and plating can inform future designs of lithium metal anodes for high areal capacity operations.
Dinuclear Gold‐Catalyzed para‐Selective C−H Arylation of Undirected Arenes by Noncovalent Interactions
Authors: Liu Duan‐Yang , Han Jie , Liu Kai , Cheng Yaohang , Tan Hairen , Yang Xiaoliang , Li Weipeng , Xie Jin 
Published: September 2023

AbstractThe regioselectivity of C−H functionalization is commonly achieved by directing groups, electronic factors, or steric hindrance, which facilitate the identification of reaction sites. However, such strategies are less effective for reactants such as simple monofluoroarenes due to their relatively low reactivity and the modest steric demands of the fluorine atom. Herein, we present an undirected gold‐catalyzed para‐C−H arylation of a wide array of monofluoroarenes using air‐stable aryl silanes and germanes at room temperature. A high para‐regioselectivity (up to 98 : 2) can be realized by utilizing a dinuclear dppm(AuOTs)2 (dppm=bis(diphenylphosphino)methane) as the catalyst and hexafluorobenzene as the solvent. This provides a general and practical protocol for the concise construction of structurally diverse para‐arylated monofluoroarenes through C−H activation manner. It features excellent functional group tolerance and a broad substrate scope (>80 examples). Besides, this strategy is also robust for other simple monosubstituted arenes and heteroarenes. Our mechanistic studies and theoretical calculations suggest that para‐C−H selectivity arises from highly electrophilic and structurally flexible dinuclear Ar−Au(III)−Au(I) species, coupled with noncovalent interaction induced by hexafluorobenzene.
Characterization of alginate from Antarctic Himantothallus grandifolius (Phaeophyceae) and preparation of polyelectrolyte complexes with chitosan
Authors: Candia Carolina , Gallardo‐Moya Daniel , Guerrero Juan , Leal David , Mansilla Andrés , Martínez‐Gómez Fabián , Matsuhiro Betty , Yáñez‐S Mauricio 
Published: September 2023

AbstractHydrogels are three‐dimensional polymeric materials with applications in various areas such as biomedicine, tissue engineering, pollutant capture systems, and so forth. However, its application is limited due to the reproducibility of its properties. Factors such as the composition of the constituents, the type of union between the polymer chains, and the crosslinking time play a crucial role in ensuring its reproducibility. In this study, the objective is to prepare a matrix with well‐defined properties that ensure controlled release processes. Treatment of Himantothallus grandifolius with Na2CO3 aqueous solution afforded in 18.9% yield alkaline extract. Hydrogels were prepared by ionic complexation of alginate from H. grandifolius, and polyguluronate enriched alginate from Desmarestia ligulata with chitosan stabilized by immersion in 0.1 M CaCl2 solution; better swelling ratio in water was found for hydrogels with low molecular weight chitosan (MW 125,000 g/mol) than those with medium molecular weight chitosan (MW450,000–500,000 g/mol). Liberation of the model drug metformin hydrochloride from alginates: chitosan complexes (3:1) at pH 1.5 was especially low for hydrogel from H. grandifolius during the first 2 h; 70% of metformin was released at pH 6.5 after 24 h. This polyelectrolyte complex constitutes a good material for potential application in biomedicine considering its cationic and anionic characteristics.
Dual Pd‐Acid Sites Confined in a Hierarchical Core‐Shell Structure for Hydrogenation of Nitrobenzene
Authors: Wang Yi‐Tian , Wu Si‐Ming , Luo Guo‐Qiang , Xiao Shi‐Tian , Pu Fu‐Fei , Wang Li‐Ying , Chang Gang‐Gang , Tian Ge , Yang Xiao‐Yu 
Published: September 2023

AbstractA core‐shell structured Pd@TS‐1@meso‐SiO2 catalyst with confined Pd nanometals has been fabricated by one‐pot synthesis, impregnation method and sol‐gel method. With the promotion of acid sites and protection of mesoporous silica shell, Pd@TS‐1@meso‐SiO2 shows higher activity than commercial comparison and higher stability than sample without mesoporous silica shell in the hydrogenation of nitrobenzene. The schematic illustration of the synergy effect is also proposed.
Metabolomics provides insights into acceleration of bone healing in fractured patients with traumatic brain injuries
Authors: Xia Demeng , Wu Rui , Xue Qian , Jiang Gehan , Xu Shuogui 
Published: September 2023

AbstractWhile clinical surveys have frequently reported that patients with traumatic brain injuries (TBIs) and comorbidities experience faster healing, the underlying mechanisms have been investigated but remain unclear. As a comprehensive comparison and analysis of the metabolic characteristics of these two pathologies have not been undertaken, we developed a rat model of fracture and TBI and collected serum samples for metabolomic analysis using ultra‐high performance liquid chromatography–quadrupole time‐of‐flight MS (UHPLC–Q‐TOF/MS). In total, we identified 40 differential metabolites and uncovered related pathways and potential mechanisms, including aminoacyl‐transfer RNA biosynthesis; differential amino acids such as leucine, cholylhistidine, aspartyl‐lysine; and related lipid metabolism, and discussed their impacts on bone formation in detail. This study highlights that the UHPLC–Q‐TOF/MS–based metabolomics approach offers a better understanding of the metabolic links between TBI and accelerated bone recovery.