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An unprecedented synthesis of axially chiral biaryls by rearrangement and aromatization of carbocations with central-to-axial conversion of chirality

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Science China Chemistry 2024年第9期67卷 2998-3003页

作者： qi liu Xue-Dong Li Liang Cheng Li liu Beijing National Laboratory for Molecular Sciences(BNLMS) CAS Key Laboratory of Molecular Recognition and FunctionCAS Research/Education Center for Excellence in Molecular SciencesInstitute of ChemistryChinese Academy of SciencesBeijing 100190China University of Chinese Academy of Sciences Beijing 100049China

The central-to-axial chirality conversion represents a fascinating class of chemical processes consisting of the destruction of stereogenic centers and the simultaneous installation of axial chiral elements,which provides efficient methods for the preparation of axially chiral ***,developing catalytic asymmetric approaches for constructing these central chirality precursors and the efficient central-to-axial chirality conversion remains a challenge due to the requirement of aromatization or elimination *** this work,we have developed an unprecedented enantioselective intramolecular FriedelCrafts alkylation with unactivated-ketone carbonyls from which a chiral tertiary alcohol was generated with high efficiency and excellent *** addition,the central-to-axial chirality conversion strategy has been successfully applied to the synthesis of enantioenriched biaryls via a less-explored carbocation-initiated rearrangement and aromatization under the promotion of Lewis *** methodology provided a straightforward and sustainable access to a broad range of biaryl-2-carboxylic acid and in excellent yields(up to 92%)and excellent central-to-axial chirality conversion(up to 99%conversion percentage).This work could be a great model for developing new methods for synthesizing axially chiral biaryls and a general protocol for the rearrangement and aromatization of carbocations for further functionalization.

关键词： br?nsted acid catalysis desymmetrization phosphoric acid axially chiral biaryls central-to-axial conversion

Strain-Compensated InGaAs/InAlAs Quantum Cascade Detector of 4.5 μm Operating at Room Temperature

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Chinese Physics Letters 2010年第3期27卷 312-315页

作者：孔宁刘俊岐李路刘峰奇王利军王占国 Key Laboratory of Semiconductor Materials Science Institute of Semiconductors Chinese Academy of Sciences P.O. Box 912 Beijing 100083

We present a strain-compensated InP-based InGaAs/InAlAs photovoltaic quantum cascade detector grown by solid source molecular beam epitaxy. The detector is based on a vertical intersubband transition and electron transfer on a cascade of quantum levels which is designed to provide longitudinal optical phonon extraction stairs. By careful structure design and growth, the whole epilayer has a residual strain toward InP substrate of only -2.8× 10^-4. A clear narrow band detection spectrum centered at 4.5 μm has been observed above room temperature for a device with 200／times 200 ×μm^2 square mesa.

关键词： Electronics and devices Surfaces interfaces and thin films Optics quantum optics and lasers Nanoscale science and low-D systems

Quantum phase transition of the Jaynes-Cummings model

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Science China(Physics,Mechanics & Astronomy) 2024年第1期67卷 1-9页

作者： Cheng liu Jin-feng Huang Key Laboratory of Low-Dimensional Quantum Structures and Quantum Control of Ministry of Education Key Laboratory for Matter Microstructure and Function of Hunan ProvinceDepartment of Physics and Synergetic Innovation Center for Quantum Effects and ApplicationsInstitute of Interdisciplinary StudiesHunan Normal UniversityChangsha 410081China

Herein,we propose an experimentally feasible scheme to show the quantum phase transition of the Jaynes-Cummings(JC)model by modulating the transition frequency of a two-level system in a quantum Rabi model with strong *** tuning the modulation frequency and amplitude,the ratio of the effective coupling strength of the rotating terms to the effective cavity(atomic transition)frequency can enter the deep-strong coupling regime,while the counter-rotating terms can be ***,a deep-strong JC model is *** ratio of the coupling strength to resonance frequencies in the deep-strong JC model is two orders of magnitude larger than the corresponding ratio in the original quantum Rabi *** scheme can be employed in atom-cavity resonance and off-resonance cases,and it is valid over a broad *** nonzero average cavity photons of the ground state indicate the emergence of a quantum phase ***,we demonstrate the dependence of the phase diagram on the atom-cavity detuning and modulation *** the parameters used in our scheme are within the reach of current experimental *** scheme provides a new mechanism for investigating the critical phenomena of finite-sized systems without requiring classical field limits,thereby opening a door for studying fundamental quantum phenomena occurring in the ultrastrong and even deep-strong coupling regimes.

关键词： Jaynes-Cummings model quantum phase transition frequency modulation

Enlarged interlayer of separator coating enabling high-performance lithiumsulfur batteries

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Frontiers of Chemical Science and Engineering 2024年第2期18卷 103-112页

作者： Yanqi feng Hui liu Xiaoting liu qiongqiong Lu School of Materials&Environment Engineering Chengdu Technological UniversityChengdu 611730China School of Materials Science and Engineering Shaanxi Key Laboratory of Green Preparation and Functionalization for Inorganic MaterialsShaanxi University of Science and TechnologyXi’an 710021China Green Catalysis Center and College of ChemistryZhengzhou UniversityZhengzhou 450001China Institute of Materials Henan Key Laboratory of Advanced Conductor MaterialsHenan Academy of SciencesZhengzhou 450046China Leibniz Institute for Solid State and Materials Research(IFW) Dresden e.V.Dresden 01069Germany

Lithiumsulfur batteries have been intensively studied due to their high theoretical energy density and abundant sulfur resources. However, their commercial application is hindered by the low redox kinetics and high sulfur losses. In principle, in the design of cathodes and separators, the adsorption toward lithium-polysulfides should be enhanced and the conversion of soluble high-order lithium-polysulfides should be catalyzed. Herein, a KV_(3)O_(8)·0.75H_(2)O separator is designed as an effective lithium-polysulfides mediator in lithiumsulfur batteries. The intercalated K+ would enlarge the interlayer spacing of vanadium oxides, preventing the collapse of the layer structure and improving the electrical/ion conductivity of the interface. Moreover, the KV_(3)O_(8)·0.75H_(2)O modified separator possess a prior adsorption and high redox kinetics toward lithium-polysulfides due to the enhanced diffusion kinetics, which guarantees the high-rate capability and efficient utilization of sulfur. As a result, lithiumsulfur batteries exhibit a high capacity of 1362 mAh·g^(-1) and a long lifespan with a low capacity loss of 0.073% per cycle. This work may provide an alternative way to establish a functional separator to balance the adsorption and conversion of polysulfides during the redox back and forth.

关键词： lithium kinetics adsorption

Sound event localization and detection based on deep learning

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Journal of Systems Engineering and Electronics 2024年第2期35卷 294-301页

作者： ZHAO Dada DING Kai qi Xiaogang CHEN Yu feng Hailin School of Mathematics and Statistics Xidian UniversityXi’an 710071China Science and Technology on Near-Surface Detection Laboratory Wuxi 214035China

Acoustic source localization(ASL)and sound event detection(SED)are two widely pursued independent research *** recent years,in order to achieve a more complete spatial and temporal representation of sound field,sound event localization and detection(SELD)has become a very active research *** paper presents a deep learning-based multioverlapping sound event localization and detection algorithm in three-dimensional ***-Mel spectrum and generalized cross-correlation spectrum are joined together in channel dimension as input *** features are classified and regressed in parallel after training by a neural network to obtain sound recognition and localization results *** channel attention mechanism is also introduced in the network to selectively enhance the features containing essential information and suppress the useless ***,a thourough comparison confirms the efficiency and effectiveness of the proposed SELD *** experiments show that the proposed algorithm is robust to reverberation and environment and can achieve higher recognition and localization accuracy compared with the baseline method.

关键词： sound event localization and detection(SELD) deep learning convolutional recursive neural network(CRNN) channel attention mechanism

A robust viscoelastic surfactant tolerating 20% HCl up to 150℃ for oil well stimulation

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Petroleum Science 2024年第3期21卷 1865-1874页

作者： Ji Wang Ning qi Hong-Yao Yin Yu-Jun feng Polymer Research Institute State Key Laboratory of Polymer Materials EngineeringSichuan UniversityChengdu610065SichuanPR.China Tianfu Yongxing Laboratory New Theory and Technology of CO_(2) Capture Research CenterChengdu610065SichuanPR China School of Petroleum Engineering China University of Petroleum(East China)Qingdao266580ShandongPR China

Viscoelastic surfactants(VES)are often used as viscous diverters in acidizing stimulation to prolong the acid consumption time and maximize zonal coverage of the acid for improving well ***,the ceiling temperature of commercial VES cannot exceed 120℃in practical use because of the poor thermal stability and fragile molecular structure,hindering their implementation in hightemperature oil reservoirs,i.e.,≥150℃.Here we synthesized a novel C22-tailed diamine,N-erucaminopropyl-N,N-dimethylamine(EDPA),and examined comparatively its rheological behavior,assemblies morphology and molecular stability in 20 wt%HCl with a commercial VES,erucyl dimethyl amidopropyl betaine(EDAB).The feasibility of EDPA for acidizing stimulation was assessed by acid etching of carbonate rock with its HCl solution at 150℃.Rheological results showed that the 2.5 wt%EDPA—20 wt%HCl solution maintains stable viscosity of 90 m Pa s at 150℃for 60 min,while that of 2.0 wt%EDAB HCl solution is just 1 m Pa s under identical conditions.1H NMR spectra and cryo-TEM observations revealed that the chemical structure and self-assembled architectures of EDPA remained intact in such context,but the EDAB suffered from degradation due to the hydrolysis of the amide group,accounting for the poor heat-resistance and *** reaction rate of 2.5 wt%EDPA HCl solution with carbonate rock was one order of magnitude lower than that of 20 wt%HCl solution at 150℃,underpinning the potential of EDPA to be used in the high-temperature reservoirs *** work improved the thermal tolerance of VES in highly concentrated HCl solution,paving a feasible way for the acidization of high-temperature reservoir environments(~150℃).

关键词： Viscoelastic surfactants Thermal stability Self-diverting acid Wormlike micelles Acidizing stimulation

A Review of NILM Applications with Machine Learning Approaches

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Computers, Materials & Continua 2024年第5期79卷 2971-2989页

作者： Maheesha Dhashantha Silva qi liu School of Electronic and Information Engineering Nanjing University of Information Science and TechnologyNanjing210044China

In recent years,Non-Intrusive LoadMonitoring (NILM) has become an emerging approach that provides affordableenergy management solutions using aggregated load obtained from a single smart meter in the power ***, by integrating Machine Learning (ML), NILM can efficiently use electrical energy and offer less ofa burden for the energy monitoring process. However, conducted research works have limitations for real-timeimplementation due to the practical issues. This paper aims to identify the contribution of ML approaches todeveloping a reliable Energy Management (EM) solution with NILM. Firstly, phases of the NILM are discussed,along with the research works that have been conducted in the domain. Secondly, the contribution of machinelearning approaches in three aspects is discussed: Supervised learning, unsupervised learning, and *** highlights the limitations in the applicability of ML approaches in the field. Then, the challenges in the realtimeimplementation are concerned with six use cases: Difficulty in recognizing multiple loads at a given time,cost of running the NILM system, lack of universal framework for appliance detection, anomaly detection andnew appliance identification, and complexity of the electricity loads and real-time demand side ***, options for selecting an approach for an efficientNILMframework are suggested. Finally, suggestionsare provided for future research directions.

关键词： Non-intrusive load monitoring transfer learning machine learning feature extraction

Visible Light Indoor Positioning System Based on Pisarenko Harmonic Decomposition and Neural Network

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Chinese Journal of Electronics 2024年第1期33卷 195-203页

作者： Li ZHAO Yi REN qi WANG Lange DENG feng ZHANG School of Electronic Information Engineering Xi’an Technological University

Visible-light indoor positioning is a new generation of positioning technology that can be integrated into smart lighting and optical communications. The current received signal strength(RSS)-based visible-light positioning systems struggle to overcome the interferences of background and indoor-reflected noise. Meanwhile, when ensuring the lighting, it is impossible to use the superposition of each light source to accurately distinguish light source information; furthermore, it is difficult to achieve accurate positioning in complex indoor environments. This study proposes an indoor positioning method based on a combination of power spectral density detection and a neural network. The system integrates the mechanism for visible-light radiation detection with RSS theory, to build a back propagation neural network model fitting for multiple reflection channels. Different frequency signals are loaded to different light sources at the beacon end, and the characteristic frequency and power vectors are obtained at the location end using the Pisarenko harmonic decomposition method. Then, a complete fingerprint database is established to train the neural network model and conduct location tests. Finally, the location effectiveness of the proposed algorithm is verified via actual positioning experiments. The simulation results show that, when four groups of sinusoidal waves with different frequencies are superimposed with white noise, the maximum frequency error is 0.104 Hz and the maximum power error is 0.0362 W. For the measured positioning stage, a 0.8 m × 0.8 m × 0.8 m solid wood stereoscopic positioning model is constructed, and the average error is 4.28 cm. This study provides an effective method for separating multi-source signal energies, overcoming background noise, and improving indoor visible-light positioning accuracies.

关键词： Neural networks Measurement uncertainty Position measurement Harmonic analysis Light emitting diodes Frequency estimation Indoor positioning systems

Diagnosis and treatment of biliary mucinous cystic neoplasms: A single-center experience

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Hepatobiliary & Pancreatic Diseases International 2024年第5期23卷 495-501页

作者： Jun-Jun Jia Ya-Fen Cheng Mei-Bao feng Li liu Ming-qi Shuai Xiao-Dong Shen Xiao-feng Tang Shu-Sen Zheng Division of Hepatobiliary and Pancreatic Surgery Department of Surgerythe First Affiliated HospitalZhejiang University School of MedicineHangzhou 310003China Department of International Healthcare Center the First Affiliated HospitalZhejiang University School of MedicineHangzhou 310003China Department of Pathology the First Affiliated HospitalZhejiang University School of MedicineHangzhou 310003China Department of Library the First Affiliated HospitalZhejiang University School of MedicineHangzhou 310003China

Background: Biliary mucinous cystic neoplasms(BMCNs) are rare hepatobiliary cystic tumors, which can be divided into noninvasive and invasive types. This study aimed to investigate the diagnosis, treatment, and prognosis of BMCNs in a large single center. Methods: We analyzed 49 patients with BMCNs confirmed by postoperative pathology at the First Afflliated Hospital, Zhejiang University School of Medicine between January 2007 and December 2021. Results: Among the 49 patients, 37 were female(75.5%), and the average age was 57.04 years. Common symptoms included abdominal discomfort, jaundice and fever, while 22 patients(44.9%) had no symptoms. Serum carbohydrate antigen(CA) 19-9 and CA125 concentrations were elevated in 34.8% and 19.6% of patients, respectively. Forty-eight patients had tumors in the intrahepatic bile ducts and only one had a tumor in the extrahepatic bile duct. Forty-eight patients with noninvasive intrahepatic BMCNs were further analyzed in terms of pathological features: 34(70.8%) had low-grade intraepithelial neoplasms(LGINs), and 14(29.2%) had high-grade intraepithelial neoplasms(HGINs). The potential immunohistochemical markers of BMCNs were cytokeratin(CK) 19, CK7, estrogen receptor and progesterone receptor. Follow-up data for 37 patients with intrahepatic BMCNs were obtained. The median overall survival(OS) of BMCNs was not reached. The longest survival time was 137 *** 5-and 10-year OS rates were 100% and 85.4%, respectively. The 5-and 10-year recurrence-free survival(RFS) rates were 93.9% and 80.2%, respectively. Conclusions: BMCNs are rare cystic neoplasms that commonly occur in middle-aged females. BMCNs can only be diagnosed and classified by postoperative pathology, as there are no specific clinical presentations, serological indicators or imaging modalities for preoperative diagnosis. Complete surgical resection is necessary for BMCNs, and the postoperative prognosis is favorable.

关键词： Biliary mucinous cystic neoplasms Low-grade intraepithelial neoplasms High-grade intraepithelial neoplasms Overall survival Recurrence-free survival