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SSRN 2023年

作者： Li, Guangxin Chu, BinBin Chen, Jinyu Xue, Lingfeng You, Longzhen Ren, Xu Wang, Yin Zhang, Yu Xu, Ruoyu Huang, Tao Yu, Aishui Laboratory of Advanced Materials Institute of New Energy Fudan University 2205 Songhu Road Shanghai200438 China Department of Chemical Engineering University College London LondonWC1E 7JE United Kingdom School of Materials Science and Engineering Linyi University Shandong Linyi276000 China Department of Chemistry Collaborative Innovation Center of Chemistry for Energy Materials Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials Fudan University 2205 Songhu Road Shanghai200438 China Department of Physics International Centre for Quantum and Molecular Structures Shanghai University China Hongzhiwei Technology Shanghai Shanghai201206 China Co. Ltd. Shanghai201206 China

Understanding the oxygen evolution of layered oxide cathode materials at high cut-off voltages is an enormous challenge. Herein, the single-crystal LiNi0.6Co0.2Mn0.2O2 (SC622) cathodes have been studied to investigate the relationship between electrochemical oxygen evolution behavior, structural degradation, and electrochemical performance at high cut-off voltages. The oxygen evolution behavior can be detected at around 4.6 V (with 84% lithium extraction) via in-situ differential electrochemical mass spectrometry and ex-situ synchrotron soft X-ray absorption spectroscopy tests. Density functional theory results show that lattice oxygen atoms are lost easily from the surficial region but stable in the bulk area at high voltages. This provides scientific theoretical fundamentals for using SC622 cathode material at high cut-off voltages. Excessive lithium extraction results in uneven distribution of lithium inside SC622 grains, leading to lattice distortion and uneven deformation, eventually causing slippage and cracks. These bulk damages accelerate oxygen release and severely degrade the electrochemical performance of SC622. Both surface doping and fluorinated electrolyte can suppress the oxygen evolution of SC622 cathode materials at an ultrahigh cut-off voltage of 4.7 V. However, an appropriately high cut-off voltage, such as 4.5 V, maybe a more pragmatic strategy, achieving high specific energy and long cycle-life of cathodes such as SC622. © 2023, The Authors. All rights reserved.

关键词： Cathodes

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Optically Tunable Many-Body Exciton-Phonon Quantum Interference

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Advanced science 2024年第40期11卷 e2404741页

作者： Chang, Si-Jie Huang, Po-Chun Su, Jia-Sian Hsieh, Yu-Wei Quiroz Reyes, Carlos Jose Fan, Ting-Hsuan Sun, Han-Sheng Nguyem, Ai-Phuong Liu, Te-I Cheng, Ho-Wen Lin, Ching-Wei Hayashi, Michitoshi Yong, Chaw-Keong Department of Physics National Taiwan University Taipei10617 Taiwan Institute of Atomic and Molecular Sciences Academia Sinica Taipei106319 Taiwan International Ph.D. Program in Biomedical Engineering College of Biomedical Engineering Taipei Medical University New Taipei235603 Taiwan Department of Chemistry National Tsing Hua University Hsinchu300044 Taiwan International Graduate Program of Molecular Science and Technology National Taiwan University Taipei106319 Taiwan Center for Condensed Matter Sciences National Taiwan University Taipei10617 Taiwan Center of Atomic Initiative for New Materials National Taiwan University Taipei10617 Taiwan National Center for Theoretical Sciences Taipei10617 Taiwan

This study introduces a novel paradigm for achieving widely tunable many-body Fano quantum interference in low-dimensional semiconducting nanostructures, beyond the conventional requirement of closely matched energy levels between discrete and continuum states observed in atomic Fano systems. Leveraging Floquet engineering, the remarkable tunability of Fano lineshapes is demonstrated, even when the original discrete and continuum states are separated by over 1 eV. Specifically, by controlling the quantum pathways of discrete phonon Raman scattering using femtosecond laser pulses, the Raman intermediate states across the excitonic Floquet band are tuned. This manipulation yields continuous transitions of Fano lineshapes from antiresonance to dispersive and to symmetric Lorentzian profiles, accompanied by significant variations in Fano parameter q and Raman intensity spanning 2 orders of magnitude. A subtle shift in the excitonic Floquet resonance is further shown, achieved by controlling the intensity of the femtosecond laser, which profoundly modifies quantum interference strength from destructive to constructive interference. The study reveals the crucial roles of Floquet engineering in coherent light-matter interactions and opens up new avenues for coherent control of Fano quantum interference over a broad energy spectrum in low-dimensional semiconducting nanostructures. © 2024 The Author(s). Advanced science published by Wiley-VCH GmbH.

关键词： Femtosecond lasers

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Estimation of the main air pollutants from different biomasses under combustion atmospheres by artificial neural networks

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Chemosphere 2024年 352卷 141484页

作者： Monteiro, Thalyssa Oliveira Alves, Pedro Augusto Araújo da Silva de Almeida Nava Barradas Filho, Alex Oliveira Villa-Vélez, Harvey Alexander Cruz, Glauber Postgraduate Program in Mechanical Engineering (PPGMEC) Department of Mechanics and Materials Federal Institute of Education Science and Technology of Maranhão (IFMA) Maranhão São Luís Brazil Postgraduate Program in Computer Science and Computational Mathematics (PPG-CCMC) Department of Computer Science University of São Paulo (USP) São Carlos São Paulo Brazil Data Analysis and Artificial Intelligence Laboratory (DARTi) Department of Computational Engineering Federal University of Maranhão (UFMA) Maranhão São Luís Brazil Department of Chemical Engineering Federal University of Maranhão (UFMA) Maranhão São Luís Brazil Processes and Thermal Systems Laboratory (LPSisTer) Department of Mechanical Engineering Federal University of Maranhão (UFMA) Maranhão São Luís Brazil

The production of biofuels to be used as bioenergy under combustion processes generates some gaseous emissions (CO, CO2, NOx, SOx, and other pollutants), affecting living organisms and requiring careful assessments. H... 详细信息

The production of biofuels to be used as bioenergy under combustion processes generates some gaseous emissions (CO, CO₂, NO_x, SO_x, and other pollutants), affecting living organisms and requiring careful assessments. However, obtaining such information experimentally for data evaluation is costly and time-consuming and its in situ obtaining for regional biomasses (e.g., those from Northeast Brazil (NEB) is still a major challenge. This paper reports on the application of artificial neural networks (ANNs) for the prediction of the main air pollutants (CO, CO₂, NO, and SO₂) produced during the direct biomass combustion (N₂/O₂:80/20%) with the use of ultimate analysis (carbon, hydrogen, nitrogen, sulfur, and oxygen). 116 worldwide biomasses were used as input data, which is a relevant alternative to overcome the lack of experimental resources in NEB and obtain such information. Cross-validation was conducted with k-fold to optimize the ANNs and performance was analyzed with the use of statistical errors for accuracy assessments. The results showed an acceptable statistical performance for all architectures of ANNs, with 0.001–12.41% MAPE, 0.001–5.82 mg Nm⁻³ MAE, and 0.03–52.30 mg Nm⁻³ RMSE, highlighting the high precision of the emissions studied. On average, the differences between predicted and real values for CO, CO₂, NO, and SO₂ emissions from NEB biomasses were approximately 0.01%, 10⁻⁶%, 0.14%, and 0.05%, respectively. Pearson coefficient provided consistent results of concentration of the ultimate analysis in relation to the emissions studied and effectiveness of the test set in the developed models. © 2024 Elsevier Ltd

关键词： Brazilian northeastern Environmental statistics Evaluation metrics Gaseous emissions Predictive models Thermoconversion

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Tip-structure coupled with hydrophobic effect synergistically regulate microenvironment for efficient CO2 electroreduction in acidic electrolytes

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Applied Catalysis B: Environmental 2025年 375卷

作者： Dong, Tian Wang, Weizhou Yang, Qin Geng, Yanling Du, Yunmei Liu, Kang Wu, Zexing Lai, Jianping Li, Bin Zheng, Gengfeng Li, Hongdong Wang, Lei Key Laboratory of Eco-Chemical Engineering International Science and Technology Cooperation Base of Eco-Chemical Engineering and Green Manufacturing Qingdao University of Science and Technology Qingdao266042 China College of Chemistry and Molecular Engineering Qingdao University of Science and Technology Qingdao266042 China Laboratory of Advanced Materials Department of Chemistry and Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials Faculty of Chemistry and Materials Science Fudan University Shanghai200438 China

In acidic CO2 electro-reduction, the strong hydrogen evolution reaction (HER) and the catalyst's susceptibility to corrosion limit its selectivity, stability and energy efficiency. We demonstrate that the enhanced the activity and stability of CO2 reduction reaction (CO2RR) with suppressed HER can be achieved by synergistically modulating the local microenvironment using tip-enhanced electric field effect and hydrophobic effect. This enabled a Faraday efficiency (FE) of 93.2 % and a cathode energy efficiency of 49.36 % for CO at the current density up to −400 mA cm−2 over 32 h on polytetrafluoroethylene (PTFE) modified silver nanoneedles catalyst (Ag-NNs@PTFE) in a flow cell with pH = 2. Finite element modelling and density functional theory revealed that silver nanoneedles catalyst could induce high local potassium ion (K+) concentration to stabilize key intermediates of CO2RR, and PTFE-modified catalyst inter faces generated energetically favorable pathways for CO2RR. Furthermore, the coated PTFE could protect catalyst against corrosion. Meanwhile, this strategy has also been well applied on bismuth-based catalyst with nanoneedle structures. The optimal Bi-NNs@PTFE exhibited the FE of HCOOH maintaining above 85 % over 32 h of operation at −1.1 V vs. RHE. This work provides a new idea for the application of CO2RR in acidic media. © 2025 Elsevier B.V.

关键词： Electrolytic reduction

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Characterization of Coulomb Interactions in Electron Transport through a Single Hetero-Helicene molecular Junction Using Scanning Tunneling Microscopy

arXiv

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arXiv 2024年

作者： Shi, Yueqing Bi, Liya Wang, Zihao Liang, Kangkai Li, Ji-Kun Wang, Xiao-Ye Li, Wan-Lu Li, Shaowei Department of Chemistry and Biochemistry University of California La Jolla San DiegoCA92093-0309 United States Program in Materials Science and Engineering University of California La Jolla San DiegoCA92093-0418 United States State Key Laboratory of Elemento-Organic Chemistry College of Chemistry Nankai University Tianjin300071 China Aiiso Yufeng Li Family Department of Chemical and Nano Engineering University of California La Jolla San DiegoCA92093-0448 United States

Characterization of the structural and electron transport properties of single chiral molecules provides critical insights into the interplay between their electronic structure and electrochemical environments, providing broader implications given the significance of molecular chirality in chiroptical applications and pharmaceutical sciences. Here, we examined the topographic and electronic features of a recently developed chiral molecule, B,N-embedded double hetero[7]helicene, at the edge of Cu(100)-supported NaCl thin film with scanning tunneling microscopy and spectroscopy. An electron transport energy gap of 3.2 eV is measured, which is significantly larger than the energy difference between the highest occupied and the lowest unoccupied molecular orbitals given by theoretical calculations or optical measurements. Through first-principles calculations, we demonstrated that this energy discrepancy results from the Coulomb interaction between the tunneling electron and the molecule's electrons. This occurs in electron transport processes when the molecule is well decoupled from the electrodes by the insulating decoupling layers, leading to a temporary ionization of the molecule during electron tunneling. Beyond revealing properties concerning a specific molecule, our findings underscore the key role of Coulomb interactions in modulating electron transport in molecular junctions, providing insights into the interpretation of scanning tunneling spectroscopy features of molecules decoupled by insulating layers. © 2024, CC BY.

关键词： Sodium chloride

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Interfacial Layer materials with a Truxene Core for Dopant-Free NiOx-Based Inverted Perovskite Solar Cells

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Small 2024年第33期20卷 e2310939页

作者： Ramanujam, Rajarathinam Hsu, Hsiang-Lin Shi, Zhong-En Lung, Chien-Yu Lee, Chin-Han Wubie, Gebremariam Zebene Chen, Chih-Ping Sun, Shih-Sheng Institute of Chemistry Academia Sinica Nankang Taipei11529 Taiwan Taiwan International Graduate Program Sustainable Chemical Science and Technology Academia Sinica Nankang Taipei11529 Taiwan Department of Applied Chemistry National Yang Ming Chiao Tung University Hsinchu30050 Taiwan Department of Materials Engineering Ming Chi University of Technology 84 Gunjuan Road Taishan New Taipei City24301 Taiwan College of Engineering and Center for Sustainability and Energy Technologies Chang Gung University Taoyuan33302 Taiwan

Nickel oxide (NiOx) is commonly used as a holetransporting material (HTM) in p-i-n perovskite solar cells. However, the weak chemical interaction between the NiOx and CH3NH3PbI3 (MAPbI3) interface results in poor crystallinity, ineffective hole extraction, and enhanced carrier recombination, which are the leading causes for the limited stability and power conversion efficiency (PCE). Herein, two HTMs, TRUX-D1 (N2,N7,N12-tris(9,9-dimethyl-9H-fluoren-2-yl)-5,5,10,10,15,15-hexaheptyl-N2,N7,N12-tris(4-methoxyphenyl)-10,15-dihydro-5H-diindeno[1,2-a:1′,2′-c]fluorene-2,7,12-triamine) and TRUX-D2 (5,5,10,10,15,15-hexaheptyl-N2,N7,N12-tris(4-methoxyphenyl)-N2,N7,N12-tris(10-methyl-10H-phenothiazin-3-yl)-10,15-dihydro-5H-diindeno[1,2-a:1′,2′-c]fluorene-2,7,12-triamine), are designed with a rigid planar C3 symmetry truxene core integrated with electron-donating amino groups at peripheral positions. The TRUX-D molecules are employed as effective interfacial layer (IFL) materials between the NiOx and MAPbI3 interface. The incorporation of truxene-based IFLs improves the quality of perovskite crystallinity, minimizes nonradiative recombination, and accelerates charge extraction which has been confirmed by various characterization techniques. As a result, the TRUX-D1 exhibits a maximum PCE of up to 20.8% with an impressive long-term stability. The unencapsulated device retains 98% of their initial performance following 210 days of aging in a glove box and 75.5% for the device after 80 days under ambient air condition with humidity over 40% at 25 °C. © 2024 Wiley-VCH GmbH.

关键词： Passivation

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Tio2 Coated Sio2 Core-Shell Stationary Phase with Uniform and Tunable Tio2 Thickness for High Performance Liquid Chromatography Separation

SSRN

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SSRN 2023年

作者： Wang, Dian Wan, Xiang Wang, Jiafei Mangelings, Debby Sun, Yuanshe Li, Tong Xu, Qin Xie, Fazhi Li, Weihua Qu, Qishu Key Laboratory of Functional Molecule Design and Interface Process Anhui Province Engineering Laboratory of Advanced Building Materials School of Materials Science and Chemical Engineering Anhui Jianzhu University Hefei230601 China Department of Analytical Chemistry Applied Chemometrics and Molecular Modelling Vrije Universiteit Brussel Laarbeeklaan 103 BrusselsB-1090 Belgium Dalian Elite Analytical Instruments Co. Ltd. Dalian116023 China College of Chemistry and Chemical Engineering Yangzhou University Yangzhou225002 China Anhui Provincial Key Laboratory of Environmental Pollution Control and Resource Reuse School of Environment and Energy Engineering Anhui Jianzhu University Hefei230601 China

In this work, SiO2 core-shell spheres with a dendritic pore structure were used as chromatographic support and TiO2 was coated into the pores of the SiO2@dSiO2 shell using tetrabutyl orthotitanate (TBOT) as the titanium source. By simply prolonging the reaction time, a TiO2 layer with a uniform and controllable thickness was obtained on the surface of SiO2 core-shell spheres by Ostwald ripening. The thickness of the TiO2 layer can be achieved by either controlling the reaction time or controlling the amount of TBOT. When the concentration of TBOT was 0.06 mol L-1, the thickness of the TiO2 layer can be tuned from 15 to about 44 nm by changing the reaction time. When the concentration of TBOT was 0.08 mol L-1, the thickness of the TiO2 layer can be tuned from 21 to about 71 nm by changing the reaction time. C18-derived core-shell spheres with a TiO2 layer thicknesses of 40 nm (C18-SST-0.5-60) and 70 nm (C18-SST-0.7-30) were used as packings to evaluate the effect of TiO2 layer thickness on the chromatographic separation performance. The separation performance of C18-SST-0.5-60 was better than that of C18-SST-0.7-30. The separation efficiency of C18-SST-0.5-60 and C18-SST-0.7-30 for fluorene was 115112 plates m-1 and 83189 plates m-1, respectively. The columns were also used for the separation of basic, acidic and nucleoside mixtures. Both TiO2-coated core-shell packings showed good peak symmetry for basic samples, with peak asymmetry factors below 1.11. The relative standard deviations of the retention time of polycyclic aromatic hydrocarbons and anilines for intraday, interday and column-to-column variation were all lower than 6%. The results demonstrate that the TiO2 based stationary phase possesses great potential for high performance liquid chromatographic separation. © 2023, The Authors. All rights reserved.

关键词： Silica

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DETECTION OF THE SARS-COV-2 SPIKE PROTEIN IN SALIVA WITH SHRINKY-DINK© ELECTRODES 25

DETECTION OF THE SARS-COV-2 SPIKE PROTEIN IN SALIVA WITH SHR...

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25th International Conference on Miniaturized Systems for Chemistry and Life sciences, MicroTAS 2021

作者： Zakashansky, Julia A. Imamura, Amanda H. Salgado, Darwin F. Romero Mercieca, Heather C. Aguas, Raphael F.L. Lao, Angelou M. Pariser, Joseph Arroyo-Currás, Netzahualcóyotl Khine, Michelle Materials Science and Engineering University of California - Irvine IrvineCA92697 United States Instituto de Química de São Carlos Universidade de São Paulo São Paulo São Carlos13566‐590 Brazil Biomedical Engineering University of California - Irvine IrvineCA92697 United States Department of Pharmacology and Molecular Sciences Johns Hopkins School of Medicine BaltimoreMD21205 United States Department of Chemical and Bio-molecular Engineering Whiting School of Engineering Institute for Nanobiotechnology Johns Hopkins University BaltimoreMD21218 United States

ISBN: (纸本)9781733419031

Our recently published1 investigation of an aptamer-based electrochemical (E-AB) assay that recognizes the spike protein of SARS-CoV-2 in saliva for viral infection detection yielded an exceptionally low limit of quantification of less than 0.001 fg mL-1 of the SARS-CoV-2 S1 subunit. Since this work, we have also been able to demonstrate detection of inactivated virus in saliva. © 2021 MicroTAS 2021 - 25th International Conference on Miniaturized Systems for Chemistry and Life sciences. All rights reserved.

关键词： Coronavirus

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Spin injection and transport in single-crystalline organic spin valves based on TIPS-pentacene

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science China materials 2021年第11期64卷 2795-2804页

作者： Ying Wang Jiarong Yao Shuaishuai Ding Siyu Guo Dapeng Cui Xinyue Wang Shuyuan Yang Lijuan Zhang Xinzi Tian Di Wu Chao Jin Rongjin Li Wenping Hu Tianjin Key Laboratory of Molecular Optoelectronic Sciences Department of ChemistrySchool of ScienceTianjin University and Collaborative Innovation Center of Chemical Science and EngineeringTianjin 300072China National Laboratory of Solid State Microstructures Department of Materials Science and Engineering and Jiangsu Key Laboratory for Artificial Functional MaterialsNanjing UniversityNanjing 210093China Tianjin Key Laboratory of Low Dimensional Materials Physics and Preparing Technology Department of PhysicsSchool of ScienceTianjin UniversityTianjin 300072China Joint School of National University of Singapore and Tianjin University International Campus of Tianjin UniversityBinhai New CityFuzhou 350207China

Single crystals of organic semiconductors with perfect crystal structure and minimal density of defects can exhibit high mobility and low spin scattering compared with their amorphous or polycrystalline ***,these materials are promising candidates as the spin transport media to obtain long spin relaxation times and spin diffusion lengths in spintronic ***,the investigation of spin injection and transport properties in organic single crystals is hindered by the inability to construct devices such as single-crystalline organic spin valves(OSVs).Herein,thin and large organic single crystals of 6,13-bis(triisopropylsilylethynyl)pentacene(TIPS-pentacene)were grown on a liquid substrate and transferred to a target substrate carrying ferromagnetic electrodes to construct single-crystalline *** magnetoresistance(MR)responses of the single crystals were investigated to study their spin injection and transport *** value as high as 17%was probed with an intermediate layer thickness of 269 *** importantly,spin transport was still observed in a single crystal of a thickness up to 457 nm,which was much larger than that of polycrystalline thin *** research provides a general methodology for constructing single-crystalline OSVs and paves the way to probe the intrinsic spin transport properties of organic semiconductors based on single crystals.

关键词： organic single crystal organic semiconductor magnetoresistance organic spin valve spintronics

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Convergence Analysis of the Stochastic Resolution of Identity: Comparing Hutchinson to Hutch++ for the Second-Order Green's Function

arXiv

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arXiv 2024年

作者： Mejía, Leopoldo Sharma, Sandeep Baer, Roi Chan, Garnet Kin-Lic Rabani, Eran Department of Chemistry University of California BerkeleyCA94720 United States Materials Sciences Division Lawrence Berkeley National Laboratory BerkeleyCA94720 United States Department of Chemistry University of Colorado Boulder BoulderCO80309 United States Fritz Haber Center for Molecular Dynamics Institute of Chemistry The Hebrew University of Jerusalem Jerusalem91904 Israel Division of Chemistry and Chemical Engineering California Institute of Technology PasadenaCA91125 United States The Raymond and Beverly Sackler Center of Computational Molecular and Materials Science Tel Aviv University Tel Aviv69978 Israel

Stochastic orbital techniques offer reduced computational scaling and memoryrequirements to describe ground and excited states at the cost of introducingcontrolled statistical errors. Such techniques often rely on two basicoperations, stochastic trace estimation and stochastic resolution of identity,both of which lead to statistical errors that scale with the number ofstochastic realizations ($N_{\\xi}$) as $\\sqrt{N_{\\xi}^{-1}}$. Reducing thestatistical errors without significantly increasing $N_{\\xi}$ has beenchallenging and is central to the development of efficient and accuratestochastic algorithms. In this work, we build upon recent progress made toimprove stochastic trace estimation based on the ubiquitous Hutchinson\'salgorithm and propose a two-step approach for the stochastic resolution ofidentity, in the spirit of the Hutch++ method. Our approach is based onemploying a randomized low-rank approximation followed by a residualcalculation, resulting in statistical errors that scale much better than$\\sqrt{N_{\\xi}^{-1}}$. We implement the approach within the second-order Bornapproximation for the self-energy in the computation of neutral excitations anddiscuss three different low-rank approximations for the two-body Coulombintegrals. Tests on a series of hydrogen dimer chains with varying lengthsdemonstrate that the Hutch++-like approximations are computationally moreefficient than both deterministic and purely stochastic (Hutchinson) approachesfor low error thresholds and intermediate system sizes. Notably, forarbitrarily large systems, the Hutchinson-like approximation outperforms bothdeterministic and Hutch++-like methods. Copyright © 2024, The Authors. All rights reserved.

关键词： Errors

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