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Elevated temperature-driven coordinative reconstruction of an unsaturated single-Ni-atom structure with low valency on a polymer-derived matrix for the electrolytic oxygen evolution reaction

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Nanoscale 2024年第15期16卷 7467-7479页

作者： Patil, Rahul Rajput, Anubha Matsagar, Babasaheb M. Chen, Norman C. R. Ujihara, Masaki Salunkhe, Rahul R. Yadav, Praveen Wu, Kevin C.-W. Chakraborty, Biswarup Dutta, Saikat Electrochemical Energy & Sensor Research Laboratory Amity Institute of Click Chemistry Research & Studies Amity University Noida India Department of Chemistry Indian Institute of Technology New Delhi India Department of Chemical Engineering National Taiwan University Taipei10617 Taiwan Molecular Science and Technology Program Taiwan International Graduate Program Academia Sinica Taiwan National Taiwan University Taiwan Graduate Institute of Applied Science and Technology National Taiwan University of Science and Technology Taipei Taiwan Materials Research Laboratory Department of Physics Indian Institute of Technology Jammu India Synchrotron X-ray Facility Raja Ramanna Centre for Advanced Technology Rajendra Nagar Madhya Pradesh 452013 Indore India

A high-temperature pyrolysis-controlled coordination reconstruction resulted in a single-Ni-atom structure with a Ni-Nx-C structural unit (x = N atom coordinated to Ni). Pyrolysis of Ni-phen@ZIF-8-RF at 700 °C resulted in NiNP-NC-700 with predominantly Ni nanoparticles. Upon elevating the pyrolysis temperature from 700 to 900 °C, a coordination reconstruction offers Ni-Nx atomic sites in NiSA-NC-900. A combined investigation with X-ray absorption spectroscopy, X-ray photoelectron spectroscopy, and soft X-ray L3-edge spectroscopy suggests the stabilization of low-valent Niδ+ (0 −2 was achieved. The cell potential recorded with Pt(−)/(+)NiSA-NC-900/NF was much lower than that obtained for other cells, i.e., Pt(−)/NF and NF(−)/(+)NF, which enhances the potentials of low-valent NiSAs for insightful understanding of the OER. At a constant applied potential of 1.61 V (vs. RHE) for 12 h, an small increase in current for initial 0.6 h followed by a constant current depicts the fair stability of catalyst for 12 h. Our results offer an insightful angle into the OER with a coordinatively reconstructed single-Ni-atom structure at lower valency ( © 2024 The Royal Society of Chemistry.

关键词： Reaction kinetics

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Polarization-contrcoled chiral trransport

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Light(science & Applications) 2025年第3期14卷 822-830页

作者： Hang Zhu Jian Wang Andrea Alu Lin Chen Wuhan National Laboratory for Optoelectronics and School of Optical and Electronic Information Huazhong University of Science and TechnologyWuhan 430074China Photonics Initiative Advanced Science Research CenterCity University of New YorkNew YorkNY 10031USA physics Program Graduate CenterCity University of New YorkNew YorkNY 10016USA Shenzhen Huazhong University of Science and Technology Research Institute Shenzhen 518063China Key Laboratory of High Temperature Electromagnetic Materials and Structure of MOE Wuhan University of Science andTechnologyWuhan430081China

Handedness-selective chiral transport is an intriguing phenomenon that not only holds signifcant importance for fundamental research but also carries application prospects in fields such as optical communications and ***,on-chip chiral transport devices are static,unable to modulate the output modes based on the input *** limits both device functionality reconfiguration and information transmission ***,we propose to use the incident polarization diversity to control the Hamiltonian evolution path,achieving polarization-dependent chiral *** mapping the evolution path of TE and TM polarizations onto elaborately engineered double-coupled waveguides,we experimentally demonstrate that different polarizations yield controllable modal *** work combines Multiple-lnput,Multiple-Output,and polarization diversity concepts with chiral transport and challenges the prevailing notion that the modal outputs are fixed to specific modes in chiral transport,thereby opening pathways for the development of on-chip reconfigurable and high-capacity handedness-selective devices.

关键词： polarization controlled handedness selective control hamilton modulate output modes incident polarization diversity optical communications chiral transport fundamental research

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Porphyrin-Grafted Poly(ethylene terephthalate) as a Reusable and Highly Selective Colorimetric Probe for Mercuric Ion Contaminants in Aqueous Samples

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ACS Applied materials and Interfaces 2024年第30期16卷 39195-39205页

作者： Atayde, Eduardo C. Takenaka, Yasumasa Abe, Hideki Wu, Ming-Rou Wu, Kevin C.-W. Molecular Science and Technology Program Taiwan International Graduate Program Academia Sinica Department of Chemistry National Tsing Hua University Department of Chemical Engineering National Taiwan University Bioplastic Research Team RIKEN Center for Sustainable Resource Science Department of Chemical Engineering and Materials Science Yuan Ze University Department of Chemical Engineering Chung Yuan Christian University

Heavy metals are the most hazardous water pollutants, with severe health and environmental consequences. Among these, mercuric (Hg2+) ions are known to cause detrimental health issues in both humans and aquatic life. ... 详细信息

Heavy metals are the most hazardous water pollutants, with severe health and environmental consequences. Among these, mercuric (Hg²⁺) ions are known to cause detrimental health issues in both humans and aquatic life. Due to this, several analytical techniques have been devised to detect and quantify the amount of this ion. However, most of these require advanced instrumentation, prolonged analysis time, and sample preparation. In this study, a low-cost and highly reusable colorimetric probe was developed by grafting porphyrin to poly(ethylene terephthalate) sheets using an oxazoline polymer as covalent adhesive. Upon exposure to trace amounts of Hg²⁺ in solution, the fabricated material visually transitioned from faint brownish pink to green by the complexation mechanism. Additionally, the transparency of this probe allowed the quantitative spectrophotometric determination of the Hg²⁺ concentration in aqueous samples. It was also shown that the material is highly stable, which can be reused for more than 50 times without significant decline in its performance, hence, making it suitable for the onsite monitoring of mercuric ion contamination in different bodies of water. © 2024 The Authors. Published by American Chemical Society.

关键词： colorimetric probe mercuric ion oxazoline PET porphyrin

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Transforming organic chemistry research paradigms:Moving from manual efforts to the intersection of automation and artificial intelligence

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National science Open 2024年第2期3卷 98-127页

作者： Chengchun Liu Yuntian Chen Fanyang Mo School of Materials Science and Engineering Peking UniversityBeijing 100871China Ningbo Institute of Digital Twin Eastern Institute of TechnologyNingbo 315000China AI for Science(AI4S)-Preferred Program Peking University Shenzhen Graduate SchoolShenzhen 518055China

Organic chemistry is undergoing a major paradigm shift,moving from a labor-intensive approach to a new era dominated by automation and artificial intelligence(AI).This transformative shift is being driven by technological advances,the ever-increasing demand for greater research efficiency and accuracy,and the burgeoning growth of interdisciplinary *** models,supported by computational power and algorithms,are drastically reshaping synthetic planning and introducing groundbreaking ways to tackle complex molecular *** addition,autonomous robotic systems are rapidly accelerating the pace of discovery by performing tedious tasks with unprecedented speed and *** article examines the multiple opportunities and challenges presented by this paradigm shift and explores its far-reaching *** provides valuable insights into the future trajectory of organic chemistry research,which is increasingly defined by the synergistic interaction of automation and AI.

关键词： organic chemistry automation platform artificial intelligence algorithms

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Unconventional assemblies of bisacylhydrazones:The role of water for circularly polarized luminescence

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Aggregate 2022年第5期3卷 185-193页

作者： Hye Jin Cho Dong Yeun Jeong Hwihyun Moon Taewoo Kim You Kyoung Chung Yeongdong Lee Zonghoon Lee Joonsuk Huh Youngmin You Changsik Song Department of Chemistry Sungkyunkwan UniversitySuwonGyeonggi 16419Republic of Korea Division of Chemical Engineering and Materials Science Graduate Program in System Health Science and EngineeringEwha Womans UniversitySeoul 03760Republic of Korea Center for Multidimensional Carbon Materials Institute for Basic Science(IBS)Department of Materials Science and EngineeringUlsan National Institute of Science and Technology(UNIST)Ulsan 44919Republic of Korea

Understanding the precise molecular arrangement of chiral supramolecular polymers is essential not only to comprehend complex superstructures like proteins and DNA but also for the development of next-generation optoelectronic materials,including materials displaying high-performance circularly polarized luminescence(CPL).Herein,we report the first chiral supramolecular polymer systems based on hydrazone–pyridinium conjugates comprising alkyl chains of different lengths,which afforded control of the apparent supramolecular *** supramolecular chirality is governed basically by the remote chiral centers of alkyl chains,helicity inversion was achieved by controlling the conditions under which the hydrazone building blocks underwent aggregation(i.e.,solvent compositions or temperature).More importantly,the addition of water to the system led to aggregationinduced hydrazone deprotonation,which resulted in a completely different selfassembly *** water molecules played an essential role,forming the assembly’s channel-like backbone,around which hydrazone molecules gathered as a result of hydrogen bonding *** co-assembly of an achiral hydrazone luminophore with the given supramolecular polymer system allowed the fabrication of a novel CPL-active hydrazone-based material exhibiting a high maximum value for the photoluminescence dissymmetry factor of -2.6×10^(-2).

关键词： circularly polarized luminescence(CPL) helicity control hydrazone self-assembly structural water supramolecular polymerization

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Unified throughout-pore microstructure enables ultrahigh separator porosity for robust high-flux lithium batteries

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Electron 2023年第1期1卷 37-49页

作者： Dongjiang Chen Yuanpeng Liu Chao Feng Yuhui He Shengyu Zhou Botao Yuan Yunfa Dong Haodong Xie Guangfeng Zeng Jiecai Han Weidong He National Key Laboratory of Science and Technology on Advanced Composites in Special Environments Harbin Institute of TechnologyHarbinChina Center for Composite Materials and Structures Harbin Institute of TechnologyHarbinChina State Key Laboratory of Electronic Thin Film and Integrated Devices University of Electronic Science and Technology of ChinaChengduChina Chongqing Research Institute Harbin Institute of TechnologyChongqingChina Interdisciplinary Graduate Program in Materials Science Vanderbilt UniversityNashvilleTennesseeUSA

With small thickness,commercial polyolefin separators own low porosity to ensure sufficient thermomechanical properties,resulting in tortuous and enlarged Li+diffusion pathways that induce large overpotentials and detrimental dendrite *** a dilemma,the exploration of highly porous separators has been challenged by their large thickness,impairing the applicability of such ***,an ultraporous architecture is designed to shorten Li+transfer pathways by impregnating electrolyteaffinitive poly(vinylidene fluoride-co-hexafluoropropylene)into ultralight~3μm 3D-polytetrafluoroethylene scaffold(abbreviated as UP3D).The UP3D separator with a porosity of 74%gives rise to 70%enhancement in Li+transference and 77%reduction in Li+transfer resistance(2.67 mΩmm^(−1))and thus enables an ultrahigh Li+flux of 22.7 mA cm^(−2),effectively alleviating Li+concentration gradient across the *** the separator,the LiFePO4 half cell delivers a capacity of 118 mAh g^(−1) with an unparalleled capacity retention of 90%after 1000 cycles at 2 C,and a graphite||LiNi_(0.6)Co_(0.2)Mn_(0.2)O_(2)pouch full cell delivers an areal energy density of 6.8 mWh cm^(−2)at 8.848 mA(1.4 mA cm^(−2))with a high cathode loading of 134.9 *** results,together with the scalable production of the separator,reflect its promising potential in high-flux battery applications of separators that require both ultrahigh porosity and reliability.

关键词： Li deposition Li-ion batteries polytetrafluoroethylene separator ultrahigh porosity

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Organic X-Ray Image Sensors Using a Medium Bandgap Polymer Donor with Low Dark Current

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Energy & Environmental materials 2024年第6期7卷 230-237页

作者： Jong-Woon Ha Seung Hun Eom Bo Kyung Cha Seyeong Song Hyeong Ju Eun Jong H.Kim Jong Mok Park BongSoo Kim Byoungwook Park Seo-Jin Ko Sung Cheol Yoon Changjin Lee In Hwan Jung Do-Hoon Hwang Department of Chemistry Chemistry Institute for Functional MaterialsPusan National UniversityBusan 46241Korea Division of Advanced Energy Materials Research Center Korea Research Institute of Chemical Technology(KRICT)Daejeon 34114Korea Electro-Medical Device Research Center Korea Electrotechnology Research Institute(KERI)Ansan 15588Korea Graduate School of Carbon Neutrality School of Energy and Chemical EngineeringUlsan National Institute of Science and Technology(UNIST)Ulsan 44919Korea Department of Molecular Science and Technology Ajou UniversitySuwon 16449Korea Research Center for Advanced Specialty Chemicals Korea Research Institute of Chemical TechnologyUlsan 44412Korea Department of Chemistry Ulsan National Institute of Science and Technology(UNIST)Ulsan 44919Korea Department of Organic and Nano Engineering Human-Tech Convergence ProgramHanyang University222 Wangsimni-roSeongdong-guSeoul 04763Korea

The development of portable X-ray detectors is necessary for diagnosing fractures in unconscious patients in emergency ***,this is quite challenging because of the heavy weight of the scintillator and silicon *** weight and thickness of X-ray detectors can be reduced by replacing the silicon layer with an organic *** study presents a novel bithienopyrroledione-based polymer donor that exhibits excellent photodetection properties even in a thick photoactive layer(~700 nm),owing to the symmetric backbone and highly soluble molecular structure of *** ability of bithienopyrroledione-based polymer donor to strongly suppress the dark current density(Jd~10−10 A cm^(−2))at a negative bias(−2.0 V)while maintaining high responsivity(R=0.29 A W−1)even at a thickness of 700 nm results in a maximum shot-noise-limited specific detectivity of D_(sh)^(*)=2.18×10^(13)Jones in the organic *** organic photodetectors are developed by slot-die coating for use in X-ray detectors,which exhibit D_(sh)^(*)=2.73×10^(12)Jones with clear rising(0.26 s)and falling(0.29 s)response times upon X-ray *** reliability is also proven by linear response of the X-ray detector,and the X-ray detection limit is 3 mA.

关键词： low dark current low detection limit organic photodetector printable X-ray

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Correlating the Ambient Conditions and Performance Indicators of the LoRaWAN via Surrogate Gaussian Process-Based Bidirectional LSTM Stacked Autoencoder

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IEEE Transactions on Network and Service Management 2023年第3期20卷 3413-3427页

作者： Bhat, Showkat Ahmad Huang, Nen-Fu Hussain, Imtiyaz Sajjad, Uzair National Tsing Hua University College of Electrical and Computer Science Hsinchu1300044 Taiwan National Tsing Hua University Department of Computer Science Hsinchu1300044 Taiwan National Taipei University of Technology Graduate Program in Energy and Opto-Electronic Materials Taipei10608 Taiwan National Taipei University of Technology Department of Energy and Refrigerating Airconditioning Engineering Taipei10608 Taiwan

LoRa's biggest advantage is its flexibility, which is the ability to increase or decrease data rate and range while decreasing or increasing sensitivity. Whenever propagation conditions change frequently, this function allows the spreading factor to be modified accordingly. Despite their efficiency and scalability, adaptive data rate algorithms ignore and fail to factor in the complex correlation between ambient weather parameters influencing the communication channel design. In this research, a Bayesian surrogate Gaussian process-based bidirectional LSTM stacked autoencoder model (BSGP-BLSTM-SAE) is proposed to estimate the channel performance indicators such as received signal strength indicator (RSSI) and signal-to-noise ratio (SNR) and to determine the correlation between the ambient weather conditions and performance indicators for the LoRaWAN network. Bayesian optimization algorithm has been used to optimize the hyper-parameters of the developed model. A LoRaWAN experimental multivariate time series dataset has been used for the evaluation of the developed model, which upon testing and validation produces high accuracy in predicting the channel performance indicators and ambient conditions of the experimental LoRaWAN network. The mean absolute error of the developed model was around 0.45. Thus, the proposed model can predict the link performance indicators and thereby assist in real-time optimization of the transmission parameters to enhance the network performance in LoRaWAN-based systems at different ambient conditions. © 2004-2012 IEEE.

关键词： Internet of things

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Mo-terminated edges in two-dimensional molybdenum disulfide for site-specific hydrolysis and DNA cleavage

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materials Today 2025年 86卷 162-171页

作者： Wang, Cong Wu, Menghan Li, Muqing Zhao, Yingcan Zhao, Mingchuang Zhang, Yunhao Bai, Yichao Gao, Jianxiang Wang, Xiaoxia Tian, Xilin Zhang, Han Chang, Liang Zou, Xiaolong Liu, Bilu Kang, Feiyu Terrones, Mauricio Lei, Yu Institute of Materials Research Shenzhen Key Laboratory of Advanced Layered Materials for Value-added Applications Guangdong Provincial Key Laboratory of Thermal Management Engineering and Materials & Center of Double Helix Tsinghua Shenzhen International Graduate School Tsinghua University Shenzhen518055 China Institute of Materials Research & Shenzhen Geim Graphene Center Shenzhen Key Laboratory of Advanced Layered Materials for Value-added Applications Tsinghua-Berkeley Shenzhen Institute and Tsinghua Shenzhen International Graduate School Tsinghua University Shenzhen518055 China Environmental Science Program Department of Life Sciences Beijing Normal University-Hong Kong Baptist University United International College Guangdong519087 China Tsinghua Shenzhen International Graduate School Tsinghua University Shenzhen518055 China Department of Physics Department of Chemistry Department of Materials Sciences Center for 2-Dimensional and Layered Materials The Pennsylvania State University University ParkPA16802 United States International Collaborative Laboratory of 2D Materials for Optoelectronics Science and Technology of Ministry of Education Institute of Microscale Optoelectronics Shenzhen University Shenzhen518060 China

The hydrolysis of DNA serves as the foundational principle for gene engineering that enable precise gene cleavage at the molecular level. This process typically occurs in biological nucleases, which exhibit nucleobase-selective and catalytic hydrolysis capabilities rarely replicated in abiotic nanomaterials. Here, we demonstrate that molybdenum-terminated (Mo-terminated) edges of molybdenum disulfide (MoS2) possess the unique ability to abstract a proton (H+) from water molecules, thereby facilitating catalytic hydrolysis reactions that cleave the phosphodiester bonds in DNA through the action of hydroxide ions. The enhanced proton absorption at Mo-terminated edges of MoS2 significantly reduces the activation energy required for the DNA hydrolysis reaction. Furthermore, the favorable interaction between the Mo-terminated edges and thymine nucleobases promotes both charge transfer and P-O bond cleavage, enabling targeted DNA hydrolysis at 'TTTTTTT' sequences under dark conditions. This discovery underscores the potential of MoS2 as a stable, efficient nanosystem for precise genetic editing, heralding advanced applications in the field of gene engineering. © 2025 The Author(s)

关键词： Activation energy

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Three-dimensional magnetization reconstruction from electron optical phase images with physical constraints

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science China(Physics,Mechanics & Astronomy) 2024年第11期67卷 122-132页

作者： Boyao Lyu Shihua Zhao Yibo Zhang Weiwei Wang Fengshan Zheng Rafal E.Dunin-Borkowski Jiadong Zang Haifeng Du Anhui Province Key Laboratory of Low-Energy Quantum Materials and Devices High Magnetic Field LaboratoryHefei Institutes of Physical ScienceChinese Academy of SciencesHefei 230031China Science Island Branch Graduate School of University of Science and Technology of ChinaHefei 230026China Department of Physics and Astronomy University of New HampshireDurham 03824USA Department of Physics The City College of New YorkNew York 10031USA Physics Program Graduate Center of the City University of New YorkNew York 10016USA Department of Chemistry University of New HampshireDurham 03824USA Institutes of Physical Science and Information Technology Anhui UniversityHefei 230601China Spin-X Institute Center for Electron MicroscopySchool of Physics and OptoelectronicsState Key Laboratory of Luminescent Materials and DevicesGuangdong-Hong Kong-Macao Joint Laboratory of Optoelectronic and Magnetic Functional MaterialsSouth China University of TechnologyGuangzhou 511442China Ernst Ruska-Centre for Microscopy and Spectroscopy with Electrons Forschungszentrum JülichJülich 52425Germany

The ability to characterize three-dimensional(3D)magnetization distributions in nanoscale magnetic materials and devices is essential to fully understand their static and dynamic magnetic *** contrast techniques in the transmission electron microscope(TEM),such as electron holography and electron ptychography,can be used to record two-dimensional(2D)projections of the in-plane magnetic induction of 3D nanoscale *** the 3D magnetic induction can in principle be reconstructed from one or more tilt series of such 2D projections,conventional tomographic reconstruction algorithms do not recover the 3D magnetization within a sample ***,we use simulations to describe the basis of an improved model-based algorithm for the tomographic reconstruction of a 3D magnetization distribution from one or more tilt series of electron optical phase images recorded in the *** algorithm allows a wide range of physical constraints,including a priori information about the sample geometry and magnetic parameters,to be *** also makes use of minimization of the micromagnetic energy in the loss *** demonstrate the reconstruction of the 3D magnetization of a localized magnetic soliton—a hopfion ring—and discuss the influence of noise,choice of magnetic constants,maximum tilt angle and number of tilt axes on the *** algorithm can in principle be adapted for other magnetic contrast imaging techniques in the TEM,as well as for other magnetic characterization techniques,such as those based on X-rays or neutrons.

关键词： three-dimensional magnetization vector field tomography differentiable programming electron holography micromagnetism

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