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CO oxidation on MXene(Mo_(2)CS_(2)) supported single-atom catalyst: A termolecular Eley-Rideal mechanism

Chinese chemical Letters 2023年第2期34卷 519-528页

作者： Shamraiz Hussain Talib Zhansheng Lu Beenish Bashir Sajjad Hussain Khalil Ahmad Salahuddin Khan Sajjad Haider Zongxian Yang Kersti Hermansson Jun Li School of Physics Henan Normal UniversityXinxiang 453007China Department of Chemistry and Key Laboratory of Organic Optoelectronics&Molecular Engineering of Ministry of Education Tsinghua UniversityBeijing 100084China Department of Materials Science and Engineering Southern University of Science and TechnologyShenzhen 518055China School of Chemistry Minhaj UniversityLahore 54000Pakistan Department of Chemistry Mirpur University of Science and Technology(MUST)MirpurAJK 10250Pakistan College of Engineering King Saud UniversityPO Box 800Riyadh 11421Saudi Arabia Chemical Engineering Department College of EngineeringKing Saud UniversityPO Box 800Riyadh 11421Saudi Arabia Department of Chemistry-Ångström Uppsala UniversityBox 538Uppsala 75121Sweden Department of Chemistry Southern University of Science and TechnologyShenzhen 518055China

Finding transition metal catalysts for effective catalytic conversion of CO to CO_(2)has attracted much *** as a new 2D layered material of early transition metal carbides,nitrides,and carbo-nitrides is a robust support for achoring metal *** this study,the electronic structure,geometries,thermodynamic stability,and catalytic activity of MXene (Mo_(2)CS_(2)) supported single noble metal atoms (NM=Ru,Rh,Pd,Ir,Pt and Au) have been systematically examined using first-principles calculations and ab initio molecular dynamic (AIMD) ***,AIMD simulations and phonon spectra demonstrate the dynamic and thermal stabilities of Mo_(2)CS_(2)*** likely reaction pathways,LangmuirHinshelwood (LH),Eley-Rideal (ER),and Termolecular Eley–Rideal (TER) for CO oxidation on the Ru1-and Ir_(1)@Mo_(2)CS_(2)SACs,have been studied in *** is found that CO oxidation mainly proceeds via the TER mechanism under mild reaction *** corresponding rate-determining steps are the dissociation of the intermediate (OCO-Ru_(1)-OCO) and formation of OCO-Ir_(1)-OCO *** downshift d-band center of Ru1-and Ir_(1)@Mo_(2)CS_(2)help to enhance activity and improve catalytst ***,a microkinetic study predicts a maximum CO oxidation rate of 4.01×10^(2)s^(-1)and 4.15×10^(3)s^(-1)(298.15K) following the TER pathway for the Ru_(1)-and Ir_(1)@Mo_(2)CS_(2)catalysts,*** work provides guideline for fabricating and designing highly efficient SACs with superb catalyts using MXene materials.

关键词： CO oxidation Quantum chemical study 2D MXene monolayer M1@Mo_(2)CS_(2) Termolecular Eley–Rideal Single-atom catalysis

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Dynamics of self-hybridized exciton–polaritons in 2D halide perovskites

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Light(science & Applications) 2024年第1期13卷 13-22页

作者： Surendra B.Anantharaman Jason Lynch Christopher E.Stevens Christopher Munley Chentao Li Jin Hou Hao Zhang Andrew Torma Thomas Darlington Francis Coen Kevin Li Arka Majumdar PJames Schuck Aditya Mohite Hayk Harutyunyan Joshua R.Hendrickson Deep Jariwala Department of Electrical and Systems Engineering University of PennsylvaniaPhiladelphiaPA19104USA KBR Inc. BeavercreekOH45431USA Air Force Research Laboratory Sensors DirectorateWright-Patterson Air Force BaseOH45433USA Department of Physics University of WashingtonSeattleWA98195USA Department of Physics Emory UniversityAtlantaGA30322USA Department of Chemical and Biomolecular Engineering Rice UniversityHoustonTX77005USA Department of Materials Science and Nanoengineering Rice UniversityHoustonTX77005USA Applied Physics Program Smalley‐Curl InstituteRice UniversityHoustonTX77005USA Department of Mechanical Engineering Columbia UniversityNew YorkNY10027USA Department of Electrical and Computer Engineering University of WashingtonSeattleWA98195USA

Excitons,bound electron–hole pairs,in two-dimensional hybrid organic inorganic perovskites(2D HOIPs)are capable of forming hybrid light-matter states known as exciton-polaritons(E–Ps)when the excitonic medium is confined in an optical *** the case of 2D HOIPs,they can self-hybridize into E–Ps at specific thicknesses of the HOIP crystals that form a resonant optical cavity with the ***,the fundamental properties of these self-hybridized E–Ps in 2D HOIPs,including their role in ultrafast energy and/or charge transfer at interfaces,remain ***,we demonstrate that>0.5µm thick 2D HOIP crystals on Au substrates are capable of supporting multiple-orders of self-hybridized E–P *** E–Ps have high Q factors(>100)and modulate the optical dispersion for the crystal to enhance sub-gap absorption and *** varying excitation energy and ultrafast measurements,we also confirm energy transfer from higher energy E–Ps to lower energy E–***,we also demonstrate that E–Ps are capable of charge transport and transfer at *** findings provide new insights into charge and energy transfer in E–Ps opening new opportunities towards their manipulation for polaritonic devices.

关键词： charge polar excitation

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Ultrasmall,elementary and highly translational nanoparticle X-ray contrast media from amphiphilic iodinated statistical copolymers

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Acta Pharmaceutica Sinica B 2023年第4期13卷 1660-1670页

作者： Lu Su Kellie S.Dalby Hannah Luehmann Sussana A.Elkassih Sangho Cho Xun He Lisa Detering Yen-Nan Lin Nari Kang Dennis A.Moore Richard Laforest Guorong Sun Yongjian Liu Karen L.Wooley Department of Chemistry Department of Materials Science and Engineeringand Department of Chemical EngineeringTexas A&M UniversityCollege StationTX 77842USA Laboratory of Macromolecular and Organic Chemistry and Institute for Complex Molecular Systems Eindhoven University of TechnologyEindhovenMB 5600The Netherlands Mallinckrodt Institute of Radiology Washington University School of MedicineSaint LouisMO 63110USA Bayer AG Creve CoeurMO 63167USA

To expand the single-dose duration over which noninvasive clinical and preclinical cancer imaging can be conducted with high sensitivity,and well-defined spatial and temporal resolutions,a facile strategy to prepare ultrasmall nanoparticulate X-ray contrast media(nano-XRCM)as dual-modality imaging agents for positron emission tomography(PET)and computed tomography(CT)has been *** from controlled copolymerization of triiodobenzoyl ethyl acrylate and oligo(ethylene oxide)acrylate monomers,the amphiphilic statistical iodocopolymers(ICPs)could directly dissolve in water to afford thermodynamically stable solutions with high aqueous iodine concentrations(>140 mg iodine/mL water)and comparable viscosities to conventional small molecule *** formation of ultrasmall iodinated nanoparticles with hydrodynamic diameters of ca.10 nm in water was confirmed by dynamic and static light scattering *** a breast cancer mouse model,in vivo biodistribution studies revealed that the64Cu-chelator-functionalized iodinated nano-XRCM exhibited extended blood residency and higher tumor accumulation compared to typical small molecule imaging ***/CT imaging of tumor over 3 days showed good correlation between PET and CT signals,while CT imaging allowed continuous observation of tumor retention even after 10 days post-injection,enabling longitudinal monitoring of tumor retention for imaging or potentially therapeutic effect after a single administration of nano-XRCM.

关键词： Amphiphilic statistical iodocopolymer CT X-ray contrast media Ultrasmall nanoassembly PET/CT Longitudinal tumor monitoring

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Electrochemical evolution of a metal oxyhydroxide surface on two-dimensional layered metal phosphorus trisulfides enables the oxidation of amine to nitrile

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Carbon Energy 2025年第3期7卷 133-147页

作者： Binglan Wu Karim Harrath Marshet Getaye Sendeku Tofik Ahmed Shifa Yuxin Huang Jing Tai Fekadu Tsegaye Dajan Kassa Belay Ibrahim Xueying Zhan Zhenxing Wang Elisa Moretti Ying Yang Fengmei Wang Alberto Vomiero State Key Laboratory of Chemical Resource Engineering College of ChemistryBeijing University of Chemical TechnologyBeijingChina CAS Key Laboratory of Nanosystem and Hierarchical Fabrication National Center for Nanoscience and Technology(NCNST)BeijingChina Shaanxi Provincial Key Laboratory of Electroanalytical Chemistry Key Laboratory of Synthetic and Natural Functional Molecule of the Ministry of EducationCollege of Chemistry&Materials ScienceNorthwest UniversityXi'anChina State Key Laboratory of Multiphase Flow in Power Engineering International Research Center for Renewable EnergyXi'an Jiaotong UniversityShaanxiChina Fundamental Science Center of Rare Earths Ganjiang Innovation AcademyChinese Academy of ScienceGanzhouChina Ocean Hydrogen Energy R&D Center Research Institute of Tsinghua University in ShenzhenShenzhenChina Department of Molecular Sciences and Nanosystems Ca'Foscari University of VeniceVenezia MestreItaly Testing and Analysis Center Institute of Chemistry Chinese Academy of SciencesBeijingChina Department of Engineering Sciences and Mathematics Division of Materials ScienceLuleåUniversity of TechnologyLuleåSweden

Selective oxidation of amines to imines through electrocatalysis is an attractive and efficient way for the chemical industry to produce nitrile compounds,but it is limited by the difficulty of designing efficient catalysts and lack of understanding the mechanism of ***,we demonstrate a novel strategy by generation of oxyhydroxide layers on two-dimensional iron-doped layered nickel phosphorus trisulfides(Ni1-xFexPS_(3))during the oxidation of benzylamine(BA).In-depth structural and surface chemical characterizations during the electrocatalytic process combined with theoretical calculations reveal that Ni(1-x)FexPS_(3) undergoes surface reconstruction under alkaline conditions to form the metal oxyhydroxide/phosphorus trichalcogenide(NiFeOOH/Ni1-xFexPS_(3))***,the generated heterointerface facilitates BA oxidation with a low onset potential of 1.39 V and Faradaic efficiency of 53%for benzonitrile(BN)*** calculations further indicate that the as-formed NiFeOOH/Ni1-xFexPS_(3) heterostructure could offer optimum free energy for BA adsorption and BN desorption,resulting in promising BN synthesis.

关键词： 2D layered materials benzylamine oxidation metal phosphorus trichalcogenides surfacereconstructed heterostructure

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Photolithography Patterning of Organic Light-Emitting Diodes Using Solvent Resistant Electron Transport materials

Photolithography Patterning of Organic Light-Emitting Diodes...

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International Symposium, Seminar, and Exhibition, Display Week 2024

作者： Yu, Hyunjin Yeong So, Eun Eun, Kyunghyun Jun Jung, Byung Kim, Myungwoong Lee, Jin-Kyun Yeob Lee, Jun School of Chemical Engineering Sungkyunkwan University 2066 Seobu-ro Jangan-gu Suwon-si Gyeonggi-do16419 Korea Republic of Department of Materials Science and Engineering University of Seoul Seoul02504 Korea Republic of Department of Chemistry and Chemical Engineering Inha University Incheon22212 Korea Republic of Program in Environment and Polymer Engineering Inha University 100 Inha-ro Michuhol-gu Incheon22212 Korea Republic of

In this paper, we develop a novel approach to achieve ultra-high resolution in organic light-emitting diodes (OLEDs) through a photolithography patterning process. It is important to apply a solvent resistant electron transport layer (ETL) in the photolithography pattering of OLED because of solution coating process of photoresist on the ETL. Therefore, a solvent resistant ETL named 2,7-bis(4,6-diphenyl-1,3,5-triazin-2-yl)-9,9′-spirobi[fluorene] (SBF-Trz) was developed and employed as the ETL of OLEDs. The SBF-Trz demonstrated excellent solvent resistance during photolithography process and enabled device performances comparable to those of the conventional OLED without any photolithography process. It was found that the SBF-Trz ETL is appropriate as the ETL of the OLED patterned by photolithography due to good electron transport property, good stability, and good solvent resistance. © 2024, John Wiley and Sons Inc. All rights reserved.

关键词： Reactive ion etching

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Cytometry in the Short-Wave Infrared

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ACS Nano 2024年第28期18卷 18534-18547页

作者： Liu, Te-I Wang, Jhih-Shan Nguyen, Ai-Phuong Raabe, Marco Quiroz Reyes, Carlos Jose Lin, Chih-Hsin Lin, Ching-Wei Institute of Atomic and Molecular Sciences Academia Sinica Taipei City106319 Taiwan Department of Materials Science and Engineering National Taiwan University Taipei City106319 Taiwan Department of Physics University of Stuttgart Stuttgart70174 Germany Department of Chemistry National Tsing Hua University Hsinchu300044 Taiwan International Ph.D. Program in Biomedical Engineering Taipei Medical University New Taipei City235603 Taiwan Graduate Institute of Nanomedicine and Medical Engineering Taipei Medical University New Taipei City235603 Taiwan

Cytometry plays a crucial role in characterizing cell properties, but its restricted optical window (400-850 nm) limits the number of stained fluorophores that can be detected simultaneously and hampers the study and utilization of short-wave infrared (SWIR;900-1700 nm) fluorophores in cells. Here we introduce two SWIR-based methods to address these limitations: SWIR flow cytometry and SWIR image cytometry. We develop a quantification protocol for deducing cellular fluorophore mass. Both systems achieve a limit of detection of ∼0.1 fg cell-1 within a 30 min experimental time frame, using individualized, high-purity (6,5) single-wall carbon nanotubes as a model fluorophore and macrophage-like RAW264.7 as a model cell line. This high-sensitivity feature reveals that low-dose (6,5) serves as an antioxidant, and cell morphology and oxidative stress dose-dependently correlate with (6,5) uptake. Our SWIR cytometry holds immediate applicability for existing SWIR fluorophores and offers a solution to the issue of spectral overlapping in conventional cytometry. © 2024 The Authors. Published by American chemical Society.

关键词： Oxygen

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Direct visualisation of metal-defect cooperative catalysis in Ru-doped defective MOF-808

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Journal of materials Chemistry A 2024年第30期12卷 19018-19028页

作者： Xu, Chirui Orbell, William Wang, Guilian Li, Boye Ng, Bryan K. Y. Wu, Tai-Sing Soo, Yun-Liang Luan, Zhao-Xue Tang, Kangjian Wu, Xin-Ping Tsang, S. C. Edman Zhao, Pu Innovation Center for Chemical Science College of Chemistry Chemical Engineering and Materials Science Soochow University Suzhou215123 China Department of Chemistry University of Oxford OxfordOX1 3QR United Kingdom State Key Joint Laboratory of Environment Simulation and Pollution Control School of Environment Tsinghua University Beijing100084 China National Synchrotron Radiation Research Center Hsinchu30076 Taiwan Department of Physics National Tsing Hua University Hsin-chu30013 Taiwan State Key Laboratory of Green Chemical Engineering and Industrial Catalysis Centre for Computational Chemistry Research Institute of Industrial Catalysis School of Chemistry and Molecular Engineering East China University of Science and Technology Shanghai200237 China

Improving the efficiency of catalytic materials is vital to the chemical and energy industries. Constructing neighbouring active sites in metal-organic framework (MOF) materials for cooperative catalysis is a promising way to achieve the above goal. However, it is difficult to fine-tune active sites at the atomic level due to the challenge of visualising their local structures and their interaction with substrates. In this article, we report the direct visualisation of metal and defect active sites and binding of the phenol substrate in Ru-doped defective MOF-808. X-ray absorption spectroscopy, X-ray pair distribution function analysis, X-ray powder diffraction, and infrared spectroscopy reveal that the enhanced selective hydrogenation originates from the specific adsorption geometry of phenol over 7-centred Ru clusters and hydroxyl or water of defect sites. This mechanism also well explains the high catalytic activity in CO2 reduction. This work represents the first example of structural elucidation of metal-defect cooperative catalysis in MOFs and will lead to the rational design of new superactive MOF catalysts. © 2024 The Royal Society of Chemistry.

关键词： Substrates

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Porous Pyrene Organic Cage with Unusual Absorption Bathochromic-Shift Enables Visible Light Photocatalysis

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CCS Chemistry 2022年第8期4卷 2588-2596页

作者： Nana Sun Dongdong Qi Yucheng Jin Hailong Wang Chiming Wang Chen Qu Jiemin Liu Yinghua Jin Wei Zhang Jianzhuang Jiang Beijing Advanced Innovation Center for Materials Genome Engineering Beijing Key Laboratory for Science and Application of Functional Molecular and Crystalline MaterialsDepartment of Chemistry and Chemical EngineeringSchool of Chemistry and Biological EngineeringUniversity of Science and Technology BeijingBeijing 100083 Department of Chemistry University of ColoradoBoulderCO 80309

We have constructed a novel porous pyrene-based organic cage,PyTC1,through the condensation reaction of cyclohexanediamine with 5,5′-(pyrene-1,6-diyl)***-crystal X-ray diffraction analysis reveals the effective intercage C–H...πinteraction between cyclohexanediimine and pyrene *** a soft intercage C–H...πinteraction,rather than a classic J-aggregate with slippedπ–π-stacking configuration,induced an unusual bathochromic shift of pyrene-based chromophore absorption from an ultraviolet region of PyTC1 in solution to the visible light region of PyTC1 in solid-state.

关键词： absorption bathochromic-shift J-aggregate porous organic cage pyrene derivatives visible light catalysis

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Zwitterionic peptides:Tunable next-generation stealth nanoparticle modifications

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Bioactive materials 2023年第9期27卷 113-124页

作者： Clyde Overby Soomin Park Austin Summers Danielle S.W.Benoit Department of Biomedical Engineering University of Rochester RochesterNYUSA Center for Musculoskeletal Research University of RochesterRochesterNYUSA Department of Biology University of Rochester RochesterNYUSA Department of Biology Duquesne UniversityPAUSA Department of Chemical Engineering University of RochesterRochesterNYUSA Materials Science Program University of RochesterRochesterNYUSA Knight Campus for Accelerating Scientific Impact Department of BioengineeringUniversity of OregonEugeneORUSA

Adsorption of proteins to nanoparticles(NPs),a complex process that results in a protein corona,is controlled by NP surface properties that define NP interactions in *** to control adsorbed protein quantity through surface modification have led to improvements in circulation time or ***,current approaches have yet to be identified to control adsorbed protein identities within the ***,we report the development and characterization of diverse zwitterionic peptides(ZIPs)for NP anti-fouling surface functionalization with specific and controllable affinity for protein adsorption profiles defined by ZIP *** serum exposure of ZIP-conjugated NPs and proteomics analysis of the resulting corona,we determined that protein adsorption profiles depend not on the exact composition of the ZIPs but on the sequence and order of charges along the sequence(charge motif).These findings pave the way for developing tunable ZIPs to orchestrate specific ZIP-NP protein adsorption profiles as a function of ZIP charge motif to better control cell and tissue specificity and pharmacokinetics and provide new tools for investigating relationships between protein corona and biological ***,overall ZIP diversity enabled by the diversity of amino acids may ameliorate adaptive immune responses.

关键词： Nanoparticles Protein corona Surface functionalization Peptide design Cellular uptake

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Synergistic photocatalytic degradation of crystal violet dye using novel medical waste-derived carbon/ZnO composite: A study on toxicological assessment

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Process Safety and Environmental Protection 2024年 187卷 145-158页

作者： Ramanathan, Subramanian Rashmitha, Robert Merlin Chuang, Ho-Chiao Kasemchainan, Jitti Arumugam, Madan Kumar Lydia, Immanuel Sharmila Pandiyarajan, Sabarison Poompradub, Sirilux Department of Chemical Technology Faculty of Science Chulalongkorn University Bangkok10330 Thailand Affiliated to Bharathidasan University Tamil Nadu Tiruchirappalli620017 India Department of Mechanical Engineering National Taipei University of Technology Taipei10608 Taiwan Cancer Biology lab Center for Molecular and Nanomedical Sciences Sathyabama Institute of Science and Technology Chennai600119 India Center of Excellence in Green Materials for Industrial Application Faculty of Science Chulalongkorn University Bangkok10330 Thailand Center of Excellence on Petrochemical and Materials Technology Faculty of Science Chulalongkorn University Bangkok10330 Thailand

The discharge of crystal violet (CV) dye effluents from textile sectors is a significant concern, as these pollutants not only diminish the aesthetic appeal of water bodies but also impede light penetration, thereby disrupting aquatic ecology. Additionally, the COVID-19 pandemic has led to increased usage of disposable face masks, further contributing to medical waste in the environment. In this state-of-the-art study, the aim was to develop a photocatalyst material using medical-waste-derived carbon (MWC) as a support matrix for zinc oxide (ZnO) nanoparticles, facilitating the photocatalytic degradation of CV dye via persulfate (PS) activation. X-ray diffraction and Raman spectroscopy were used to analyze the crystalline and chemical bonding properties of the synthesized photocatalysts, whilst field-emission scanning electron microscopy and transmission electron microscopy with energy-dispersive X-ray spectroscopy mapping were employed to examine the samples’ surface morphology and composition. The UV–vis spectroscopy and photoluminescence spectroscopy were used to confirm the optical properties of the photocatalysts. The degradation analyses showed that the MWC/ZnO nanocomposite achieved a higher degradation efficiency of 94.4%, with a reusability performance of 91.0% in the fifth cycle. Toxicology assessment was performed using seedling Vigna mungo plants and zebrafish, which revealed significant developmental deformities in the embryos and adults of zebrafish treated with the CV solution, but not when grown with the degraded CV solution or water, supporting the non-toxic nature of the degraded dye water. Therefore, the proposed MWC/ZnO nanocomposite could be suggested as a potential catalyst for CV dye degradation and an ideal solution for both aquatic and medical waste pollutants. © 2024 The Institution of chemical Engineers

关键词： Scanning electron microscopy

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