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arXiv 2025年

作者： Acharya, Anupama Said, Madhukar Barker, Sylwia J. Utz, Marcel Linclau, Bruno Kuprov, Ilya School of Chemistry and Chemical Engineering University of Southampton University Road SouthamptonSO17 1BJ United Kingdom Department of Organic and Macromolecular Chemistry Ghent University Krijgslaan 281-S4 Ghent9000 Belgium Institute of Microstructure Technology Karlsruhe Institute of Technology Hermann-von-Helmholtz-Platz 1 Eggenstein-Leopoldshafen76344 Germany Department of Chemical and Biological Physics Weizmann Institute of Science 234 Herzl Street Rehovot76100 Israel

Quantum mechanical equations of motion are strictly linear in state descriptors, such as wavefunctions and density matrices, but equations describing chemical kinetics and hydrodynamics may be non-linear in concentrations. This incompatibility is fundamental, but special cases can be handled – for example, in magnetic resonance where nuclear spin interactions may be too weak influence concentration dynamics. For processes involving single spins and first-order chemical reactions, this is a well-researched topic, but time evolution of complex nuclear spin systems in the presence of second-order kinetics, diffusion, and flow has so far remained intractable. This creates obstacles in microfluidics, homogeneous catalysis, and magnetic resonance imaging of metabolic processes. In this communication we report a numerically stable formalism for time-domain quantum mechanical description of nuclear spin dynamics and decoherence in the simultaneous presence of diffusion, flow, and second-order chemical reactions. The formalism is implemented in versions 2.11 and later of the open-source Spinach library. As an illustration, we use Diels-Alder cycloaddition of acrylonitrile to cyclopentadiene, yielding endo- and exo-norbornene carbonitrile, in the presence of diffusion and flow in the detection chamber of a microfluidic NMR probe (a finite element model with thousands of Voronoi cells) with a spatially localised stripline radiofrequency coil. Copyright © 2025, The Authors. All rights reserved.

关键词： Magic angle spinning

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Correction: NaCMC-decorated ZnO nanocomposite polymer membranes for the separation of reactive dyes from textile water

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New Journal of Chemistry 2023年第3期48卷 1443-1443页

作者： R. Robin Vinoth Kumar Raja R. Sathish Kumar G. Arthanareeswaran Wirach Taweepreda Membrane Research Laboratory Department of Chemical Engineering National Institute of Technology Tiruchirappalli 620015 India Department of Chemical Engineering National Institute of Technology Andhra Pradesh Tadepalligudem Andhra Pradesh 534101 India Polymers & Composites Lab Department of Biomaterials Saveetha Dental College and Hospitals Saveetha Institute of Medical and Technical Sciences Saveetha University Chennai 600077 India Polymer Science Program Division of Physical Science Faculty of Science Prince of Songkla University Hat-Yai Songkhla 90110 Thailand

Correction for ‘NaCMC-decorated ZnO nanocomposite polymer membranes for the separation of reactive dyes from textile water’ by R. Robin et al., New J. Chem., 2023, 47, 20517–20526, https://***/10.1039/D3NJ03783E.

Correction for ‘NaCMC-decorated ZnO nanocomposite polymer membranes for the separation of reactive dyes from textile water’ by R. Robin et al., New J. Chem., 2023, 47, 20517–20526, https://***/10.1039/D3NJ03783E.

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De-Linker-Enabled Exceptional Volumetric Acetylene Storage Capacity and Benchmark C2H2/C2H4and C2H2/CO2Separations in Metal–Organic Frameworks

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Angewandte Chemie 2023年第10期135卷

作者： Dr. Jia-Wen Wang Dr. Shu-Cong Fan Dr. Hai-Peng Li Prof. Xianhui Bu Dr. Ying-Ying Xue Prof. Quan-Guo Zhai Key Laboratory of Macromolecular Science of Shaanxi Province Key Laboratory of Applied Surface and Colloid Chemistry Ministry of Education School of Chemistry & Chemical Engineering Shaanxi Normal University Xi'an Shaanxi 710062 China Department of Chemistry and Biochemistry California State University Long Beach CA-90840 USA

An ideal adsorbent for separation requires optimizing both storage capacity and selectivity, but maximizing both or achieving a desired balance remain challenging. Herein, a de-linker strategy is proposed to address this issue for metal–organic frameworks (MOFs). Broadly speaking, the de-linker idea targets a class of materials that may be viewed as being intermediate between zeolites and MOFs. Its feasibility is shown here by a series of ultra-microporous MOFs (SNNU-98-M, M=Mn, Co, Ni, Zn). SNNU-98 exhibit high volumetric C 2 H 2 uptake capacity under low and ambient pressures (175.3 cm 3 cm −3 @ 0.1 bar, 222.9 cm 3 cm −3 @ 1 bar, 298 K), as well as extraordinary selectivity (2405.7 for C 2 H 2 /C 2 H 4 , 22.7 for C 2 H 2 /CO 2 ). Remarkably, SNNU-98-Mn can efficiently separate C 2 H 2 from C 2 H 2 /CO 2 and C 2 H 2 /C 2 H 4 mixtures with a benchmark C 2 H 2 /C 2 H 4 (1/99) breakthrough time of 2325 min g −1 , and produce 99.9999 % C 2 H 4 with a productivity up to 64.6 mmol g −1 , surpassing values of reported MOF adsorbents.

关键词： Acetylene Storage Acetylene/Carbon Dioxide Separation Acetylene/Ethylene Separation De-Linker Strategy Metal–Organic Frameworks (MOFs)

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Precise Supramolecular Nanoarchitectonics for Simultaneous Enhanced Photoluminescence and Photocatalysis in a Co-Assembly by a Biomimetic Isolation-Conduction Strategy

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Angewandte Chemie 2024年第12期137卷

作者： Dr. Zhao Gao Jianxiang Sun Lulu Shi Wei Yuan Prof. Hongxia Yan Prof. Wei Tian Shaanxi Key Laboratory of Macromolecular Science and Technology Xi'an Key Laboratory of Hybrid Luminescent Materials and Photonic Device MOE Key Laboratory of Material Physics and Chemistry under Extraordinary Conditions School of Chemistry and Chemical Engineering Northwestern Polytechnical University Xi'an 710072 P. R. China Department of Chemistry National University of Singapore 3 Science Drive 3 Singapore 117543 Singapore

Limited by the two mutually exclusive physicochemical processes of separation and recombination of photogenerated carriers, achieving photoluminescence and photocatalysis simultaneously is extremely challenging but essential for ever-growing complex issues and specialized scenarios. Here we proposed a biomimetic isolation-conduction strategy induced by an arene-perfluoroarene (A−P) interaction for enabling photoluminescence and photocatalytic hydrogen evolution reaction (HER) activity in the co-assembly of aromatic monomers and octafluoronapthalene ( OFN ). Inspired by the isolation-conduction effect of periodic isolation of myelin sheaths on the axons of vertebrate nerve fibers by node of Ranvier, we use OFN as a molecular isolator embedded in the aromatic monomers array to block the singlet-to-triplet pathway, while the enlarged intermolecular dipoles resulting from the A−P interactions facilitate the conduction of photogenerated carriers in the isolated regions. The resultant co-assembly exhibits an enhanced monomeric green emission compared to the corresponding monocomponent self-assembly with weak red emission. Meanwhile, it also has an enhanced photocatalytic HER performance with a rate of 2.45 mmol g −1 h −1 , which is 15.2 times more than the self-assembled one. On this basis, a sequential fluoric wastewater reuse system that includes real-time fluorescence detection/removal of perfluorooctanoic acids and photocatalytic HER device is constructed.

关键词： Self-assembly Arene-Perfluoroarene Interactions Molecular Recognition Photocatalysis Perfluoroalkyl Compounds

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Synthesis of curcumin polyprodrug via click chemistry and construction of dual-drug-loaded nano platform for highly efficient tumor treatment

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Chinese chemical Letters 2025年第8期36卷

作者： Haijiao Li Mingzu Zhang Jinlin He Jian Liu Xingwei Sun Peihong Ni College of Chemistry Chemical Engineering and Materials Science State and Local Joint Engineering Laboratory for Novel Functional Polymeric Materials Jiangsu Key Laboratory of Advanced Functional Polymer Design and Application Suzhou Key Laboratory of Macromolecular Design and Precision Synthesis Soochow University Suzhou 215123 China Institute of Functional Nano and Soft Materials (FUNSOM) Soochow University Suzhou 215123 China Intervention Department The Second Affiliated Hospital of Soochow University Suzhou 215004 China

Micellar nanostructures formed by amphiphilic polymers are prone to dissociation when the in vivo environment changes. Polyprodrug micelles can cross-link with other hydrophobic drugs through non-covalent bonds, which has the advantage of fixed structure and avoids the use of chemical cross-linking agents. In this study, we prepared a polyprodrug with hydrophobic curcumin (CUR) and hydrophilic poly(ethylene glycol) (PEG) in the main chain through a click reaction between CUR derivatives containing azide groups and di-alkynly-capped PEG. Due to the presence of benzene rings in the structure of CUR, the polyprodrug can form non-covalent cross-linked nanoparticles (NCCL-CUR NPs) through hydrophobic and π - π stacking interaction. The structure, molecular weight, and self-assembly properties of the polyprodrug were characterized. The anti-cancer drug camptothecin (CPT) was encapsulated in the polyprodrug nanoparticles, producing dual-drug-loaded nanoparticles (abbreviated as CPT@NCCL-CUR NPs). The test results indicate that the NPs have reductive responsiveness and can release the original drugs CUR and CPT in phosphate buffer (PB) solution containing glutathione (GSH), while remaining stability in physiological environment. Cell and in vivo experiments further demonstrate that the dual-drug-loaded CPT@NCCL-CUR NPs can inhibit the growth of tumor through synergistic effects. This work provides a valuable approach for the preparation of amphiphilic polyprodrug with anti-tumor CUR as the backbone, and the stable dual-drug-loaded NPs containing both CUR and CPT through non-covalent cross-linking for synergistic therapy.

关键词： Camptothecin Click reaction Curcumin Non-covalent cross-linking Polyprodrug Stimuli responsiveness Synergistic therapy

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High-performance nitrogen selectivity through selective nitrate reduction on nickel-supported copper foam architectures

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Process Safety and Environmental Protection 2025年 199卷

作者： Thi Nhat-Tuyen Nguyen Kiruthika Mariappan Jih-Hsing Chang TsingHai Wang Subramanian Sakthinathan Chao-Lin Liu Ching-Lung Chen International Ph.D. Program in Innovative Technology of Biomedical Engineering and Medical Devices Ming Chi University of Technology New Taipei City 243303 Taiwan Department of Safety Health and Environmental Engineering Ming Chi University of Technology New Taipei City 243303 Taiwan Department of Environmental Engineering and Management Chaoyang University of Technology Taichung 413310 Taiwan Department of Chemical Engineering and Materials Science Yuan Ze University Zhongli 32003 Taiwan Department of Materials and Mineral Resources Engineering National Taipei University of Technology No.1 Section 3 Chung-Hsiao East Road Taipei 106 Taiwan Department of Chemical Engineering Ming Chi University of Technology New Taipei City 243303 Taiwan R&D Center of Biochemical Engineering Technology Ming Chi University of Technology New Taipei City 243303 Taiwan Department of Chemical and Materials Engineering Chang Gung University Taoyuan 33302 Taiwan Center for Environmental Sustainability and Human Health Ming Chi University of Technology New Taipei City 243303 Taiwan Center for Sustainability and Energy Technologies Chang Gung University Taoyuan 33302 Taiwan

In this study, Nickel@Copper (Ni@Cu) bimetallic electrodes were fabricated via electrodeposition to assess their efficacy in electrochemical nitrate reduction (ENR). The Ni@Cu 3 m electrodes achieved a remarkable nitrate (NO 3 − ) reduction efficiency of 96.09 % and nitrogen selectivity of 96.08 % at a current density of 1.36 mA/cm² over an 8-hour reaction period. Extensive characterization techniques, including TEM, XPS, and XRD, were employed to analyze the structural and morphological features of the electrodes. Cyclic voltammetry was used to examine electron transfer interactions between surface nitrogen (N 2 ) species and copper foam electrodes, nitrate (NO 3 − ) reduction commenced within a potential range of −0.8 V to 0.1 V. The Ni loading on copper foam was optimized to enhance catalytic performance, and the effect of different pH levels on activity was systematically studied. The Ni@Cu 3 m electrodes demonstrated excellent long-term stability over 10 cycles, maintaining high efficiency and selectivity over multiple cycles. These results highlight the strong potential of bimetallic electrodes as efficient and reliable candidates for NO 3 − reduction in wastewater treatment applications.

关键词： Cyclic voltammetry

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CRISPR/Cas9 mediated somatic gene therapy for insertional mutations:the vibrator mouse model

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Precision Clinical Medicine 2021年第3期4卷 168-175页

作者： Xin Fu Jie Zhu Yaou Duan Paul Lu Kang Zhang Spine Center Xin Hua Hospital Affiliated to Shanghai Jiao Tong University School of MedicineShanghai 200092China Guangzhou Women and Children’s Medical Center Guangzhou Medical UniversityGuangzhou 510623China Department of Nanoengineering Chemical Engineering Programand Moores Cancer CenterUniversity of California at San DiegoLa JollaCA 92093USA VA-San Diego Healthcare System San DiegoCA 92161USA Department of Neurosciences University of California at San DiegoLa JollaCA 92093USA Center for Biomedicine and Innovations Faculty of MedicineMacao University of Science and TechnologyMacaoChina

Somatic gene therapy remains technically challenging,especially in the central nervous system(CNS).Efficiency of gene delivery,efficacy in recipient cells,and proportion of cells required for overall benefit are the key points needed to be considered in any therapeutic *** efforts have demonstrated the efficacy of RNA-guided nucleases such as CRISPR/Cas9 in correcting point mutations or removing dominant *** we used viral delivered Cas9 plasmid and two guide RNAs to remove a recessive insertional mutation,vibrator(vb),in the mouse *** vb mice expressed∼20%of normal levels of phosphatidylinositol transfer protein,α(PITPα)RNA and protein due to an endogenous retrovirus inserted in intron 4,resulting in early-onset tremor,degeneration of brainstem and spinal cord neurons,and juvenile *** in situ CRISPR/Cas9 viral treatment effectively delayed neurodegeneration,attenuated tremor,and bypassed juvenile *** studies demonstrate the potential of CRISPR/Cas9-mediated gene therapy for insertional mutations in the postnatal brain.

关键词： somatic gene editing neurodegenerative disease vibrator mouse model CRISPR/Cas9 Pitpna

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How the dynamics of attachment to the substrate influence stress in metal halide perovskites

APL Energy

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APL Energy 2023年第3期1卷

作者： Gabriel R. McAndrews Boyu Guo Daniel A. Morales Aram Amassian Michael D. McGehee Materials Science and Engineering Program University of Colorado Boulder 4001 Discovery Drive Boulder Colorado 80303 USA Department of Materials Science and Engineering North Carolina State University 911 Partners Way Room 3002 Engineering Building I Raleigh North Carolina 27695 USA Renewable and Sustainable Energy Institute (RASEI) University of Colorado Boulder 4001 Discovery Drive Boulder Colorado 80303 USA Department of Chemical and Biological Engineering University of Colorado Boulder Boulder Colorado 80303 USA

Metal halide perovskites have the potential to contribute to renewable energy needs as a high efficiency, low-cost alternative for photovoltaics. Initial power conversion efficiencies are superb, but improvements to the operational stability of perovskites are needed to enable extensive deployment. Mechanical stress is an important, but often misunderstood factor impacting chemical degradation and reliability during thermal cycling of perovskites. In this manuscript, we find that a commonly used equation based on the coefficient of thermal expansion (CTE) mismatch between perovskite and substrate fails to accurately predict residual stress following solution-based film formation. For example, despite similar CTEs there is a 60 MPa stress difference between narrow bandgap “SnPb perovskite” Cs0.25FA0.75Sn0.5Pb0.5I3 and “triple cation perovskite” Cs0.05MA0.16FA0.79Pb(I0.83Br0.17)3. A combination of in situ absorbance and substrate curvature measurements are used to demonstrate that partial attachment prior to the anneal can reduce residual stress and explain wide stress variations in perovskites.

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Coulombic Condensation of Liquefied Gas Electrolytes for Li Metal Batteries at Ambient Pressure

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Angewandte Chemie 2024年第8期137卷

作者： Yijie Yin John Holoubek Kangwoon Kim Alex Liu Bhargav Bhamwala Shen Wang Bingyu Lu Kunpeng Yu Hongpeng Gao Mingqian Li Ganesh Raghavendran Guorui Cai Weikang Li Ping Liu Ying Shirley Meng Zheng Chen Program of Materials Science and Engineering University of California San Diego La Jolla CA 92093 USA Aiiso Yufeng Li Family Department of Chemical and Nano Engineering University of California San Diego La Jolla CA 92093 USA Sustainable Power and Energy Center University of California San Diego La Jolla CA 92093 USA Pritzker School of Molecular Engineering University of Chicago Chicago IL 60637 USA

The concept of employing highly concentrated electrolytes has been widely incorporated into electrolyte design, due to their enhanced Li-metal passivation and oxidative stability compared to their diluted counterparts. However, issues such as high viscosity and sub-optimal wettability, compromise their suitability for commercialization. In this study, we present a highly concentrated dimethyl ether-based electrolyte that appears as a liquid phase at ambient conditions via Li + - solvents ion-dipole interactions (Coulombic condensation). Unlike conventional high salt concentration ether-based electrolytes, it demonstrates enhanced transport properties and fluidity. The anion-rich solvation structure also contributes to the formation of a LiF-rich salt-derived solid electrolyte interphase, facilitating stable Li metal cycling for over 1000 cycles at 0.5 mA cm −2 , 1 mAh cm −2 condition. When combined with a sulfurized polyacrylonitrile (SPAN) electrode, the electrolyte effectively reduces the polysulfide shuttling effect and ensures stable performance across a range of charging currents, up to 6 mA cm −2 . This research underscores a promising strategy for developing an anion-rich, high concentration ether electrolyte with decreased viscosity, which supports a Li metal anode with exceptional temperature durability and rapid charging capabilities.

关键词： Li/Sulfur Batteries Electrolyte Solvation structure Ion-dipole interaction Fast Charge

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Active Fischer-Tropsch synthesis Fe-Cu-K/SiO_2 catalysts prepared by autocombustion method without a reduction step

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Journal of Energy Chemistry 2018年第2期27卷 432-438页

作者： Suthasinee Pengnarapat Peipei Ai Prasert Reubroycharoen Tharapong Vitidsant Yoshiharu Yoneyama Noritatsu Tsubaki Program in Petrochemistry Faculty of ScienceChulalongkorn University Department of Applied Chemistry School of EngineeringUniversity of Toyama Department of Chemical Technology Faculty of ScienceChulalongkorn University

The purpose of this study was to prepare iron-based catalysts supported on silica by autocombustion method for directly using for Fischer-Tropsch synthesis（FTS） without a reduction step. The effect of different citric acid（CA）：iron nitrate（N） molar ratios and acid types on the FTS performance of catalysts were investigated. The CA：N molar ratios had an important influence on the formation of iron active phases and FTS activity. The iron carbide（FexC）, which is known to be one of the iron active phases, was demonstrated by the X-ray diffraction and X-ray photoelectron spectroscopy. Increasing the CA：N molar ratios up to 0.1 increased CO conversion of catalyst to 86.5%, which was then decreased markedly at higher CA：N molar ratios. An excess of CA resulted in carbon residues covering the catalyst surface and declined FTS activity. The optimal catalyst（CA：N molar ratio = 0.1） achieved the highest CO conversion when compared with other autocombustion catalysts as well as reference catalyst prepared by impregnation method, followed by a reduction step. The autocombustion method had the advantage to synthesize more efficient catalysts without a reduction step. More interestingly, iron-based FTS catalysts need induction duration at the initial stage of FTS reaction even after reduction, because metallic iron species need time to be transformed to FexC. But here, even if without reduction, FexC was formed directly by autocombustion and induction period was eliminated during FTS reaction.

关键词： Fischer-Tropsch synthesis Iron-based catalysts Autocombustion Iron carbide SiO2

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