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2D and 3D phthalocyanine covalent organic frameworks for electrocatalytic carbon dioxide reduction

Chinese chemical Letters 2024年

作者： Qi Zhang Bin Han Yucheng Jin Mingrun Li Enhui Zhang Jianzhuang Jiang Beijing Advanced Innovation Center for Materials Genome Engineering Beijing Key Laboratory for Science and Application of Functional Molecular and Crystalline Materials Department of Chemistry and Chemical Engineering School of Chemistry and Biological Engineering University of Science and Technology Beijing Beijing 100083 China

Dimensionality has great influence on the photo/electro-catalysts properties of covalent organic frameworks (COFs) because of the different electronic and porous structures. However, very rare attention has been paid on the dimensionality and function correlations of COF materials. In the present work, one new two-dimensional phthalocyanine COF, namely 2D-NiPc-COF, and one new three-dimensional phthalocyanine COF, namely 3D-NiPc-COF, were fabricated according to the imide reaction between tetraanhydrides of 2,3,9,10,16,17,23,24-octacarboxyphthalocyaninato nickel(II) with [2,2-bipyridine]-5,5-diamine and tetrakis(4-aminophenyl) methane, respectively. The crystalline structures of both COFs are verified by the powder X-ray diffraction analysis, computational simulation, and high resolution transmission electron microscopy measurement. Notably, 3D-NiPc-COF with dispersed conjugated modules has high utilization efficiency of NiPc electroactive sites of 26.8%, almost two times higher than the in-plane stacking 2D-NiPc-COF measured by electrochemical measurement, in turn resulting in its superior electrocatalytic performance with high CO 2 -to-CO Faradaic efficiency over 90% in a wide potential window, a large partial CO current density of −13.97 mA/cm 2 at −0.9 V ( vs . reversible hydrogen electrode) to 2D-NiPc-COF. Moreover, 3D-NiPc-COF has higher turnover number and turnover frequency of 5741.6 and 0.18 s -1 at −0.8 V during 8 h lasting measurement. The present work provides an example for the investigation on the correlation between dimensionality and electrochemical properties of 2D and 3D phthalocyanine COFs.

关键词： Phthalocyanine Dimensionality Covalent organic framework Electrocatalysis Carbon dioxide reduction

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Novel synthesis of manganese cobalt layered double hydroxide and sulfur-doped nickel cobalt layered double hydroxide composite as efficient active material of battery supercapacitor hybrids

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Journal of Energy Storage 2023年 57卷

作者： Hsiao, Yu-Cheng Liao, Chen-Hao Hsu, Chia-Shuo Yougbaré, Sibidou Lin, Lu-Yin Wu, Yung-Fu International PhD Program in Biomedical Engineering College of Biomedical Engineering Taipei Medical University Taipei11031 Taiwan Stanford Byers Center for Biodesign Stanford University CA94305-5428 United States Graduate Institute of Biomedical Optomechatronics College of Biomedical Engineering Taipei Medical University Taipei11031 Taiwan Cell Physiology and Molecular Image Research Center Wan Fang Hospital Taipei Medical University Taipei11696 Taiwan Department of Chemical Engineering and Biotechnology National Taipei University of Technology Taipei Taiwan Department of Chemical Engineering National Taiwan University of Science and Technology Taipei106 Taiwan /Nanoro 03 B.P 7192 Ouagadougou03 Burkina Faso Department of Chemical Engineering Ming Chi University of Technology New Taipei City24301 Taiwan

Nickel and cobalt layered double hydroxide (NiCo-LDH) is one of promising active materials of battery supercapacitor hybrids (BSH) as the clean renewable energy. Designing composites and doping heteroatoms are widely applied to solve poor conductivity, serious agglomeration, and structural defects of NiCo-LDH. In this work, manganese cobalt LDH (MnCo-LDH) is firstly incorporated in sulfur-doped NiCo-LDH (S-NiCo-LDH) on Ni foam (NF) via the hydrothermal process as a binder-free electrode of BSH. Favorable morphology with nanowires covered on the vertical grown nanosheet array is successfully designed for MnCo-LDH/S-NiCo-LDH with the large specific surface area and the well-established pore structure. The specific capacitances (CF) of 681.4, 953.9 and 1581.3 F/g are respectively achieved for the NiCo-LDH, S-NiCo-LDH, MnCo-LDH/S-NiCo-LDH electrodes at the current density of 1 A/g. The larger CF value of MnCo-LDH/S-NiCo-LDH is due to larger conductivity and effective charge transfer paths. A BSH assembled using MnCo-LDH/S-NiCo-LDH/NF and graphene/NF electrodes shows a wide potential window of 1.6 V, a large maximum energy density of 46.6 Wh/kg at 0.8 kW/kg, and an excellent cyclic stability with the CF retention of 81% and the Coulombic efficiency higher than 87% after 10,000 times charge/discharge process at the current density of 7 A/g. © 2022

关键词： Supercapacitor

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Photo-Fenton Induced Multi-Site Peroxymonosulfate Activation Via High Redox Pair Cycling Modified Biochar Nanoarchitecture Nbc@Tio2@Femn for Boosting Degradation of Tetrachloroguaiacol

SSRN

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SSRN 2023年

作者： Bai, He Yang, Yuxiang Zhang, Jining Yang, Yubing Wang, Chengyin Yuan, Hongming Dong, Mengyang Ni, Chaoying School of Chemistry and Molecular Engineering East China University of Science & Technology Shanghai200237 China Ecoenvironmental Protection Research Institute Shanghai Academy of Agricultural Sciences Shanghai201403 China Liuzhou Institute of technology Liuzhou Guangxi545616 China College of Chemistry and Chemical Engineering Yangzhou University Yangzhou225002 China State Key Laboratory of Inorganic Synthesis and Preparative Chemistry Jilin University Changchun130012 China Department of Materials Science and Engineering University of Delaware DE19716 United States

Traditional PMS activation was verified as an efficient method to degrade the refractory pollutant, however, singular active site and total dependence of PMS to promote the circulation of redox pair were the main defects in wastewater treatment. In this work, an attractive strategy was proposed to construct a multi-site and photo-Fenton like nanoarchitecture NBC@TiO2@FeMn (NBTF) with high redox pair cycling rate. Degradation efficiency revealed that the pulp wastewater Tetrachloroguaiacol (TeCG) was removed in the presence of peroxymonosulfate (PMS) and visible light. The multi-sites including NBC and redox pairs (Fe(II)/Fe(III), Mn(II)/Mn(III)/Mn(IV)) play vital roles in degradation. Various influencing factors including pH, temperature and interfering substance were investigated systematically. Quench experiments and EPR spectroscopy revealed that 1O2 and NBTF-4 mediated direct electron transfer played a dominant role in the system. The universality and energy consumption (EEO) of NBTF-4 were also evaluated. Such nanoarchitecture has promising application prospects in emerging contaminants. © 2023, The Authors. All rights reserved.

关键词： Wastewater treatment

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Bifunctional Moni4/Nickel Foam Electro-Catalyst for Ultra-Efficient Oxidation of High-Concentration 5-Hydroxymethylfurfural and Her

SSRN

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SSRN 2024年

作者： Liu, Xiaohui Liu, Hao Xia, Jie Hu, Yongfeng Shakouri, Mohsen Wu, Haoran Zhu, Minghui Guo, Yong Chen, Jingye Chen, Ning Wang, Haifeng Wang, Yanqin Shanghai Key Laboratory of Functional Materials Chemistry Research Institute of Industrial Catalysis School of Chemistry and Molecular Engineering East China University of Science and Technology Shanghai200237 China Sinopec Shanghai Research Institute of Petrochemical Technology Shanghai201208 China Canadian Light Source Inc. 44 Innovation Boulevard SaskatoonSKS7N 2V3 Canada State Key Laboratory of Chemical Engineering East China University of Science and Technology Shanghai China Department of Chemical and Biological Engineering University of Saskatchewan 57 Campus Drive SaskatoonSKS7N 5A9 Canada

The electro-catalytic oxidation of biomass-derived 5-hydroxymethylfurfural (HMF) provides an attractive route to produce 2, 5-furandicarboxylic acid (FDCA) as a substitute for terephthalic acid used in the plastics industry. Herein, we prepared MoNi4 alloy on nickel foam (NF) using a simple hydrothermal method followed by hydrogen reduction. Applied MoNi4/NF as the bifunctional electrodes for the electro-catalytic HMF oxidation reaction (HMFOR) and HER, 98.7% FDCA yield and 97.3% Faraday efficiency (FE) can be achieved even with HMF concentration as high as 200 mM. Notably, no obvious deactivation was observed after ten consecutive cycles. In-situ Raman, XANES and EXAFS results show that the nickel species of MoNi4/NF is first oxidized to Ni3+ species under the applied voltage, and after undergoing the electro-catalytic HMFOR, then reduced to Ni2-δ state (with a valence between 0 and +2) due to the electron-donating effect from Mo. MoNi4/NF with more than one electron transfer between Ni3+ and Ni2-δ during the HMFOR enables it to have excellent electro-catalytic oxidation ability toward HMFOR. © 2024, The Authors. All rights reserved.

关键词： Nickel

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Synthesis of a New Cobalt Based Metal-Organic Framework for Efficient Gas Adsorption and Separation

SSRN

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SSRN 2025年

作者： Tylianakis, Emmanuel Mahmoudi, Ghodrat Doustkhah, Esmail Zangrando, Ennio Batten, Stuart R. White, Jonathan M. Department of Chemistry Faculty of Science University of Maragheh P.O. Box 55136-83111 Maragheh Iran Chemistry Department Faculty of Engineering and Natural Sciences Istinye University Sarıyer Istanbul34396 Turkey Department of Technical Sciences Western Caspian University Baku1001 Azerbaijan Department of Materials Science and Engineering University of Crete Voutes Campus Crete HeraklionGR-70013 Greece Department of Chemical and Pharmaceutical Sciences University of Trieste Via L. Giorgieri 1 Trieste34127 Italy School of Chemistry Monash University VIC3800 Australia BIO-21 Molecular Science and Biotechnology University of Melbourne ParkvilleVIC3052 Australia Koç University Turkey

In this study, we report on a new synthesized open porous metal–organic framework (MOF) of formulation [Co(L)(SCN)(H2O)]n (where HL = N′-(1-(pyridin-3-yl)aminomethylidene)isonicotino-hydrazide), which has been structural characterized by single crystal X-ray analysis. The MOF is a 2D layered structure of 4,4 topology, subsequently expanded to 3D dimensionality by H-bond interactions. Taking into account that the crystal presents a void fraction of 36.3% in the unit cell, the MOF has been investigated by using computational methods for gas adsorption properties. Grand Canonical Monte Carlo simulations at various thermodynamic conditions show that this MOF can effectively adsorb light gases reaching its maximum loading capacity of 2.5 and 19.7 mmol/g for H2 at 298 K and 77 K respectively, and of 4.7, 5.6, 3.3, 4.2 mmol/g for CH4, CO2, N2 and C2H2, respectively at 298 K. Similar simulations on binary mixtures of CO2 with the other non-polar gases examined here, prove that this framework can be used for selective adsorption of CO2 over the other gases. In fact, the selectivity of CO2 in the CO2/CH4, CO2/C2H2, CO2/N2, and CO2/H2 binary mixtures, was calculated to reach a maximum value of 8, 5, 55 and 534, respectively over the other gas. © 2025, The Authors. All rights reserved.

关键词： Binary mixtures

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Soft-lock drawing of super-aligned carbon nanotube bundles for nanometre electrical contacts (vol 17, pg 278, 2022)

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NATURE NANOTECHNOLOGY 2022年第3期17卷 331-331页

作者： Guo, Yunfan Shi, Enzheng Zhu, Jiadi Shen, Pin-Chun Wang, Jiangtao Lin, Yuxuan Mao, Yunwei Deng, Shibin Li, Baini Park, Ji-Hoon Lu, Ang-Yu Zhang, Shuchen Ji, Qingqing Li, Zhe Qiu, Chenguang Qiu, Song Li, Qingwen Dou, Letian Wu, Yue Zhang, Jin Palacios, Tomas Cao, Anyuan Kong, Jing Department of Electrical Engineering and Computer Science Massachusetts Institute of Technology Cambridge MA USA Research Institute of Frontier Technology College of Micro-Nano Electronics Zhejiang University Hangzhou China Taiwan Semiconductor Manufacturing Company (TSMC) Hsinchu Taiwan Key Laboratory of 3D Micro/Nano Fabrication and Characterization of Zhejiang Province School of Engineering Westlake University Hangzhou China School of Materials Science and Engineering Peking University Beijing China Davidson School of Chemical Engineering Purdue University West Lafayette IN USA Department of Mechanical Engineering Massachusetts Institute of Technology Cambridge MA USA Department of Chemistry Purdue University West Lafayette IN USA College of Chemistry and Molecular Engineering Peking University Beijing China Department of Chemical and Biological Engineering Iowa State University Ames IA USA Key Laboratory for the Physics and Chemistry of Nanodevices and Department of Electronics Peking University Beijing China Division of Advanced Nano-Materials Suzhou Institute of Nano-Tech and Nano-Bionics Chinese Academy of Sciences Suzhou China

The assembly of single-walled carbon nanotubes (CNTs) into high-density horizontal arrays is strongly desired for practical applications, but challenges remain despite myriads of research efforts. Herein, we developed a non-destructive soft-lock drawing method to achieve ultraclean single-walled CNT arrays with a very high degree of alignment (angle standard deviation of ~0.03°). These arrays contained a large portion of nanometre-sized CNT bundles, yielding a high packing density (~400 µm−1) and high current carrying capacity (∼1.8 × 108A cm−2). This alignment strategy can be generally extended to diverse substrates or sources of raw single-walled CNTs. Significantly, the assembled CNT bundles were used as nanometre electrical contacts of high-density monolayer molybdenum disulfide (MoS2) transistors, exhibiting high current density (~38 µA µm−1), low contact resistance (~1.6 kΩ µm), excellent device-to-device uniformity and highly reduced device areas (0.06 µm2per device), demonstrating their potential for future electronic devices and advanced integration technologies.

关键词： Locks (fasteners)

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Optimizing Host–Guest Selectivity Through Side-Chain Modification of PillarArenes for O-Ethyltoluene/M-Ethyltoluene Separation

SSRN

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SSRN 2023年

作者： Liu, Yang Fang, Shuai Shao, Li Wang, Jianwei Li, Ming Stoikov, Ivan I. Wang, Mengbin Hua, Bin Stoddart Institute of Molecular Science Department of Chemistry Zhejiang University Hangzhou310058 China Zhejiang-Israel Joint Laboratory of Self-Assembling Functional Materials ZJU-Hangzhou Global Scientific and Technological Innovation Center Zhejiang University Hangzhou311215 China Department of Materials Science and Engineering Zhejiang Sci-Tech University Hangzhou310018 China A.M. Butlerov Chemical Institute Kazan Federal University Kremlevskaya 18 Kazan420008 Russia

Separation of o-ethyltoluene (OET) and m-ethyltoluene (MET) poses a significant challenge in industrial applications due to their closely matched boiling points and similar chemical structures. In this study, we successfully achieve selective adsorpive separation of OET over MET by tuning the host–guest interactions of pillar[6]arenes with ethyltoluene isomers. Experimental results demonstrate that perbromoethylated pillar[6]arene (BrP6) can effectively separate OET and MET, yielding an impressive OET purity of 94.0%. Unlike conventional alkyl chain-modified pillar[6]arenes such as perethylated pillar[6]arene (EtP6) and n-perpropylated pillar[6]arene (PrP6), the improved selectivity of BrP6 arises from the electron-withdrawing effect induced by the bromine atoms present on the side chain. The presence of bromine atoms enhances the electropositivity of the side chain in BrP6, amplifies the contrast in electron cloud density between the branched chains and the cavity of BrP6, and further facilitates the favorable binding of OET with BrP6 due to the concentrated electron density in OET's branched chain. © 2023, The Authors. All rights reserved.

关键词： Supramolecular chemistry

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Cell- And Serum-Derived Proteins Act as DAMPs to Activate RAW 264.7 Macrophages in the Foreign Body Response to Silicone Implants

SSRN

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SSRN 2023年

作者： Blackman, Samuel A. Miles, Dalton Suresh, Joshita Calve, Sarah Bryant, Stephanie J. Department of Chemical and Biological Engineering University of Colorado Boulder 3415 Colorado Ave BoulderCO80309-0596 United States Paul M. Rady Department of Mechanical Engineering University of Colorado Boulder 1111 Engineering Dr BoulderCO80309-0427 United States BioFrontiers Institute University of Colorado Boulder 3415 Colorado Ave BoulderCO80309-0596 United States Materials Science and Engineering Program University of Colorado Boulder 4001 Discovery Dr BoulderCO80300-0613 United States

Protein adsorption after biomaterial implantation is the first stage of the foreign body response (FBR). However, the source(s) of the adsorbed proteins that lead to damaged associated molecular patterns (DAMPs) and induce inflammation has not been fully elucidated. This study examined the effects of different protein sources: cell-derived (from a NIH/3T3 fibroblast cell lysate) and serum-derived (from fetal bovine serum), which were compared to implant-derived proteins (after a 30-min subcutaneous implantation in mice) on activation of RAW 264.7 macrophages cultured in minimal (serum-free) medium. Both cell-derived and serum-derived protein sources when pre-adsorbed to either tissue culture polystyrene or medical grade silicone induced macrophage activation. The combination led to an even higher expression of pro-inflammatory cytokines genes and proteins. Implant-derived proteins on silicone explants induced a rapid inflammatory response that then subsided more quickly and to a greater extent than the studies with in vitro cell-derived or serum-derived protein sources. Proteomic analysis of the implant-derived proteins identified proteins that included cell-derived and serum-derived, but also other protein sources (e.g., extracellular matrix), suggesting the latter may help to temper the inflammatory response in vivo. These findings indicate that both serum-derived and cell-derived proteins can act as DAMPs to drive inflammation in the FBR, but that other protein sources may play an important role in controlling inflammation. © 2023, The Authors. All rights reserved.

关键词： Proteins

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Phase Segregation Dynamics in Mixed-Halide Perovskites Revealed by Plunge-Freeze Cryogenic Electron Microscopy

arXiv

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arXiv 2024年

作者： Fan, Qingyuan Li, Yanbin Vigil, Julian A. Jiang, Zhiqiao Nandi, Partha Colby, Robert Zhang, Chensong Cui, Yi Karunadasa, Hemamala I. Lindenberg, Aaron M. Department of Materials Science and Engineering Stanford University StanfordCA94305 United States SLAC National Accelerator Laboratory Menlo ParkCA94025 United States Stanford PULSE Institute SLAC National Accelerator Laboratory Menlo ParkCA94025 United States Department of Chemistry Stanford University StanfordCA94305 United States Department of Chemical Engineering Stanford University StanfordCA94305 United States Corporate Strategic Research ExxonMobil Research and Engineering 1545 US Highway 22 East AnnandaleNJ08807 United States ExxonMobil Technology and Engineering Company AnnandaleNJ08801 United States Department of Molecular and Cellular Physiology StanfordCA94305 United States

Mixed-halide lead perovskites, with photoexcited charge-carrier properties suitable for high-efficiency photovoltaics, hold significant promise for high-efficiency tandem solar cells. However, phase segregation under illumination, where an iodide-rich phase forms carrier trap states, remains a barrier to applications. This study employs plunge-freeze cryogenic electron microscopy to visualize nanoscale phase segregation dynamics in CsPb(BrxI1–x)3 films. By rapidly freezing the illuminated samples, we preserve transient photoexcited ion distributions for high-resolution structural and compositional analysis at the nanoscale. Cryogenic scanning transmission electron microscopy techniques (EELS, 4D-STEM) captured the dynamics of photo-induced iodine migration from grain boundaries to centers, identified the buildup of anisotropic strain, and captured the heterogeneous evolution of this process within a single grain. These findings provide new insights into microscopic phase segregation mechanisms and their dynamics, enhancing our understanding of mixed-halide perovskite photostability. © 2024, CC BY-NC-ND.

关键词： Grain boundaries

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Cold atmospheric plasma-enabled platelet vesicle incorporated iron oxide nano-propellers for thrombolysis

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materials Today Bio 2023年 23卷 100876页

作者： Jheng, Pei-Ru Chiang, Chia-Che Kang, Jiunn-Horng Fan, Yu-Jui Wu, Kevin C.-W. Chen, Yan-Ting Liang, Jia-Wei Bolouki, Nima Lee, Jyh-Wei Hsieh, Jang-Hsing Chuang, Er-Yuan Graduate Institute of Nanomedicine and Medical Engineering Graduate Institute of Biomedical Materials and Tissue Engineering Institute of Biomedical Optomechatronics International Ph.D. Program in Biomedical Engineering School of Biomedical Engineering College of Biomedical Engineering Professional Master Program in Artificial Intelligence in Medicine College of Medicine Taipei Medical University Taipei11031 Taiwan Department of Physical Medicine and Rehabilitation Taipei Medical University Hospital Taipei Taiwan Institute of Biomedical Engineering & Nanomedicine National Health Research Institute Keyan Road Zhunan Miaoli City350 Taiwan Department of Chemical Engineering National Taiwan University No.1 Sec. 4 Roosevelt Rd Taipei10617 Taiwan Department of Plasma Physics and Technology Faculty of Science Masaryk University Brno Czech Republic Center for Plasma and Thin Film Technologies Ming Chi University of Technology New Taipei City Taiwan Department of Materials Engineering Ming Chi University of Technology New Taipei City Taiwan Cell Physiology and Molecular Image Research Center Taipei Medical University-Wan Fang Hospital Taipei11696 Taiwan

A new approach to treating vascular blockages has been developed to overcome the limitations of current thrombolytic therapies. This approach involves biosafety and multimodal plasma-derived theranostic platelet vesicle incorporating iron oxide constructed nano-propellers platformed technology that possesses fluorescent and magnetic features and manifold thrombus targeting modes. The platform is capable of being guided and visualized remotely to specifically target thrombi, and it can be activated using near-infrared phototherapy along with an actuated magnet for magnetotherapy. In a murine model of thrombus lesion, this proposed multimodal approach showed an approximately 80 % reduction in thrombus residues. Moreover, the new strategy not only improves thrombolysis but also boosts the rate of lysis, making it a promising candidate for time-sensitive thrombolytic therapy. © 2023 The Authors

关键词： Infrared devices

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