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Modular Construction of a Tessellated Octahedron, its Hierarchical Spherical Aggregate Behavior, and Electrocatalytic CO2Reduction Activity

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Angewandte Chemie 2022年第43期134卷

作者： Guotao Wang Yunna Yang Prof. Dr. Hui Liu Dr. Mingzhao Chen Dr. Zhiyuan Jiang Qixia Bai Dr. Jie Yuan Dr. Zhilong Jiang Dr. Yiming Li Prof. Dr. Pingshan Wang School of Metallurgy and Environment Central South University Changsha Hunan 410083 China Chinese National Engineering Research Center for Control & Treatment of Heavy Metal Pollution Changsha Hunan 410083 China Institute of Environmental Research at Greater Bay Area Key Laboratory for Water Quality and Conservation of the Pearl River Delta Ministry of Education Guangzhou Key Laboratory for Clean Energy and Materials Guangzhou University Guangzhou 510006 China Department of Organic and Polymer Chemistry Hunan Key Laboratory of Micro & Nano Materials Interface Science College of Chemistry and Chemical Engineering Central South University Changsha Hunan 410083 China School of Chemistry and Chemical Engineering Henan Normal University Xinxiang Henan 453007 China

Coordination-driven self-assembly has led to the formation of various aesthetical polyhedrons and compounds with advanced functions. Whereas two-dimensional supramolecules with complex and giant skeletons are plentiful, the constructions of polyhedrons are limited by using basic polygons as the panels. Herein, we report the modular synthesis of a tessellated triangle and tessellated octahedron with metal-organic modules as the panels and formed via template-driven self-assembly. These architectures have diameters on the order of 10.9 nm and molecular weights greater than 84 kDa. Interestingly, fiber and spherical-like nanostructures could be formed from the tessellated triangles and octahedrons, respectively, through hierarchical self-assembly. In addition, after hybridization with carbon nanotubes, the supramolecules exhibit electrochemical reduction activity for CO 2 to CO.

关键词： Nano-Fiber Self-Assembly Self-Healing Template Oriented Terpyridine

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Molecular Level Modulation of Anthraquinone-containing Resorcinol-formaldehyde Resin Photocatalysts for H2O2Production with Exceeding 1.2 % Efficiency

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Angewandte Chemie 2022年第12期135卷

作者： Chen Zhao Xinyao Wang Dr. Yanfeng Yin Prof. Wenming Tian Dr. Guang Zeng Dr. Haitao Li Prof. Sheng Ye Prof. Limin Wu Prof. Jian Liu State Key Laboratory of Catalysis Dalian Institute of Chemical Physics Chinese Academy of Sciences 457 Zhongshan Road Dalian 116023 China Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of Sciences Beijing 100049 P. R. China State Key Laboratory of Molecular Reaction Dynamics and the Dynamic Research Center for Energy and Environmental Materials Dalian Institute of Chemical Physics Chinese Academy of Sciences Dalian 116023 China College of Science & School of Plant Protection Anhui Agricultural University Hefei 230036 China Department of Materials Science and State Key Laboratory of Molecular Engineering of Polymers Fudan University 200433 Shanghai China Inner Mongolia University Hohhot Inner Mongolia 010021 P. R. China DICP-Surrey Joint Centre for Future Materials Department of Chemical and Process Engineering and Advanced Technology Institute University of Surrey Guilford Surrey GU27XH UK

Designing polymeric photocatalysts at the molecular level to modulate the photogenerated charge behavior is a promising and challenging strategy for efficient hydrogen peroxide (H 2 O 2 ) photosynthesis. Here, we introduce electron-deficient 1,4-dihydroxyanthraquinone (DHAQ) into the framework of resorcinol-formaldehyde (RF) resin, which modulates the donor/acceptor ratio from the perspective of molecular design for promoting the charge separation. Interestingly, H 2 O 2 can be produced via oxygen reduction and water oxidation pathways, verified by isotopic labeling and in situ characterization techniques. Density functional theory (DFT) calculations elucidate that DHAQ can reduce the energy barrier for H 2 O 2 production. RF-DHAQ exhibits excellent overall photosynthesis of H 2 O 2 with a solar-to-chemical conversion (SCC) efficiency exceeding 1.2 %. This work opens a new avenue to design polymeric photocatalysts at the molecular level for high-efficiency artificial photosynthesis.

关键词： Donor/Acceptor Ratio H2O2 Production Molecular Level Modulation Photocatalysis Resorcinol-Formaldehyde Resin

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Laccase immobilized on magnetic nanoparticles by dopamine polymerization for 4-chlorophenol removal

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Green Energy & Environment 2017年第4期2卷 393-400页

作者： Di Zhang Manfeng Deng Hongbin Cao Songping Zhang He Zhao Beijing Engineering Research Center of Process Pollution Control Division of Environment Technology and Engineering Institute of Process EngineeringChinese Academy of Sciences Collaborative Innovation Center of Chemical Science and Engineering State Key Laboratory of Biochemical Engineering Institute of Process Engineering Chinese Academy of Sciences

In this work, a new immobilization method based on dopamine(DA) self-polymerization was developed for laccase immobilization on magnetic nanoparticles(Fe_3O_4 NPs). To optimize the immobilization condition including reaction pH, DA concentration and enzyme concentration, a central composite response surface method was applied. The optimal condition was determined as p H value of 5.92, laccase concentration of 0.25 mg mL^(-1) and DA concentration of 12.74 mg mL^(-1), under which a high enzyme activity recovery of 88.17% was *** comparing with free laccase, the stabilities of immobilized laccase towards p H, thermostability, storage were enhanced *** 60% of relative activity for immobilized laccase was remained after being incubated for 6 h at 50℃, but the free laccase only remained 25%. After 40 days of storage at 4℃, the laccase immobilized by DA kept about 89% of its original activity, but the free laccase only retained 48%. After recycled 10 times, the relative activity of immobilized laccase still retained 70%. The immobilized laccase was then applied to catalyze the degradation of 4-chlorophenol(4-CP), 86% percentage of 4-CP was removed within 2 h. After degraded 10 times, the relative activity of immobilized laccase still remained 64% of its initial activity, which exhibits an excellent reusability and operational stability.

关键词： Magnetic nanoparticle Laccase Dopamine Immobilization 4-Chlorophenol removal

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Adsorption of Reactive Brilliant Red X-3B from Aqueous Solution by Polypyrrole/Calcium Rectorite Composites: Adsorption Behavior and Mechanism

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IOP Conference Series: Earth and Environmental Science 2020年第1期453卷

作者： Qihua Guo Yaolei Xu Kun Yong Ran Chen Xiaofeng Wang Jinyi Chen School of Chemistry and Environmental Engineering Wuhan Institute of Technology Wuhan China Hubei Environmental Engineering Technology Research Center for Engineering Pollution Control Wuhan China Key Laboratory of Green Chemical Engineering Process of Ministry of Education Wuhan China

In this study, polypyrrole/calcium rectorite clay composites (PPy/REC composites) were prepared by in-situ polymerization of pyrrole monomer to adsorb reactive brilliant red X-3B from aqueous solution. The results of XRD showed that the clay flakes exfoliated in the prepared composites. The SEM results showed that PPy had good dispersibility on clay sheets. The adsorption mainly depended on the initial pH value of the solution, and the optimal adsorption of reactive brilliant red X-3B was achieved when the pH value was 2.0. The removal rate of PPy/REC composite was much higher than that of PPy homopolymer. The adsorption kinetic data of reactive brilliant red X-3B at three initial concentrations (100, 150 and 200 mg/L) were best fitted by the pseudo-second-order model, indicating that the concentration gradient of the adsorbent was the driving force of the adsorption process. The adsorption isotherm accorded with the Langmuir isotherm model, and the maximum adsorption capacity was 232.56 mg/g at 298 K. The PPy/REC composites could be regenerated and reused for 5 continuous adsorption-desorption cycles without losing the removal efficiency of the original reactive brilliant red X-3B. XPS, zeta potential and FT-IR results showed that the removal mechanism of reactive brilliant red X-3B was related to electrostatic interaction and ion exchange.

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Environmental considerations and current status of grouping and regulation of engineered nanomaterials

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Environmental Nanotechnology, Monitoring and Management 2022年 18卷

作者： Tschiche, Harald R. Bierkandt, Frank S. Creutzenberg, Otto Fessard, Valerie Franz, Roland Giese, Bernd Greiner, Ralf Haas, Karl‑Heinz Haase, Andrea Hartwig, Andrea Hund‑Rinke, Kerstin Iden, Pauline Kromer, Charlotte Loeschner, Katrin Mutz, Diana Rakow, Anastasia Rasmussen, Kirsten Rauscher, Hubert Richter, Hannes Schoon, Janosch Schmid, Otmar Som, Claudia M.Tovar, Günter E. Westerhoff, Paul Wohlleben, Wendel Luch, Andreas Laux, Peter German Federal Institute for Risk Assessment (BfR) Department of Chemical and Product Safety Berlin Germany Fraunhofer Institute for Toxicology and Experimental Medicine (ITEM) Hannover Germany French Agency for Food Environmental and Occupational Health & Safety (ANSES) Fougères Laboratory Toxicology of contaminants Unit Fougères France Fraunhofer Institute for Process Engineering and Packaging (IVV) Freising Germany University of Natural Resources and Life Sciences (BOKU) Institute of Safety and Risk Sciences (ISR) Vienna Austria Max Rubner-Institut Department of Food Technology and Bioprocess Engineering Karlsruhe Germany Fraunhofer Institute for Silicate Research (ISC) Würzburg Germany Karlsruhe Institute of Technology (KIT) Institute of Applied Biosciences (IAB) Food Chemistry and Toxicology Germany Fraunhofer Institute for Molecular Biology and Applied Ecology (IME) Schmallenberg Germany Nanid Scientific Consulting Germany National Food Institute Technical University of Denmark Lyngby Denmark German Federal Institute for Risk Assessment (BfR) Research Strategy and Coordination Berlin Germany Charité - Universitätsmedizin Berlin Center for Musculoskeletal Surgery Berlin Germany University Medicine Greifswald Center for Orthopaedics Trauma Surgery and Rehabilitation Medicine Greifswald Germany European Commission Joint Research Centre (JRC) Ispra Italy Fraunhofer IKTS - Institute for Ceramic Technologies and Systems Hermsdorf Germany Berlin Institute of Health at Charité - Universitätsmedizin Berlin Julius Wolff Institute Berlin Germany Comprehensive Pneumology Center (CPC-M) Member of the German Center for Lung Research (DZL) Munich Germany Institute of Lung Health and Immunity Helmholtz Zentrum München – German Research Center for Environmental Health Neuherberg Germany Swiss Federal Laboratories for Materials Science and Technology (Empa) Technology and Society Laboratory St. Gallen Switzerland Fraunhofer Institute for Interfacial Engineering and Biot

This article reviews the current status of nanotechnology with emphasis on application and related environmental considerations as well as legislation. Application and analysis of nanomaterials in infrastructure (construction, building coatings, and water treatment) is discussed, and in particular nanomaterial release during the lifecycle of these applications. Moreover, possible grouping approaches with regard to ecotoxicological and toxicological properties, and the fate of nanomaterials in the environment are evaluated. In terms of potential exposure, the opportunities that arise from leveraging advances in several key areas, such as water treatment and construction are addressed. Additionally, this review describes challenges with regard to the European Commission's definition of ‘nanomaterial’. The revised REACH information requirements, intended to enable a comprehensive risk assessment of nanomaterials, are outlined. © 2022 The Author(s)

关键词： Engineered Nanomaterials Environmental Nanotechnology Grouping Regulation

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Spontaneous Molecular Bromine Production in Sea-Salt Aerosols

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Angewandte Chemie 2024年第39期136卷

作者： Yiqun Cao Zhuo Wang Jiarong Liu Qingxin Ma Shuying Li Jun Liu Hao Li Peng Zhang Tianzeng Chen Yonghong Wang Biwu Chu Xiuhui Zhang Alfonso Saiz-Lopez Joseph S. Francisco Hong He State Key Joint Laboratory of Environment Simulation and Pollution Control Research Center for Eco-Environmental Sciences Chinese Academy of Sciences Beijing 100085 China College of Resources and Environment University of Chinese Academy of Sciences Beijing 100049 China These authorscontributed equally to this work Key Laboratory of Cluster Science Ministry of Education of China School of Chemistry and Chemical Engineering Beijing Institute of Technology Beijing 100081 China Department of Atmospheric Chemistry and Climate Institute of Physical Chemistry Blas Cabrera CSIC Madrid 28006 Spain Department of Earth and Environmental Science and Department of Chemistry University of Pennsylvania Philadelphia Pennsylvania 19104 United States Institute of Urban Environment Chinese Academy of Sciences Xiamen 361021 China

Bromine chemistry is responsible for the catalytic ozone destruction in the atmosphere. The heterogeneous reactions of sea-salt aerosols are the main abiotic sources of reactive bromine in the atmosphere. Here, we present a novel mechanism for the activation of bromide ions (Br − ) by O 2 and H 2 O in the absence of additional oxidants. The laboratory and theoretical calculation results demonstrated that under dark conditions, Br − , O 2 and H 3 O + could spontaneously generate Br and HO 2 radicals through a proton–electron transfer process at the air–water interface and in the liquid phase. Our results also showed that light and acidity could significantly promote the activation of Br − and the production of Br 2 . The estimated gaseous Br 2 production rate was up to 1.55×10 10 molecules cm −2 ⋅ s −1 under light and acidic conditions; these results showed a significant contribution to the atmospheric reactive bromine budget. The reactive oxygen species (ROS) generated during Br − activation could promote the multiphase oxidation of SO 2 to produce sulfuric acid, while the increase in acidity had a positive feedback effect on Br − activation. Our findings highlight the crucial role of the proton-electron transfer process in Br 2 production; here, H 3 O + facilitates the activation of Br − by O 2 , serves as a significant source of atmospheric reactive bromine and exerts a profound impact on the atmospheric oxidation capacity.

关键词： halogens photochemistry environmental chemistry sulfates interfacial oxidation

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Efficient treatment of pure terephthalic acid wastewater with Na 2 S 2 O 8 based on thermal activation

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Environmental Technology & Innovation 2020年 19卷

作者： Xi Chen Zhi-Hui Huang Zhi-Yong Ji Xiao-Fu Guo Li-Ming Zhao Jun-Sheng Yuan State Key Laboratory of Petroleum Pollution Control Beijing 102206 China Engineering Research Center of Seawater Utilization of Ministry of Education School of Chemical Engineering and Technology Hebei University of Technology Tianjin 300130 China Hebei Collaborative Innovation Center of Modern Marine Chemical Technology 300130 Tianjin China National-Local Joint Engineering Laboratory for Energy Conservation in Chemical Process Integration and Resources Utilization School of Chemical Engineering and Technology Hebei University of Technology 300130 Tianjin China

Terephthalic acid (TA) is an important industrial raw material. A large amount of wastewater, mainly containing TA, is generated in the pure terephthalic acid (PTA) producing process. In this study, an advanced oxidation process based on persulfate like Na 2 S 8 O 8 was proposed to degrade TA. The result showed that higher temperature was conducive to degrade TA due to better thermal activation effect, causing more radicals to generate, and the removal ratio of TA reached to a high level of 95.2% at 80 °C. Meanwhile, the TA removal efficiency (maximum 97.4%) at alkaline conditions was better than that in both acidic conditions (about 94%) and neutral condition (85%) at 80 °C. It implied the removal of TA could be carried out effectively in thermal activation mode, and further intensified in the alkaline environment on the basis of thermal activation. The generation of free radicals with thermal activation could be used to explain the degradation mechanism of the organic. Overall, a max total organic carbon (TOC) removal of 97.7% could be achieved, and a probable reaction pathway was proposed with the identification of the intermediate products during TA oxidation. These results could provide a theoretical basis for lower energy consumption and effective treatment of PTA industrial wastewater , which is usually at 75–85 °C and suitable for thermal activation.

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Visible light-driven removal of methylene blue through photocatalytic reaction using CuFe₂O₄/N-TiO₂

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Environmental Challenges 2025年 20卷

作者： Nurhaqi, Abda Ali, Badrut Tamam Ibnu Subagyo, Riki Rasyid, Herlina Maharani, Rani Kartikowati, Christina Wahyu Umaningrum, Dewi Fatmawati, Sri Ediati, Ratna Gunawan, Triyanda Asih, Retno Akhlus, Syafsir Kusumawati, Yuly Department of Chemistry Faculty of Science and Data Analytics Institut Teknologi Sepuluh Nopember Kampus ITS Keputih-Sukolilo East Java Surabaya 60111 Indonesia Research Center for Process and Manufacturing Industry Technology National Research and Innovation Agency 625 Building Technology Energy Cluster PUSPIPTEK South Tangerang Banten 15314 Indonesia Department of Chemistry Faculty of Mathematics and Natural Sciences Hasanuddin University South Sulawesi Makassar 90245 Indonesia Department of Chemistry Faculty of Mathematics and Natural Sciences Universitas Padjadjaran Jatinangor West Java Sumedang 45363 Indonesia Department of Chemical Engineering Brawijaya University East Java Malang 65145 Indonesia Department of Chemistry Faculty of Mathematics and Natural Sciences Universitas Lambung Mangkurat Jl. Ahmad Yani Km. 35 8 Banjarbaru East Kalimantan 70714 Indonesia Department of Physics Faculty of Science and Data Analytics Institut Teknologi Sepuluh Nopember Jl. Arif Rahman Hakim Kampus ITS Keputih-Sukolilo Surabaya 60111 Indonesia

CuFe2O4/N-TiO2 photocatalyst was used for the removal of methylene blue (MB) dye under visible light. Various characterisation techniques were performed, including X-ray diffraction (XRD), UV Diffuse Reflectance Spect... 详细信息

CuFe₂O₄/N-TiO₂ photocatalyst was used for the removal of methylene blue (MB) dye under visible light. Various characterisation techniques were performed, including X-ray diffraction (XRD), UV Diffuse Reflectance Spectroscopy (UV-DRS), scanning electron microscopy (SEM) and vibrating-sample magnetometry (VSM). UV-DRS results showed a reduced TiO₂ bandgap after nitrogen doping and addition of CuFe₂O₄. The photocatalytic removal of MB was achieved 98.7 % after 180 min irradiation for nitrogen doped TiO₂ (N-TiO₂). The addition of CuFe₂O₄ improved the magnetic properties. The optimal composition of 5 % CuFe₂O₄/N-TiO₂, exhibited good magnetic properties and 97.56 % of MB removal efficiency. The 5 % CuFe₂O₄/N-TiO₂ also exhibit maintaining over 90 % of MB removal efficiency across three cycles process. The proposed degradation pathway was presented based on Liquid Chromatography Mass Spectrophotometer (LCMS). Based on the obtained results, 5 % CuFe₂O₄/N-TiO₂ can be proposed as photocatalyst for MB removal and its magnetic properties is beneficial for quick separation from the solution after photocatalytic process. © 2025 The Authors

关键词： CuFe2O4/N-TiO2 Magnetic photocatalytic Methylene blue removal Visible Light driven Wastewater treatment

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Back Cover: Promoter-controlled Synthesis and Conformational Analysis of Cyclic Mannosides up to a 32-mer (Angew. Chem. Int. Ed. 43/2023)

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Angewandte Chemie International Edition 2023年第43期62卷

作者： Dr. Xiaona Li Cristina Di Carluccio He Miao Lvfeng Zhang Jintao Shang Prof. Dr. Antonio Molinaro Prof. Dr. Peng Xu Prof. Dr. Alba Silipo Prof. Dr. Biao Yu Prof. Dr. You Yang Shanghai Frontiers Science Center of Optogenetic Techniques for Cell Metabolism Shanghai Key Laboratory of New Drug Design Engineering Research Center of Pharmaceutical Process Chemistry Ministry of Education School of Pharmacy East China University of Science and Technology 130 Meilong Road Shanghai 200237 China Department of Chemical Sciences University of Naples Federico II Via Cintia 4 80126 Napoli Italy Department of Chemistry School of Science Osaka University 1-1 Osaka University Machikaneyama Toyonaka Osaka 560-0043 Japan State Key Laboratory of Bioorganic and Natural Products Chemistry Shanghai Institute of Organic Chemistry Chinese Academy of Sciences 345 Lingling Road Shanghai 200032 China

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Rapid Access to Ordered Mesoporous Carbons for chemical Hydrogen Storage

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Angewandte Chemie 2021年第41期133卷

作者： Dr. Uiseok Jeong HyeonJi Kim Dr. Sreerangappa Ramesh Dr. Nesibe A. Dogan Sirinapa Wongwilawan Sungsu Kang Jungwon Park Prof. Eun Seon Cho Prof. Cafer T. Yavuz Department of Chemical and Biomolecular Engineering Korea Advanced Institute of Science and Technology (KAIST) Daejeon 34141 Republic of Korea Graduate School of EEWS Korea Advanced Institute of Science and Technology (KAIST) Daejeon 34141 Republic of Korea Department of Bioproducts and Biosystems School of Chemical Engineering Aalto University P.O. Box 16300 00076 Aalto Finland School of Chemical and Biological Engineering and Institute of Chemical Process Seoul National University Seoul 08826 Republic of Korea Center for Nanoparticle Research Institute for Basic Science (IBS) Seoul 08826 Republic of Korea Advanced Membranes & Porous Materials Center Physical Science & Engineering (PSE) King Abdullah University of Science and Technology (KAUST) Thuwal 23955 Saudi Arabia KAUST Catalysis Center Physical Science & Engineering (PSE) King Abdullah University of Science and Technology (KAUST) Thuwal 23955 Saudi Arabia

Ordered mesoporous carbon materials offer robust network of organized pores for energy storage and catalysis applications, but suffer from time-consuming and intricate preparations hindering their widespread use. Here we report a new and rapid synthetic route for a N-doped ordered mesoporous carbon structure through a preferential heating of iron oxide nanoparticles by microwaves. A nanoporous covalent organic polymer is first formed in situ covering the hard templates of assembled nanoparticles, paving the way for a long-range order in a carbonaceous nanocomposite precursor. Upon removal of the template, a well-defined cubic mesoporous carbon structure was revealed. The ordered mesoporous carbon was used in solid state hydrogen storage as a host scaffold for NaAlH 4 , where remarkable improvement in hydrogen desorption kinetics was observed. The state-of-the-art lowest activation energy of dehydrogenation as a single step was attributed to their ordered pore structure and N-doping effect.

关键词： hard template synthesis hydrogen storage microwave heating nanoconfinement nitrogen doped carbon

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