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chemical and engineering bases for green H2O2 production and related oxidation and ammoximation of olefins and analogues

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National Science Review 2024年第8期11卷 304-321页

作者： Minghua Qiao Xinggui Zhou Zexue Du Peng Wu Baoning Zong Collaborative Innovation Center of Chemistry for Energy Materials Department of Chemistry and Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials Fudan University State Key Laboratory of Chemical Engineering East China University of Science and Technology State Key Laboratory of Petroleum Molecular& Process Engineering Research Institute of Petroleum ProcessingSINOPEC State Key Laboratory of Petroleum Molecular& Process Engineering School of Chemistry and Molecular Engineering East China Normal University

Plastics,fibers and rubber are three mainstream synthetic materials that are essential to our daily lives and contribute significantly to the quality of our *** production of the monomers of these synthetic polymers usually involves oxidation or ammoximation reactions of olefins and ***,the utilization of C,O and N atoms in current industrial processes is <80%,which represents the most environmentally polluting processes for the production of basic *** innovation and integration of catalytic materials,new reaction pathways,and reaction engineering,the research Institute of Petroleum processing,Sinopec Co.,Ltd.（RIPP） and its collaborators have developed unique H2O2-centered oxidation/ammoximation technologies for olefins and analogues,which has resulted in a ￥500 billion emerging industry and driven trillions of ￥s' worth of downstream *** chemical and engineering bases of the production technologies mainly involve the integration of slurry-bed reactors and microsphere catalysts to enhance H2O2production,H2O2propylene/chloropropylene epoxidation for the production of propylene oxide/epichlorohydrin,and integration of H2O2cyclohexanone ammoximation and membrane separation to innovate the caprolactam production *** review briefly summarizes the whole process from the acquisition of scientific knowledge to the formation of an industrial production technology by ***,the scientific frontiers of H2O2production and related oxidation/ammoximation processes of olefins and analogues are reviewed,and new technological growth points are envisaged,with the aim of maintaining China's standing as a leader in the development of the science and technologies of H2O2production and utilization.

关键词： hydrogen peroxide oxidation ammoximation propylene oxide epichlorohydrin cyclohexanone oxime

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Synergistic optimization framework for the process synthesis and design of biorefineries

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Frontiers of chemical Science and engineering 2022年第2期16卷 251-273页

作者： Nikolaus IVollmer Resul Al Krist V.Gernaey Gürkan Sin Process and Systems Engineering(PROSYS)Research Center Department of Chemical and Biochemical EngineeringTechnical University of Denmark2800 Kgs.LyngbyDenmark Novo Nordisk A/S 2880 BagsværdDenmark

The conceptual process design of novel bioprocesses in biorefinery setups is an important task,which remains yet challenging due to several *** propose a novel framework incorporating superstructure optimization and simulation-based optimization *** this context,several approaches for superstructure optimization based on different surrogate models can be *** means of a case study,the framework is introduced and validated,and the different superstructure optimization approaches are *** results indicate that even though surrogate-based optimization approaches alleviate the underlying computational issues,there remains a potential issue regarding their *** development of appropriate surrogate models,comprising the selection of surrogate type,sampling type,and size for training and cross-validation sets,are essential *** this aspect,satisfactory validation metrics do not ensure a successful outcome from its embedded use in an optimization ***,the framework’s synergistic effects by sequentially performing superstructure optimization to determine candidate process topologies and simulationbased optimization to consolidate the process design under uncertainty offer an alternative and promising *** findings invite for a critical assessment of surrogatebased optimization approaches and point out the necessity of benchmarking to ensure consistency and quality of optimized solutions.

关键词： biotechnology surrogate modelling superstructure optimization simulation-based optimization process design

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Porous 3D carbon-based materials:An emerging platform for efficient hydrogen production

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Nano research 2023年第1期16卷 127-145页

作者： Fangyi Li Jizhou Jiang Jiamei Wang Jing Zou Wei Sun Haitao Wang Kun Xiang Pingxiu Wu Jyh-Ping Hsu School of Environmental Ecology and Biological Engineering School of Chemistry and Environmental EngineeringKey Laboratory of Green Chemical Engineering Process of Ministry of EducationEngineering Research Center of Phosphorus Resources Development and Utilization of Ministry of EducationWuhan Institute of TechnologyWuhan 430205China Semiconductor Electronic Special Gas of Hubei Engineering Research Center Jingzhou 434000China Department of Chemical Engineering “National Taiwan University”Taipei 10617

Due to their unique properties and uninterrupted breakthrough in a myriad of clean energy-related applications,carbon-based materials have received great ***,the low selectivity and poor conductivity are two primary difficulties of traditional carbon-based materials(zero-dimensional(0D)/one-dimensional(1D)/two-dimensional(2D)),enerating inefficient hydrogen production and impeding the future commercialization of carbon-based *** improve hydrogen production,attempts are made to enlarge the surface area of porous three-dimensional(3D)carbon-based materials,achieve uniform interconnected porous channels,and enhance their stability,especially under extreme *** this review,the structural advantages and performance improvements of porous carbon nanotubes(CNTs),g-C_(3)N_(4),covalent organic frameworks(COFs),metal-organic frameworks(MOFs),MXenes,and biomass-derived carbon-based materials are firstly summarized,followed by discussing the mechanisms involved and assessing the performance of the main hydrogen production *** include,for example,photo/electrocatalytic hydrogen production,release from methanolysis of sodium borohydride,methane decomposition,and *** role that the active sites of porous carbon-based materials play in promoting charge transport,and enhancing electrical conductivity and stability,in a hydrogen production process is *** current challenges and future directions are also discussed to provide guidelines for the development of next-generation high-efficiency hydrogen 3D porous carbon-based materials prospected.

关键词： porous three-dimensional(3D)carbon-based materials hydrogen production advanced synthesis

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Green innovation unleashed:Harnessing tungsten-based nanomaterials for catalyzing solar-driven carbon dioxide conversion

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Chinese chemical Letters 2025年第2期36卷 108-117页

作者： Weidan Meng Yanbo Zhou Yi Zhou State Environmental Protection Key Laboratory of Environmental Risk Assessment and Control on Chemical Process East China University of Science and TechnologyShanghai 200237China National Engineering Research Center of Industrial Wastewater Detoxication and Resource Recovery East China University of Science and TechnologyShanghai 200237China Shanghai Engineering Research Center for Multi-media Environmental Catalysis and Resource Utilization East China University of Science and TechnologyShanghai 200237China Shanghai Institute of Pollution Control and Ecological Security Shanghai 200092China

Carbon dioxide photocatalytic reduction (CO_(2)-PR) is an efficient method for controlling CO_(2)emissions and generating cleaner energy while mitigating global *** oxides (WxOy) have attracted considerable attention for CO_(2)-PR due to their excellent spectral ***,comprehensive reviews are lacking on the use of WxOyfor CO_(2)-***,this review provides a detailed summary of t research progress made with WxOy-based catalysts in CO_(2)-*** also explains the fundamental principles of CO_(2)-PR and evaluates key performance indicators that affect the activity of WxOy-based photocatalysts,including yield,selectivity,stability,and apparent quantum ***,this review explores opportunities for synthesizing high-performance WxOy-based photocatalysts and highlights their potential for the green preparation of C1/C2 products through CO_(2)-*** innovative strategies aim to address the challenges and pressures associated with energy and environmental issues,particularly by enhancing artificial photosynthesis efficiency.

关键词： Carbon dioxide photoreduction Tungsten-based nanocatalyst Mechanism Performance evaluation Selectivity

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A pyrazine based metal-organic framework for selective removal of copper from strongly acidic solutions

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Frontiers of Environmental Science & engineering 2023年第3期17卷 75-86页

作者： Jiachuang Shao Penghui Shao Mingming Peng Min Li Ziwei Yao Xiuqin Xiong Caiting Qiu Yufan Zheng Liming Yang Xubiao Luo Key Laboratory of Jiangxi Province for Persistent Pollutants Control and Resources Recycle National-Local Joint Engineering Research Center of Heavy Metals Pollutants Control and Resource utilizationNanchang Hangkong UniversityNanchang 330063China Department of Chemical Engineering Chongqing University of Science and TechnologyChongqing 401331China

The selective capture of copper from strongly acidic solutions is of vital importance from the perspective of sustainable development and environmental *** organic frameworks(MOFs)have attracted the interest of many scholars for adsorption due to their fascinating physicochemical characteristics,including adjustable structure,strong stability and ***,pz-UiO-66 containing a pyrazine structure is successfully synthesized for the efficient separation of copper from strongly acidic *** copper removal at low pH values is accomplished by using this material that is not available in previously reported metal–organic ***,the material exhibits excellent adsorption capacity,with a theoretical maximum copper uptake of 247 mg/*** proven by XPS and FT-IR analysis,the coordination of pyrazine nitrogen atoms with copper ions is the dominant adsorption mechanism of copper by *** work provides an opportunity for efficient and selective copper removal under strongly acidic conditions,and promises extensive application prospects for the removal of copper in the treatment for acid metallurgical wastewater.

关键词： Pyrazine Metal-organic frameworks Copper removal Strong acidity High selectivity

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Magnetic Porous Material Derived from Ni-MOF for the Removal of Tetracycline from Aqueous Solution

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ACS Applied Nano Materials 2024年第7期7卷 7614-7621页

作者： Xue, Yuhui Wang, Jingjing Wang, Meng Li, Jiang Wang, Kefu Hassan, Afaq Guo, Changyan Wang, Jide Xinjiang Key Laboratory of Oil and Gas Fine Chemicals College of Chemistry and Chemical Engineering Xinjiang University Urumqi 830046 China Technical Center of Urumqi Customs Urumqi 830063 China Xinjiang Uygur Autonomous Region Center for Disease Control and Prevention Urumqi 830002 China Department of Process Engineering and Chemical Technology Chemical Faculty Gdansk University of Technology Gdansk 80-233 Poland

The efficient removal of antibiotic residues from aqueous solution is very important for water security. Studies have found that adsorption is widely used for the removal of antibiotics due to its cost-effectiveness, low energy consumption, simplicity of operation, and environmental friendliness. In this study, a novel magnetic porous carbon adsorbent (Ni-MPC-400) with a high adsorption capacity and saturation magnetization was synthesized via direct carbonization of Ni-MOF at 400 °C pyrolysis temperature and used to efficiently remove tetracycline from an aqueous solution. Adsorption experiments showed that Ni-MPC-400 exhibited excellent tetracycline adsorption capacity (441.51 mg·g^-1) from the aqueous solution. Possible adsorption mechanisms were proposed through characterization and analysis. The adsorption mechanisms mainly involved π-π interactions, hydrogen bonding, metal-organic complexation, and pore filling effects. In addition, Ni-MPC-400 showed rapid and sufficient adsorption at a low concentration of tetracycline (5 mg·L^-1) and good adsorption performance over a wide pH range. In addition, the material has been tested to have good immunity to interference and regenerative capacity, demonstrating a potential application in the removal of tetracycline contaminants from aqueous solutions. © 2024 American chemical Society.

关键词： aqueous solutions magnetic porous material Ni-MOF Ni-MPC-400 tetracycline

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Oxygen vacancy engineering for tuning the catalytic activity of LaCoO_(3) perovskite

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Journal of Rare Earths 2024年第3期42卷 506-514,I0003页

作者： Jeong Hyun Cho Minjae Kim Inchan Yang Kyung Tae Park Chang Houn Rhee Hai Woong Park Ji Chul Jung Department of Chemical Engineering Myongji UniversityYongin 17058Republic of Korea Institute of Advanced Composite Materials Korea Institute of Science and TechnologyWanju-gunJeollabuk-do 55324Republic of Korea Iron&Steel Process Engineering Research Group POSCOPohang 37859Republic of Korea Hydrogen Research Center Research Institute of Industrial Science&Technology(RIST)Pohang 37673Republic of Korea

Herein, we attempted to engineer oxygen vacancies on the surface of LaCoO_(3) perovskite through simple post-treatments(acid or reductive thermal treatments). Acid treatment induces oxygen vacancies through the selective etching of the La cations, whereas thermal treatment in a reducing atmosphere generates oxygen vacancies by directly removing lattice oxygen. The characterization results confirm that the number of surface oxygen vacancies, which are crucial in various catalytic oxidation reactions,considerably increases in the LaCoO_(3) catalysts treated with acid or reducing gas. Acid treatment enriches the oxygen vacancies while maintaining the structure of the LaCoO_(3) catalysts, which can not be achieved through reductive thermal treatment. Therefore, the acid treatment is considered a promising technique for oxygen vacancy engineering of perovskite catalysts for tuning their catalytic activities. Furthermore,the catalytic activities of the posttreated LaCoO_(3) catalysts for CO oxidation were evaluated and are noted to be considerably better than those of the pristine LaCoO_(3) catalyst due to their abundant oxygen vacancies. Consequently, we conclude that the oxygen vacancies of perovskite catalysts can be effectively engineered via two simple methods and play a significant role in CO oxidation.

关键词： LaCoO_(3)perovskite Acid treatment Reductive thermal treatment Oxygen vacancy CO oxidation Rare earths

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Oxidative torrefaction of woody biomass: introducing a modified severity factor

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Biomass Conversion and Biorefinery 2025年第6期15卷 9353-9366页

作者： Devaraja, Udya Madhavi Aravindi Dissanayake, Chamini Lakshika Wickramarathna Gunarathne, Duleeka Sandamali Chen, Wei-Hsin Department of Chemical and Process Engineering University of Moratuwa Moratuwa10400 Sri Lanka Department of Aeronautics and Astronautics National Cheng Kung University Tainan701 Taiwan Research Center for Smart Sustainable Circular Economy Tunghai University Taichung407 Taiwan Department of Mechanical Engineering National Chin-Yi University of Technology Taichung411 Taiwan

Torrefaction experiments of Rubberwood and Gliricidia were conducted at 250–300 °C for 30–60 min in a 3–9% oxygen environment to study the oxidative torrefaction behavior. The higher heating value of the torrefied Rubberwood increased from 18.9 to 24.68 MJ/kg and from 19.46 to 23.19 MJ/kg for Gliricidia under the most severe oxidative conditions. Effects of torrefaction conditions on the solid yield, VM removal, C enhancement, HHV enhancement, and energy yield were modeled using response surface methodology, and temperature and oxygen concentration mainly affected the torrefied biomass properties. Rubberwood recorded a significantly greater energy mass co-benefit index (EMCI) than Gliricidia. EMCI of oxidative torrefaction of Gliricidia showed no significant difference from that of inert conditions. A new severity factor was introduced for oxidative torrefaction, and the normalized severity factor showed a linear correlation with torrefied biomass properties, which could facilitate oxidative torrefaction modeling. © The Author(s), under exclusive licence to Springer-Verlag GmbH Germany, part of Springer Nature 2024.

关键词： Biomass

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Efficient chemical Synthesis and Folding of Mirror-Image Tropomyosin Receptor Kinase A Using the Strategy of Removable Glycosylation Modification

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Chinese Journal of Chemistry 2024年第19期42卷 2316-2322页

作者： Tongyue Wang Weiwei Shi Guo-Chao Chu Yi-Ming Li Ministry of Education Key Laboratory of Bioorganic Phosphorus Chemistry and Chemical Biology Department of ChemistryTsinghua UniversityBeijing 100084China School of Food and Biological Engineering Engineering Research Center of Bio-processMinistry of EducationKey Laboratory of Animal Source of Anhui ProvinceHefei University of TechnologyHefeiAnhui 230009China

Comprehensive Summary The strategy of removable glycosylation modification was used to overcome the low-efficiency problem encountered in the chemical synthesis of the mirror-image D-version of the immunoglobulin(Ig)-like domain of tropomyosin receptor kinase A(DlgCTrkA),a protein molecule needed for mirror-image screening of D-peptide ligands targeting this cell membrane *** was found that O-linked-β-N-acetyl-D-glucosamine(O-GlcNAc)modification at^(D)Ser^(312),or^(D)Ser^(320)can significantly improve the efficiency of DlgCTrkA synthesis and folding,while O-GlcNAc modification at^(D)Ser^(330)showed barely any *** study provides a new example demonstrating the power of the removable glycosylation modification strategy in the chemical synthesis and folding of difficult-to-obtain *** also presents evidence that removable glycosylation modification at different sites would significantly affect the efficiency of protein folding promoted by this strategy.

关键词： chemical protein synthesis Removable glycosylation modification Synthetic methods Protein folding D-protein

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Very low Ru loadings boosting performance of Ni-based dual-function materials during the integrated CO_(2)capture and methanation process

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Journal of Energy Chemistry 2025年第3期102卷 309-328页

作者： Anastasios I.Tsiotsias Eleana Harkou Nikolaos D.Charisiou Victor Sebastian Dhanaji R.Naikwadi Bart van der Linden Atul Bansode Dragos Stoian George Manos Achilleas Constantinou Maria A.Goula Laboratory of Alternative Fuels and Environmental Catalysis(LAFEC) Department of Chemical EngineeringUniversity of Western MacedoniaKozani 50100Greece Department of Chemical Engineering Cyprus University of Technology57 Corner of Athinon and AnexartisiasLimassol 3036Cyprus Department of Chemical Engineering and Environmental Technology Universidad de ZaragozaCampus RióEbro-Edificio I+DZaragoza 50018Spain Instituto de Nanociencia y Materiales de Aragón(INMA) Universidad de ZaragozaCSICc/Mariáde Luna 3Zaragoza 50018Spain Networking Research Center on Bioengineering Biomaterials and NanomedicineCIBERBBN28029 MadridSpain Department of Chemical Engineering Delft University of TechnologyVan der Massweg 9Delft 2629 HZthe Netherlands The Swiss-Norwegian Beamlines(SNBL) European Synchrotron Radiation Facility(ESRF)Grenoble 38000France Department of Chemical Engineering University College LondonLondon WCIE7JEUnited Kingdom Centre for Research&Technology Hellas(CERTH) Chemical Process and Energy Resources Institute(CPERI)52 Egialias strMaroussiAthens 15125Greece School of Science and Technology Hellenic Open UniversityParodos Aristotelous 18Patras 26335Greece

Herein,the effect of the Ru:Ni bimetallic composition in dual-function materials(DFMs)for the integrated CO_(2)capture and methanation process(ICCU-Methanation)is systematically evaluated and combined with a thorough material characterization,as well as a mechanistic(in-situ diffuse reflectance infrared fourier-transform spectroscopy(in-situ DRIFTS))and computational(computational fluid dynamics(CFD)modelling)investigation,in order to improve the performance of Ni-based *** bimetallic DFMs are comprised of a main Ni active metallic phase(20 wt%)and are modified with low Ru loadings in the 0.1-1 wt%range(to keep the material cost low),supported on Na_(2)O/Al_(2)O_(3).It is shown that the addition of even a very low Ru loading(0.1-0.2 wt%)can drastically improve the material reducibility,exposing a significantly higher amount of surface-active metallic sites,with Ru being highly dispersed over the support and the Ni phase,while also forming some small Ru *** manifests in a significant enhancement in the CH_(4)yield and the CH_(4)production kinetics during ICCU-Methanation(which mainly proceeds via formate intermediates),with 0.2 wt%Ru addition leading to the best *** bimetallic DFM also shows high stability and a relatively good performance under an oxidizing CO_(2)capture *** formation rate of CH_(4)during hydrogenation is then further validated via CFD modelling and the developed model is subsequently applied in the prediction of the effect of other parameters,including the inlet H_(2)concentration,inlet flow rate,dual-fu nction material weight,and reactor internal diameter.

关键词： Dual-function materials Integrated CO_(2)capture and methanation Bimetallic materials Nickel-ruthenium Reducibility in-situ DRIFTS CFD modelling

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