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Magnetic activated carbon for the removal of methyl orange from water via adsorption and Fenton-like degradation

Particuology 2024年第11期94卷 314-326页

作者： Qianyu Wang Yuming Zhang Yuhua Zheng Emmanuel Oluwaseyi Fagbohun Yanbin Cui State Key Laboratory of Heavy Oil Processing China University of Petroleum(Beijing)Beijing102249China State Key Laboratory of Mesoscience and Engineering Institute of Process EngineeringChinese Academy of SciencesBeijing100190China Laboratory for Nanomaterials and Molecular Plasmonics Department of Chemistry and BiologyToronto Metropolitan University350 Victoria StTorontoONM5B2K3Canada

Water pollution caused by organic dyes is a critical environmental *** activated carbon(AC)is commonly used for dye adsorption,its effectiveness is limited by challenges in separation and *** address these limitations,a convenient recyclable magnetic activated carbon(MAC)was fabricated via co-precipitation and calcination method,serving as adsorbent and catalyst for methyl orange(MO)removal through a Fenton-like degradation *** techniques,including XRD,FTIR,SEM and TEM,confirmed that Fe_(3)O_(4) nanoparticles(10–20 nm)were uniformly dispersed on AC *** MAC maintaining a high surface area(997 m^(2)/g)and pore volume(0.795 cm^(3)/g)and exhibited superparamagnetic properties with a saturated magnetization of 5.52 emu/g,enabling effective separation from aqueous solutions by *** adsorption studies revealed that MO adsorption onto MAC followed pseudo-second-order kinetic and Freundlich isotherm model,with a maximum adsorption capacity of 205 mg/g at 25℃.Thermodynamic analysis showed that the adsorption process was spontaneous and *** degradation of MO and in-situ regeneration of MAC were achieved via Fenton-like reaction using sodium persulfate(PS).Under a PS concentration of 9 mmol/L,the MO removal efficiency near 95%after 60 min,with a total organic carbon(TOC)reduction of 83.1%.The reaction of Fe_(3)O_(4) and oxygen functional groups on AC surface with PS facilitated the generation of SO_(4)^(·-),thereby enhancing catalytic degradation of *** degradation efficiency improved as the temperature increased from 25℃ to 45℃.Cycle tests demonstrated that the MO removal efficiency of MAC remained above 90%after 5 cycles of ***,this study highlights the potential of MAC for efficient removal of organic dyes from water through the coupling of adsorption and Fenton-like degradation,providing a promising solution for addressing water pollution challenges.

关键词： Magnetic activated carbon Methyl orange Adsorption Sodium persulfate Fenton-like degradation

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Exfoliated metal oxide ultrathin nanosheets with supported Pd nanoparticles enabling the one-pot reaction of phenol into caprolactam

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Science China Chemistry 2025年第6期68卷 2636-2643页

作者： Xiaomeng Cheng Bingfeng Chen Lei Zhang Tianjiao Wang Sen Luan Yang Sun Huizhen Liu Buxing Han Beijing National Laboratory for Molecular Sciences CAS Laboratory of Colloid and Interface and Thermodynamics CAS Research/Education Center for Excellence in Molecular Sciences Center for Carbon Neutral Chemistry Institute of Chemistry Chinese Academy of Sciences School of Chemistry and Chemical Engineering University of Chinese Academy of Sciences Shanghai Key Laboratory of Green Chemistry and Chemical Processes State Key Laboratory of Petroleum Molecular & Process EngineeringSchool of Chemistry and Molecular Engineering East China Normal University

Two-dimensional（2D） oxide nanomaterials have great potential for various applications but face challenges due to strong interlayer interactions. In this work, we propose a novel and facile method to exfoliate layered transition metal oxides into ultrathin nanosheets functionalized with phosphate species by the combination of ball-milling and liquid-exfoliation with phosphoric acid. The resulting HNb Mo O6nanosheets with supported Pd nanoparticles displayed excellent catalytic performance in the one-pot conversion of phenol into caprolactam（CPL）, achieving a yield of up to 71.9%. This one-pot route avoids the energy-intensive intermediate separation process in conventional multi-step approaches to CPL. The superior catalytic performance of the catalysts is attributed to the tunable Br?nsted acid/Lewis acid ratio and readily accessible active sites on the ultrathin nanosheets. This research demonstrates a new methodology for constructing ultrathin nanosheets and preparing bifunctional catalysts for tandem reactions, which opens the way for one-pot production of CPL.

关键词： two-dimensional oxides ultrathin nanosheets bifunctional catalysts tandem reaction caprolactam

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Behavior and mechanism of pre-oxidation improvement on fluidization in the fluidized reduction of titanomagnetite

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International Journal of Minerals,Metallurgy and Materials 2024年第11期31卷 2458-2465页

作者： Haoyan Sun Ajala Adewole Adetoro Zhiqiang Wang Qingshan Zhu State Key Laboratory of Mesoscience and Engineering Institute of Process EngineeringChinese Academy of SciencesBeijing 100190China School of Chemical Engineering University of Chinese Academy of SciencesBeijing 100049China Data Science AI modeling CentreUniversity of HullHull HU67RXUK

The direct reduction process is an important development direction of low-carbon ironmaking and efficient comprehensive utilization of poly-metallic iron ore,such as ***,the defluidization of reduced iron particles with a high metallization degree at a high temperature will seriously affect the operation of fluidized bed *** the pre-oxidation enhancing reduction and the particle surface modification of titanomagnetite,the behavior and mechanism of pre-oxidation improvement on fluidization in the fluidized bed reduction of titanomagnetite are systematically studied in this ***-oxidation treatment of titanomagnetite can significantly lower the critical stable reduction fluidization gas velocity to 0.17 m/s,which is reduced by 56%compared to that of titanomagnetite reduction without pre-oxidation,while achieving a metallization degree of>90%,Corresponding to the different reduction fluidization behaviors,three pre-oxidation operation regions have been divided,taking oxidation degrees of 26%and 86%as the *** on the particle surface morphology evolution in the pre-oxidation-reduction process,the relationship between the surface morphology of pre-oxidized ore and the reduced iron with fluidization properties is *** improving method of pre-oxidation on the reduction fluidization provides a novel approach to prevent defluidization by particle surface modification,especially for the fluidized bed reduction of poly-metallic iron ore.

关键词： fluidization direct reduction pre-oxidation titanomagnetite iron whisker

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Tuning the atomic configuration environment of MnN_(4) sites by Co cooperation for efficient oxygen reduction

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Journal of Energy Chemistry 2023年第7期82卷 547-559,I0012页

作者： Jing Wang Haihong Zhong Jun Yang Huiyu Li Pinggui Tang Yongjun Feng Dianqing Li State Key Laboratory of Chemical Resource Engineering Beijing Engineering Center for Hierarchical CatalystsCollege of ChemistryBeijing University of Chemical TechnologyBeijing 100029China College of Science Hainan UniversityHaikou 570228HainanChina State Key Laboratory of Multiphase Complex Systems Institute of Process EngineeringChinese Academy of SciencesBeijing 100190China

Carbon-based N-coordinated Mn(Mn-N_(x)/C)single-atom electrocatalysts are considered as one of the most desirable non-precious oxygen reduction reaction(ORR)candidates due to their insignificant Fenton reactivity,high abundance,and intriguing electrocatalytic ***,current MnN_(x)/C single-atom electrocatalysts suffer from high overpotentials because of their low intrinsic activity and unsatisfactory chemical ***,through an in-situ polymerization-assisted pyrolysis,the Co as a second metal is introduced into the Mn-N_(x)/C system to construct Co,Mn-N_(x)dual-metallic sites,which atomically disperse in N-doped 1D carbon nanorods,denoted as Co,Mn-N/CNR and *** electron microscopy and X-ray absorption spectroscopy(XAS)techniques,we verify the uniform dispersion of CoN4and MnN4atomic sites and confirm the effect of Co doping on the MnN_(4) electronic *** functional theory(DFT)calculations further elucidate that the energy barrier of ratedetermining step(^(*)OH desorption)decreases over the 2 N-bridged MnCoN_(6) moieties related to the pure MnN_(4).This work provides an effective strategy to modulate the local coordination environment and electronic structure of MnN_(4) active sites for improving their ORR activity and stability.

关键词： Dual-atom sites Oxygen reduction reaction M-Nx/C catalysts Coordination environment Electronic structure Synergistic effect

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Reinforcement learning for optimal tracking of large-scale systems with multitime scales

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Science China(Information Sciences) 2023年第7期66卷 5-29页

作者： Jinna LI Hao NIE Tianyou CHAI Frank L.LEWIS School of Information and Control Engineering Liaoning Petrochemical University State Key Laboratory of Synthetical Automation for Process Industries Northeastern University UTA Research Institute University of Texas at Arlington

This paper aims to solve an optimal tracking control(OTC) problem of large-scale systems with multitime scales and coupled subsystems using singular perturbation(SP) theory and reinforcement learning(RL) techniques. A considerable contribution of this paper is the development of a data-driven SP-based RL method for the OTC of unknown large-scale systems with multitime scales. To achieve this, a multitime scale tracking problem was decomposed into a linear quadratic tracker problem for slow subsystems and a dynamical game problem for fast subsystems using the SP theory. Then, the distributed composite feedback controllers were found using a distributed off-policy integral RL algorithm that uses only measured data from the system in real time. Thus, the operational index can follow its prescribed target value via an approximately optimal approach. Theoretical analysis and proof are presented to demonstrate that the sum of the performances of reduced-order subsystems is approximately equal to the performance of the original large-scale system. Finally, numerical and practical examples are provided to validate the effectiveness of the proposed method.

关键词： reinforcement learning singular perturbation multitime scales data-driven control

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Balanced Polysulfide Containment and Lithium Ion Transport in Lithium-Sulfur Batteries via Nitrogen-doped Carbon Hollow Multi-shelled Structures on Modified Separators

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Chemical Research in Chinese Universities 2024年第4期40卷 690-698页

作者： RAO Fu XIAO Qian WEI Yanze WANG Jiangyan YU Ranbo WANG Dan State Key Laboratory of Biochemical Engineering Institute of Process EngineeringChinese Academy of SciencesBeijing100190P.R.China Key Laboratory of Biopharmaceutical Preparation and Delivery Chinese Academy of SciencesBeijing100190P.R.China University of Chinese Academy of Sciences Beijing100049P.R.China Department of Physical Chemistry School of Metallurgical and Ecological EngineeringUniversity of Science&Technology BeijingBeijing100083P.R.China

Representing the next-generation technology in lithium-ion batteries,lithium-sulfur(Li-S)batteries offer increased specific energy without relying on scarce metals like nickel and cobalt,but suffer from a low practical specific energy due to poor conductivity and a short lifespan due to the shuttle effect of *** the confinement of polysulfides and the transport of lithium ions requires highly elaborate modifiers for *** multi-shelled structures(HoMSs)show promise as hierarchical mesostructures for separators,offering multiple shell layers and internal cavities that effectively inhibit polysulfide *** design of these structures is crucial to address these challenges *** this study,nitrogen-doped carbon HoMS(NC HoMS)was created using polymer templates through a precisely controlled polymerization *** featuring NC HoMS-modified separators exhibit improved capacity and cycling stability in comparison to those utilizing commercial ***,triple-shelled NC HoMS strikes a balance in polysulfide containment and lithium ion *** a sulfur loading of 6.34 mg/cm^(2),the Li-S battery can consistently complete 100 charge-discharge cycles,starting with a discharge capacity of 966.4 mA·h/g with a 75.8%capacity retention *** HoMS holds potential as the separator modifier in addressing the polysulfide shuttle problem and facilitating the Li-ion transportation for advanced Li-S batteries.

关键词： Hollow multi-shelled structure Carbon material Li-S battery Separator modification Shuttle effect

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Machine learning-based solubility prediction and methodology evaluation of active pharmaceutical ingredients in industrial crystallization

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Frontiers of Chemical Science and engineering 2022年第4期16卷 523-535页

作者： Yiming Ma Zhenguo Gao Peng Shi Mingyang Chen Songgu Wu Chao Yang Jing-Kang Wang Jingcai Cheng Junbo Gong School of Chemical Engineering and Technology State Key Laboratory of Chemical EngineeringTianjin UniversityTianjin 300072China The Co-Innovation Center of Chemistry and Chemical Engineering of Tianjin Tianjin 300072China Key Laboratory of Green Process and Engineering Institute of Process EngineeringChinese Academy of SciencesBeijing 100190China

Solubility has been widely regarded as a fundamental property of small molecule drugs and drug candidates,as it has a profound impact on the crystallization *** prediction,as an alternative to experiments which can reduce waste and improve crystallization process efficiency,has attracted increasing ***,there are still many urgent challenges thus *** we used seven descriptors based on understanding dissolution behavior to establish two solubility prediction models by machine learning *** solubility data of 120 active pharmaceutical ingredients(APIs)in ethanol were considered in the prediction models,which were constructed by random decision forests and artificial neural network with optimized data structure and model ***,a comparison with traditional prediction methods including the modified solubility equation and the quantitative structure-property relationships model was carried *** highest accuracy shown by the testing set proves that the ML models have the best solubility prediction *** linear regression and stepwise regression were used to further investigate the critical factor in determining solubility *** results revealed that the API properties and the solute-solvent interaction both provide a nonnegligible contribution to the solubility value.

关键词： solubility prediction machine learning artificial neural network random decision forests

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Carbon nanofiber catalysts containing high-entropy metal phosphides with low-content Ru for highly efficient hydrogen evolution reaction

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Rare Metals 2025年第1期44卷 324-335页

作者： Peng Wang Jie Zheng Xue-Hao Li Wen-Bo Cui Jin-Hua Liu Yong Wan Jun Zhang Yusuke Yamauchi Zhong-Li Wang Mang Niu Yun-Ze Long Shandong Key Laboratory of Medical and Health Textile Materials College of PhysicsQingdao UniversityQingdao 266071China Industrial Research Institute of Nonwovens and Technical Textiles Shandong Center for Engineered Nonwovens(SCEN)College of Textiles ClothingQingdao UniversityQingdao 266071China State Key Laboratory of Bio-Fibers and Eco-textiles Institute of Biochemical EngineeringCollege of Materials Science and EngineeringQingdao UniversityQingdao 266071China School of Chemical Engineering and Australian Institute for Bioengineering and Nanotechnology(AIBN) The University of QueenslandBrisbaneQLD 4072Australia Department of Chemical and Biomolecular Engineering Yonsei UniversitySeoul 03722Republic of Korea Department of Materials Process Engineering Graduate School of EngineeringNagoya UniversityNagoya 464-8603Japan Tianjin Key Laboratory of Applied Catalysis Science and Technology School of Chemical Engineering and TechnologyTianjin UniversityTianjin300072China

High-entropy metal phosphide(HEMP)has considerable potential as an electrocatalyst owing to its beneficial properties,including high-entropy alloy synergy as well as the controllable structure and high conductivity of ***,electrospinning and in situ phosphating were employed to prepare three-dimensional(3D)networks of self-supporting HEMP nanofibers with varying degrees of phosphate *** characterizations via X-ray diffraction and X-ray photoelectron spectroscopy,as well as density functional theory calculations,demonstrate that the introduction of phosphorus(P)atoms to HEMP carbon nanofibers mediates their electronic structure,leads to lattice expansion,which in turn enhances their catalytic performance in the hydrogen evolution reaction(HER).Moreover,the formation of metal-P bonds weakens metal-metal interaction and decreases the free energy of hydrogen adsorption,contributing to the exceptional activity observed in the HEMP *** measurements demonstrate that the HEMP-0.75 catalyst with an ultralow loading of 1.22 wt%ruthenium(Ru)exhibits the highest HER catalytic activity and stability in a 1 M KOH electrolyte,achieving a minimal overpotential of 26 mV at a current density of 10 mA·cm^(-2)and Tafel slope of 50.9 mV·dec^(-1).

关键词： High-entropy metal phosphide Electrospinning Hydrogen evolution reaction Self-supporting carbon nanofibers

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engineering W/O/W pickering emulsion for the enhanced antigen delivery and immune responses

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Particuology 2024年第9期92卷 224-233页

作者： Sihua Wu Xiaonan Huang Yin Ma Naoki Asakawa Yufei Xia State Key Laboratory of Biochemical Engineering Institute of Process EngineeringChinese Academy of SciencesBeijing100081China Key Laboratory of Biopharmaceutical Preparation and Delivery Chinese Academy of SciencesBeijing100190China Division of Molecular Science Graduate School of Science and TechnologyGunma University1-5-1Tenjin-choKiryu376-8515Japan Sinovac Biotech Ltd. Beijing100085China School of Chemical Engineering Nanjing Tech UniversityNanjing211816China School of Chemical Engineering University of Chinese Academy of SciencesBeijing100049China

Tumor immunotherapy,particularly cancer vaccines,holds promise for combating cancer by harnessing tailored immune responses against malignant ***,conventional approaches face challenges in efficiently delivering antigens for optimal immune *** adjuvants,like MF59,enhance cellular uptake but struggle to induce robust CD8^(+)T cell ***,we introduce a novel strategy employing a water-in-oil-in-water(W/O/W)multiple Pickering emulsion(mPE)for antigen *** mPE,utilizing biocompatible,pH-sensitive particles,encapsulates antigens within the inner water phase,ensuring enhanced intracellular processing and dictating the intracellular fate of antigens for improved *** vitro and in vivo studies demonstrated that mPEs induced robust dendritic cells activation and antigen cross-presentation,leading to a significantly enhanced immune ***,calcium phosphate-stabilized mPE(CaP-mPE)illustrated the more robust IFN-γ^(+)T cell *** comparison with traditional surfactant-stabilized multiple emulsions,CaP-mPE significantly inhibit tumor growth and effectively prolong the survival of tumor-bearing *** innovative approach offers a promising avenue for the development of effective cancer vaccines with potent cellular immune responses.

关键词： Cancer vaccine Multiple pickeringemulsion Adjuvant Antigen delivery Anti-tumor response

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Facile and effective synthesis strategy for terbium-doped hydroxyapatite toward photoelectric devices and flexible functional fibers

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Rare Metals 2024年第4期43卷 1713-1723页

作者： Xiao-Dong Zhang Kun Nie Zi-Yao Hu Ran-Ran Zhou Xiu-Qiang Duan Wu-Bin Dai Song-Song Nie Song-Jun Yao Luo-Xin Wang Le-Fu Mei Hua Wang Yi-Yi Yao Xiao-Xue Ma Hubei Key Laboratory for New Textile Materials and Applications and State Key Laboratory of New Textile Materials and Advanced Processing Technology School of Materials Science and EngineeringWuhan Textile UniversityWuhan430200China Key Laboratory of Testing and Tracing of Rare Earth Products for State Market Regulation Jiangxi University of Science and TechnologyGanzhou341000China Hubei Key Laboratory of Plasma Chemistry and Advanced Materials and Key Laboratory of Green Chemical Engineering Process of Ministry of Education Wuhan Institute of TechnologyWuhan430205China

As a material with good biocompatibility,hydroxyapatite(HAP)can have optical properties after doping with various rare earth *** a biocompatible fluorescent material,doped HAP could have broad applications in biological probes,drug delivery,optoelectronic materials,fluorescence anti-counterfeiting,and other *** this paper,we put forward the preparation of HAP doped with terbium(Ⅲ)ions(Tb^(3+))by hydrothermal *** controlling the Tb^(3+)doping content in reaction and the reaction time,the changes in HAP's structure,morphology,and luminescence properties under different conditions were *** the doping amount of Tb^(3+)reached an optimal value,the dipole-quadrupole would occur and the concentration would be *** control experiment showed that the optimal Tb3+content was 7.5×10^(-5)mol,which showed the best fluorescence ***,a non-luminous material,was rarely used in the field of fluorescent anti-counterfeiting and photoelectric *** proposed to prepare a luminescent aramid/polyphenylene sulfide(ACFs/PPS)fiber paper and a new light-emitting diode(LED)using the Tb-doped HAP *** composite sample exhibited an excellent stability and fluorescence performance,which also demonstrated a possibility of HAP applications in anticounterfeiting and *** introduction of Tb3+dopant HAP was done to give HAP optical properties and broaden the application range of HAP.

关键词： Hydroxyapatite Rare earth luminescence Photoelectric device Aramid Polyphenylene sulfide fiber paper Luminescent fiber

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