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Development of anti-corrosive coating on AZ31 Mg alloy modified by MOF/LDH/PEO hybrids

Journal of Magnesium and Alloys 2024年第2期12卷 586-607页

作者： Muhammad Ali Khan Ananda Repycha Safira Mohammad Aadil Mosab Kaseem Corrosion and electrochemistry Laboratory Department of Nanotechnology and Advanced Materials EngineeringSejong UniversitySeoul 05006Republic of Korea

The self-assembly of hybrid inorganic-organic materials on stationary platforms plays a critical role in improving their structural stability and wide usability.In this work,a novel two-step hydrothermal approach is proposed for synthesizing stable and advanced hybrid coatings on metal-oxide platforms through the surface modification of layered double hydroxide(LDH)films using novel metal-organic frameworks(MOFs).Initially,Mg-Al LDH nanocontainers,grown on a magnesium oxide layer produced through plasma electrolytic oxidation(PEO)of AZ31 Mg alloy substrate,were intercalated with cobalt via an oxidation route,providing the metallic coordination center for the MOF formation.In the subsequent step,a pioneering technique is introduced,utilizing tryptophan as the organic linker for the first time at a pH of 10.The self-assembly of cobalt-tryptophan complex,driven by the strong bonding between electrophilic sites of monomers and nucleophilic sites,facilitated the formation of a MOF network having a cloud-like structure on the surface of MgAl LDH's film.The resulting MOF-LDH encapsulation containers demonstrate exceptional electrochemical stability when exposed to a 3.5 wt.%NaCl solution,surpassing the performance of PEO and pure LDH coatings.This enhanced stability is attributed to the development of a dense top layer and a stable composition within the self-assembled MOF,effectively sealing flaws and preventing the infiltration of corrosive ions into the underlying metallic substrate.The formation mechanism of MOFs on LDH galleries is investigated using density functional theory calculations.

关键词： Mg alloy Layered double hydroxide Metal-organic frameworks Corrosion DFT

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Enhanced electrochemical and photocatalytic performance achieved through dual incorporation of SnO2 and WO3 nanoparticles into LDH layer fabricated on PEO-coated AZ31 Mg alloy

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Journal of Magnesium and Alloys 2024年第5期12卷 1880-1898页

作者： Muhammad Ali Khan Ananda Repycha Safira Mosab Kaseem Arash Fattah-alhosseini Corrosion and electrochemistry Laboratory Department of Nanotechnology and Advanced Materials Engineering Sejong University Department of Materials Engineering Faculty of Engineering Bu-Ali Sina University

This study explores the potential of LDH flakes decorated with metallic oxide nanoparticles to function as both anti-corrosion barriers against chloride anions and heterogeneous photocatalysts for tetracycline degradation under visible light. The process involves modifying the primarily MgO-based inorganic porous film by growing a MgFe LDH film, followed by the individual and dual incorporation of SnO2and WO3nanoparticles. The dual incorporation of these nanoparticles into the LDH matrix leads to synergistic interactions, effectively sealing pre-existing defects within LDH flakes and facilitating the in-situ formation of catalytic sites through oxidation and the induction of surface oxygen vacancy defects, which synergistically contribute to the enhancement of both electrochemical and photocatalytic activities. The enhanced electrochemical stability is reflected in a significant reduction in corrosion current density by 4 orders of magnitude compared to unmodified porous film. Additionally, the decorated film demonstrates sustained photocatalytic functionality, achieving significant degradation（95.5%） of tetracycline within two hours. This study presents a novel approach, highlighting the dual effectiveness of LDHs decorated by dual metal oxides as an anti-corrosive agent and photocatalyst, with promising implications for environmental remediation and wastewater purification.

关键词： Porous film LDH film Anti corrosive Photocatalysis Oxygen vacancy Tetracycline

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Novel interface engineering of LDH-based materials on Mg alloy for efficient photocatalytic systems considering the geometrical linearity of condensed phosphates

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Journal of Magnesium and Alloys 2024年第1期12卷 267-280页

作者： Mosab Kaseem Ananda Repycha Safira Arash Fattah-alhosseini Department of Nanotechnology and Advanced Materials Engineering Corrosion and Electrochemistry LaboratorySejong UniversitySeoul 05006Republic of Korea Department of Materials Engineering Bu-Ali Sina UniversityHamedan 65178-38695Iran

This study presents a facile and rapid method for synthesizing novel Layered Double Hydroxide(LDH)nanoflakes,exploring their application as a photocatalyst,and investigating the influence of condensed phosphates'geometric linearity on their photocatalytic properties.Herein,the Mg O film,obtained by plasma electrolysis of AZ31 Mg alloys,was modified by growing an LDH film,which was further functionalized using cyclic sodium hexametaphosphate(CP)and linear sodium tripolyphosphate(LP).CP acted as an enhancer for flake spacing within the LDH structure,while LP changed flake dispersion and orientation.Consequently,CP@LDH demonstrated exceptional efficiency in heterogeneous photocatalysis,effectively degrading organic dyes like Methylene blue(MB),Congo red(CR),and Methyl orange(MO).The unique cyclic structure of CP likely enhances surface reactions and improves the catalyst's interaction with dye molecules.Furthermore,the condensed phosphate structure contributes to a higher surface area and reactivity in CP@LDH,leading to its superior photocatalytic performance compared to LP@LDH.Specifically,LP@LDH demonstrated notable degradation efficiencies of 93.02%,92.89%,and 88.81%for MB,MO,and CR respectively,over a 40 min duration.The highest degradation efficiencies were observed in the case of the CP@LDH sample,reporting 99.99%for MB,98.88%for CR,and 99.70%for MO.This underscores the potential of CP@LDH as a highly effective photocatalyst for organic dye degradation,offering promising prospects for environmental remediation and water detoxification applications.

关键词： Plasma electrolysis Layered Double Hydroxide Condensed phosphates Adsorption capacity Photocatalytic efficiency

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Advancing oxygen separation:insights from experimental and computational analysis of La_(0.7)Ca_(0.3)Co_(0.3)Fe_(0.6)M_(0.1)O_(3-δ)(M=Cu,Zn)oxygen transport membranes

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Frontiers of Chemical Science and Engineering 2024年第6期18卷 17-29页

作者： Guoxing Chen Wenmei Liu Marc Widenmeyer Xiao Yu Zhijun Zhao Songhak Yoon Ruijuan Yan Wenjie Xie Armin Feldhoff Gert Homm Emanuel Ionescu Maria Fyta Anke Weidenkaff Fraunhofer Research Institution for Materials Recycling and Resource Strategies IWKS Alzenau 63755Germany electrochemistry Laboratory Paul Scherrer InstituteVilligen PSI 5232Switzerland Department of Materials and Earth Sciences Materials and ResourcesTechnical University of DarmstadtDarmstadt 64287Germany Institute of Physical Chemistry and electrochemistry Leibniz University HannoverHannover 30167Germany Institute for Computational Physics University of StuttgartStuttgart 70569Germany Computational Biotechnology RWTH AachenAachen 52074Germany

In this study,perovskite-type La_(0.7)Ca_(0.3)Co_(0.3)Fe_(0.6)M_(0.1)O_(3-δ)(M=Cu,Zn)powders were synthesized using a scalable reverse co-precipitation method,presenting them as novel materials for oxygen transport membranes.The comprehensive study covered various aspects including oxygen permeability,crystal structure,conductivity,morphology,CO_(2) tolerance,and long-term regenerative durability with a focus on phase structure and composition.The membrane La_(0.7)Ca_(0.3)Co_(0.3)Fe_(0.6)M_(0.1)O_(3-δ)exhibited high oxygen permeation fluxes,reaching up to 0.88 and 0.64 mL·min^(−1)·cm^(−2) under air/He and air/CO_(2) gradients at 1173 K,respectively.After 1600 h of CO_(2) exposure,the perovskite structure remained intact,showcasing superior CO_(2) resistance.A combination of first principles simulations and experimental measurements was employed to deepen the understanding of Cu/Zn substitution effects on the structure,oxygen vacancy formation,and transport behavior of the membranes.These findings underscore the potential of this highly CO_(2)-tolerant membrane for applications in high-temperature oxygen separation.The enhanced insights into the oxygen transport mechanism contribute to the advancement of next-generation membrane materials.

关键词： perovskite oxygen permeation membrane oxygennionsdiffusiono xygen vacancy formation energy energy barrier

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Innovative approach to boosting the chemical stability of AZ31 magnesium alloy using polymer-modified hybrid metal oxides

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Journal of Magnesium and Alloys 2024年第3期12卷 1068-1081页

作者： Mosab Kaseem Ananda Repycha Safira Mohammad Aadil Tehseen Zehra Muhammad Ali Khan Arash Fattah-alhosseini Corrosion and electrochemistry Laboratory Department of Nanotechnology and Advanced Materials EngineeringSejong UniversitySeoul 05006Republic of Korea Department of Materials Engineering Bu-Ali Sina UniversityHamedan 65178-38695Iran

Meeting the demands of complex and advanced applications requires the development of high-performance hybrid materials with unique properties.However,the integration of polymeric frameworks with MgO/WO_(3) composite layers faces challenges due to the lack of understanding of the formation mechanism and the challenge of determining the impact of self-assembled architecture on anticorrosive properties.In this study,we aimed to enhance the corrosion resistance of the MgO layer produced by plasma electrolysis(PE)of AZ31 Mg alloy by incorporating WO_(3) with partially phosphorated poly(vinyl alcohol)(PPVA).Two types of porous MgO layers were produced using the PE process with an alkaline-phosphate electrolyte,one with and one without WO_(3) nanoparticles,which were subsequently immersed in an aqueous solution of PPVA.Incorporating PPVA into the WO_(3)-MgO layer resulted in hybrids being deposited in a fragmented manner,creating a“laminar reef-like structure”that sealed most of the structural defects in the layer.The PPVA-sealed WO_(3)-based coating exhibited superior corrosion resistance compared to the other samples.Computational analyses were employed to explore the mechanism underlying the formation of PPVA/WO_(3) hybrids on the MgO layer.These findings suggest that PPVA-WO_(3)-MgO hybrid coatings can potentially improve corrosion resistance in various fields.

关键词： Plasma electrolysis Poly(vinyl alcohol) Tungsten trioxide Sealing Corrosion DFT.

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In-situ construction of grass-like hybrid architecture responsible for extraordinary corrosion performance: Experimental and theoretical approach

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Nano Materials Science 2024年第1期6卷 44-59页

作者： T.Suhartono F.Hazmatulhaq Y.Sheng A.Chaouiki M.P.Kamil Y.G.Ko Materials electrochemistry Group School of Materials Science and EngineeringYeungnam UniversityGyeongsan38541Republic of Korea Research Center for Advanced Materials National Research and Innovation Agency(BRIN)South TangerangBanten15314Indonesia

Despite the engineering potential by the co-existence of inorganic and organic substances to protect vulnerable metallic materials from corrosive environments,both their interaction and in-situ formation mechanism to induce the nature-inspired composite remained less understood.The present work used three distinctive mercaptobenzazole(MB)compounds working as corrosion inhibitors,such as 2-mercaptobenzoxazole(MBO),2-mercaptobenzothiazole(MBT),and 2-mercaptobenzimidazole(MBI)in a bid to understand how the geometrical structure arising from O,S,and N atoms affected the interaction toward inorganic layer.MB compounds that were used here to control the corrosion kinetics would be interacted readily with the pre-existing MgO layer fabricated by plasma electrolysis.This phenomenon triggered the nucleation of the root network since MB compounds were seen to be adsorbed actively on the defective surface through the active sites in MB compound.Then,the molecule with twin donor atoms adjacent to the mercapto-sites affected the facile growth of the grass-like structures with‘uniform’distribution via molecular self-assembly,which showed better corrosion performance than those with having dissimilar donor atoms with the inhibition efficiency(η)of 97%approximately.The formation mechanism underlying nucleation and growth behavior of MB molecule was discussed concerning the theoretical calculation of density functional theory.

关键词： Nature-inspired composite Organic-inorganic interaction Corrosion inhibitor Density functional theory electrochemistry

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Aerosol deposition technology and its applications in batteries

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Nano Materials Science 2024年第1期6卷 24-37页

作者： Xinyu Wang Ramon Alberto Paredes Camacho Xiaoyu Xu Yumei Wang Yi Qiang Hans Kungl Ruediger-AEichel Yunfeng Zhang Li Lu National University of Singapore(Chongqing)Research Institute Chongqing401123PR China National University of Singapore Singapore117576 Fundamental electrochemistry(IEK-9) Institute of Energy and Climate ResearchForschungszentrum Jülich52425JülichGermany

Aerosol deposition(AD)method is a kind of additive manufacturing technology for fabricating dense films such as metals and ceramics at room temperature.It resolves the challenge of integrating ceramic films onto temperaturesensitive substrates,including metals,glasses,and polymers.It should be emphasized that the AD is a spray coating technology that uses powder without thermal assistance to generate films with high density.Compared to the traditional sputter-based approach,the AD shows several advantages in efficiency,convenience,better interfacial bonding and so on.Therefore,it opens some possibilities to the field of batteries,especially all-solidstate batteries(ASSBs)and draws much attention not only for research but also for large scale applications.The purpose of this work is to provide a critical review on the science and technology of AD as well as its applications in the field of batteries.The process,mechanism and effective parameters of AD,and recent developments in AD applications in the field of batteries will be systematically reviewed so that a trend for AD will be finally provided.

关键词： Aerosol deposition Room temperature impact consolidation Ceramic film All-solid-state battery Spray coating technology

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Two positive effects with one arrow:Modulating crystal and interfacial decoration towards high-potential cathode material

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Journal of Energy Chemistry 2024年第5期92卷 216-223页

作者： Xuexiu Gu Xuan-Wen Gao Dongrun Yang Qinfen Gu YSong Hong Chen Tianzhen Ren Wen-Bin Luo Institute for Energy electrochemistry and Urban Mines Metallurgy School of MetallurgyNortheastern UniversityShenyang 110819LiaoningChina Australian Synchrotron(ANSTO) 800 Blackburn RdClaytonVictoria 3168Australia School of Science and Engineering University of DundeeNethergateDundee DD14HNScotlandUK

As the primary suppliers of cyclable sodium ions,O3-type layer-structured manganese-based oxides are recognized as highly competitive cathode candidates for sodium-ion batteries.To advance the development of high-energy sodium-ion batteries,it is crucial to explore cathode materials operating at high voltages while maintaining a stable cycling behavior.The orbital and electronic structure of the octahedral center metal element plays a crucial role in maintaining the octahedra structural integrity and improving Na^(+)ion diffusion by introducing heterogeneous chemical bonding.Inspired by the abundant configuration of extra nuclear electrons and large ion radius,we employed trace amounts of tungsten in this study.The obtained cathode material can promote the reversibility of oxygen redox reactions in the high-voltage region and inhibit the loss of lattice oxygen.Additionally,the formation of a Na_(2)WO_(4) coating on the material surface can improve the interfacial stability and interface ions diffusion.It demonstrates an initial Coulombic efficiency(ICE)of 94.6%along with 168.5 mA h g^(-1 )discharge capacity within the voltage range of 1.9-4.35 V.These findings contribute to the advancement of high-energy sodium-ion batteries by providing insights into the benefits of tungsten doping and Na_(2)WO_(4) coating on cathode materials.

关键词： Sodium ion battery Layer-structured manganese-based oxides Cathodematerial Surface modification Elements doping

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Green Synthesis of Silver Nanoparticles Using Aqueous Orange and Lemon Peel Extract and Evaluation of Their Antimicrobial Properties

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Advances in Nanoparticles 2024年第2期13卷 11-28页

作者： Amra Bratovcic Amna Dautovic Department of Physical Chemistry and electrochemistry Faculty of Technology University of Tuzla Tuzla Bosnia and Herzegovina Multilab Tuzla Bosnia and Herzegovina

Green synthesis of silver nanoparticles (AgNPs) using aqueous extracts of orange and lemon peels, as a reducing agent, and silver nitrate salts as a source of silver ions is a promising field of research due to the versatility of biomedical applications of metal nanoparticles. In this paper, AgNPs were synthetized at different reaction parameters such as the type and concentration of the extracts, metal salt concentration, temperature, speed stirring, and pH. The antibacterial properties of the obtained silver nanoparticles against E. coli, as well as the physical and chemical characteristics of the synthesized silver nanoparticles, were investigated. UV-Vis spectroscopy was used to confirm the formation of AgNPs. In addition to green biogenic synthesis, chemical synthesis of silver nanoparticles was also carried out. The optimal temperature for extraction was 65˚C, while for the synthesis of AgNPs was 35˚C. The synthesis is carried out in an acidic environment (pH = 4.7 orange and pH = 3.8 lemon), neutral (pH = 7) and alkaline (pH = 10), then for different concentrations of silver nitrate solution (0.5 mM - 1 mM), optimal time duration of the reaction was 60 min and optimal stirring speed rotation was 250 rpm on the magnetic stirrer. The physical properties of the synthesized silver nanoparticles (conductivity, density and refractive index) were also studied, and the passage of laser light through the obtained solution and distilled water was compared. Positive inhibitory effect on the growth of new Escherichia coli colonies have shown AgNPs synthesized at a basic pH value and at a 0.1 mM AgNO3 using orange or lemon peel extract, while for a 0.5 mM AgNO3 using lemon peel extract.

关键词： Green Synthesis Silver Nanoparticles Orange and Lemon Peel Extract Antibacterial Activity Escherichia coli

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Classification and technical target of water electrolysis for hydrogen production

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Journal of Energy Chemistry 2024年第8期95卷 554-576页

作者： Kahyun Ham Sooan Bae Jaeyoung Lee Ertl Center for electrochemistry and Catalysis Gwangju Institute of Science and Technology(GIST) Department of Heterogeneous Reactions Max Planck Institute for Chemical Energy Conversion School of Earth Sciences and Environmental Engineering GIST International Future Research Center of Chemical Energy Storage and Conversion Processes GIST eSuS Co. Ltd. #408 S6 Building School of Environment and Energy Engineering GIST

Continuous efforts are underway to reduce carbon emissions worldwide in response to global climate change. Water electrolysis technology, in conjunction with renewable energy, is considered the most feasible hydrogen production technology based on the viable possibility of large-scale hydrogen production and the zero-carbon-emission nature of the process. However, for hydrogen produced via water electrolysis systems to be utilized in various fields in practice, the unit cost of hydrogen production must be reduced to $1/kg H2. To achieve this unit cost, technical targets for water electrolysis have been suggested regarding components in the system. In this paper, the types of water electrolysis systems and the limitations of water electrolysis system components are explained. We suggest guideline with recent trend for achieving this technical target and insights for the potential utilization of water electrolysis technology.

关键词： electrochemistry Hydrogen production Technical target Water electrolysis

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