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Boosting hydrogen Storage Performance of MgH_(2) by Oxygen Vacancy-Rich H-V_(2)O_(5) Nanosheet as an Excited H-Pump

Nano-Micro Letters 2024年第8期16卷 398-416页

作者： Li Ren Yinghui Li Zi Li Xi Lin Chong Lu Wenjiang Ding Jianxin Zou National Engineering Research center of Light Alloys Net Forming&State Key Laboratory of Metal Matrix Composites Shanghai Jiao Tong UniversityShanghai 200240People’s Republic of China shanghai Engineering Research center of Mg Materials and Applications&School of Materials science and Engineering Shanghai Jiao Tong UniversityShanghai 200240People’s Republic of China center of hydrogen science Shanghai Jiao Tong UniversityShanghai 200240People’s Republic of China Instrumental Analysis center of SJTU Shanghai Jiao Tong UniversityShanghai 200240People’s Republic of China

MgH_(2) is a promising high-capacity solid-state hydrogen storage material,while its application is greatly hindered by the high desorption temperature and sluggish ***,intertwined 2D oxygen vacancy-rich V_(2)O_(5) nanosheets(H-V_(2)O_(5))are specifically designed and used as catalysts to improve the hydrogen storage properties of MgH_(2).The as-prepared MgH_(2)-H-V_(2)O_(5) composites exhibit low desorption temperatures(Tonset=185℃)with a hydrogen capacity of 6.54 wt%,fast kinetics(Ea=84.55±1.37 kJ mol^(-1) H_(2) for desorption),and long cycling ***,hydrogen absorption can be achieved at a temperature as low as 30℃ with a capacity of 2.38 wt%within 60 ***,the composites maintain a capacity retention rate of~99%after 100 cycles at 275℃.Experimental studies and theoretical calculations demonstrate that the in-situ formed VH_(2)/V catalysts,unique 2D structure of H-V_(2)O_(5) nanosheets,and abundant oxygen vacancies positively contribute to the improved hydrogen sorption ***,the existence of oxygen vacancies plays a double role,which could not only directly accelerate the hydrogen ab/de-sorption rate of MgH_(2),but also indirectly affect the activity of the catalytic phase VH_(2)/V,thereby further boosting the hydrogen storage performance of MgH_(2).This work highlights an oxygen vacancy excited“hydrogen pump”effect of VH_(2)/V on the hydrogen sorption of Mg/MgH_(2).The strategy developed here may pave a new way toward the development of oxygen vacancy-rich transition metal oxides catalyzed hydride systems.

关键词： hydrogen storage MgH_(2) V_(2)O_(5)nanosheets Oxygen vacancies VH_(2)

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Exciting lattice oxygen of nickel–iron bi-metal alkoxide for efficient electrochemical oxygen evolution reaction

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Journal of Energy Chemistry 2024年第1期88卷 194-201,I0005页

作者： Saihang Zhang Senchuan Huang Fengzhan Sun Yinghui Li Li Ren Hao Xu Zhao Li Yifei Liu Wei Li Lina Chong Jianxin Zou National Engineering Research center of Light Alloy Net Forming&State Key Laboratory of Metal Matrix Composites Center of Hydrogen ScienceSchool of Materials Science and EngineeringShanghai Jiao Tong UniversityShanghai 200240China Department of Chemistry Laboratory of Advanced MaterialsShanghai Key Laboratory of Molecular Catalysis and Innovative MaterialsiChEM and State Key Laboratory of Molecular Engineering of PolymersCollege of Chemistry and MaterialsFudan UniversityShanghai 200433China

High efficiency,cost-effective and durable electrocatalysts are of pivotal importance in energy conversion and storage *** electro-oxidation of water to oxygen plays a crucial role in such energy conversion ***,we report a robust method for the synthesis of a bimetallic alkoxide for efficient oxygen evolution reaction(OER)for alkaline electrolysis,which yields current density of 10 mA cm^(-2)at an overpotential of 215 mV in 0.1 M KOH *** catalyst demonstrates an excellent durability for more than 540 h operation with negligible degradation in *** spectra revealed that the catalyst underwent structure reconstruction during OER,evolving into oxyhydroxide,which was the active site proceeding OER in alkaline ***-situ synchrotron X-ray absorption experiment combined with density functional theory calculation suggests a lattice oxygen involved electrocatalytic reaction mechanism for the in-situ generated nickel–iron bimetal-oxyhydroxide *** mechanism together with the synergy between nickel and iron are responsible for the enhanced catalytic activity and *** findings provide promising strategies for the rational design of nonnoble metal OER catalysts.

关键词： Oxygen evolution reaction Nickel-iron bi-metal alkoxide Lattice oxygen-mediated reaction mechanism Alkaline electrolysis Electrocatalysts

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Efficient Preconstruction of Three‑Dimensional Graphene Networks for Thermally Conductive Polymer Composites

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Nano-Micro Letters 2022年第8期14卷 72-111页

作者： Hao‑Yu Zhao Ming‑Yuan Yu Ji Liu Xiaofeng Li Peng Min Zhong‑Zhen Yu Beijing Key Laboratory of Advanced Functional Polymer Composites Beijing University of Chemical TechnologyBeijing 100029People’s Republic of China College of Materials science and Engineering Beijing University of Chemical TechnologyBeijing 100029People’s Republic of China School of Chemistry CRANN and AMBERTrinity College DublinDublinIreland

Electronic devices generate heat during operation and require efficient thermal management to extend the lifetime and prevent performance *** by its exceptional thermal conductivity,graphene is an ideal functional filler for fabricating thermally conductive polymer composites to provide efficient thermal *** studies have been focusing on constructing graphene networks in polymer composites to achieve high thermal *** with conventional composite fabrications by directly mixing graphene with polymers,preconstruction of three-dimensional graphene networks followed by backfilling polymers represents a promising way to produce composites with higher performances,enabling high manufacturing flexibility and *** this review,we first summarize the factors that affect thermal conductivity of graphene composites and strategies for fabricating highly thermally conductive graphene/polymer ***,we give the reasoning behind using preconstructed three-dimensional graphene networks for fabricating thermally conductive polymer composites and highlight their potential ***,our insight into the existing bottlenecks and opportunities is provided for developing preconstructed porous architectures of graphene and their thermally conductive composites.

关键词： Graphene networks Thermal conductivity Thermal interface materials Phase change composites Anisotropic aerogels

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Designing strategy for corrosion-resistant Mg alloys based on film-free and film-covered models

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Journal of Magnesium and Alloys 2023年第9期11卷 3120-3129页

作者： Pengyu Zhao Tao Ying Fuyong Cao Xiaoqin Zeng Wenjiang Ding National Engineering Research center of Light Alloys Shanghai Jiao Tong UniversityShanghai 200240PR China center for Marine Materials Corrosion and Protection College of MaterialsXiamen University361005PR China

Mathematical models were proposed to clarify the effect of alloying on corrosion of magnesium alloys based on film-free and film-covered status. The models are applicable to explain the “barrier effect” by cathodes and the “analogous Hall-Petch relationship” between corrosion rates and grain size. The slope of corrosion rates versus alloying content is determined by the dissolution ability of film-free substrate and the hindering effects by corrosion product film. Designing strategy for corrosion-resistant Mg alloys is established.

关键词： Magnesium Corrosion Modeling Electrochemistry

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Revealing the GHG reduction potential of emerging biomass-based CO_(2) utilization with an iron cycle system

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Frontiers of Environmental science & Engineering 2023年第10期17卷 119-131页

作者： Jing Xu Jiong Cheng Runtian He Jiaqi Lu Chunling Wang Heng Zhong Fangming Jin School of Environmental science and Engineering State Key Laboratory of Metal Matrix CompositesShanghai Jiao Tong UniversityShanghai 200240China Innovation Centre for Environment and Resources Shanghai University of Engineering ScienceShanghai 201620China center of hydrogen science Shanghai Jiao Tong UniversityShanghai 200240China shanghai Institute of Pollution Control and Ecological Security Shanghai 200092China

CO_(2) utilization becomes a promising solution for reducing anthropogenic greenhouse gas (GHG) emissions. Biomass-based CO_(2) utilization (BCU) even has the potential to generate negative emissions, but the corresponding quantitative evaluation is limited. Herein, the biomass-based CO_(2) utilization with an iron cycle (BCU-Fe) system, which converts CO_(2) into formate by Fe under hydrothermal conditions and recovers Fe with biomass-derived glycerin, was investigated. The GHG reduction potential under various process designs was quantified by a multidisciplinary method, including experiments, simulations, and an ex-ante life-cycle assessment. The results reveal that the BCU-Fe system could bring considerable GHG emission reduction. Significantly, the lowest value is −34.03 kg CO_(2)-eq/kg absorbed CO_(2) (−2.44 kg CO_(2)-eq/kg circulated Fe) with the optimal yield of formate (66%) and Fe (80%). The proposed ex-ante evaluation approach not only reveals the benefits of mitigating climate change by applying the BCU-Fe system, but also serves as a generic tool to guide the industrialization of emerging carbon-neutral technologies.

关键词： Carbon dioxide utilization Hydrothermal reactions Biomass-based CO_(2)reduction Simulation Ex-ante LCA

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In situ revealing the reconstruction behavior of monolayer rocksalt CoO nanosheet as water oxidation catalyst

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Journal of Energy Chemistry 2022年第7期31卷 373-381,I0010页

作者： Weiqi Guo Haolin Luo Dongxu Fang Zhi Jiang Jiasheng Chi Wenfeng Shangguan Research center for Combustion and Environment Technology Shanghai Jiao Tong UniversityShanghai 200240China center of hydrogen science Shanghai Jiao Tong UniversityShanghai 200240China

The reconstruction during oxygen evolution reaction (OER) significantly affects the electronic and local geometry structure of metal sites in *** with well-investigated cobalt-based materials,the reconstruction of rocksalt CoO with purely Co^(2+) in octahedral (Oh) coordination has not been revealed in ***,monolayer Co O supported on reduced graphene oxide (r GO) was synthesized via a one-pot hydrothermal strategy with calcinating in Ar *** structure evolution of twodimension (2D) Co O/r GO during OER was revealed by in situ X-ray absorption spectroscopy (XAS).The transition from Co O toward Co3O_(4) already occurred at open circuit potential,further enhanced at 1.23 V (***).The Co Ox(OH)ywas determined as the active phase at 1.53 V,displaying a tetrahedral Co coordination defective spinel Co_(3)O_(4) with the Co-O shell that featured the (oxy)hydroxide,not the standard Co *** OER,the irreversible transition from CoO to Co_(3)O_(4) was *** contrast,in situ Raman spectra revealed a reversible amorphization process on Co_(3)O_(4)/r GO under operation ***,this study indicated that the reconstruction behavior could be more effectively revealed by XAS using 2D materials.

关键词： Oxygen evolution reaction Two-dimension materials Rocksalt CoO X-ray absorption spectroscopy In situ experiments

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Organic cathode materials for rechargeable magnesium-ion batteries:Fundamentals, recent advances, and approaches to optimization

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Journal of Magnesium and Alloys 2023年第12期11卷 4359-4389页

作者： Xiaoqian He Ruiqi Cheng Xinyu Sun Hao Xu Zhao Li Fengzhan Sun Yang Zhan Jianxin Zou Richard M.Laine National Engineering Research center of Light Alloys Net Forming and State Key Laboratory of Metal Matrix Composites Shanghai Engineering Research Center of Mg Materials and Applications and School of Materials Science and EngineeringCenter of Hydrogen ScienceShanghai Jiao Tong UniversityShanghai 200240PR China Department of Materials science and Engineering University of Michigan Ann ArborMI 48109-2136USA shanghai Key Laboratory of Advanced High-temperature Materials and Precision Forming School of Materials Science and EngineeringShanghai Jiao Tong UniversityShanghai 200240PR China

Rechargeable magnesium-ion batteries(MIBs) are favorable substitutes for conventional lithium-ion batteries(LIBs) because of abundant magnesium reserves, a high theoretical energy density, and great inherent safety. Organic electrode materials with excellent structural tunability,unique coordination reaction mechanisms, and environmental friendliness offer great potential to promote the electrochemical performance of MIBs. However, research on organic magnesium battery cathode materials is still preliminary with many significant challenges to be resolved including low electrical conductivity and unwanted but severe dissolution in useful electrolytes. Herein, we provide a detailed overview of reported organic cathode materials for MIBs. We begin with basic properties such as charge storage mechanisms(e.g., n-, p-, and bipolartype), moving to recent advances in various types of organic cathodes including carbonyl-, nitrogen-, and sulfur-based materials. To shed light on the diverse strategies targeting high-performance Mg-organic batteries, elaborate summaries of various approaches are ***, these strategies include molecular design, polymerization, mixing with carbon, nanosizing and electrolyte/separator *** review provides insights on exploring high-performance organic cathodes in rechargeable MIBs.

关键词： Mg-organic batteries Organic cathode materials Energy storage Charge storage mechanism Electrochemical optimization approaches

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In situ High-Energy Synchrotron X-ray Studies in Thermodynamics of Mg-In-Ti hydrogen Storage System

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Energy Material Advances 2023年第1期4卷 548-558页

作者： Wen Zhu Li Ren Yinghui Li Chong Lu Xi Lin Qiuyu Zhang Xue Yang Zhigang Hu Tao Cheng Yingyan Zhao Jianxin Zou National Engineering Research center of Light Alloys Net Forming&State Key Laboratory of Metal Matrix Composites Shanghai Jiao Tong UniversityShanghai200240PR China shanghai Engineering Research center of Mg Materials and Applications and School of Materials science and Engineering Shanghai Jiao Tong UniversityShanghai200240PR China shanghai Key Laboratory of hydrogen science and center of hydrogen science Shanghai Jiao Tong UniversityShanghai200240PR China Sinopec Research Institute of Petroleum Processing Co. Ltd.Beijing100083PR China

Achieving dual regulation of the kinetics and thermodynamics of MgH_(2) is essential for the practical *** this study,a novel nanocomposite(In@Ti-MX)architected from single-/few-layered Ti_(3)C_(2) MXenes and ultradispersed indium nanoparticles was prepared by a bottom-up self-assembly strategy and introduced into MgH_(2) to solve the above-mentioned *** MgH_(2)+In@Ti-MX composites demonstrate excellent hydrogen storage performance:The resultant In@Ti-MX demonstrated a positive effect on the hydrogen storage performance of MgH_(2)/Mg:the dehydrogenated rate of MgH_(2)+15 wt%In@Ti-MX reached the maximum at 330°C,which was 47°C lower than that of commercial MgH_(2);The hydrogenation enthalpy of the dehydrided MgH_(2)+15 wt%In@Ti-MX and MgH_(2)+25 wt%In@Ti-MX were determined to be−66.2±1.1 and−61.7±1.4 kJ·mol^(−1) H_(2).In situ high-energy synchrotron x-ray diffraction technique together with other microstructure analyses revealed that synergistic effects from Ti_(3)C_(2) MXenes and In nanoparticles(NPs)contributed to the improved kinetics and thermodynamics of MgH_(2)(Mg):Ti/TiH_(2) derived from Ti_(3)C_(2) MXenes accelerated the dissociation and recombination of hydrogen molecule/atoms,while In NPs reduced the thermodynamic stability of MgH_(2) by forming the Mg-In *** a strategy of using dual-active hybrid structures to modify MgH_(2)/Mg provides a new insight for tuning both the hydrogen storage kinetics and thermodynamics of Mg-based hydrides.

关键词： microstructure kinetics thermodynamics

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Recent advances of hydrogen production through particulate semiconductor photocatalytic overall water splitting

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Frontiers in Energy 2022年第1期16卷 49-63页

作者： Zhi JIANG Zhen YE Wenfeng SHANGGUAN Research center for Combustion and Environment Technology Shanghai Jiao Tong UniversityShanghai 200240China

Solar energy-driven photocatalytic water splitting has been investigated for decades to produce clean and renewable green *** this paper,the cutting-edge research within the overall water splitting system is summarized from the one-step photocatalytic overall water splitting(POWS)system to the two-step system and the cocatalysts research in this *** addition,the photocatalytic reaction engineering study is also reviewed which is crucial for future *** mini-review provides a picture of survey of recent progress of relevant overall water splitting system,with particular attention paid to material system and mechanistic breakthroughs,and highlights the challenge and opportunity of the current system.

关键词： photocatalysis overall water splitting hydrogen

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Nanostructuring of Mg-Based hydrogen Storage Materials:Recent Advances for Promoting Key Applications

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Nano-Micro Letters 2023年第7期15卷 30-56页

作者： Li Ren Yinghui Li Ning Zhang Zi Li Xi Lin Wen Zhu Chong Lu Wenjiang Ding Jianxin Zou National Engineering Research center of Light Alloys Net Forming and State Key Laboratory of Metal Matrix Composites Shanghai Engineering Research Center of Mg Materials and Applications and School of Materials Science and EngineeringCenter of Hydrogen ScienceShanghai Jiao Tong UniversityShanghai 200240People’s Republic of China Instrumental Analysis center of SJTU Shanghai Jiao Tong UniversityShanghai 200240People’s Republic of China

With the depletion of fossil fuels and global warming,there is an urgent demand to seek green,low-cost,and high-efficiency energy *** has been considered as a potential candidate to replace fossil fuels,due to its high gravimetric energy density(142 MJ kg^(-1)),high abundance(H_(2)O),and ***,due to its low volume density,effective and safe hydrogen storage techniques are now becoming the bottleneck for the"hydrogen economy".Under such a circumstance,Mg-based hydrogen storage materials garnered tremendous interests due to their high hydrogen storage capacity(~7.6 wt%for MgH_(2)),low cost,and excellent ***,the high thermodynamic stability(ΔH=-74.7 kJ mol^(-1)H_(2))and sluggish kinetics result in a relatively high desorption temperature(>300℃),which severely restricts widespread applications of MgH_(2).Nano-structuring has been proven to be an effective strategy that can simultaneously enhance the ab/de-sorption thermodynamic and kinetic properties of MgH_(2),possibly meeting the demand for rapid hydrogen desorption,economic viability,and effective thermal management in practical ***,the fundamental theories,recent advances,and practical applications of the nanostructured Mg-based hydrogen storage materials are *** synthetic strategies are classified into four categories:free-standing nano-sized Mg/MgH_(2)through electrochemical/vapor-transport/ultrasonic methods,nanostructured Mg-based composites via mechanical milling methods,construction of core-shell nano-structured Mg-based composites by chemical reduction approaches,and multi-dimensional nano-sized Mg-based heterostructure by nanoconfinement *** applying these strategies,near room temperature ab/de-sorption(6 wt%)has been achieved in nano Mg/MgH_(2)*** perspectives on the future research and development of nanostructured hydrogen storage materials are also provided.

关键词： Mg-based hydrogen storage materials Nanostructure hydrogen storage Thermodynamics Kinetics On-board hydrogen storage

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