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Stability of dimensionally stable anode for chlorine evolution reaction

Nano Research 2024年第3期17卷 949-959页

作者： Ziliang Deng Shuying Xu Chuhao Liu Xueqiang Zhang Mufan Li Zipeng Zhao beijing key laboratory of Construction Tailorable Advanced Functional materials and Green Applications Experimental Center of Advanced MaterialsSchool of Materials Science and EngineeringBeijing Institute of TechnologyBeijing 100081China beijing National laboratory for Molecular Sciences College of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China Laser Micro/Nano-Fabrication laboratory School of Mechanical EngineeringBeijing Institute of TechnologyBeijing 10081China

Chlorine(Cl2)is one of the most important chemicals produced by the electrolysis of brine solutions and is a key raw material for many areas of industrial chemistry.For nearly half a century,dimensionally stable anode(DSA)made from a mixture of RuO_(2) and TiO_(2) solid oxides coated on Ti substrate has been the most widely used electrode for chlorine evolution reaction(CER).In harsh operating environments,the stability of DSAs remains a major challenge greatly affecting their lifetime.The deactivation of DSAs significantly increases the cost of the chlor-alkali industry due to the corrosion of Ru and the formation of the passivation layer TiO_(2).Therefore,it is urgent to develop catalysts with higher activity and stability,which requires a thorough understanding of the deactivation mechanism of DSA catalysts.This paper reviews existing references on the deactivation mechanisms of DSA catalysts,including both experimental and theoretical studies.Studies on how CER selectivity affects electrode stability are also discussed.Furthermore,studies on the effects of the preparation process,elemental composition,and surface/interface structures on the DSA stability and corresponding improvement strategies are summarized.The development of other non-DSA-type catalysts with comparable stability is also reviewed,and future opportunities in this exciting field are also outlined.

关键词： chlorine evolution reaction(CER) dimensionally stable anode(DSA) RuO_(2)-TiO_(2) metal oxide anode stability

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Interactive effect of thermal aging and proton irradiation on microstructural evolution and hardening ofδ-ferrite in 308L stainless steel weld metal

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Journal of materials Science & technology 2024年第3期170卷 140-155页

作者： Xiaodong Gao Xiaodong Lin Tao Guo Lining Xu Yaolei Han Baolong Jiang Xingyuan Mei Qunjia Peng Lijie Qiao beijing Advanced Innovation Center for materials Genome Engineering Institute of Advanced Materials and TechnologyUniversity of Science and Technology BeijingBeijing 100083China Institute of materials Shanghai UniversityShanghai 200072China School of materials Science and Engineering University of Science and Technology BeijingBeijing 100083China Suzhou Nuclear Power Research Institute Suzhou 215004China State key laboratory for Advanced Metals and materials University of Science and Technology BeijingBeijing 100083China

In the harsh service environment of high temperature and intense neutron irradiation in water-cooled nuclear reactors,the austenitic stainless steel weld overlay cladding on the inner surface of the reactor pressure vessel suffers from thermal aging and irradiation damage simultaneously,which can induce microstructural evolution and hardening of the material.Since it is quite difficult to achieve this simul-taneous process out of the pile,two kinds of combined experiments,i.e.,post-irradiation thermal aging and post-aging irradiation were performed on 308 L stainless steel weld metals in this work.The interactive effect of thermal aging and proton irradiation on microstructural evolution and hardening ofδ-ferrite in 308 L weld metal was investigated by combining atom probe tomography,transmission elec-tron microscopy and nanoindentation tests.The results revealed that thermal aging could eliminate the dislocation loops induced by irradiation and affect the phase transition process by accelerating spinodal decomposition and G-phase precipitation,thus enhancing hardening of irradiatedδ-ferrite.For the effect of irradiation on the microstructure and hardening of thermally agedδ-ferrite,however,intensive collision cascades can intensify G-phase precipitation and dislocation loop formation but decrease spinodal decomposition,leading to a limited effect on hardening of thermally agedδ-ferrite.Furthermore,the interaction of thermal aging and irradiation can promote G-phase precipitation.Meanwhile,the interaction can causeδ-ferrite hardening,which is mainly influenced by spinodal decomposition,followed by G-phase and dislocation loops,where spinodal decomposition and G-phase cause hardening by inducing strain fields.

关键词： Austenitic stainless steel weld metals Thermal aging Proton irradiation Interaction Microstructural evolution Hardening

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Recent Advances in Biomass-derived Porous Carbon materials:Synthesis,Composition and Applications

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Chemical Research in Chinese Universities 2024年第1期40卷 3-19页

作者： ZHAI Ziqi LU Yumiao LIU Guangyong DING Wei-Lu CAO Bobo HE Hongyan CAS key laboratory of Green process and Engineering State Key Laboratory of Mesoscience and EngineeringBeijing Key Laboratory of Ionic Liquids Clean ProcessInstitute of Process EngineeringChinese Academy of SciencesBeijing 100190P.R.China University of Chinese Academy of Sciences Beijing 100049P.R.China Longzihu New Energy laboratory Zhengzhou Institute of Emerging Industrial TechnologyZhengzhou 450000P.R.China

Porous carbon materials(PCMs)play a pivotal role in diverse applications,such as energy storage,adsorption,catalysis,environmental remediation,and microwave adsorption.The selection of carbon precursors,in particular,is crucial for tailoring porous structures with specific functionalities.Biomass,with its rich carbon feedstock,abundant availability,renewability,and versatile structures,has emerged as a promising precursor for porous carbon material synthesis.This review comprehensively summarizes the recent advances in biomass-derived porous carbon materials(BPCMs)encompassing synthetic strategy,morphology,structural composition,and multiple applications.We first review synthetic approaches aiming at regulating porosity,followed by morphological and composition features of BPCMs,with a special emphasis on elucidating the dimensional clarification and heteroatom doping effects.The discussion then extends to the wide-ranging applications of BPCMs,covering energy-related applications and CO_(2) adsorption to environmental remediation.Finally,the review outlines the existing challenges and prospects in the field.In summary,this review systematically describes BPCMs and provides valuable guidance for researchers to select and synthesize BPCMs that meet specific functional requirements.

关键词： Biomass Porous carbon Pyrolysis Heteroatom-doping Supercapacitor CO_(2)adsorption

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Bio-inspired surface manipulation of halloysite nanotubes for highperformance flame retardant polylactic acid nanocomposites

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Nano Research 2024年第3期17卷 1595-1606页

作者： Yaru Sun Bin Yu Yan Liu Junbo Yan Zixi Xu Bo Cheng Fenglei Huang Jun Wang State key laboratory of Explosion Science and technology Beijing Institute of TechnologyBeijing 100081China State key laboratory of Fire Science University of Science and Technology of ChinaHefei 230026China beijing Institute of technology Chongqing Innovation Center Chongqing 401120China National Engineering Research Center of Flame Retardant materials Beijing Institute of TechnologyBeijing 100081China

High-performance flame-retardant polylactic acid(PLA)bio-composites based on biobased fillers to meet usage requirements represents a promising direction for creating a sustainable world.Although flame retardant PLA composites have been reported extensively,it still remains a huge challenge to develop mechanically robust.The flame retardant PLA composites due to plastication effect of organic flame retardants and poor compatibility of organic fillers with the matrix lead to the severe deterioration in mechanical properties.In this work,a bio-inspired surface manipulation strategy for halloysite nanotubes(HNTs)was proposed via a facile and green self-assembly process.The structure and morphology of bio-inspired HNTs(b-HNTs)proved that biomass nanofillers(PA-NA-Fe)grew well both within the lumen and on the surface of HNTs.The growth of biomass on the inner and outer surfaces of HNTs was inspired from wooden towards enhancing the interface compatibility and imparting multi-properties to PLA biopolymer.Excellent mechanical properties(tensile,thermomechanical and anti-impact mechanical),great fire safety(heat release and smoke emission),thermostability and improved electromagnetic interference shielding effectiveness of this well-designed PLA nanocomposite were realized.The mechanisms of the enhanced performances of the PLA bio-composites by loading b-HNTs were proposed.This work presents a facile and environmentally-friendly bio-inspired modification strategy for HNTs to fabricate high-performance,multi-functional polymer composites,which is also suitable for surface modification of many other nanomaterials,including nanofibers,nanotubes,nanowires,and nanosheets.

关键词： mechanical properties thermostability fire safety electromagnetic interference shielding biomass

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Porous metal oxides in the role of electrochemical CO_(2) reduction reaction

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Journal of Energy Chemistry 2024年第1期88卷 373-398,I0009页

作者： Ziqi Zhang Jinyun Xu Yu Zhang Liping Zhao Ming Li Guoqiang Zhong Di Zhao Minjing Li Xudong Hu Wenju Zhu Chunming Zheng Xiaohong Sun School of Chemical Engineering and technology Tianjin Key Laboratory of Green Chemical Technology and Process EngineeringState Key Laboratory of Separation Membrane and Membrane ProcessesTiangong UniversityTianjin 300387China School of materials Science and Engineering Key Laboratory of Advanced Ceramics and Machining TechnologyMinistry of EducationTianjin UniversityTianjin 300072China

The global energy-related CO_(2) emissions have rapidly increased as the world economy heavily relied on fossil fuels.This paper explores the pressing challenge of CO_(2) emissions and highlights the role of porous metal oxide materials in the electrocatalytic reduction of CO_(2)(CO_(2)RR).The focus is on the development of robust and selective catalysts,particularly metal and metal-oxide-based materials.Porous metal oxides offer high surface area,enhancing the accessibility to active sites and improving reaction kinetics.The tunability of these materials allows for tailored catalytic behavior,targeting optimized reaction mechanisms for CO_(2)RR.The work also discusses the various synthesis strategies and identifies key structural and compositional features,addressing challenges like high overpotential,poor selectivity,and low stability.Based on these insights,we suggest avenues for future research on porous metal oxide materials for electrochemical CO_(2) reduction.

关键词： CO_(2)reduction Carbon dioxide Transformation Porous metal oxides Electrocatalysis

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Constructing inter-diffusive PtCuNi/WO_(3)interface to enhance the catalytic activity and stability in oxygen reduction

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Tungsten 2024年第2期6卷 293-303页

作者： Hao-Zhe Xu Dong Li Ying Chen Pin Fang Xiao-Xing Ke Olga Demidenko Yu-Jing Li beijing key laboratory of Construction Tailorable Advanced Functional materials and Green Applications Experimental Center of Advanced MaterialsSchool of Materials Science and EngineeringBeijing Institute of TechnologyBeijing 100081China Faculty of materials and Manufacturing Beijing University of TechnologyBeijing 100124China Scientifi c-Practical materials Research Centre National Academy of Sciences of Belarus220072 MinskBelarus

Platinum-group-metal-based alloy nanocrystals have been considered as the most effi cient catalysts for oxygen reduction reaction(ORR).However,the poor stability issues limit their further deployment in industrialization.Tungsten oxide(WO_(3))has received attention due to its intrinsic electrochemical stability and proton absorption/desorption capability.In this work,we prepared PtCuNi/WO_(3)/C hybrid catalyst with inter-diff usive alloy/WO_(3)interface on carbon.The catalyst exhibits enhanced activity and stability associated with the WO_(3)content.The characterization results suggest that the increased activity originates from the complementary proton supply of non-stoichiometric H_(x)WO_(3).Moreover,WO_(3)prevents the particle from dissolution and detachment under vigorous electrochemical polarizations.The enhanced stability originates from the electronic interaction established between Pt and W.This work provides new strategies to design high-performance ORR catalysts by taking the merits of WO_(3)。

关键词： Tungsten oxide PtCuNi Interface Electronic interaction

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Solvation Engineering via Fluorosurfactant Additive Toward Boosted Lithium-Ion Thermoelectrochemical Cells

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Nano-Micro Letters 2024年第4期16卷 253-268页

作者： Yinghong Xu Zhiwei Li Langyuan Wu Hui Dou Xiaogang Zhang Jiangsu key laboratory of electrochemical Energy Storage Technologies College of Material Science and TechnologyNanjing University of Aeronautics and AstronauticsNanjing 211106People’s Republic of China

Lithium-ion thermoelectrochemical cell(LTEC), featuring simultaneous energy conversion and storage, has emerged as promising candidate for low-grade heat harvesting. However, relatively poor thermosensitivity and heat-to-current behavior limit the application of LTECs using LiPF_6 electrolyte. Introducing additives into bulk electrolyte is a reasonable strategy to solve such problem by modifying the solvation structure of electrolyte ions. In this work, we develop a dual-salt electrolyte with fluorosurfactant(FS) additive to achieve high thermopower and durability of LTECs during the conversion of low-grade heat into electricity. The addition of FS induces a unique Li~+ solvation with the aggregated double anions through a crowded electrolyte environment,resulting in an enhanced mobility kinetics of Li~+ as well as boosted thermoelectrochemical performances. By coupling optimized electrolyte with graphite electrode, a high thermopower of 13.8 mV K^(-1) and a normalized output power density of 3.99 mW m^(–2) K^(–2) as well as an outstanding output energy density of 607.96 J m^(-2) can be obtained.These results demonstrate that the optimization of electrolyte by regulating solvation structure will inject new vitality into the construction of thermoelectrochemical devices with attractive properties.

关键词： Solvation engineering Fluorosurfactant Ionic thermoelectric Lithium-ion thermoelectrochemical cell Low-grade heat

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Designed imidazole-based supramolecular catalysts for accelerating oxidation/hydrolysis cascade reactions

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Nano Research 2024年第6期17卷 4916-4923页

作者： Yuanxi Liu Wenjie Xu Shichao Xu Haifeng Wu Baoli Zhang Li Song Zhen-Gang Wang State key laboratory of Organic-Inorganic Composites Key Lab of Biomedical Materials of Natural Macromolecules(Ministry of Education)Beijing Laboratory of Biomedical MaterialsCollege of Materials Science and EngineeringBeijing University of Chemical TechnologyBeijing 100029China National Synchrotron Radiation laboratory CAS Center for Excellence in NanoscienceUniversity of Science and Technology of ChinaHefei 230029China

Reconstructing enzymatic active sites presents a significant challenge due to the intricacies involved in achieving enzyme-like scaffold folding and spatial arrangement of essential functional groups.There is also a growing interest in building biocatalytic networks,wherein multiple enzymatic active sites are localized within a single artificial system,allowing for cascaded transformations.In this work,we report the self-assembly of imidazole or its derivatives with fluorenylmethyloxycarbonyl-modified histidine and Cu2+to fabricate a supramolecular catalyst,which possesses catechol oxidase-like dicopper center with multiple imidazole as the coordination sphere.Transmission electron microscopy,low-temperature X-band continuous-wave electron paramagnetic resonance,K-edge X-ray absorption spectra/the extended X-ray absorption fine structure analysis,and density functional theory modeling were used for the structural characterization of the catalyst.The phenol derivatives and the dissolved oxygen were used as the substrates,with the addition of 4-aminoantipyrine to generate a red adduct with a maximum absorbance at 510 nm,for obtaining time-dependent absorbance change curves and estimating the activities.The results reveal that the addition of imidazole synergistically accelerates the oxidative activity about 10-fold and the hydrolysis activity about 14-fold than fluorenylmethyloxycarbonyl modified-histidine/Cu2+.The supramolecular nanoassembly also exhibits the ability to catalyze oxidation/hydrolysis cascade reactions,converting 2′,7′-dichlorofluorescin diacetate into 2′,7′-dichlorofluorescein.This process can be regulated through the methylation of the imidazole component at various positions.This work may contribute to the design of advanced biomimetic catalysts,and shed light on early structural models of the active sites of the primitive copper-dependent enzymes.

关键词： enzyme mimic self-assembly supramolecular catalyst cascade reactions

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Activatable photoacoustic bioprobe for visual detection of aging in vivo

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Chinese Chemical Letters 2024年第4期35卷 324-329页

作者： Zihong Li Jie Cheng Ping Huang Guoliang Wu Weiying Lin Institute of Optical materials and Chemical Biology Guangxi Key Laboratory of Electrochemical Energy MaterialsSchool of Chemistry and Chemical EngineeringGuangxi UniversityNanning 530004China

Aging is a natural physiological process with various challenges, related to the loss of homeostasis within the organism, which is not a disease, but a significantly strong risk factor for multiple diseases, including myocardial infarction, stroke, some age-related cancers, macular degeneration, osteoarthritis, neurodegeneration, and many others. In the body, the main manifestation of aging is cellular aging, which exists within tissues and has a local or global impact on tissue function. However, the lack of effective aging detection tools has always been an issue that cannot be ignored in the field of aging research. Therefore,it is necessary to construct a non-invasive tool for in vivo detection of aging. Here, we show that the photoacoustic probe(LGAL), which has peak excitation and emission wavelengths in the near-infrared optical window, binds in vivo and at high contrast to the hallmark of aging, and allows for the microscopic imaging of aging through the intact mice. Firstly, this tool LGAL has been successfully applied to detect senescence in cells, displaying stronger photoacoustic signals than normal cells. Then, by using the photoacoustic probe, the blood vessels and tissues inside the mice can be visualized. Young and elderly mice exhibit varying intensities of photoacoustic signals, marking the first time a probe has been used to explore the aging of blood vessels and tissues inside the mice. Finally, we monitored the changes in the degree of aging during tumor treatment under photoacoustic(PA) imaging for the first time. As the treatment time increased, the degree of aging of the tumor gradually deepened. We expect the powerful tool could be a noninvasive and powerful tool for the study of aging biology.

关键词： Near-infrared Photoacoustic Aging Senescence Tumor Sa-β-gal

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Physicochemical principles of hydrogen metallurgy in blast furnace

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Journal of Iron and Steel Research(International) 2024年第1期31卷 46-63页

作者： Han-jie Guo School of Metallurgical and Ecological Engineering University of Science and Technology BeijingBeijing100083China beijing key laboratory of Special Melting and Preparation of High-End Metal materials Beijing100083China

Based on the stoichiometric method and the free energy minimization method,an ideal model for the reduction of iron oxides by carbon and hydrogen under blast furnace conditions was established,and the reduction efficiency and theoretical energy consumption of the all-carbon blast furnace and the hydrogen-rich blast furnace were compared.The results show that after the reduction reaction is completed at the bottom of the blast furnace,the gas produced by reduction at 1600℃still has a certain excessive reduction capacity,which is due to the hydrogen brought in by the hydrogen-rich blast as well as the excess carbon monoxide generated by the reaction of the coke and the oxygen brought in by the blast.During the process of the gas with excessive reduction capacity rising from the bottom of the blast furnace and gas reduction process,the excessive reduction capacity of the gas gradually decreases with the increase in the dydrogen content in the blast.In the all-carbon blast furnace,the excess gas reduction capacity is the strongest,and the total energy consumption per ton of iron reduction is the lowest.This shows that,for the current operation mode of the blast furnace,adding hydrogen in the blast furnace cannot reduce the consumption of carbon required for reduction per ton of iron,but rather increases the consumption of carbon.

关键词： Hydrogen metallurgy Excess gas reduction capacity Theoretical energy consumption Hydrogen-rich blast furnace Thermodynamic model Gibbs minimum free energy method

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