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Pb induced dislocation defects of PtCo systems: Strain-triggered oxygen reduction reaction for PEMFC

Nano Research 2024年第4期17卷 2462-2472页

作者： Chun Jin Qiheng Wang Jingjun Liu Beijing Key laboratory of electrochemical Process and technology for Materials Beijing 100029China Beijing University of Chemical technology Beijing 100029China

Design and development of advanced electrocatalysts with high performance and low Pt consumption are crucial for reducing the kinetic energy barrier of the cathode oxygen reduction reaction(ORR)and improving the efficiency of proton exchange membrane fuel cells(PEMFC).In this study,we demonstrate a Pb-modulated PtCo system for efficient ORR,in which the inclusion of Pb in ternary alloys induces dislocation defects due to the significant difference in atomic radius.Dislocation-PtCoPb was confirmed to exhibit significantly higher ORR activity and stability in acidic ORR.In practical PEMFC applications,it outperforms the corresponding commercial Pt/C with a mass activity of 0.58 A·mgPt^(-1),making it a promising alternative to state-of-the-art Pt-based catalysts.The combination of experimental results and density functional theory(DFT)calculations offers valuable atomic-level insights into the dislocation structures.Pb with a larger atomic radius is located in the lattice stretching region below the dislocation slip plane,forming a structure similar to a Cottrell atmosphere,which reduces the dislocation energy and puts the system in a lower energy state.The Cottrell atmosphere pins the dislocation structure and stabilizes the ternary alloy.By adjusting the amount of added Pb,a moderate level of dislocation density induces a tuned strain effect,thereby enhancing the electrocatalytic mechanism by optimizing the electronic structure of the alloy surface and the adsorption and desorption of oxygen species.This work provides valuable insights into the design and development of lattice dislocation defect structures to trigger strain effects for improving ORR performance.

关键词： dislocation defect strain effect Pb-modulated oxygen reduction reaction

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Novel self-assembled porous yolk-shell NiO nanospheres with excellent electrochromic performance for smart windows

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Particuology 2024年第1期84卷 72-80页

作者： Baoshun Wang Ya Huang Siming Zhao Run Li Di Gao Hairong Jiang Rufan Zhang Beijing Key laboratory of Green Chemical reaction Engineering and technology Department of Chemical EngineeringTsinghua UniversityBeijing100084China

With the rapid development of optoelectronics,electrochromic(EC)materials(ECMs)with the advan-tages of low power consumption,easy viewing,high contrast ratio,etc have attached more and more attention from the fields of smart windows,electronic billboards,emerging wearable and portable electronics,and other next-generation displays.Nickel oxide(NiO)is a promising candidate for high-performance ECMs because of its neutral-colored states and low cost.However,NiO-based ECMs still face the problem of slow switching speed due to their low electrical conductivity and small lattice spacing.Metal-organic frameworks(MOFs)are promising candidates to fabricate hollow and porous transition metal oxides(TMOs)with high ion transport efficiency,excellent specific capacitance,and electrochemical activities.In this work,porous yolk-shell NiO nanospheres(PYS-NiO NSs)were syn-thesized via a solvothermal and subsequent calcination process of Ni-MOF,which exhibited outstanding EC performance.Because the large specific surface areas and hollow porous nanostructures were conducive to ionic transport,PYS-NiO NSs exhibited a fast coloring/bleaching speed(3.6/3.9 s per one coloring/bleaching cycle)and excellent cycling stability(82%of capacity retention after 3000 cycles).These superior EC properties indicated that the PYS-NiO NSs was a promising candidate for high-performance EC devices.This work provides a new and feasible strategy for the efficient preparation of TMOs ECMs with good EC performance,especially fast switching speed.

关键词： Electrochromic Nickel oxide Metal-organic frameworks Hollow structure Smart windows

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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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Lotus root-like RuIr alloys with close-packed(0001)branches:Strain-driven performance for acidic water oxidation

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Journal of Energy Chemistry 2024年第5期92卷 579-590页

作者： Mingyue Xiao Wanli Xu Rongchao Li Yanhui Sun Jingjun Liu Feng Liu Jun Gan Shixin Gao Beijing Key laboratory of electrochemical Process and technology for Materials Beijing University of Chemical TechnologyBeijing 100029China Yunnan Precious Metals Lab Kunming 650100YunnanChina

Achieving composition tunability and structure editability of nanoalloys with high level strain may be an efficient strategy to remarkably boost catalytic performance toward oxygen evolution reaction(OER)in acidic water oxidation.Herein,lotus root-like RuIr alloys with native micro-strain were constructed by an epitaxial growth of Ru-richened hcp-(0001)branches on Ir-richened fcc-(111)seeds using a polyol thermal synthesis strategy.The resultant Ru_(60)Ir_(40) alloy shows an OER overpotential of 197 mV at 10 mA cm^(-2) and a Tafel slope of 46.59 mV dec^(-1),showing no obvious activity decay for 80 h continuous chronopotentiometry test in 0.5 M H_(2)SO_(4).The related characterizations including X-ray absorption fine structure(XAFS)spectroscopy and density functional theory(DFT)calculations show that that the remarkably improved activity of the lotus root-like alloy can be attributed to the(0001)facet-triggered strain,which can efficiently optimize the electronic band structure of the active metal and the weakening of the chemisorption of oxygen-containing substances to boost OER electrocatalysis.Therefore,this work provides a new strategy to designing a class of advanced electrocatalysts with high strain using diverse nanostructures as building materials for carbon-free clean energy conversion systems.

关键词： Rulr alloy Lotusroot-like structure Strain Oxygene volution reaction Activity

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Stretchable and self-healing conductive fibers from hierarchical silver nanowires-assembled network

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Nano Research 2024年第2期17卷 763-770页

作者： Ying-Ying Wu Hong Chen Fan Zhang Pan Guo Haili Qin Huai-Ping Cong Anhui Province Key laboratory of Advanced Catalytic Materials and reaction Engineering School of Chemistry and Chemical EngineeringHefei University of TechnologyHefei 230009China

Conductive fibers(CFs)with features of high conductivity,stretchability,self-healability,and electromechanical stability are key components of the increasingly popular wearable electronics.However,since the lack of structural design of conductive network and interfacial interaction between soft polymer and conductive additives,it is still hard to enable CFs to meet above requirements.Here,we describe a facial drawing method from a hydrogel reservoir which is remolded into ultrathin and stretchable CFs with excellent multi-responsive self-healability.The hydrogel reservoir was fabricated in synergy of an ice-templating method and in situ polymerization using the assembled framework as a crosslinker.Relying on the effective fabrication mechanism,the diameter of CFs could be well-tuned from 90 to 400μm by adjusting the dipping depth of the glass rod,accompanied with conductivity increased from 0.75 to 2.5 S/m.Since the hierarchical network structure was well maintained in the CFs,professional performances have been proved on the stretchability and electromechanical stability.The presence of massive hydrogen bonding and Ag–S bond enabled the CFs with excellent self-healability under the conditions of contact,electric field,and near infrared light,respectively.Excitingly,the CFs with high sensing property could be integrated into an advanced textile sensor through an effective healing-induced integration strategy,demonstrating its great potentials as superior two-dimensional(2D)electronic skins.

关键词： conductive fibers self-assembled silver nanowires Ag–S coordination self-healing flexible sensors

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Dual-filler reinforced PVDF-HFP based polymer electrolyte enabling high-safety design of lithium metal batteries

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Nano Research 2024年第6期17卷 5251-5260页

作者： Chang Fang Kangsheng Huang Jing Zhao Shiqi Tian Hui Dou Xiaogang Zhang Jiangsu Key laboratory of electrochemical Energy Storage Technologies College of Materials Science and TechnologyNanjing University of Aeronautics and AstronauticsNanjing 210016China

Despite the high energy density of lithium metal batteries(LMBs),their application in rechargeable batteries is still hampered due to insufficient safety.Here,we present a novel flame-retardant solid-state electrolyte based on polyvinylidene fluoride-hexafluoropropylene(PVDF-HFP)with nano SiO_(2)aerogel as an inert filler but Li_(6.4)La_(3)Zr_(1.4)Ta_(0.6)O_(12)(LLZTO)as an auxiliary component to enhance the ion conductivity.The introduction of SiO_(2)aerogels imparts the polymer electrolyte with exceptional thermal stability and flame retardancy.Simultaneously,the interaction between hydroxyl groups of SiO_(2)particles and PVDF-HFP creates a strong cross-linking structure,enhancing the mechanical strength and stability of the electrolyte.Furthermore,the presence of SiO_(2)aerogel and LLZTO facilitates the dissociation of lithium salts through Lewis acid-base interactions,resulting in a high ionic conductivity of 1.01×10^(−3)S·cm^(−1)and a wide electrochemical window of~5.0 V at room temperature for the prepared electrolytes.Remarkably,the assembled Li|Li cell demonstrates the excellent resistance to lithium dendrite and runs stablly for over 1500 h at a current density of 0.25 mA·cm^(−2).Thus,we prepare a pouch cell with high safety,which can work normally after short-circuiting under the external folding and cutting.

关键词： polymer electrolyte SiO_(2)/Li_(6.4)La_(3)Zr_(1.4)Ta_(0.6)O_(12)(LLZTO)dual-filler non-flammable long cycle life lithium metal battery

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Bifunctional interstitial phosphorous doping strategy boosts platinum-zinc alloy for efficient ammonia oxidation reaction and hydrogen evolution reaction

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Nano Research 2024年第3期17卷 1182-1189页

作者： Tianqi Yu Kexin Tan Jia Wu Yongjin Zou Shibin Yin Guangxi Key laboratory of electrochemical Energy Materials School of Chemistry and Chemical EngineeringGuangxi UniversityNanning 530004China Guangxi Key laboratory of Information Materials Guilin University of Electronic TechnologyGuilin 541004China

It is still a lack of bifunctional catalysts for ammonia oxidation reaction(AOR)and hydrogen evolution reaction(HER)due to their different reaction mechanisms.In this work,P is doped into PtZn alloy by calcination with NaH_(2)PO_(2) as P source to induce the lattice tensile strain of Pt and the electronic interaction between P and Zn,which optimizes the AOR and HER activity simultaneously.The sample with the optimal P content can drive the AOR peak current density of 293.6 mA·mgPt^(-1),which is almost 2.7 times of Pt.For HER,the overpotential at^(-1)0 mA·cm^(-2) is only 23 mV with Tafel slope of 34.1 mV·dec^(-1).Furthermore,only 0.59 V is needed to obtain 50 mA·mgPt^(-1) for ammonia electrolysis under a two-electrode system.Therefore,this work shows an ingenious method to design bifunctional catalysts for ammonia electrolysis.

关键词： PtZn alloy phosphorous doping ammonia oxidation reaction hydrogen evolution reaction bifunctional catalyst

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NIR-Ⅱ responsive Janus nanoparticles amplify immunogenic cell death for enhanced cancer immunotherapy

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Science China(Technological Sciences) 2024年第1期67卷 321-329页

作者： CHEN BeiBei GUO KangLi WANG HaoRan XU Fu-Jian WANG JuLin ZHAO NaNa State Key laboratory of Chemical Resource Engineering Beijing University of Chemical TechnologyBeijing 100029China Key laboratory of Biomedical Materials of Natural Macromolecules(Beijing University of Chemical technology) Beijing Laboratory of Biomedical MaterialsBeijing University of Chemical TechnologyBeijing 100029China College of Materials Sciences and Engineering Beijing University of Chemical TechnologyBeijing 100029China Beijing Key laboratory of electrochemical Process and technology for Materials Beijing University of Chemical TechnologyBeijing 100029China

Immunotherapy brings new hope for tumor treatment by inducing immunogenic cell death(ICD)of tumor cells.However,insufficient immunogenicity and low immune response rate greatly limit antitumor immunity.Herein,by optimizing the composition and morphology,the rational design of Janus nanoparticles composed of Fe_(3)O_(4) nanospheres and SiO_(2)nanorods was realized for enhanced cancer immunotherapy through amplified ICD.After glucose oxidase(GOx)was loaded by the Janus nanoparticles,the resultant M-FS-GOx consumes glucose at tumor sites to generate gluconic acid and hydrogen peroxide(H_(2)O_(2))for starvation therapy while the H_(2)O_(2)supply promotes the production of highly toxic·OH to achieve effective chemodynamic therapy(CDT).Under a 1064 nm light irradiation,the photothermal effect of M-FS-GOx enhances the enzyme activity of GOx for improved starvation therapy.Furthermore,both tumor-associated antigens released during the process of ICD and the intrinsic immunoadjuvant property of M-FS-GOx stimulate dendritic cell maturation to activate antitumor immune responses.This work provides a promising strategy for the construction of Janus nanoparticles to achieve enhanced cancer immunotherapy through combination therapy-amplified ICD.

关键词： Janus nanoparticles immunogenic cell death cancer immunotherapy

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Mass transfer enhancement and hydrodynamic performance with wire mesh coupling solid particles in bubble column reactor

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Chinese Journal of Chemical Engineering 2024年第3期67卷 195-205页

作者： Chuanjun Di Jipeng Dong Fei Gao Guanghui Chen Pan Zhang Jianlong Li Key laboratory of Multiphase Flow reaction and Separation Engineering of Shandong Province College of Chemical EngineeringQingdao University of Science and TechnologyQingdao 266042China College of Electromechanical Engineering Qingdao University of Science and TechnologyQingdao 266043China

It is of vital significance to investigate mass transfer enhancements for chemical engineering processes.This work focuses on investigating the coupling influence of embedding wire mesh and adding solid particles on bubble motion and gas-liquid mass transfer process in a bubble column.Particle image velocimetry(PIV)technology was employed to analyze the flow field and bubble motion behavior,and dynamic oxygen absorption technology was used to measure the gas-liquid volumetric mass transfer coefficient(kLa).The effect of embedding wire mesh,adding solid particles,and wire mesh coupling solid particles on the flow characteristic and kLa were analyzed and compared.The results show that the gas-liquid interface area increases by 33%-72%when using the wire mesh coupling solid particles strategy compared to the gas-liquid two-phase flow,which is superior to the other two strengthening methods.Compared with the system without reinforcement,kLa in the bubble column increased by 0.5-1.8 times with wire mesh coupling solid particles method,which is higher than the sum of kLa increases with inserting wire mesh and adding particles,and the coupling reinforcement mechanism for affecting gas-liquid mass transfer process was discussed to provide a new idea for enhancing gas-liquid mass transfer.

关键词： Fluid mechanics Bubble Mass transfer Wire mesh coupling solid particles Particle image velocimetry Hydrodynamics

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Mechanical reliable,NIR light-induced rapid self-healing hydrogel electrolyte towards flexible zinc-ion hybrid supercapacitors with low-temperature adaptability and long service life

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Journal of Energy Chemistry 2024年第5期92卷 63-73页

作者： Tengjia Gao Na Li Yang Yang Jing Li Peng Ji Yunlong Zhou Jianxiong Xu School of Materials and Advanced Manufacturing Hunan Key Laboratory of Electrochemical Green Metallurgy TechnologyHunan University of TechnologyZhuzhou 412007HunanChina School of Life Sciences and Chemistry Hunan Key Laboratory of Biomedical Nanomaterials and DevicesHunan University of TechnologyZhuzhou 412007HunanChina

Hydrogel electrolytes hold great potential in flexible zinc ion supercapacitors(ZICs)due to their high conductivity,good safety,and flexibility.However,freezing of electrolytes at low temperature(subzero)leads to drastic reduction in ionic conductivity and mechanical properties that deteriorates the performance of flexible ZICs.Besides,the mechanical fracture during arbitrary deformations significantly prunes out the lifespan of the flexible device.Herein,a Zn^(2+)and Li^(+)co-doped,polypyrrole-dopamine decorated Sb_(2)S_(3)incorporated,and polyvinyl alcohol/poly(N-(2-hydroxyethyl)acrylamide)double-network hydrogel electrolyte is constructed with favorable mechanical reliability,anti-freezing,and self-healing ability.In addition,it delivers ultra-high ionic conductivity of 8.6 and 3.7 S m^(-1)at 20 and−30°C,respectively,and displays excellent mechanical properties to withstand tensile stress of 1.85 MPa with tensile elongation of 760%,together with fracture energy of 5.14 MJ m^(-3).Notably,the fractured hydrogel electrolyte can recover itself after only 90 s of infrared illumination,while regaining 83%of its tensile strain and almost 100%of its ionic conductivity during−30–60°C.Moreover,ZICs coupled with this hydrogel electrolyte not only show a wide voltage window(up to 2 V),but also provide high energy density of 230 Wh kg^(-1)at power density of 500 W kg^(-1)with a capacity retention of 86.7%after 20,000 cycles under 20°C.Furthermore,the ZICs are able to retain excellent capacity even under various mechanical deformation at−30°C.This contribution will open up new insights into design of advanced wearable flexible electronics with environmental adaptability and long-life span.

关键词： Flexible zinc ion supercapacitor Hydrogel electrolyte Self-healing Anti-freezing

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