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Surface reconstruction of heterostructures in alkaline medium towards enhanced electrocatalytic hydrogen evolution

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Rare Metals 2024年第6期43卷 2636-2647页

作者： Ming-Yang Yang Ji Yuan Xue-Lian Fu Jing-Jing Chen Jing Hu Zhou-Guang Lu Chen Liu Guangdong Research Center for Interfacial engineering of Functional materials Shenzhen Key Laboratory of Polymer Science and TechnologyShenzhen Key Laboratory of Energy Electrocatalytic MaterialsCollege of Materials Science and EngineeringShenzhen UniversityShenzhen 518060China Shenzhen key laboratory of Interfacial science and engineering of materials Department of Materials Science and EngineeringSouthern University of Science and TechnologyShenzhen 518055China

Constructing heterostructures has proved to be a successful strategy to fabricate electrocatalysts with high efficiency for water ***,the structure evolution in alkaline hydrogen evolution reaction lacks investigation and the specific active center remains ***,we take the well-designed Ni_(3)S_(2)@VO_(2) heterostructures as a model to investigate the electrocatalytic activity and the surface reconstruction process of heterostructure catalysts in alkaline *** Ni_(3)S_(2)@VO_(2) heterostructures,with Ni_(3)S_(2) nanorods as the core and VO_(2) nanoflakes as the shell,coupled with the high conductive Ni_(3)S_(2),the hydrophilic VO_(2) and modulated electronic structures at the interfaces,exhibited prominent activity and superior stability at various current ***,the ex-situ characterizations confirmed that the surface reconstruction from Ni_(3)S_(2)@VO_(2) into Ni_(3)S_(2)@amorphous-Ni(OH)_(2) in alkaline media could optimize the water dissociation barrier and exposed large active area,thereby contributing to improved electrocatalytic *** study not only introduces novel high-performance electrocatalysts for hydrogen evolution reaction(HER),but also provides a new avenue for re-examining hetero-structural catalysts in alkaline solutions.

关键词： Heterostructures Ni_(3)S_(2)@VO_(2) Surface reconstruction Water dissociation Alkaline hydrogen evolution

Crystalline-amorphous M@MN_x(M=Co,Fe,Ni)encapsulated in nitrogen-doped carbon for enhanced efficient and durable hydrogen evolution reaction

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Rare Metals 2024年第4期43卷 1547-1556页

作者： Yang Yang Xiao-Chuan Duan Shao-Hui Guo Xian-Ming Zhang college of materials science and engineering College of ChemistryKey Laboratory of Interface Science and Engineering in Advanced MaterialsTaiyuan University of TechnologyYuci030600China

Developing earth-abundant electrocatalysts for hydrogen evolution reaction(HER)is important for the sustainable energy ***,efficient and stable heterocatalysts consisting of crystalline-amorphous M@MN_(x)(M=Co,Fe,Ni)encapsulated in N-doped carbon layers supported with N-doped graphene sheets(denoted as M@MN_(x)@NC-NG)are synthesized by facile hydrothermal reaction and nitridation *** the nitriding process,metal ions in M(tzbc)_2(H_(2)O)_4(tzbc=4-(1H-1,2,4-triazol-1-yl)benzoic acid)complexes are reduced to crystalline M cores,accompanied by the formation of amorphous MN_(x)shells;the tzbc ligands are insitu carbonized to form outermost N-doped carbon(NC)layers that connect with inner MN_(x)via M-N-C motifs inherited from the complex precursors and inhibit the transition of MN_(x)from amorphous to crystalline *** Co@CoN_(x)@NC-NG catalyst exhibits excellent HER activity with small overpotentials of 45 and 64 mV at a cathode current density of 10 mA·cm^(-2)and low Tafel slopes of 40 and 85 mV·dec^(-1)in 0.5 mol·L^(-1)H_(2)SO_4 and1.0 mol·L^(-1)KOH electrolytes,*** Co@CoN_(x)@NC-NG retains 97%of the initial overpotential after 100,000 s in both acidic and alkaline *** outstanding HER performance originates from the crystalline-amorphous Co@CoN_(x)that redistributes electrons around the heterointerfaces,facilitating the conversion process of H^(+)/H_(2)O to hydrogen and thereby promoting HER *** outermost NC layers serve as the armor of Co@CoN_(x),and graphene nanosheets act as carriers of egg-like Co@CoN_(x)@NC and conduction paths for electron shuttles,ensuring stable and continuous electrocatalytic hydrogen production.

关键词： Hydrogen evolution reaction Electrocatalysts Iron group metals Heterojunction Crystalline-amorphous structure

An intermittent lithium deposition model based on CuMnbimetallic MOF derivatives for composite lithium anode with ultrahigh areal capacity and current densities

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Nano Research 2024年第4期17卷 2763-2769页

作者： Tao Wei Yanyan Zhou Cheng Sun Xingtong Guo Shoudong Xu Daifen Chen Yongfu Tang School of Energy and Power Jiangsu University of Science and TechnologyZhenjiang 212003China State key laboratory of metastable materials science and technology(MMST) Hebei Key Laboratory of Applied ChemistryYanshan UniversityQinhuangdao 066004China college of materials science and engineering Taiyuan University of TechnologyTaiyuan 030024China

Recently,three-dimensional(3D)conductive frameworks have been chosen as the host for composite lithium(Li)metal anode because of their exceptional electrical conductivity and remarkable thermal and electrochemical ***,Li tends to accumulate on the top of the 3D frameworks with homogenous lithiophilicity and Li dendrite still *** work firstly designed a bimetallic metal-organic framework(MOF)(CuMn-MOF)derived Cu_(2)O and Mn_(3)O_(4) nanoparticles decorated carbon cloth(CC)substrates(CC@Cu_(2)O/Mn_(3)O_(4))to fabricate a composite Li *** to the synergistic effects of lithiophilic Cu_(2)O and Mn_(3)O_(4),the CC@Cu_(2)O/Mn_(3)O_(4)@Li symmetrical cell can afford a prolonged cycling lifespan(1400 h)under an ultrahigh current density and areal capacity(6 mA·cm^(-2)/6 mAh·cm^(-2)).When coupled with the LiFePO_(4)(LFP)cathode,the LFP||CC@Cu_(2)O/Mn_(3)O_(4)@Li full cell demonstrated a superior performance of 89.7 mAh·g^(-1) even at an extremely high current density(10 C).Furthermore,it can also be matched well with LiNi_(0.5)Co^(0).2Mn_(0.3)O_(2)(NCM523)***,to explain the excellent performances of the CC@Cu_(2)O/Mn_(3)O_(4)@Li composite anode,an intermittent model was also *** study offers a novel model that can enhance our comprehension of the Li deposition behavior and pave the way to attain stable and safe Li metal anodes by employing bimetallic MOF-derived materials to construct 3D frameworks.

关键词： lithium metal anode(LMA) three-dimensional(3D)frameworks intermittent lithiophilic model high areal capacity bimetallic metal-organic frameworks(MOFs)

In situ observation of the electrochemical behavior of Li–CO_(2)/O_(2)batteries in an environmental transmission electron microscope

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Carbon Energy 2024年第4期6卷 244-255页

作者： Peng Jia Yunna Guo Dongliang Chen Jingming Yao Xuedong Zhang Jianguo Lu Yuqing Qiao Liqiang Zhang Hebei key laboratory of Applied Chemistry College of Environmental and Chemical EngineeringYanshan UniversityQinhuangdaoChina State key laboratory of metastable materials science and technology Clean Nano Energy CenterYanshan UniversityQinhuangdaoChina State key laboratory of Silicon and Advanced Semiconductor materials School of Materials Science and EngineeringZhejiang UniversityHangzhouChina key laboratory of Low Dimensional materials and Application technology of Ministry of Education School of Materials Science and EngineeringXiangtan UniversityXiangtanChina

Li–CO_(2)/O_(2)batteries,a promising energy storage technology,not only provide ultrahigh discharge capacity but also capture CO_(2)and turn it into renewable *** electrochemical reaction pathways'ambiguity,however,creates a hurdle for their practical *** study used copper selenide(CuSe)nanosheets as the air cathode medium in an environmental transmission electron microscope to in situ study Li–CO_(2)/O_(2)(mix CO_(2)as well as O_(2)at a volume ratio of 1:1)and Li–O_(2)batteries as well as Li–CO_(2)*** discharge reactions take place successively in the Li–CO_(2)/O_(2)–CuSe nanobattery:(I)4Li^(+)+O_(2)+4e^(−)→2Li_(2)O;(II)Li_(2)O+CO_(2)→Li_(2)CO_(3).The charge reaction proceeded via(III)2Li_(2)CO_(3)→4Li^(+)+2CO_(2)+O_(2)+4e^(−).However,Li–O_(2)and Li–CO_(2)nanobatteries showed poor cycling stability,suggesting the difficulty in the direct decomposition of the discharge *** fluctuations of the Li–CO_(2)/O_(2)battery's electrochemistry were also shown to depend heavily on O_(2).The CuSe‐based Li–CO_(2)/O_(2)battery showed exceptional electrochemical *** Li^–CO_(2)/O_(2)battery offered a discharge capacity apex of 15,492 mAh g^(−1) and stable cycling 60 times at 100 mA g^(−1).Our research offers crucial insight into the electrochemical behavior of Li–CO_(2)/O_(2),Li–O_(2),and Li–CO_(2)nanobatteries,which may help the creation of high‐performance Li–CO_(2)/O_(2)batteries for energy storage applications.

关键词： CuSe nanosheets electrochemical reaction in situ environmental transmission electron microscopy Li-CO_(2)battery Li-CO_(2)/O_(2)battery Li-O_(2)battery

Converting intercalation-type cathode in spent lithium-ion batteries into conversion-type cathode

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Nano Research 2024年第5期17卷 4602-4609页

作者： Dingding Zhu Yong Su Jingzhao Chen Xiangze Ou Xuedong Zhang Wen Xie Yuyan Zhou Yunna Guo Qiushi Dai Peng Jia Jitong Yan Lin Geng Baiyu Guo Liqiang Zhang Yongfu Tang Qiao Huang Jianyu Huang School of materials science and engineering Xiangtan UniversityXiangtan 411105China Clean Nano Energy Center State Key Laboratory of Metastable Materials Science and TechnologyYanshan UniversityQinhuangdao 066000China

The widespread applications of lithium-ion batteries(LIBs)generate tons of spent ***,recycling LIBs is of paramount importance in protecting the environment and saving the *** commercialized LIBs mostly adopt layered oxides such as LiCoO_(2)(LCO)or LiNi_(x)Co_(y)Mn_(1-x-y)O_(2)(NMC)as the cathode *** the intercalation-type spent oxides into conversion-type cathodes(such as metal fluorides(MFs))offers a valid recycling strategy and provides substantially improved energy densities for ***,two typical Co-based cathodes,LCO and LiNi_(0.6)Co_(0.2)Mn_(0.2)O_(2)(NMC622),in spent LIBs were successfully converted to CoF_(2) and(Ni_(x)Co_(y)Mn_(z))F_(2) cathodes by a reduction and fluorination *** as converted CoF_(2) and(Ni_(x)Co_(y)Mn_(z))F_(2) delivered cell energy densities of 650 and 700 Wh/kg,*** atomic-level electron microscopy revealed that the used LCO and NMC622 were converted to highly phase pure Co metal and Ni_(0.6)Co_(0.2)Mn_(0.2) alloys in the used graphite-assisted reduction roasting,simultaneously producing the important product of Li_(2)CO_(3) using only environment friendly *** study provided a versatile strategy to convert the intercalation-type Co-based cathode in the spent LIBs into conversion-type MFs cathodes,which offers a new avenue to recycle the spent LIBs and substantially increase the energy densities of next generation LIBs.

关键词： spent lithium-ion batteries recycling energy densities conversion-type cathode

Kinetic-boosted CO_(2) electroreduction to formate via synergistic electric-thermal field on hierarchical bismuth with amorphous layer

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Journal of Energy Chemistry 2024年第3期90卷 233-243,I0007页

作者： Bing Yang Junyi Zeng Zhenlin Zhang Lin Meng Donglin Shi Liang Chen Youju Huang college of Material Chemistry and Chemical EngineeringKey Laboratory of Organosilicon Chemistry and Material TechnologyMinistry of EducationHangzhou Normal UniversityHangzhou 311121ZhejiangChina State key laboratory of metastable materials science and technology College of Materials Science and EngineeringYanshan UniversityQinhuangdao 066004HebeiChina

Electrocatalytic converting CO_(2) into chemical products has emerged as a promising approach to achieving carbon ***,we report a bismuth-based catalyst with high curvature terminal and amorphous layer which fabricated via two-step electrodeposition achieves stable formate output in a wide voltage window of 600 *** Faraday efficiency(FE) of formate reached up to 99.4% at-0.8 V *** and it remained constant for more than 92 h at-15 mA cm^(-2).More intriguingly,FE formate of95.4% can be realized at a current density of industrial grade(-667.7 mA cm^(-2)) in flow *** special structure promoted CO_(2) adsorption and reduced its activation energy and enhanced the electric-thermal field and K^(+) enrichment which accelerated the reaction *** situ spectroscopy and theoretical calculation further confirmed that the introduction of amorphous structure is beneficial to adsorpting CO_(2)and stabling*OCHO *** work provides special insights to fabricate efficient electrocatalysts by means of structural and crystal engineering and makes efforts to realize the industrialization of bismuth-based catalysts.

关键词： CO_(2) electroreduction Hierarchical bismuth Amorphous layer Electric-thermal field Kinetic-boosting

Effect of Ti_(p) Content on the Work Hardening and Softening Behavior of Mg-Zn-Ca Alloy

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Acta Metallurgica Sinica(English Letters) 2024年第3期37卷 551-560页

作者： Jin-Kai Zhang Cui-Ju Wang Yi-Dan Fan Chao Xu Kai-Bo Nie Kun-Kun Deng Shanxi key laboratory of Advanced Magnesium-Based materials College of Materials Science and EngineeringTaiyuan University of TechnologyTaiyuan 030024China School of materials science and engineering Harbin Institute of TechnologyHarbin 150001China

The Ti_(p)/ZX60 composites with different Ti_(p) contents were prepared by semi-solid stirring *** extrusion,the microstructure,work hardening and softening behavior of the Ti_(p)/ZX60 composites were analyzed compared with the ZX60(Mg-6Zn-0.2Ca)*** results showed that the addition of Ti_(p) could not only promote the nucleation of dynamic recrystallized(DRXed)grains,but also be propitious to the refinement of DRXed *** increasing Ti_(p) content,the size of DRXed grains decreased accompanied with increasing volume fraction of DRXed *** the Ti_(p) content increased to 15 vol.%,the average size and volume fraction of DRXed grains reached to~0.32μm and 93.2%,***,both the strength and elongation were improved by the addition of Ti_(p).With increasing content of Ti_(p),a substantial increase in the strength was achieved with little change in the ***,the elongation decreased sharply when the Ti_(p) content further increased to 15 vol.%.The addition of Ti_(p) led to an increase in the work hardening rate,which gradually increased with increasing Ti_(p) ***,the softening rate did not demonstrate the same tendency with increasing Ti_(p) *** the conventional ceramic particles,the Ti_(p) can be deformed in coordination with the matrix alloy,which imparted a higher softening rate to the matrix *** though the softening rate improved as the Ti_(p) content increased from 5 to 10 vol.%,it dropped deeply as the Ti_(p) content increased to 15 vol.%owing to the fracture of Ti_(p) during extrusion.

关键词： Titanium particle content Particle reinforced magnesium matrix composites Work hardening Softening behavior Mechanical properties

Negative enthalpy alloys and local chemical ordering:a concept and route leading to synergy of strength and ductility

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National science Review 2024年第4期11卷 172-184页

作者： Zibing An Tao Yang Caijuan Shi Shengcheng Mao Lihua Wang Ang Li Wei Li Xianmeng Xue Ming Sun Yifan Bai Yapeng He Fuzeng Ren Zhouguang Lu Ming Yan Yang Ren Chain-Tsuan Liu Ze Zhang Xiaodong Han Beijing key Lab of Microstructure and Property of Advanced materials College of Materials Science &Engineering Beijing University of Technology Department of materials science and engineering City University of Hong Kong key laboratory of Partial Acceleration Physics& technology Institute of High Energy PhysicsChinese Academy of Sciences Department of materials science &engineering Southern University of Science and Technology Department of Physics City University of Hong Kong State key laboratory of Silicon materials Department of Materials Science and Engineering Zhejiang University

Solid solutions are ubiquitous in metals and alloys. Local chemical ordering(LCO) is a fundamental sub-nano/nanoscale process that occurs in many solid solutions and can be used as a microstructure to optimize strength and ductility. However, the formation of LCO has not been fully elucidated, let alone how to provide efficient routes for designing LCO to achieve synergistic effects on both superb strength and ductility. Herein, we propose the formation and control of LCO in negative enthalpy alloys. With engineering negative enthalpy in solid solutions, genetic LCO components are formed in negative enthalpy refractory high-entropy alloys(RHEAs). In contrast to conventional ‘trial-and-error' approaches, the control of LCO by using engineering negative enthalpy in RHEAs is instructive and results in superior strength(1160 MPa) and uniform ductility(24.5%) under tension at ambient temperature, which are among the best reported so far. LCO can promote dislocation cross-slip, enhancing the interaction between dislocations and their accumulation at large tensile strains; sustainable strain hardening can thereby be attained to ensure high ductility of the alloy. This work paves the way for new research fields on negative enthalpy solid solutions and alloys for the synergy of strength and ductility as well as new functions.

关键词： negative enthalpy alloys local chemical ordering strength ductility dislocation

Constructing a 3D multichannel structure to enhance performance of Ni–Co–Mn hydroxide electrodes for flexible supercapacitors

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Rare Metals 2024年第1期43卷 148-163页

作者： Zhi-Hui Xu Shi-Shuai Sun Xue-Lei Li Zhi-Hui Zhang Hai-Ying Li Shuang-Ting Ruan Shou-Gen Yin key laboratory of Display materials and Photoelectric Devices(Ministry of Education)and Tianjin key laboratory for Photoelectric materials and Devices School of Materials Science and EngineeringTianjin University of TechnologyTianjin 300384China college of science Tianjin University of TechnologyTianjin 300384China School of materials science and engineering Inner Mongolia University of TechnologyHohhot 010051China

The balancing of the electrochemical performance,mechanical stability,and processing technology for applying supercapacitors to flexible and wearable electronics continues to encounter severe ***,we prepare Ni-Co-Mn hydroxide electrodes with a threedimensional multichannel structure via a simple hydrothermal *** are constructed using vertically contiguous nano sheets with a uniform thickness and rough *** electrodes can provide numerous electroactive sites and accelerate the transmission of electrolyte *** relationship between the structure and electrochemical performances is verified by experiments and theoretical ***-dimensional(2D)planar and one-dimensional(1D)fiber electrodes are prepared using a flexible carbon cloth(CC)and carbon fiber(CF),respectively,as *** assembled quasi-solid-state flexible asymmetric supercapacitor(FASC)with a twodimensional sandwich structure using NiCoMn-OH/CC as the electrode achieves a remarkable energy density of73.8 Wh·kg^(-1)at a power density of 1.03 kW·kg^(-1).The quasi-solid-state FASC with a 1D linear structure using NiCoMn-OH/CF as the electrode also attains a high energy density(12.9 Wh·kg^(-1)at a power density of0.75 W·kg^(-1)).Moreover,the electrochemical performances of the NiCoMn/CC//AC/CC and NiCoMn/CF//AC/CF FASCs are not disturbed at different bending angles(0°,45°,90°,135°and 180°),This indicates the superior flexibility of the *** also assemble a self-powered energy-harvesting storage system by integrating FASCs and commercial solar cells to verify its *** displays sustainable development potential for energy storage.

关键词： Supercapacitors Flexible Ni–Co–Mn hydroxide 3D multichannel structure High performances