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

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

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“Blocking and rebalance” mechanism-guided design strategies of bimetallic doped 2D a-phosphorus carbide as efficient catalysts for N2 electroreduction

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Journal of Energy Chemistry 2024年第10期97卷 68-78页

作者： Cheng He Jianglong Ma Shen Xi Wenxue Zhang State Key laboratory for Mechanical Behavior of materials School of Materials Science and Engineering Xi'an Jiaotong University School of materials science and engineering Chang'an University

Compared to single atom catalysts（SACs）,the introduction of dual atom catalysts（DACs） has a significantly positive effect on improving the efficiency in the electrocatalytic nitrogen reduction reaction（NRR） which provides an environmental alternative to the Haber-Bosch ***,the research on the mechanism and strategy of designing bimetallic combinations for better performance is still in its early ***,based on "blocking and rebalance" mechanism,45 combinations of bimetallic pair doped α-phosphorus carbide（TMATMB@PC） are investigated as efficient NRR catalysts through density functional theory and machine learning *** a multi-step screening,the combinations of TiV,TiFe,MnMo,and FeW exhibit highly efficient catalytic performance with significantly lower limiting potentials（-0.17,-0.18,-0.14,and-0.30 V,respectively）.Excitingly,the limiting potential for CrMo and CrW combinations is 0 V,which are considered to be extremely suitable for the NRR *** mechanism of "blocking and rebalance" is revealed by the exploration of charge transfer for phosphorus atoms in electron blocking ***,the descriptor φ is proposed with machine learning,which provides design strategies and accurate prediction for finding efficient *** work not only offers promising catalysts TMATMB@PC for NRR process but also provides design strategies by presenting the descriptor φ.

关键词： 2D α-phosphorus carbide DACs Inherent attributes Machine learning Nitrogen reduction reaction

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Highly Stretchable and Tunable Thermo-fluorochromic Polymer Elastomer through Eu3+ Dynamic Coordination Cross-linking

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Chinese Journal of Polymer science 2024年第10期42卷 1449-1458页

作者： Qiu-Li Tan Kai Gou Jing-Zhi Tang Ming-Hui Wei Chong Wang Yi-Jing Nie Geng-Sheng Weng School of materials science and Chemical engineering State Key Laboratory Base of Novel Functional Materials and Preparation Science Ningbo University Institute of Polymer materials School of Materials Science and Engineering Jiangsu University

Thermochromic polymers with tunable thermochromism, high stretchability and mechanical strength are of interests for optical information storage and encryption. In this work, we demonstrate a new design of thermo-fluorochromic carboxylated nitrile butadiene rubber(XNBR) elastomer cross-linked by Eu3+-COOH dynamic coordination with deprotonated imidazole (DPIm) as the ancillary ligand. The presence of DPIm not only improves the mechanical strength and stretchability, but also dramatically intensifies the fluorescence emission and lifetime of the Eu-containing elastomer. The elastomer behaves reversible thermo-fluorochromism with easily tunable transition temperature and emission intensity by the simple change of the deprotonation degree of imidazole. The facile tunable thermo-fluorochromism, exceptional mechanical strength, and high stretchability (up to about 5000%) enable the Eu-containing XNBR elastomer with potential applications in soft electronics where optical information storage and encryption are required.

关键词： Dynamic coordination Elastomer Europium Highly stretchable Thermochromism

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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

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Self-Healable and Stretchable PAAc/XG/Bi2Se0.3Te2.7 Hybrid Hydrogel Thermoelectric materials

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Energy & Environmental materials 2024年第2期7卷 184-190页

作者： Jinmeng Li Tian Xu Zheng Ma Wang Li Yongxin Qian Yang Tao Yinchao Wei Qinghui Jiang Yubo Luo Junyou Yang State Key laboratory of materials Processing and Die & Mould Technology School of Materials Science and Engineering Huazhong University of Science and Technology

Thermoelectric power generators have attracted increasing interest in recent years owing to their great potential in wearable electronics power *** is noted that thermoelectric power generators are easy to damage in the dynamic service process,resulting in the formation of microcracks and performance ***,we prepare a new hybrid hydrogel thermoelectric material PAAc/XG/Bi2Se0.3Te2.7by an in situ polymerization method,which shows a high stretchable and self-healable performance,as well as a good thermoelectric *** the sample with Bi2Se0.3Te2.7content of 1.5 wt%(i.e.,PAAc/XG/Bi2Se0.3Te2.7（1.5 wt%）),which has a room temperature Seebeck coefficient of-0.45 mV K-1,and exhibits an opencircuit voltage of-17.91 mV and output power of 38.1 nW at a temperature difference of 40 *** being completely cut off,the hybrid thermoelectric hydrogel automatically recovers its electrical characteristics within a response time of 2.0 s,and the healed hydrogel remains more than 99% of its initial power *** stretchable and self-healable hybrid hydrogel thermoelectric materials show promising potential for application in dynamic service conditions,such as wearable electronics.

关键词： bismuth telluride self healing thermoelectric material

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Enhanced Ion-Selective Diffusion Achieved by Supramolecular Interaction for High Thermovoltage and Thermal Stability

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Energy & Environmental materials 2024年第2期7卷 204-212页

作者： Jiale Ke Xing Zhao Jie Yang Kai Ke Yu Wang Mingbo Yang Wei Yang College of Polymer science and engineering Sichuan University State Key Laboratory of Polymer Materials Engineering

Thermoelectric（TE） generators capable of converting thermal energy into applicable electricity have gained great popularity among emerging energy conversion ***-based ionic thermoelectric（i-TE）materials are promising candidates for energy conversion systems because of their wide sources,innocuity,and low manufacturing ***,common physically crosslinked biopolymer gels induced by single hydrogen bonding or hydrophobic interaction suffer from low differential thermal voltage and poor thermodynamic ***,we develop a novel i-TE gel with supramolecular structures through multiple noncovalent interactions between ionic liquids（ILs） and gelatin molecular *** thermopower and thermoelectric power factor of the ionic gels are as high as 2.83 mV K-1and 18.33 μW m-1K-2,*** quasi-solid-state gelatin-[EMIM]DCA i-TE cells achieve ultrahigh 2 h output energy density(E2h=9.9 mJ m-2) under an optimal temperature ***,the remarkable stability of the supramolecular structure provides the i-TE hydrogels with a thermal stability of up to 80 ℃.It breaks the limitation that biopolymer-based i-TE gels can only be applied in the low temperature range and enables biopolymer-based i-TE materials to pursue better performance in a higher temperature range.

关键词： biopolymer gel ionic liquid multiple noncovalent interactions supramolecular structure thermoelectric conversion

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Critical role of carbon support in metal nanoaggregate facilitating Fe-N-C catalyst for PEM fuel cell application

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Journal of Energy Chemistry 2024年第10期97卷 669-676页

作者： Liming Guo Xin Wan Qingtao Liu Xiaofang Liu Jiaxiang Shang Ronghai Yu Jianglan Shui School of materials science and engineering Beihang University Tianmushan laboratory

Metal nanoaggregates can simultaneously enhance the activity and stability of Fe-N-C catalysts in proton-exchange-membrane fuel cells（PEMFC）.Previous studies on the relevant mechanism have focused on the direct interaction between FeN4active sites and metal ***,the role of carbon support that hosts metal nanoaggregates and active sites has been ***,a Fe-N-C catalyst encapsulating inactive gold nanoparticles is prepared as a model catalyst to investigate the electronic tuning of Au nanoparticles（NPs） towards the carbon *** NPs donate electrons to carbon support,making it rich in π electrons,which reduces the work function and regulates the electronic configuration of the FeN4sites for an enhanced ORR ***,the electron-rich carbon support can mitigate the electron depletion of FeN4sites caused by carbon support oxidation,thereby preserving its high *** yield and accumulation of H2O2are thus alleviated,which delays the oxidation of the catalyst and benefits the *** to the electron-rich carbon support,the composite catalyst achieves a top-level peak power density of 0.74 W/cm2in a 1.5 bar H2-air PEMFC,as well as the improved *** work elucidates the key role of carbon support in the performance enhancement of the FeN-C/metal nanoaggregate composite catalysts for fuel cell application.

关键词： Carbon support Fe-N-C Fuel cells Hetero-structure catalyst Oxygen reduction reaction

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Rheological Behaviors of Polymers with Nanoparticles Tethered at Each End

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Chinese Journal of Polymer science 2024年第3期42卷 400-406,I0009页

作者： Song-Qi Zhang Wen-Qing Wang Jia-Ping Lin Li-Quan Wang Shanghai Key laboratory of Advanced Polymeric materials Key Laboratory for Ultrafine Materials of Ministry of EducationSchool of Materials Science and EngineeringEast China University of Science and TechnologyShanghai 200237China

The polymer with nanoparticles tethered at each end is a unique model for unraveling the effect of chain ends on the polymer dynamics. We investigated the rheological behavior of this kind of polymer by using nonequilibrium molecular dynamics simulation. The effect of polymer lengths and nanoparticle radii on the complex moduli and viscosity was examined. The dependence of complex moduli on the frequency becomes less pronounced as the polymer is short or the nanoparticle is large. The shear thinning behavior was revealed for these systems, and the scaling exponent of complex viscosity with respect to the frequency was found to change from-1/2 to-3/4 as the polymer shortens or the nanoparticle enlarges. The rheological behavior was further explained by analyzing the mean square distance of nanoparticles. The simulation results were compared with the existing experimental finding, showing an agreement. The work provides information for understanding the chain end effect on polymer rheology.

关键词： Polymer rheology Modulus Viscosity Molecular dynamics

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Precise phase adjustment and antibacterial property of copper sulfide particles in confined mesoporous silica nanoreactor

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Particuology 2024年第2期85卷 113-121页

作者： Shiyu Xu Jinyong Wu Zhongzhen Ren Dechao Niu Low Dimensional materials Chemistry laboratory Key Laboratory for Ultrafine Materials of Ministry of EducationFrontier Science Center of the Materials Biology and Dynamic ChemistryShanghai Engineering Research Center of Hierarchical NanomaterialsSchool of Materials Science and EngineeringEast China University of Science and TechnologyShanghai200237China

Bacteria-caused wound infection greatly threatens human health,thus developing an efficient and safe antibacterial agent without drug resistance is still a great ***,a confined vulcanization strategy is proposed to construct copper sulfides-loaded dual-mesoporous silica nanospheres(Cux-Sy@DMSNs)with various crystal phases for reactive oxygen species(ROS)-mediated and photothermal antibacterial *** the pore confinement of DMSNs,the crystal phases of copper sulfides including CuS,Cu_(9)S_(5)and Cui.96S can be easily controlled by changing the vulcanization *** relationships between the crystal phases and photothermal properties as well as peroxidase-like activity of copper sulfides were systematically *** show that the obtained CuS@DMSNs exhibited higher photothermal ability with remarkable photothermal conversion efficiency of 36.86%in the second near-infrared region(NIR-II)and better peroxidase-like activity,compared to those of Cu_(9)S_(5)@DMSNs and Cu_(1.96)S@*** a result,the in vitro experiments showed the good antibacterial effect against both gram-negative *** and gram-positive *** under 1064 nm laser irradiation and the presence of H_(2)O_(2).Besides,the CCK-8 assay indicated that CuS@p-DMSNs have minimal cytotoxicity against normal human umbilical vein endothelial cells at the ranged ***,the resultant CuS@p-DMSNs could act as a promising antibacterial agent for deep wound bacterial infection treatment.

关键词： Copper sulfides Mesoporous silica Photothermal Reactive oxygen species Antibacterial agent

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In situ Hydrothermal Oxidation of Ternary FeCoNi Alloy Electrode for Overall Water Splitting

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Energy & Environmental materials 2024年第2期7卷 165-174页

作者： Yuwei Chen Lixia Yang Chao Li Yuqiu Wu Xiao Lν Hairen Wang Jun'e Qu Key laboratory for the Green Preparation and Application of Functional materials Hubei Key Laboratory of Polymer Materials School of Materials Science and Engineering Hubei University Faculty of Material science and Chemistry China University of Geosciences

Exploring noble metal-free catalyst materials for high efficient electrochemical water splitting to produce hydrogen is strongly desired for renewable energy *** this article,a novel bifunctional catalytic electrode of insitu-grown type for alkaline water splitting based on FeCoNi alloy substrate has been successfully prepared via a facile one-step hydrothermal oxidation route in an alkaline hydrogen peroxide *** shows that the matrix alloy with the atom ratio 4:3:3 of Fe:Co:Ni can obtain the best catalytic performance when hydrothermally treated at 180℃ for18 h in the solution containing 1.8 M hydrogen peroxide and 3.6 M sodium *** as-prepared Fe0.4Co0.3Ni0.3-1.8 electrode exhibits small overpotentials of only 184 and 175 mV at electrolysis current density of10 mA cm-2for alkaline OER and HER processes,*** overall water splitting at electrolysis current density of 10 mA cm-2can be stably delivered at a low cell voltage of 1.62 *** characteristics including the large specific surface area,the high surface nickel content,the abundant catalyst species,the balanced distribution between bivalent and trivalent metal ions,and the strong binding of in-situ naturally growed catalytic layer to matrix are responsible for the prominent catalytic performance of the Fe0.4Co0.3Ni0.3-1.8 electrode,which can act as a possible replacement for expensive noble metal-based materials.

关键词： alkaline water electrolysis bifunctional electrocatalyst FeCoNi alloy hydrothermal oxidation in-situ growing

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