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Rapid and controllable in-situ self-assembly of main-group metal nanofilms for highly efficient CO_(2)electroreduction to liquid fuel in flow cells

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Nano Research 2024年第6期17卷 5718-5725页

作者： Miao Wang Huaizhu Wang Yaoda Wang Junchuan Liang Mengfei Zhu Jiarui Li Zuoxiu Tie Zhong Jin State key laboratory of Coordination Chemistry MOE Key Laboratory of Mesoscopic ChemistryMOE Key Laboratory of High Performance Polymer Materials and TechnologyJiangsu Key Laboratory of Advanced Organic MaterialsTianchang New Materials and Energy Technology Researc

The electrocatalytic reduction of CO_(2)is a promising pathway to generate renewable fuels and chemicals.However,its advancement is impeded by the absence of electrocatalysts with both high selectivity and stability.Here,we present a scalable in-situ thermal evaporation technique for synthesizing series of Bi,In,and Sn nanofilms on carbon felt(CF)substrates with a high-aspect-ratio structure.The resulting main-group metal nanofilms exhibit a homogeneously distributed and highly exposed catalyst surface with ample active sites,thereby promoting mass transport and ad-/desorption of reaction intermediates.Benefiting from the unique fractal morphology,the Bi nanofilms deposited on CF exhibit optimal catalytic activities for CO_(2)electroreduction among the designed metal nanofilms electrodes,with the highest Faradaic efficiency of 96.9%for formate production at−1.3 V vs.reversible hydrogen electrode(RHE)in H-cell.Under an industrially relevant current density of 221.4 mA·cm−2 in flow cells,the Bi nanofilms retain a high Faradaic efficiency of 81.7%at−1.1 V(vs.RHE)and a good long-term stability for formate production.Furthermore,a techno-economic analysis(TEA)model shows the potential commercial viability of electrocatalytic CO_(2)conversion into formate using the Bi nanofilms catalyst.Our results offer a green and convenient approach for in-situ fabrication of stable and inexpensive thin-film catalysts with a fractal structure applicable to various industrial settings.

关键词： CO_(2)electroreduction non-noble metal nanofilms flow cells efficiency and selectivity techno-economic analysis

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Kinetically and thermodynamically expediting elementary steps via high-valence Cr-incorporated of nickel selenide for water electrolysis

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Nano Research 2024年第3期17卷 1199-1208页

作者： Huafeng Fan Dongxu Jiao Jinchang Fan Dewen Wang Bilal Zaman Wei Zhang Lei Zhang Weitao Zheng Xiaoqiang Cui State key laboratory of Automotive Simulation and Control School of Materials Science and EngineeringKey Laboratory of Automobile Materials of MOEJilin Provincial International Cooperation Key Laboratory of High-Efficiency Clean Energy MaterialsElectron Microscopy CenterJilin UniversityChangchun 130012China College of Chemistry Jilin UniversityChangchun 130012China

Designing high-performance electrocatalysts toward hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)is essential to reduce the activation barrier and optimize free adsorption energy of reactive intermediates.Herein,we report that incorporating high-valence Cr into NiSe_(2)(Cr_(x)Ni_(1-x)Se_(2))kinetically and thermodynamically expedites elementary steps of both HER and OER.The as-prepared Cr_(0.05)Ni_(0.95)Se_(2) catalyst displays excellent HER and OER activities,with low overpotentials of 89 and 272 mV at the current density of 10 mA·cm^(-2)(j10),respectively,and remains stable during operation for 30 h.A low cell voltage of only 1.59 V is required to drive j10 in alkaline media.In situ Raman spectroscopy reveals that Cr incorporation facilitates the formation of NiOOH active species during the OER process.Meanwhile,theoretical explorations demonstrate that high-valence Cr incorporation efficiently accelerates water dissociation kinetics and improves H*adsorption during HER process,lowering the activation barrier of OER and optimizing the adsorption energy of oxygen-based intermediate,thus kinetically and thermodynamically enhancing the intrinsic performance of NiSe_(2) for over water splitting.This strategy provides a new horizon to design transition metal based electrocatalysts in the clean energy field.

关键词： nickel selenide electrocatalytic water splitting high-valence Cr density functional theory(DFT)calculation

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Optimizing high-coordination shell of Co-based single-atom catalysts for efficient ORR and zinc-air batteries

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Journal of Energy Chemistry 2024年第8期95卷 306-314页

作者： Yugang Qi Qing Liang Kexin Song Xinyan Zhou Meiqi Liu Wenwen Li Fuxi Liu Zhou Jiang Xu Zou Zhongjun Chen Wei Zhang Weitao Zheng key laboratory of automobile materials moe School of Materials Science & Engineering Electron Microscopy Center and International Center of Future Science Jilin Provincial International Cooperation Key Laboratory of High-Efficiency Clean Energy Materials Jilin University Institute of High Energy Physics Chinese Academy of Sciences

Atom-level modulation of the coordination environment for single-atom catalysts(SACs) is considered as an effective strategy for elevating the catalytic performance. For the MNxsite, breaking the symmetrical geometry and charge distribution by introducing relatively weak electronegative atoms into the first/second shell is an efficient way, but it remains challenging for elucidating the underlying mechanism of interaction. Herein, a practical strategy was reported to rationally design single cobalt atoms coordinated with both phosphorus and nitrogen atoms in a hierarchically porous carbon derived from metal-organic frameworks. X-ray absorption spectrum reveals that atomically dispersed Co sites are coordinated with four N atoms in the first shell and varying numbers of P atoms in the second shell(denoted as Co-N/P-C).The prepared catalyst exhibits excellent oxygen reduction reaction(ORR) activity as well as zinc-air battery performance. The introduction of P atoms in the Co-SACs weakens the interaction between Co and N,significantly promoting the adsorption process of *OOH, resulting in the acceleration of reaction kinetics and reduction of thermodynamic barrier, responsible for the increased intrinsic activity. Our discovery provides insights into an ultimate design of single-atom catalysts with adjustable electrocatalytic activities for efficient electrochemical energy conversion.

关键词： Electrocatalytic Oxygen reduction reaction Shell coordination optimization Single atom catalyst

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Inhibiting shuttle effect of lithium polysulfides by double metal selenides for high-performance lithium-sulfur batteries

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Rare Metals 2024年第6期43卷 2546-2559页

作者： Lei Li Xue-Jing Yang Yi-Yang Li Bo Jin Hui Liu Meng-Yang Cui Dong-Bo Guan Xing-You Lang Qing Jiang key laboratory of automobile materials Ministry of Educationand College of Materials Science and EngineeringJilin University

Lithium-sulfur batteries（LSBs） have attracted the attention of more and more researchers due to the advantages of high energy density,environmental friendliness,and low production cost.However,the low electronic conductivity of active material and shuttling effect of lithium polysulfides（LiPSs） limit the commercial development of LSBs.To solve these problems,we design a core-shell composite with nitrogen-doped carbon（NC） and two types of selenides（FeSe2-NC@ZnSe-NC）.The FeSe2-NC@ZnSe-NC has a strong adsorption capacity,and can effectively adsorb LiPSs.At the same time,it also effectively alleviates the shuttling effect of LiPSs,and improves the utilization of the active substance during the charge/discharge reaction processes.The mechanism involved in FeSe2-NC@ZnSe-NC is demonstrated by both experiments and density-functional theory（DFT） calculations.The electrochemical test results indicate that LSB with S/FeSe2-NC@ZnSe-NC delivers an initial discharge capacity of 1260 mAh·g-1at 0.2C.And after 500 cycles at 1C,the capacity decay rate per cycle is 0.031%,and the capacity retention rate is 85%.The FeSe2-NC@ZnSe-NC core-shell structure verifies a rational strategy to construct an electrode material for high-performance LSBs.

关键词： Lithium–sulfur batteries Shuttling effect Metal selenide Nitrogen-doped carbon Lithium polysulfides

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Moiré superlattices arising from growth induced by screw dislocations in layered materials

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Chinese Physics B 2024年第7期 82-88页

作者：田伏钰 Muhammad Faizan 贺欣孙远慧张立军 State key laboratory of Integrated Optoelectronics key laboratory of automobile materials of moe and College of materials Science and Engineering Jilin University Suzhou laboratory

Moiré superlattices（MSLs） are modulated structures produced from homogeneous or heterogeneous two-dimensional layers stacked with a twist angle and/or lattice mismatch. Enriching the methods for fabricating MSL and realizing the unique emergent properties are key challenges in its investigation. Here we recommend that the spiral dislocation driven growth is another optional method for the preparation of high quality MSL samples. The spiral structure stabilizes the constant out-of-plane lattice distance, causing the variations in electronic and optical properties. Taking SnS2MSL as an example, we find prominent properties including large band gap reduction（～ 0.4 e V） and enhanced optical activity. Firstprinciples calculations reveal that these unusual properties can be ascribed to the locally enhanced interlayer interaction associated with the Moiré potential modulation. We believe that the spiral dislocation driven growth would be a powerful method to expand the MSL family and broaden their scope of application.

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pH Induced Self-assembly of AIE Fluorescent Probe for Tumor Imaging

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Chinese Journal of Polymer Science 2024年第1期42卷 7-13,I0005页

作者： Jing-Yuan Xiang Wen-Long Zhang He-Ting Li Ya-Ning He Department of Chemical Engineering Key Laboratory of Advanced Materials(MOE)Tsinghua UniversityBejing 100084China

This work reported an AIE fluorescent probe for tumor imaging based on the p H induced self-assembly strategy. The fluorescent probe was composed of an acid-responsive soluble copolymer PEG-b-PAMA-DMMA with a maleic acid amide group and an anionic soluble aggregation-induced emission fluorogen(AIEgen) TPE-2SO_(3)^(-). The polymer could be transformed into a protonated amine-containing polymer after the hydrolysis of maleic acid amide in acidic tumor microenvironment, which would be further self-assembled with TPE-2SO_(3)^(-)to form aggregated nanoparticles. The transition of TPE-2SO_(3)^(-)from dispersed state to aggregated state led to an obvious increase in fluorescence intensity due to its AIE characteristics.

关键词： p H-responsive Self-assembly Fluorescent probe AIE Tumor imaging

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High-frequency magnetic properties of biphase Ce_(2)Fe_(17)N_(3)/α-Fe microflakes with easy-plane anisotropy

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Journal of Rare Earths 2024年第1期42卷 110-115,I0004页

作者： Ke Wang Hang Zhang Yuandong Huang Zhibiao Xu Fashen Li Tao Wang key laboratory for Magnetism and Magnetic materials of moe Lanzhou UniversityLanzhou730000China key laboratory of Special Function materials and Structure Design Ministry of EducationLanzhou UniversityLanzhou730000China

Soft magnetic composites(SMCs)are effective as magnetic powder cores in an inductor.Due to high saturation magnetization,large magnetocrystalline anisotropy and high operating frequency of M(metal)-RE(rear earth)soft magnetic composites,it is possible to miniaturize inductor cores by reducing total loss,especially eddy current loss and excess loss at high frequencies.In this article,the characteristics of Ce_(2)Fe_(17)N_(3)/α-Fe(CFN/F)loss per volume and effective permeability reaching a high frequency of 3 MHz are investigated.The biphase CFN/F composite exhibits a high permeability of 16 at 70 MHz,which is two times greater than that of pure Ce_(2)Fe_(17)N_(3)(CFN)powders.The total loss is as low as 545 mW/cm^(3)at 3 MHz and 6 mT.The direct current(DC)-bias properties have a percent of permeability exceeding 65% at H=7960 A/m.This phenomenon indicates that our material has a higher working frequency and lower core loss than other materials;the biphase CFN/F structure is a promising and efficient approach for developing the miniaturized radio frequency(RF)inductor core.

关键词： High frequency Soft magnetic composites Easy-plane anisotropy Permeability spectra Core loss Rare earths

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Topological laser on square lattice with gain–loss-induced higher-order corner modes

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Chinese Physics B 2024年第6期33卷 189-195页

作者：廖明杰韦梅松王帅领许静平羊亚平 moe key laboratory of Advanced Micro-Structured materials School of Physics Science and EngineeringTongji UniversityShanghai 200092China

We investigate the higher-order topological laser in the two-dimensional(2D) coupled-cavity array. By adding staggered on-site gain and loss to the 2D Hermitian array with a trivial phase, the system will emerge degenerate topological corner modes, which are protected by bulk band gap. For such a non-Hermitian model, by adjusting the parameters of the system and introducing the pumping into the cavity at the corner, a single-mode lasing with topological protection emerges.Furthermore, single-mode lasing exists over a wide range of pumping strengths. No matter where the cavity is initially stimulated, after enough time evolution, all the cavities belonging to the topological corner mode can emit a stable laser.

关键词： topological corner modes nonlinear saturated gain single-mode lasing

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Spin logic devices based on negative differential resistance -enhanced anomalous Hall effect

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International Journal of Minerals,Metallurgy and materials 2024年第6期31卷 1437-1448页

作者： Hongming Mou Ziyao Lu Yuchen Pu Zhaochu Luo Xiaozhong Zhang key laboratory of Advanced materials(moe) School of Materials Science and EngineeringTsinghua UniversityBeijing 100084China State key laboratory of Artificial Microstructure and Mesoscopic Physics School of PhysicsPeking UniversityBeijing 100871China

Owing to rapid developments in spintronics,spin-based logic devices have emerged as promising tools for next-generation computing technologies.This paper provides a comprehensive review of recent advancements in spin logic devices,particularly focusing on fundamental device concepts rooted in nanomagnets,magnetoresistive random access memory,spin–orbit torques,electric-field modu-lation,and magnetic domain walls.The operation principles of these devices are comprehensively analyzed,and recent progress in spin logic devices based on negative differential resistance-enhanced anomalous Hall effect is summarized.These devices exhibit reconfigur-able logic capabilities and integrate nonvolatile data storage and computing functionalities.For current-driven spin logic devices,negative differential resistance elements are employed to nonlinearly enhance anomalous Hall effect signals from magnetic bits,enabling reconfig-urable Boolean logic operations.Besides,voltage-driven spin logic devices employ another type of negative differential resistance ele-ment to achieve logic functionalities with excellent cascading ability.By cascading several elementary logic gates,the logic circuit of a full adder can be obtained,and the potential of voltage-driven spin logic devices for implementing complex logic functions can be veri-fied.This review contributes to the understanding of the evolving landscape of spin logic devices and underscores the promising pro-spects they offer for the future of emerging computing schemes.

关键词： spin logic spin–orbit torque negative differential resistance full-adder

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Supramolecular Bonding Competition Enabled Nanostructure Evolution and Mechanical Reinforcement

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CCS Chemistry 2024年第1期6卷 157-164页

作者： Yuting Wang Peng Meng Aidan Brock Yanan Xu Hang Meng Zixuan Liu Kan Zhang John McMurtrie Jingsan Xu School of Chemistry and Physics and Centre for materials Science Queensland University of TechnologyBrisbaneQueensland 4000 Central Analytical Research Facility Institute for Future EnvironmentsQueensland University of TechnologyBrisbaneQueensland 4000 State key laboratory of Superhard materials Department of Materials Science and Key Laboratory of Automobile MaterialsMOEJilin UniversityChangchun 130012

In this work,competition between different supramolecular interactions is investigated based on a fibrous crystal composed of hydrogen-bonded cyanuric acid(CA)and amidinothiourea(ADT).Melamine(M)is found to prevail over ADT and bond to CA due to its stronger triple H-bonding affiliation,forming hollow microtubes assembled by oriented CAM crystalline arrays,as guided by the directionality of peripheral hydrogen bonds.Furthermore,competitive interaction between hydrogen bonding and ionic/covalent bonding is demonstrated by mixing Ag+ions with the CA-ADT fibers,where sulfur atoms are abstracted from ADT molecules to produce Ag_(2)S ligaments.The in situ-formed Ag_(2)S serves as a binding glue to generate CA-ADT/Ag_(2)S composites with significantly enhanced mechanical strength compared to the pristine CA-ADT fiber pellet.

关键词： supramolecular interaction hydrogen bonds chemical bond competition hollow crystal array organic-inorganic composite

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