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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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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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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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β-C(sp^(3))−H chlorination of amide derivatives via photoinduced copper charge transfer catalysis

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Chinese Chemical Letters 2024年第2期35卷 361-365页

作者： Yuhang He Chao Tian Guanghui An Guangming Li key laboratory of Functional Inorganic Material Chemistry (moe) School of Chemistry and Materials ScienceHeilongjiang UniversityHarbin 150080China

An atom economicβ-C(sp^(3))−H chlorination of amide derivatives has been developed.This mild protocol employs CuCl_(2) instead of palladium catalysts with atom-economic HCl as chlorine sources and enables the late-stage functionalization of medicine derivatives.Mechanism studies suggest a plausible visible light triggered ligand-to-metal charge transfer(LMCT)/1,4-hydrogen atom transfer(HAT)cascade.

关键词： Photoinduced copper catalysis Ligand-to-metal charge transfer 1,4-Hydrogen atom transfer β-Halogenated amide Late-stage functionalization

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Realizing efficient emission and triple-mode photoluminescence switching in air-stable tin(IV)-based metal halides via antimony doping and rational structural modulation

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Aggregate 2024年第1期5卷 257-269页

作者： Xuefei He Hui Peng Qilin Wei Zhijie Zhou Guolun Zhang Zhentao Du Jialong Zhao Bingsuo Zou Department of materials Physics and Chemistry State Key Laboratory of Featured Metal Materials and Life-cycle Safety for Composite StructuresMOE Key Laboratory of New Processing Technology for Nonferrous Metals and Materialsand School of ResourcesEnvironment and MaterialsGuangxi UniversityNanningChina

Recently,many lead-free metal halides with diverse structures and highly efficient emission have been reported.However,their poor stability and single-mode emission color severely limit their applications.Herein,three homologous Sb^(3+)-doped zero-dimensional(0D)air-stable Sn(IV)-based metal halides with different crystal structures were developed by inserting a single organic ligand into SnCl_(4)lattice,which brings different optical properties.Under photoexcitation,(C_(25)H_(22)P)SnC_(l5)@Sb⋅CH_(4O)(Sb^(3+)−1)does not emit light,(C_(25)H_(22)P)_(2)SnC_(l6)@Sb-α(Sb^(3+)−2α)shines bright yellow emission with a photoluminescence quantum yield(PLQY)of 92%,and(C_(25)H_(22)P)_(2)SnC_(l6)@Sb-β(Sb^(3+)−2β)exhibits intense red emission with a PLQY of 78%.The above three compounds show quite different optical properties should be due to their different crystal structures and the lattice distortions.Particularly,Sb^(3+)−1 can be successfully converted into Sb^(3+)−2αunder the treatment of C_(25)H_(22)PCl solution,accompanied by a transition from nonemission to efficient yellow emission,serving as a“turn-on”photoluminescence(PL)switching.Parallelly,a reversible structure conversion between Sb^(3+)−2αand Sb^(3+)−2βwas witnessed after dichloromethane or volatilization treatment,accompanied by yellow and red emission switching.Thereby,a triple-mode tunable PL switching of off-onI-onII can be constructed in Sb^(3+)-doped Sn(IV)-based compounds.Finally,we demonstrated the as-synthesized compounds in fluorescent anticounterfeiting,information encryption,and optical logic gates.

关键词： information encryption Sb^(3+)-doping Sn(IV)-based metal halides structural modulation triple-mode

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Antimony doped CsPbI_(2)Br for high-stability all-inorganic perovskite solar cells

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Nano Research 2024年第3期17卷 1508-1515页

作者： Mengfei Zhu Lina Qin Yuren Xia Junchuan Liang Yaoda Wang Daocheng Hong Yuxi Tian Zuoxiu Tie Zhong Jin State key laboratory of Coordination Chemistry Ministry of Education(MOE)Key Laboratory of Mesoscopic ChemistryMOE Key Laboratory of High Performance Polymer Materials and TechnologyJiangsu Key Laboratory of Advanced Organic MaterialsSchool of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210023China Nanjing Tieming Energy Technology Co. Ltd.Nanjing 210093China Suzhou Tierui New Energy Technology Co. Ltd.Suzhou 215228China

All-inorganic perovskites,adopting cesium(Cs+)cation to completely replace the organic component of A-sites of hybrid organic–inorganic halide perovskites,have attracted much attention owing to the excellent thermal stability.However,all-inorganic iodine-based perovskites generally exhibit poor phase stability in ambient conditions.Herein,we propose an efficient strategy to introduce antimony(Sb^(3+))into the crystalline lattices of CsPbI_(2)Br perovskite,which can effectively regulate the growth of perovskite crystals to obtain a more stable perovskite phase.Due to the much smaller ionic radius and lower electronegativity of trivalent Sb^(3+)than those of Pb^(2+),the Sb^(3+)doping can decrease surface defects and suppress charge recombination,resulting in longer carrier lifetime and negligible hysteresis.As a result,the all-inorganic perovskite solar cells(PSCs)based on 0.25%Sb^(3+)doped CsPbI_(2)Br light absorber and screen-printable nanocarbon counter electrode achieved a power conversion efficiency of 11.06%,which is 16%higher than that of the control devices without Sb^(3+)doping.Moreover,the Sb^(3+)doped all-inorganic PSCs also exhibited greatly improved endurance against heat and moisture.Due to the use of low-cost and easy-to-process nanocarbon counter electrodes,the manufacturing process of the all-inorganic PSCs is very convenient and highly repeatable,and the manufacturing cost can be greatly reduced.This work offers a promising approach to constructing high-stability all-inorganic PSCs by introducing appropriate lattice doping.

关键词： all-inorganic perovskite solar cells Sb doped cesium lead halide perovskites foreign B-site ions hole-conductor-free phase stability improvement

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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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