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Synergistic enhancement of alkaline hydrogen evolution reaction by role of Ni-Fe LDH introducing frustrated Lewis pairs via vacancy-engineered

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Chinese Chemical Letters 2025年第3期36卷 512-516页

作者： Mianfeng Li Haozhi Wang Zijun Yang Zexiang Yin Yuan Liu Yingmei Bian Yang Wang Xuerong Zheng Yida Deng State Key Laboratory of Marine Resource Utilization in South China Sea School of Materials Science and EngineeringHainan UniversityHaikou 570228China Tianjin Key Laboratory of Composite and Functional Materials Key Laboratory of Advanced Ceramics and Machining Technology(Ministry of Education)School of Materials Science and EngineeringTianjin UniversityTianjin 300072China

The alkaline hydrogen evolution reaction(HER)is a crucial process for sustainable hydrogen production,yet it requires efficient and stable electrocatalysts to overcome the high activation energy *** article discusses a novel strategy for enhancing the performance of Ni-Fe layered double hydroxide(Ni-Fe LDH)in the alkaline HER by modifying it with a frustrated Lewis acid-base pair(FLP)constructed through vacancy *** study found that the modified Ni-Fe LDH exhibited improved alkaline HER *** functional theory(DFT)calculations demonstrate that the introduction of FLP can activate water and protons more efficiently than monometallic sites,thus reducing the alkaline HER energy barrier and *** HER under alkaline conditions,the Volmer step involves an additional hydrolysis dissociation compared to acidic conditions,which is one of the factors contributing to the slow reaction *** paper demonstrates that FLPs can alter the rate-determining step in alkaline HER from the Volmer step to a step with a lower energy barrier,more suitable for hydrogen *** work provides new insights into the role of FLPs in regulating the mechanism and kinetics of HER and opens a new direction for the design and optimization of LDH-based and other electrocatalysts.

关键词： Ni-Fe LDH Frustrated Lewis acid-base pair Density functional theory The ab initio molecular dynamics The alkaline hydrogen evolution reaction

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Enhancing microwave absorption performance of MoS_(2)by synergistic effect of Fe doping

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Journal of advanced Ceramics 2025年第3期14卷 79-90页

作者： Yuefeng Yan Guangyu Qin Kaili Zhang Boshi Gao Guansheng Ma Xiaoxiao Huang Yu Zhou National Key Laboratory of Precision Welding&Joining of Materials and Structures Harbin Institute of Technology Harbin 150001China School of Materials Science and Engineering Harbin Institute of Technology Harbin 150001China MIIT Key Laboratory of Advanced Structural-Functional Integration Materials&Green Manufacturing TechnologyHarbin Institute of TechnologyHarbin 150001China

Owing to its unique two-dimensional structure and tunable electronic properties,MoS_(2)has emerged as a promising electromagnetic wave(EMW)-absorbing material that can be extensively combined with various other substances to construct effective EMW ***,research on cation substitution doping in MoS_(2)remains relatively limited,which impedes the design and development of high-performance MoS_(2)-based EMW absorbing *** this study,MoS_(2)was synthesized with various concentrations of doped Fe via a facile hydrothermal *** thoroughly investigated the effects of Fe doping,which induced lattice distortion and collapse,triggered a 1T‒2H phase transition,and led to the formation and evolution of second *** modulation of phase transitions,coupled with doping-induced lattice defects that enhance polarization and interfacial polarization from second phases,enabled the Fe-doped MoS_(2)samples to exhibit remarkable EMW absorption ***,the sample FM3 achieved an effective absorption bandwidth(EAB)of 5.1 GHz and a minimum reflection loss(RLmin)of−60.6 dB,underscoring the critical role of Fe doping in increasing the EMW absorption *** research provides valuable pathways and unique insights for the advancement of transition metal dichalcogenides(TMDs)as high-performance EMW-absorbing materials.

关键词： microwave absorption Fe-doped MoS_(2) dielectric property impedance characteristic second phase

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Crystalline@amorphous core-shell structure of WO3@WO_(3-x)S_(x) established via doping strategy for enhancing magnesium ions storage performance

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Journal of Magnesium and Alloys 2025年第3期13卷 1353-1363页

作者： Shiqi Ding Yuxin Tian Jiankang Chen Guofeng Wang Bing Sun He Lv Lei Wang Guicun Li Alan Meng Zhenjiang Li College of Materials Science and Engineering Key Laboratory of Optic-electric Sensing and Analytical Chemistry for Life ScienceMOEShandong Key Laboratory of Biochemical AnalysisCollege of Chemistry and Molecular EngineeringQingdao University of Science and TechnologyQingdao 266042ShandongPR China Qingdao Engineering Research Center for New Metallic Functional Materials Characteristic Laboratory of Advanced Metal Functional Materials and Processing in Universities of ShandongQingdao Binhai UniversityQingdao 266555ShandongPR China

Designing cathode possessing crystalline@amorphous core-shell structure with both active core and shell is a meaningful work for resolving the low speciﬁc capacity,unstable cycling performance and sluggish reaction kinetics issues of rechargeable magnesium batteries(RMBs)by providing more active sites as well as releasing inner stress during ***,WO_(3)@WO_(3-x)S_(x) owning crystalline@amorphous core-shell structure containing both active core and active shell is constructed successfully by introducing S into metastable WO3 structure under temperatureﬁeld *** such structure,amorphous shell would provide continuous Mg^(2+)diffusion channels due to its isotropy property for most Mg^(2+)migrating rapidly to interface and then adsorb at ions reservoir formed by interfacial electricﬁeld for increasing speciﬁc *** also makes security for stable structure of WO_(3)@WO_(3-x)S_(x) by alleviating volume expansion of crystalline core WO_(3) during cycling to prolong cycling ***,“softer”ions S^(2-)would weaken interaction between hard acid Mg2+and ionic lattice to enhance Mg^(2+)storage ***,WO_(3)@WO_(3-x)S_(x) delivers the superior cycling performance(1000 cycles with 83.3%),rate capability(88.5 mAh g^(-1) at 1000 mA g^(-1))and speciﬁc capacity(about 150 mAh g^(-1) at 50 mA g^(-1)),which is near 2 times higher than that of *** is believed that the crystalline@amorphous core-shell structure with both active core and shell designing via doping strategy is enlightening for the development of high-performance RMBs,and such design can be extended to other energy storage devices for better electrochemical performance.

关键词： Doping Sulfuration Crystalline@amorphous core-shell structure WO_(3) Rechargeable magnesium batteries

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Abnormal dielectric behavior of glaserite-type Ba_(3−x)Sr_(x)MgSi_(2)O_(8)solid solution

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Journal of advanced Ceramics 2025年第2期14卷 77-86页

作者： Jiaqing Yang Peng Lei Xiaoqiang Song Changzhi Yin Meng Zhang Weicheng Lei Yiyang Cai Mingfei Cheng Yaodong Liu Zihang Chen Yaqing Hu Wenzhong Lu Wen Lei School of Optical and Electronic Information Key Lab of Functional Materials for Electronic Information(B)of MOEHuazhong University of Science and TechnologyWuhan 430074China Wenzhou Key Laboratory of Microwave Communication Materials and Devices Wenzhou Advanced Manufacturing Institute of HUSTWenzhou 325035China

The temperature coefficient of the resonant frequency(τ_(f))of low-permittivity(ε_(r))microwave dielectric ceramics is required to be near 0 ppm/℃for practical ***,owing to the polarization mechanism,τ_(f)of low-ε_(r)microwave dielectric ceramics is generally ***,a novel microwave dielectric ceramic,Ba_(3−x)Sr_(x)MgSi_(2)O_(8),with an abnormal positiveτ_(f)at the applied temperature is *** this study,Sr^(2+)with a relatively small ionic radius was introduced to replace Ba^(2+),and a single-phase solid solution was formed(x>0.5).Ba_(3−x)Sr_(x)MgSi_(2)O_(8)ceramics were discussed in glaserite-type topology with space groups of P_(3)^(-)for x≤0.5,relatively high symmetry P_(3)^(-)m1 for 0.5functional theory simulation calculations revealed that the preferential occupation of Sr^(2+)ions could decrease the intrinsic formation energy and improve the microwave dielectric properties by mitigating the ionic size mismatch within the crystal *** present research offers a strategy for discovering novel microwave dielectric ceramics with abnormalτ_(f)values,which could serve as τ_(f)regulators in practical applications because of their low cost and excellent microwave dielectric properties.

关键词： microwave dielectric ceramics abnormal dielectric behavior ion size mismatch [SiO4]tetrahedra tilting phase transition density functional theory(DFT)

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Achieving a large field-induced polarization and energy density in BaTiO_(3)films sputter-deposited on Si at 200℃ via a buffer-layer technique

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Journal of advanced Ceramics 2025年第3期14卷 69-78页

作者： Chao Liu Jun Ouyang Yuyao Zhao Hanfei Zhu Hongbu Cheng Zhenyan Liang Li Wang Institute of Advanced Energy Materials and Chemistry Jinan Engineering Laboratory for Multi-scale Functional MaterialsShandong Provincial Key Laboratory of Molecular EngineeringSchool of Chemistry and Chemical EngineeringQilu University of Technology(Shandong Academy of Sciences)Jinan 250353China Key Laboratory of Key Film Materials&Application for Equipments(Hunan Province) Hunan Provincial Key Laboratory of Thin Film Materials and DevicesSchool of Material Sciences and EngineeringXiangtan UniversityXiangtan 411105China Key Laboratory for Liquid–Solid Structure Evolution and Processing of Materials(Ministry of Education) School of Materials Science and EngineeringShandong UniversityJinan 250061China

Ferroelectric oxide films with a large field-induced polarization can be used in dielectric capacitors for charge or energy storage in microelectronic systems and hence have attracted intense research interest.A high processing temperature is usually required to produce a well-crystallized polar phase and hence a large polarization in the film,corresponding to a high charge or energy ***,high processing temperature not only reduces the charge‒discharge efficiency by producing a sizable remnant polarization but is also incompatible with the integration *** this study,we address this problem by creating a large field-induced polarization(~55.8μC/cm^(2))in BaTiO_(3)films sputter-deposited on Si at 200℃ via a buffer-layer *** large polarization led to a high energy density and efficiency(Wrec≈94.7 J/cm^(3),η≈78.2%@4 MV/cm).The thickness of LaNiO_(3)buffer layer was revealed to be the key factor determining the electric polarization(remnant and field-induced ones).A 50 nm LaNiO_(3)thickness,corresponding to the aforementioned polarization and energy storage performance,not only ensures proper crystallization in the BaTiO_(3)film,but also leads to an optimal combination of polycrystalline grains with a high dielectric *** latter accounts for the majority of the field-induced *** results revealed the key role of a buffer layer in tuning the microstructure of a low-temperature deposited ferroelectric oxide ***,the excellent charge/energy storage performance of these 200℃-deposited BaTiO_(3)films has provided many opportunities for this simple dielectric in microelectronics.

关键词： ferroelectric oxide films field-induced polarization BaTiO_(3) LaNiO3 energy density

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Insight into the metal-free electrocatalysis of heteroatom-doped carbon nanocages in competitive CO_(2) reduction and H_(2) evolution

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Nano Research 2025年第2期18卷 255-262页

作者： Liu Jiao Chenghui Mao Biao Feng Fengfei Xu Shuo Li Jun Zhong Mingqi Xia Ruonan Cui Xizhang Wang Lijun Yang Qiang Wu Zheng Hu Key Laboratory of Mesoscopic Chemistry of Ministry of Education(MOE)and Jiangsu Provincial Laboratory for Nanotechnology School of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210023China Institute of Functional Nano and Soft Materials Laboratory(FUNSOM) Jiangsu Key Laboratory of Advanced Negative Carbon TechnologiesSoochow UniversitySuzhou 215123China

Metal-free carbon-based catalysts exhibit diverse electrocatalytic performances in CO_(2) reduction reaction(CO_(2)RR),but the attributions and contributions of active sites are still confusing to ***,the hierarchical carbon nanocages(hCNC)doped with different heteroatoms(B,N,P,S)are prepared to examine the impact of dopants on the competitive CO_(2)RR and hydrogen evolution reaction(HER).The hCNC and P-doped hCNC show little CO_(2)RR activity,B-and S-doped hCNC show weak CO_(2)RR activity,while N-doped hCNC presents high CO_(2)RR *** CO Faradaic efficiency(FECO)of N-containing hCNC increases almost linearly with increasing the N content,even with the co-existing B or P.S and SN-doped hCNC more facilitate the HER.16 doping configurations are constructed,and up to 53 sites are examined CO_(2) H2O H2 CO*H*COOH*CO for the electrochemical activities with a constant potential modelling *** pyridinic-N(N^(*))is the best active site for CO_(2)RR to CO,while CBO_(2)H_(2)-1(αC^(*)),CBO_(2)H_(2)-2(γC^(*)),NO-1(βC^(*)),PO_(2)H-3(αC^(*))and SO_(3)H-3(δC^(*))are active for *** optimized FECO achieves 83.6%for N-doped hCNC with 9.54 at.%nitrogen,and S-doped hCNC reaches ca.30 mA·cm^(-2) current density for *** study unveils the structure-performance correlation of heteroatom-doped hCNC,which is conducive to the rational design of advanced metal-free carbon-based catalysts.

关键词： heteroatom-doping metal-free carbon-based catalyst CO_(2)reduction reaction hydrogen evolution reaction active sites density functional theory(DFT)

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Synthesis of Proline-Derived Helical Copolyacetylenes as Chiral Stationary Phases for HPLC Enantioseparation

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Chinese Journal of Polymer Science 2025年第1期43卷 61-69,I0007页

作者： Yue Li Shu-Ming Kang Ge Shi Yi-Fu Chen Bo-Wen Li Jie Zhang Xin-Hua Wan Beijing National Laboratory for Molecular Sciences Key Laboratory of Polymer Chemistry and Physics of Ministry of EducationCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing100871China School of Materials Science and Engineering Henan Joint International Research Laboratory of Living Polymerizations and Functional NanomaterialsHenan Key Laboratory of Advanced Nylon Materials and ApplicationZhengzhou UniversityZhengzhou450001China

A series of optically active copolymers with various feed ratios have been synthesized through helix-sense-selective copolymerization catalyzed by[Rh(norbornadiene)Cl]*** process involves two proline-derived acetylene monomers,(S)-N-(4-chlorophenyl)carbamoyl-2-ethynyl pyrrolidine(MCl)and(S)-N-(tert-butoxycarbonyl)-2-ethynyl pyrrolidine,followed by acidic deprotection and *** copolymers adopt helical conformations with a preferred handedness,as demonstrated by nuclear magnetic resonance spectroscopy and a series of spectroscopic *** chiroptical activity intensity of copolymer has been found to increase with MCl ***,the enantioseparation capabilities of copolymers containing 95 mol%,90 mol%,and 85 mol%MCl units have been assessed as chiral stationary phases in high-performance liquid chromatography because of their good chiroptical *** chiral stationary phases effectively enantioseparate racemic alcohols,sulfoxides,amides,and metal ***,the copolymer with 90 mol%MCl shows superior chiral recognition ability,especially for 1-(2,4-dichlorophenyl)-2-(1H-imidazol-1-yl)ethanol(α=1.19)and 4-methylbenzenesulfinamide(α=1.47).Insights from molecular dynamic simulation and autodock analysis indicate that hydrogen bonding andπ-πstacking interactions between the chiral stationary phases and enantiomers play a key role for successful chiral *** contribution not only demonstrates the importance of hydrogen bonding donor and copolymer chiroptical activity of chiral stationary phases for chiral resolution,but will also provide valuable insights for the future development of novel stationary phases.

关键词： Helical copolyacetylene Chiral stationary phase High performance liquid chromatography Enantioseparation Hydrogen bonding

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Developing High-Energy, Stable All-Solid-State Lithium Batteries Using Aluminum-Based Anodes and High-Nickel Cathodes

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Nano-Micro Letters 2025年第1期17卷 1-15页

作者： Wu, Xin Wang, Meiyu Pan, Hui Sun, Xinyi Tang, Shaochun Zhou, Haoshen He, Ping Center of Energy Storage Materials & Technology Department of Energy Science and Engineering College of Engineering and Applied Sciences Jiangsu Key Laboratory of Artificial Functional Materials National Laboratory of Solid-State Microstructures and Collaborative Innovation Center of Advanced Microstructures Nanjing University Nanjing210093 China Department of Materials Science and Engineering College of Engineering and Applied Sciences Jiangsu Key Laboratory of Artificial Functional Materials National Laboratory of Solid-State Microstructures and Collaborative Innovation Center of Advanced Microstructures Nanjing University Nanjing210093 China

Aluminum (Al) exhibits excellent electrical conductivity, mechanical ductility, and good chemical compatibility with high-ionic-conductivity electrolytes. This makes it more suitable as an anode material for all-solid-state lithium batteries (ASSLBs) compared to the overly reactive metallic lithium anode and the mechanically weak silicon anode. This study finds that the pre-lithiated Al anode demonstrates outstanding interfacial stability with the Li6PS5Cl (LPSCl) electrolyte, maintaining stable cycling for over 1200 h under conditions of deep charge–discharge. This paper combines the pre-lithiated Al anode with a high-nickel cathode, LiNi0.8Co0.1Mn0.1O2, paired with the highly ionic conductive LPSCl electrolyte, to design an ASSLB with high energy density and stability. Using anode pre-lithiation techniques, along with dual-reinforcement technology between the electrolyte and the cathode active material, the ASSLB achieves stable cycling for 1000 cycles at a 0.2C rate, with a capacity retention rate of up to 82.2%. At a critical negative-to-positive ratio of 1.1, the battery’s specific energy reaches up to 375 Wh kg−1, and it maintains over 85.9% of its capacity after 100 charge–discharge cycles. This work provides a new approach and an excellent solution for developing low-cost, high-stability all-solid-state batteries. (Figure presented.) © The Author(s) 2025.

关键词： Solid-State Batteries

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Enhancing performance of fullerene-based organic electrochemical transistors via side-chain engineering

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Nano Research 2025年第2期18卷 905-912页

作者： Wenxin Fang Zijie Li Chengdong Wang Xiaowei Zhao Junyu Li Gang Ye Fengwei Huo Li Qiu Yanxi Zhang Wei Huang Institute of Flexible Electronics(IFE Future Technologies)Xiamen UniversityXiamen 361005China Yunnan Key Laboratory of Electromagnetic Materials and Devices National Center for International Research on Photoelectric and Energy MaterialsSchool of Materials and EnergyYunnan UniversityKunming 650091China Sinopec Shanghai Research Institute of Petrochemical Technology Shanghai 201028China Key Laboratory for the Green Preparation and Application of Functional Materials Hubei Key Laboratory of Polymer MaterialsSchool of Materials Science and EngineeringHubei UniversityWuhan 430062China Key Laboratory of Flexible Electronics(KLOFE)&Institute of Advanced Materials(IAM) Jiangsu National Synergetic Innovation Center for Advanced Materials(SICAM)Nanjing Tech University(NanjingTech)Nanjing 211800China Frontiers Science Center for Flexible Electronics MIIT Key Laboratory of Flexible Electronics(KLoFE)Northwestern Polytechnical UniversityXi'an 710072China

The performance of organic electrochemical transistors(OECTs)relies on the interaction between organic semiconductors and ***,hydrophilic ethylene glycol(EG)side chains are incorporated into organic semiconductors to improve the channel’s capacity to absorb ***,the EG substituted organic semiconductors tend to swell when immersed in aqueous electrolytes and exhibit microstructural changes induced by dopant *** our research,we introduce an alkyl spacer to create distance between the fullerene and EG *** approach is designed to reduce the negative effects of swelling and balance the ion and electron *** conducted an analysis of OECTs using four fullerene derivatives:no alkyl spacer,butyl,hexyl,and octyl *** OECTs based on fullerene derivatives with butyl and hexyl spacers exhibit enhanced transconductance(g_(m)=11.8 and 19.4 mS)compared to the ones without alkyl *** has also been observed that the butyl and hexyl spacers lead to a more than tenfold increase in volumetric *** increasing the alkyl spacer(octyl group)leads to no transistor *** study uncovers the relationship between alkyl spacers and the performance of OECTs based on fullerene *** will serve as a guideline for designing n-type small molecules for ***,we showcased the potential of utilizing OECTs based on these fullerene derivatives in cation sensing,which is promising for developing sweat sensors.

关键词： organic electrochemical transistors fullerene derivatives ethylene glycol side chains ion and electron conduction

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Crystalline/Non-Crystalline Carbon Co-Modified Strategy to Construct N,S Co-Doped Carbon Layer Wrapped Fe_(0.95)S_(1.05)/Carbon Nanotubes for Enhanced Lithium Storage Property

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Acta Metallurgica Sinica(English Letters) 2025年第1期38卷 93-101页

作者： Liang Chen Lan−Yun Yang Li−Ting Zeng Xu Liu Xin−Rui Li Yu−Shan Tian Wei Wang Gang−Yong Li Chen−Xi Xu Zhao−Hui Hou Key Laboratory of Hunan Province for Advanced Carbon‒based Functional Materials School of Chemistry and Chemical EngineeringHunan Institute of Science and TechnologyYueyang414006China College of Materials Science and Engineering Central South University of Forestry and TechnologyChangsha410004China

Due to their high theoretical capacity and abundant resources,transition metal sulfides are regarded as a prospering alternative to replace the commercial graphite anode in lithium-ion batteries(LIBs),particularly for large-scale energy storage and conversion ***,low conductivity,easy agglomeration and obvious volume change greatly impede their practical *** this work,a novel crystalline/non-crystalline carbon co-modified strategy is proposed to fabricate N,S co-doped carbon(NSC)layer wrapped Fe_(0.95)S_(1.05)/carbon nanotubes(CNTs)composite(Fe_(0.95)S_(1.05)/CNTs@NSC)through a simple Fenton reaction followed by a sulfurization *** characterizations and analyses reveal that this strategy well combines the advantages of crystalline CNTs and non-crystalline NSC,ensuring good conductivity and a high contribution to capacity from the carbon ***,the joint encapsulation of Fe_(0.95)S_(1.05)by both CNTs and NSC can significantly mitigate the agglomeration and volume change of Fe_(0.95)S_(1.05)during the continuous charge/discharge *** from these advantageous features,the resultant Fe_(0.95)S_(1.05)/CNTs@NSC composite displays much improved cycling stability and rate capability when compared to the ***,our research offers a distinct and innovative approach to design and construct advanced transition metal sulfides/carbon composite anodes for LIBs.

关键词： Lithium-ion batteries Crystalline/non-crystalline carbon Joint encapsulation Fe_(0.95)S_(1.05)/CNTs@NSC Lithium storage property

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