Wide-temperature applications of sodium-ion batteries(SIBs)are severely limited by the sluggish ion insertion/diffusion kinetics of conversion-type anodes.Quantum-sized transition metal dichalcogenides possess unique ...Wide-temperature applications of sodium-ion batteries(SIBs)are severely limited by the sluggish ion insertion/diffusion kinetics of conversion-type anodes.Quantum-sized transition metal dichalcogenides possess unique advantages of charge delocalization and enrich uncoordinated electrons and short-range transfer kinetics,which are crucial to achieve rapid low-temperature charge transfer and high-temperature interface stability.Herein,a quantum-scale FeS_(2) loaded on three-dimensional Ti_(3)C_(2) MXene skeletons(FeS_(2) QD/MXene)fabricated as SIBs anode,demonstrating impressive performance under wide-temperature conditions(−35 to 65).The theoretical calculations combined with experimental characterization interprets that the unsaturated coordination edges of FeS_(2) QD can induce delocalized electronic regions,which reduces electrostatic potential and significantly facilitates efficient Na+diffusion across a broad temperature range.Moreover,the Ti_(3)C_(2) skeleton reinforces structural integrity via Fe-O-Ti bonding,while enabling excellent dispersion of FeS_(2) QD.As expected,FeS_(2) QD/MXene anode harvests capacities of 255.2 and 424.9 mAh g^(−1) at 0.1 A g^(−1) under−35 and 65,and the energy density of FeS_(2) QD/MXene//NVP full cell can reach to 162.4 Wh kg^(−1) at−35,highlighting its practical potential for wide-temperatures conditions.This work extends the uncoordinated regions induced by quantum-size effects for exceptional Na^(+)ion storage and diffusion performance at wide-temperatures environment.展开更多
Optimizing charge migration and alleviating volume expansion in anode materials are the key to improve the electrochemical performance for sodium-ion storage devices.Herein,a hierarchical porous conducting matrix conf...Optimizing charge migration and alleviating volume expansion in anode materials are the key to improve the electrochemical performance for sodium-ion storage devices.Herein,a hierarchical porous conducting matrix confining defect-rich selenium doped cobalt dichalcogenide(CoSe_(0.5)S_(1.5)/GA)is constructed as a promising SICs anode based on the guidance of theoretical calculation analysis.The increased defect concentration significantly enhanced the disorder degree of the compound and presented electron aggregation around the S atoms,which effectively modulated the electronic structure,further enabling high rate and ultra-capacity sodium storage.Moreover,strong interfacial coupling could construct spatial constraint to alleviate volume expansion as well as maintain electrode integrity and stability.The CoSe_(0.5)S_(1.5)/GA electrode can deliver a high capacity of 310.1 mA h g^(-1)after 2000 cycles at 1 A g^(-1),and the CoSe_(0.5)S_(1.5)/GA//AC sodium ion capacitor can exhibit an outstanding energy density of 237.5 W h kg^(-1).A series of characterization and theoretical calculation convincingly reveal that the defect moieties can regulate the Na^(+)storage and diffusion kinetics,which prove that our defect manufacture coupling with space-confined strategy can provide deep insights into the development of high-performance Na^(+)storage devices.展开更多
This paper characterises and evaluates Si_(3)N_(4)/Ti composites during thermal treatment using an in situ neutron diffraction technique.The composites were developed using a conventional press and sinter technique.Pu...This paper characterises and evaluates Si_(3)N_(4)/Ti composites during thermal treatment using an in situ neutron diffraction technique.The composites were developed using a conventional press and sinter technique.Pure titanium(Ti)was chosen as the matrix,and different concentrations of Si_(3)N_(4)were used as the reinforcement.The effects of sintering temperature and the concentration of Si_(3)N_(4)in the Ti matrix were investigated with respect to phase constituents.The Si_(3)N_(4)mass fraction in the Ti matrix was found to be the key parameter for the reaction.Because of its instability in Ti at higher temperatures,in situ reactions between the reinforcing particles and matrix led to the formation of intermetallic compounds,such as Ti_(5)Si_(3)and possibly Ti3Si,in the composites containing higher weight fractions of Si_(3)N_(4).展开更多
Considering the tremendous applications and purification requirement of acetylene(C_(2)H_(2)),seeking appropriate adsorbents with high capacity and selectivity is a vital task and remains an enduring challenge.Herein,...Considering the tremendous applications and purification requirement of acetylene(C_(2)H_(2)),seeking appropriate adsorbents with high capacity and selectivity is a vital task and remains an enduring challenge.Herein,we designed and synthesized a robust three-dimensional(3D)indium-organic framework([(Me)_(2)NH_(2)][In(L6)_(0.5)(IPA)_(0.5)]·DMA·2H_(2)O(In-L6-IPA,DMA=dimethylammonium,IPA=isopropyl alcohol))featuring two types of one-dimensional(1D)tubular channels.The activated In-L6-IPA displayed high loading for C_(2)H_(2)(104.4 cm^(3)·g^(-1),the second highest value among all reported indium-based metal-organic frameworks(MOFs))and simultaneously selective adsorption for C_(2)H_(2) over CO_(2),C_(2)H_(6),and ethylene(C_(2)H_(4))at 298 K under 100 kPa.Molecular modelling revealed that the porous wall of In-L6-IPA provides more and stronger multiple interactions for C_(2)H_(2) than CO_(2),C_(2)H_(6),and C_(2)H_(4) containing C–H···π,C–H···O,and O···πinteractions.Breakthrough experiments validated the actual separation ability for various ratios of binary C_(2)H_(2)/C_(2)H_(4) and C_(2)H_(2)/CO_(2) mixtures as well as equimolar ternary C_(2)H_(2)/C_(2)H_(4)/CO_(2) and C_(2)H_(2)/C_(2)H_(4)/C_(2)H_(6) mixtures with excellent reusability.展开更多
Erratum to Nano Research,2024,17(4):3139–3146 https://doi.org/10.1007/s12274-023-6061-8 In the first page of the original version of this paper,the corresponding authors should be“Yanwei Sui”and“Lei Hou”,instead...Erratum to Nano Research,2024,17(4):3139–3146 https://doi.org/10.1007/s12274-023-6061-8 In the first page of the original version of this paper,the corresponding authors should be“Yanwei Sui”and“Lei Hou”,instead of“Lei Hou”and“Yao-Yu Wang”.And“Address correspondence to:Lei Hou,lhou2009@nwu.edu.cn;Yao-Yu Wang,wyds123456@outlook.com”should be corrected to“Address correspondence to:Lei Hou,lhou2009@nwu.edu.cn;Yanwei Sui,wyds123456@outlook.com”.展开更多
探索具有优异导电性和稳定性的非贵金属电催化剂对氢经济至关重要.本研究将杂原子掺杂和石墨烯包覆相结合,以控制NiCo_(2)S_(4)(NCS)蛋黄壳微球的电子性能,并抵抗酸性介质中H_(2)O和O_(2)的腐蚀.密度泛函理论(DFT)模拟结合综合表征和实...探索具有优异导电性和稳定性的非贵金属电催化剂对氢经济至关重要.本研究将杂原子掺杂和石墨烯包覆相结合,以控制NiCo_(2)S_(4)(NCS)蛋黄壳微球的电子性能,并抵抗酸性介质中H_(2)O和O_(2)的腐蚀.密度泛函理论(DFT)模拟结合综合表征和实验首次揭示了在NCS中引入P杂原子不仅加速了电子从体相向表面的转移动力学,而且降低了掺杂P原子附近活性S位上的析氢反应势垒.利用DFT计算的穿透能垒预测了rGO覆盖层在P掺杂NCS(P-NCS)表面对质子的渗透性和对H_(2)O和O_(2)分子的抵抗性等重要功能,并用X射线光电子能谱对新催化剂和回收催化剂进行了验证.利用P掺杂剂和rGO覆盖层分别辅助电荷传递和质子传递,通过二者的协同作用获得了催化活性和耐久性之间的平衡.因此,优化后的P-NCS/rGO在70 mV的低过电位下实现了10 mA cm^(-2)的电流密度,并具有令人满意的80小时耐用性.本工作阐明了石墨烯覆盖硫化物催化剂可通过调控电子结构和质子/分子穿透提高电催化性能.展开更多
基金supported by the National Nature Science Foundation of China(Nos.52202335 and 52171227)Natural Science Foundation of Jiangsu Province(No.BK20221137)National Key R&D Program of China(2024YFE0108500).
文摘Wide-temperature applications of sodium-ion batteries(SIBs)are severely limited by the sluggish ion insertion/diffusion kinetics of conversion-type anodes.Quantum-sized transition metal dichalcogenides possess unique advantages of charge delocalization and enrich uncoordinated electrons and short-range transfer kinetics,which are crucial to achieve rapid low-temperature charge transfer and high-temperature interface stability.Herein,a quantum-scale FeS_(2) loaded on three-dimensional Ti_(3)C_(2) MXene skeletons(FeS_(2) QD/MXene)fabricated as SIBs anode,demonstrating impressive performance under wide-temperature conditions(−35 to 65).The theoretical calculations combined with experimental characterization interprets that the unsaturated coordination edges of FeS_(2) QD can induce delocalized electronic regions,which reduces electrostatic potential and significantly facilitates efficient Na+diffusion across a broad temperature range.Moreover,the Ti_(3)C_(2) skeleton reinforces structural integrity via Fe-O-Ti bonding,while enabling excellent dispersion of FeS_(2) QD.As expected,FeS_(2) QD/MXene anode harvests capacities of 255.2 and 424.9 mAh g^(−1) at 0.1 A g^(−1) under−35 and 65,and the energy density of FeS_(2) QD/MXene//NVP full cell can reach to 162.4 Wh kg^(−1) at−35,highlighting its practical potential for wide-temperatures conditions.This work extends the uncoordinated regions induced by quantum-size effects for exceptional Na^(+)ion storage and diffusion performance at wide-temperatures environment.
基金financially supported by the National Nature Science Foundation of China(No.52202335)Natural Science Foundation of Jiangsu Province(No.BK20221137,BK20221139)。
文摘Optimizing charge migration and alleviating volume expansion in anode materials are the key to improve the electrochemical performance for sodium-ion storage devices.Herein,a hierarchical porous conducting matrix confining defect-rich selenium doped cobalt dichalcogenide(CoSe_(0.5)S_(1.5)/GA)is constructed as a promising SICs anode based on the guidance of theoretical calculation analysis.The increased defect concentration significantly enhanced the disorder degree of the compound and presented electron aggregation around the S atoms,which effectively modulated the electronic structure,further enabling high rate and ultra-capacity sodium storage.Moreover,strong interfacial coupling could construct spatial constraint to alleviate volume expansion as well as maintain electrode integrity and stability.The CoSe_(0.5)S_(1.5)/GA electrode can deliver a high capacity of 310.1 mA h g^(-1)after 2000 cycles at 1 A g^(-1),and the CoSe_(0.5)S_(1.5)/GA//AC sodium ion capacitor can exhibit an outstanding energy density of 237.5 W h kg^(-1).A series of characterization and theoretical calculation convincingly reveal that the defect moieties can regulate the Na^(+)storage and diffusion kinetics,which prove that our defect manufacture coupling with space-confined strategy can provide deep insights into the development of high-performance Na^(+)storage devices.
基金the Australian Institute of Nuclear Science and Engineering(AINSE)Ltd.for providing financial assistance(Award No.P7317)to enable work on WOMBAT to be conducted.Peng Cao acknowledges the support from the International Cooperation Programs of Guangzhou City(Grant number 20190710030)Guangdong Province,China(Grant No.108A050506010).
文摘This paper characterises and evaluates Si_(3)N_(4)/Ti composites during thermal treatment using an in situ neutron diffraction technique.The composites were developed using a conventional press and sinter technique.Pure titanium(Ti)was chosen as the matrix,and different concentrations of Si_(3)N_(4)were used as the reinforcement.The effects of sintering temperature and the concentration of Si_(3)N_(4)in the Ti matrix were investigated with respect to phase constituents.The Si_(3)N_(4)mass fraction in the Ti matrix was found to be the key parameter for the reaction.Because of its instability in Ti at higher temperatures,in situ reactions between the reinforcing particles and matrix led to the formation of intermetallic compounds,such as Ti_(5)Si_(3)and possibly Ti3Si,in the composites containing higher weight fractions of Si_(3)N_(4).
基金supported by the Fundamental Research Funds for the Central Universities(No.2022QN1089).
文摘Considering the tremendous applications and purification requirement of acetylene(C_(2)H_(2)),seeking appropriate adsorbents with high capacity and selectivity is a vital task and remains an enduring challenge.Herein,we designed and synthesized a robust three-dimensional(3D)indium-organic framework([(Me)_(2)NH_(2)][In(L6)_(0.5)(IPA)_(0.5)]·DMA·2H_(2)O(In-L6-IPA,DMA=dimethylammonium,IPA=isopropyl alcohol))featuring two types of one-dimensional(1D)tubular channels.The activated In-L6-IPA displayed high loading for C_(2)H_(2)(104.4 cm^(3)·g^(-1),the second highest value among all reported indium-based metal-organic frameworks(MOFs))and simultaneously selective adsorption for C_(2)H_(2) over CO_(2),C_(2)H_(6),and ethylene(C_(2)H_(4))at 298 K under 100 kPa.Molecular modelling revealed that the porous wall of In-L6-IPA provides more and stronger multiple interactions for C_(2)H_(2) than CO_(2),C_(2)H_(6),and C_(2)H_(4) containing C–H···π,C–H···O,and O···πinteractions.Breakthrough experiments validated the actual separation ability for various ratios of binary C_(2)H_(2)/C_(2)H_(4) and C_(2)H_(2)/CO_(2) mixtures as well as equimolar ternary C_(2)H_(2)/C_(2)H_(4)/CO_(2) and C_(2)H_(2)/C_(2)H_(4)/C_(2)H_(6) mixtures with excellent reusability.
文摘Erratum to Nano Research,2024,17(4):3139–3146 https://doi.org/10.1007/s12274-023-6061-8 In the first page of the original version of this paper,the corresponding authors should be“Yanwei Sui”and“Lei Hou”,instead of“Lei Hou”and“Yao-Yu Wang”.And“Address correspondence to:Lei Hou,lhou2009@nwu.edu.cn;Yao-Yu Wang,wyds123456@outlook.com”should be corrected to“Address correspondence to:Lei Hou,lhou2009@nwu.edu.cn;Yanwei Sui,wyds123456@outlook.com”.
基金supported by the National Key R&D Program of China(2021YFA1501900)the National Natural Science Foundation of China-Yunnan Joint Fund(U2102215)+4 种基金the National Natural Science Foundation of China(22209203)China Postdoctoral Science Foundation(2021M693419)Jiangsu Key Laboratory of Coal-based Greenhouse Gas Control and Utilization(PCSX202202)the Material Science and Engineering Discipline Guidance Fund of China University of Mining and Technology(CUMTMS202202 and CUMTMS202207)the Open Sharing Fund for the Large-scale Instruments and Equipment of China University of Mining and Technology。
文摘探索具有优异导电性和稳定性的非贵金属电催化剂对氢经济至关重要.本研究将杂原子掺杂和石墨烯包覆相结合,以控制NiCo_(2)S_(4)(NCS)蛋黄壳微球的电子性能,并抵抗酸性介质中H_(2)O和O_(2)的腐蚀.密度泛函理论(DFT)模拟结合综合表征和实验首次揭示了在NCS中引入P杂原子不仅加速了电子从体相向表面的转移动力学,而且降低了掺杂P原子附近活性S位上的析氢反应势垒.利用DFT计算的穿透能垒预测了rGO覆盖层在P掺杂NCS(P-NCS)表面对质子的渗透性和对H_(2)O和O_(2)分子的抵抗性等重要功能,并用X射线光电子能谱对新催化剂和回收催化剂进行了验证.利用P掺杂剂和rGO覆盖层分别辅助电荷传递和质子传递,通过二者的协同作用获得了催化活性和耐久性之间的平衡.因此,优化后的P-NCS/rGO在70 mV的低过电位下实现了10 mA cm^(-2)的电流密度,并具有令人满意的80小时耐用性.本工作阐明了石墨烯覆盖硫化物催化剂可通过调控电子结构和质子/分子穿透提高电催化性能.
