Remarkable advances in fast magic-angle spinning(MAS)techniques significantly improve the resolution of^(1)H solid-state nuclear magnetic resonance(NMR)spectra.Here,we introduce a heteronuclear-filtered^(1)H homonucle...Remarkable advances in fast magic-angle spinning(MAS)techniques significantly improve the resolution of^(1)H solid-state nuclear magnetic resonance(NMR)spectra.Here,we introduce a heteronuclear-filtered^(1)H homonuclear multi-quantum(MQ)correlation strategy available at a MAS rate of 100 kHz by combining^(1)H{X}heteronuclear-filtered methods and^(1)H homonuclear MQ correlation experiments.The proposed strategy was applied to selectively extract^(1)H signals of aluminum lactate(Al-Lac)in a mixture of Al-Lac and zinc lactate(Zn-Lac)using 27Al-filtered methods(i.e.,^(1)H{27Al}heteronuclear multiple quantum correlation(HMQC)or^(1)H{27Al}symmetry-based resonance-echo saturationpulse double-resonance(S-RESPDOR)).We demonstrate that incorporating these 27Al-filtered methods into two-dimensional(2D)^(1)He^(1)H double-quantum(DQ)/single-quantum(SQ),triple-quantum(TQ)/SQ,and even three-dimensional(3D)27Al/^(1)H(DQ)/^(1)H(SQ)experiments can facilitate the acquisition of spectra without signal overlap and targeted characterization of the^(1)H species surrounding 27Al sites.The proposed strategy is considered to efficiently extract key structural information from complex spin systems.展开更多
Developing sustainable and clean electrochemical energy conversion technologies is a crucial step in addressing the challenges of energy shortage and environmental pollution. Exploring and developing new electrocataly...Developing sustainable and clean electrochemical energy conversion technologies is a crucial step in addressing the challenges of energy shortage and environmental pollution. Exploring and developing new electrocatalysts with excellent performance and low cost will facilitate the commercial use of these energy conversion technologies. Recently, dual-atom catalysts(DACs) have attracted considerable research interest since they exhibit higher metal atom loading and more flexible active sites compared to single-atom catalysts(SACs). In this paper, the latest preparation methods and characterization techniques of DACs are systematically reviewed. The advantages of homonuclear and heteronuclear DACs and the catalytic mechanism and identification technologies between the two DACs are highlighted. The current applications of DACs in the field of electrocatalysis are summarized. The development opportunities and challenges of DACs in the future are prospected. The ultimate goal is to provide new ideas for the preparation of new catalysts with excellent properties by customizing diatomic catalysts for electrochemical applications.展开更多
The coexisting densities of equilibrium liquid and vapor phases,density profile,interfacial thickness and surface tension of homonuclear diatomic molecular fluids were studied by using the isothermal-isochoric molecul...The coexisting densities of equilibrium liquid and vapor phases,density profile,interfacial thickness and surface tension of homonuclear diatomic molecular fluids were studied by using the isothermal-isochoric molecular dynamics（MD）simulation method.It was found that the equilibrium densities of liquid and vapor phases were in agreement with the results from Monte Carlo（MC）simulation.The thickness of Liquid-vapor interface increased as temperature went up,but surface tension showed the opposite tendency.The influence of temperature on interfacial thickness was stronger in the range of higher reduced temperature.In addition,the molecular anisotropy also had an effect on interfacial properties of homonuclear diatomic molecular fluids.展开更多
We report the experimental preparations of the absolute ground states of 87Rb and 40K atoms （｜F = 1, mF = 1 ） ＋ ｜F = 9/2, rnF ： -9/2）） by means of the radio-frequency and microwave adiabatic rapid passages, an...We report the experimental preparations of the absolute ground states of 87Rb and 40K atoms （｜F = 1, mF = 1 ） ＋ ｜F = 9/2, rnF ： -9/2）） by means of the radio-frequency and microwave adiabatic rapid passages, and the observation of magnetic Feshbach resonances in an ultracold mixture of bosonic STRb and fermionic 40K atoms between 0 T and 6.0 × 10^-2 T, including 7 homonuclear and 4 heteronuclear Feshbach resonances. The resonances are identified by the abrupt trap loss of atoms induced by the strong inelastic three-body collisions. These Feshbach resonances should enable the experimental control of interspecies interactions.展开更多
Geometrical configurations play a crucial role in dual-atom catalysts(DACs)for electrocatalytic applications.Significant progress has been made to design DACs electrocatalysts with various geometri-cal configurations,...Geometrical configurations play a crucial role in dual-atom catalysts(DACs)for electrocatalytic applications.Significant progress has been made to design DACs electrocatalysts with various geometri-cal configurations,but in-depth understanding the relationship between geometrical configurations and metal-metal interaction mechanisms for designing targeted DACs is still required.In this review,the recent progress in engineering of geometrical configurations of DACs is systematically summarized.Based on the polarity of geometrical configuration,DACs can be classified into two different types that are homonuclear and heteronuclear DACs.Furthermore,with regard to the geometrical configurations of the active sites,homonuclear DACs are identified into adjacent and bridged configurations,and heteronuclear DACs can be classified into adjacent,bridged,and separated configurations.Subsequently,metal-metal interactions in DACs with different geometrical configurations are introduced.Additionally,the applications of DACs in different electrocatalytic reactions are discussed,including the oxygen reduction reaction(ORR),oxygen evolution reaction(OER),hydrogen evolution reaction(HER),and other catalysis.Finally,the future challenges and perspectives for advancements in DACs are high-lighted.This review aims to provide inspiration for the design of highly effcient DACs towards energy relatedapplications.展开更多
基金the National Natural Science Foundation of China(Grants,22161132028,221721177,22127801,U1932218 and 21733013)Hubei Provincial Natural Science Foundation(2021CFA021)Youth Innovation Promotion Association,Chinese Academy of Sciences(2019326)。
文摘Remarkable advances in fast magic-angle spinning(MAS)techniques significantly improve the resolution of^(1)H solid-state nuclear magnetic resonance(NMR)spectra.Here,we introduce a heteronuclear-filtered^(1)H homonuclear multi-quantum(MQ)correlation strategy available at a MAS rate of 100 kHz by combining^(1)H{X}heteronuclear-filtered methods and^(1)H homonuclear MQ correlation experiments.The proposed strategy was applied to selectively extract^(1)H signals of aluminum lactate(Al-Lac)in a mixture of Al-Lac and zinc lactate(Zn-Lac)using 27Al-filtered methods(i.e.,^(1)H{27Al}heteronuclear multiple quantum correlation(HMQC)or^(1)H{27Al}symmetry-based resonance-echo saturationpulse double-resonance(S-RESPDOR)).We demonstrate that incorporating these 27Al-filtered methods into two-dimensional(2D)^(1)He^(1)H double-quantum(DQ)/single-quantum(SQ),triple-quantum(TQ)/SQ,and even three-dimensional(3D)27Al/^(1)H(DQ)/^(1)H(SQ)experiments can facilitate the acquisition of spectra without signal overlap and targeted characterization of the^(1)H species surrounding 27Al sites.The proposed strategy is considered to efficiently extract key structural information from complex spin systems.
文摘Developing sustainable and clean electrochemical energy conversion technologies is a crucial step in addressing the challenges of energy shortage and environmental pollution. Exploring and developing new electrocatalysts with excellent performance and low cost will facilitate the commercial use of these energy conversion technologies. Recently, dual-atom catalysts(DACs) have attracted considerable research interest since they exhibit higher metal atom loading and more flexible active sites compared to single-atom catalysts(SACs). In this paper, the latest preparation methods and characterization techniques of DACs are systematically reviewed. The advantages of homonuclear and heteronuclear DACs and the catalytic mechanism and identification technologies between the two DACs are highlighted. The current applications of DACs in the field of electrocatalysis are summarized. The development opportunities and challenges of DACs in the future are prospected. The ultimate goal is to provide new ideas for the preparation of new catalysts with excellent properties by customizing diatomic catalysts for electrochemical applications.
文摘The coexisting densities of equilibrium liquid and vapor phases,density profile,interfacial thickness and surface tension of homonuclear diatomic molecular fluids were studied by using the isothermal-isochoric molecular dynamics（MD）simulation method.It was found that the equilibrium densities of liquid and vapor phases were in agreement with the results from Monte Carlo（MC）simulation.The thickness of Liquid-vapor interface increased as temperature went up,but surface tension showed the opposite tendency.The influence of temperature on interfacial thickness was stronger in the range of higher reduced temperature.In addition,the molecular anisotropy also had an effect on interfacial properties of homonuclear diatomic molecular fluids.
基金supported by the National Natural Science Foundation for Distinguished Young Scholars of China (Grant No. 10725416)the National Basic Research Program of China (Grant No. 2006CB921101)the National Natural Science Foundation of China for Excellent Research Team, China (Grant No. 60821004)
文摘We report the experimental preparations of the absolute ground states of 87Rb and 40K atoms （｜F = 1, mF = 1 ） ＋ ｜F = 9/2, rnF ： -9/2）） by means of the radio-frequency and microwave adiabatic rapid passages, and the observation of magnetic Feshbach resonances in an ultracold mixture of bosonic STRb and fermionic 40K atoms between 0 T and 6.0 × 10^-2 T, including 7 homonuclear and 4 heteronuclear Feshbach resonances. The resonances are identified by the abrupt trap loss of atoms induced by the strong inelastic three-body collisions. These Feshbach resonances should enable the experimental control of interspecies interactions.
基金supported by the Natural Science Foundation of China (22179062,52125202,and U2004209)the Natural Science Foundation of Jiangsu Province (BK20230035)+1 种基金the Fundamental Research Funds for the Central Universities (30922010303)the Intergovernmental Cooperation Projects in the National Key Research and Development Plan of the Ministry of Science and Technology of PRC (2022YFE0196800)
文摘Geometrical configurations play a crucial role in dual-atom catalysts(DACs)for electrocatalytic applications.Significant progress has been made to design DACs electrocatalysts with various geometri-cal configurations,but in-depth understanding the relationship between geometrical configurations and metal-metal interaction mechanisms for designing targeted DACs is still required.In this review,the recent progress in engineering of geometrical configurations of DACs is systematically summarized.Based on the polarity of geometrical configuration,DACs can be classified into two different types that are homonuclear and heteronuclear DACs.Furthermore,with regard to the geometrical configurations of the active sites,homonuclear DACs are identified into adjacent and bridged configurations,and heteronuclear DACs can be classified into adjacent,bridged,and separated configurations.Subsequently,metal-metal interactions in DACs with different geometrical configurations are introduced.Additionally,the applications of DACs in different electrocatalytic reactions are discussed,including the oxygen reduction reaction(ORR),oxygen evolution reaction(OER),hydrogen evolution reaction(HER),and other catalysis.Finally,the future challenges and perspectives for advancements in DACs are high-lighted.This review aims to provide inspiration for the design of highly effcient DACs towards energy relatedapplications.
