The activation and reduction of N_(2)to produce ammonia under mild conditions is of great interest,but challenges remain.Here,we report a breakthrough in efficient dinitrogen cleavage by employing small Ptn+(n=1–4)cl...The activation and reduction of N_(2)to produce ammonia under mild conditions is of great interest,but challenges remain.Here,we report a breakthrough in efficient dinitrogen cleavage by employing small Ptn+(n=1–4)clusters and convenient plasma assistance.The reactivity of Pt3+is found to be substantially higher than that of other clusters,and the formed Pt3N7+shows prominent mass abundance among the odd-nitrogen products.We illustrate that a chain reaction path within dual cluster cooperation,especially via a“3+2”mode,is beneficial to N≡N triple bond dissociation,embodying efficient synergistic catalysis.A key intermediate containing a bridged N_(2)of binding with two Pt clusters facilitates N_(2)activation with significantly enhanced interactions between the d orbitals of Pt and the antibondingπ*-orbitals of N_(2).Furthermore,by reacting the Pt_(n)N_(m)+clusters with H_(2),we observed hydrogenation products of both evenand odd-hydrogen species,indicative of ammonia release.The in situ synthesized platinum nitride clusters,typically Pt_(3)N_(7)+,induce a highly active N site for hydrogen anchoring,enabling a cost-effective hydrotreating process for ammonia synthesis.展开更多
This paper presents a single-electromagnet levitation device to measure the densities and detect the internal defects of antimagnetic materials.The experimental device has an electromagnet in its lower part and a pure...This paper presents a single-electromagnet levitation device to measure the densities and detect the internal defects of antimagnetic materials.The experimental device has an electromagnet in its lower part and a pure iron core in the upper part.When the electromagnet is activated,samples can be levitated stably in a paramagnetic solution.Compared with traditional magnetic levitation devices,the single-electromagnet levitation device is adjustable.Different currents,electromagnet shapes,and distances between the electromagnet and iron core are used in the experiment depending on the type of samples.The magnetic field formed by the electromagnet is strong.When the concentration of the MnCl aqueous solution is 3 mol/L,the measuring range of the single-electromagnet levitation device ranges from 1.301 to 2.308 g/cm.However,with the same concentration of MnCl aqueous solution(3 mol/L),the measuring range of a magnetic levitation device built with permanent magnets is only from 1.15 to 1.50 g/cm.The single-electromagnet levitation device has a large measuring range and can realize accurate density measurement and defect detection of high-density materials,such as glass and aluminum alloy.展开更多
Advances in cluster science have enabled the preparation of atomically precise metal clusters with one to a hundred atoms under controllable expansion conditions.After introducing typical gas-phase cluster preparation...Advances in cluster science have enabled the preparation of atomically precise metal clusters with one to a hundred atoms under controllable expansion conditions.After introducing typical gas-phase cluster preparation and reaction apparatuses,this work summarized recent progress in preparing pure metal clusters of single-atom resolution,including neutral and ionic ones,with typical examples of Al,V,Nb,Fe,Co,Ni,Rh,Pt,Ag,Cu,and Pb.With the development of soft-landing deposition technology,the size-selective pure metal clusters with strict atomic precision and predictive property will benefit nanomanufacturing down to atomic and near-atomic scales.This work serves as a modest motivation to stimulate the interest of scientists focusing on interdisciplinary subjects.展开更多
基金This work was financially supported by the National Natural Science Foundation of China(grant nos.21802146 and 21722308)the CAS Key Research Project of Frontier Science(CAS grant no.QYZDB-SSW-SLH024)the Frontier Cross Project of national laboratory for molecular sciences(grant no.051Z011BZ3).
文摘The activation and reduction of N_(2)to produce ammonia under mild conditions is of great interest,but challenges remain.Here,we report a breakthrough in efficient dinitrogen cleavage by employing small Ptn+(n=1–4)clusters and convenient plasma assistance.The reactivity of Pt3+is found to be substantially higher than that of other clusters,and the formed Pt3N7+shows prominent mass abundance among the odd-nitrogen products.We illustrate that a chain reaction path within dual cluster cooperation,especially via a“3+2”mode,is beneficial to N≡N triple bond dissociation,embodying efficient synergistic catalysis.A key intermediate containing a bridged N_(2)of binding with two Pt clusters facilitates N_(2)activation with significantly enhanced interactions between the d orbitals of Pt and the antibondingπ*-orbitals of N_(2).Furthermore,by reacting the Pt_(n)N_(m)+clusters with H_(2),we observed hydrogenation products of both evenand odd-hydrogen species,indicative of ammonia release.The in situ synthesized platinum nitride clusters,typically Pt_(3)N_(7)+,induce a highly active N site for hydrogen anchoring,enabling a cost-effective hydrotreating process for ammonia synthesis.
基金supported by the National Key Research and Development Program of China(2020YFA0714602)the National Natural Science Foundation of China(21802146 and 21722308)+1 种基金National Project Development of Advanced Scientific Instruments Based on Deep Ultraviolet Laser Source(Y31M0112C1)CAS Key Research Project of Frontier Science(QYZDB-SSW-SLH024).
基金support provided by the Key Research and Development Plan of Zhejiang Province(Grant No.2020C01113)the National Natural Science Foundation of China(Grant Nos.51821093 and 51875519)Zhejiang Provincial Natural Science Foundation of China(Grant No.LZ18E050002).
文摘This paper presents a single-electromagnet levitation device to measure the densities and detect the internal defects of antimagnetic materials.The experimental device has an electromagnet in its lower part and a pure iron core in the upper part.When the electromagnet is activated,samples can be levitated stably in a paramagnetic solution.Compared with traditional magnetic levitation devices,the single-electromagnet levitation device is adjustable.Different currents,electromagnet shapes,and distances between the electromagnet and iron core are used in the experiment depending on the type of samples.The magnetic field formed by the electromagnet is strong.When the concentration of the MnCl aqueous solution is 3 mol/L,the measuring range of the single-electromagnet levitation device ranges from 1.301 to 2.308 g/cm.However,with the same concentration of MnCl aqueous solution(3 mol/L),the measuring range of a magnetic levitation device built with permanent magnets is only from 1.15 to 1.50 g/cm.The single-electromagnet levitation device has a large measuring range and can realize accurate density measurement and defect detection of high-density materials,such as glass and aluminum alloy.
基金the Ministry of Science and Technology of the People's Republic of China(No.2020YFA0714602)the National Natural ScienceFoundationof China(Grant No.21722308and 22003072),the Key Research Program of CAS Frontier Sciences(CAS Grant QYZDBSSWSLHO024)+1 种基金the National Project Development of Advanced Scientific Instruments Based on Deep Ultraviolet Laser Source(Y31M0112C1)and the CAS Instrument Development Project(Y5294512C1).
文摘Advances in cluster science have enabled the preparation of atomically precise metal clusters with one to a hundred atoms under controllable expansion conditions.After introducing typical gas-phase cluster preparation and reaction apparatuses,this work summarized recent progress in preparing pure metal clusters of single-atom resolution,including neutral and ionic ones,with typical examples of Al,V,Nb,Fe,Co,Ni,Rh,Pt,Ag,Cu,and Pb.With the development of soft-landing deposition technology,the size-selective pure metal clusters with strict atomic precision and predictive property will benefit nanomanufacturing down to atomic and near-atomic scales.This work serves as a modest motivation to stimulate the interest of scientists focusing on interdisciplinary subjects.
