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Nano Research 2021年第12期14卷 4822-4827页

作者： lijun geng Baoqi Yin Hanyu Zhang Zhen-Dong Sun Zhixun Luo School of Physics Shandong UniversityJinan250100China Beijing National Laboratory for Molecular Sciences(BNLMS) State Key Laboratory for Structural Chemistry of Unstable and Stable SpeciesInstitute of ChemistryChinese Academy of SciencesBeijing100190China School of Physics and Electrical Engineering Kashi UniversityKashgar844006China University of Chinese Academy of Sciences Beijing100049China

Due to challenges in preparing pure metal clusters and in controlling reactions,the oxides produced by metal clusters reacting with oxygen are often different from traditional ion-molecule products in the gas phase and their reactivity pattern is also largely unveiled *** this work,utilizing a customized Re-TOFMS having a home-made cluster source and a flow tube reactor,we have observed the gaseous reactions of Nin±clusters with oxygen and found magic clusters of Ni_(13)O_(8)±that dominate the mass *** quantum chemistry calculations,we find that both Ni_(13)O_(8)−and Ni_(13)O_(8)+clusters bear a regular cubic structure with 8 oxygen anchoring the eight angles,however,they have rather different spin *** Ni_(13)O_(8)−clusters have 15 unpaired spin-up electrons exhibiting cubic aromaticity and decent ferromagnetism,while the Ni_(13)O_(8)+clusters take a lower-spin ground state(11 unpaired electrons),with spin-down population on the central Ni atom pertaining to *** is a class of metalloxocube clusters that hold properties of aromaticity and ferromagnetism/ferrimagnetism charcterized by a few spin electrons,which embodies the bonding nature of superatomic compounds and enables to develop cluster-genetic materials of multi-functionality.

关键词： metalloxocube superatomic compounds aromaticity ferromagnetism cluster materials

Plasma-Assisted Dinitrogen Activation via Dual Platinum Cluster Catalysis:A Strategy for Ammonia Synthesis under Mild Conditions

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CCS Chemistry 2023年第3期5卷 682-694页

作者： Chaonan Cui Yuhan Jia Hanyu Zhang lijun geng Zhixun Luo Beijing National Laboratory for Molecular Sciences(BNLMS) State Key Laboratory for Structural Chemistry of Unstable and Stable SpeciesInstitute of ChemistryChinese Academy of SciencesBeijing 100190 University of Chinese Academy of Sciences Beijing 100049

The activation and reduction of N_(2)to produce ammonia under mild conditions is of great interest,but challenges ***,we report a breakthrough in efficient dinitrogen cleavage by employing small Ptn+(n=1–4)clusters and convenient plasma *** 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 *** 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 *** 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.

关键词： dual-metal cluster nitrogen activation ammonia synthesis platinum nitride clusters plasma-assistance

Pure Metal Clusters with Atomic Precision for Nanomanufacturing

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Nanomanufacturing and Metrology 2022年第3期5卷 230-239页

作者： Haiming Wu Hanyu Zhang lijun geng Yuhan Jia Benben Huang Mengzhou Yang Baoqi Yin Xin Lei Zhixun Luo Beijing National Laboratory for Molecular Sciences(BNLMS)and State Key Laboratory for Structural Chemistry of Unstable and Stable Species Institute of ChemistryChinese Academy of SciencesBeijing 100190China University of Chinese Academy of Sciences Beijing 100049China

Advances in cluster science have enabled the preparation of atomically precise metal clusters with one to a hundred atoms under controllable expansion *** 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 *** 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 *** work serves as a modest motivation to stimulate the interest of scientists focusing on interdisciplinary subjects.

关键词： Metal cluster Gas phase Cluster assembly Deposition Printing

Superatomic Signature and Reactivity of Silver Clusters with Oxygen:Double Magic Ag_(17)^– with Geometric and Electronic Shell Closure

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CCS Chemistry 2021年第12期3卷 219-229页

作者： Baoqi Yin Qiuying Du lijun geng Hanyu Zhang Zhixun Luo Si Zhou Jijun Zhao State Key Laboratory for Structural Chemistry of Unstable and Stable Species Institute of ChemistryChinese Academy of SciencesBeijing 100190 University of Chinese Academy of Sciences Beijing 100049 Key Laboratory of Materials Modification by Laser Ion and Electron BeamsMinistry of EducationDalian University of TechnologyDalian 116024

Understanding the stability and reactivity of silver clusters toward oxygen provides insights to design new materials of coinage metals with atomic ***,we report a systematic study on anionic silver clusters,Ag_(n)^(−)(n=10-34),by reacting them with O_(2) under multiple-collision *** spectrometry observation presents the odd-even alternation effect on the reaction rates of these Agn−clusters.

关键词： metal cluster superatom gas-phase reaction Ag_(17)^– shell closure

Formation of Al^(+)(C_(6)H_(6))_(13):The Origin of Magic Number in Metal-Benzene Clusters Determined by the Nature of the Core

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CCS Chemistry 2019年第5期1卷 571-581页

作者： Hanyu Zhang Arthur C.Reber lijun geng Daniel Rabayda Haiming Wu Zhixun Luo Jiannian Yao Shiv N.Khanna Beijing National Laboratory of Molecular sciences(BNLMS) State Key Laboratory for Structural Chemistry of Unstable and Stable SpeciesInstitute of ChemistryChinese Academy of SciencesUniversity of Chinese Academy of SciencesBeijing 100190 Department of Physics Virginia Commonwealth UniversityRichmondVA 23284

The identification of highly abundant,“magic”spe-cies in the mass spectra of clusters have proven to be valuable in nanoscience,leading to the discovery of new stable species such as fullerenes and the elec-tronic s... 详细信息

关键词： magic number benzene cluster noncova-lent interaction Al^(+)(C_(6)H_(6))_(13)

Co13O8—metalloxocubes:a new class of perovskite-like neutral clusters with cubic aromaticity

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National Science Review 2021年第1期8卷 89-97页

作者： lijun geng Mouyi Weng Cong-Qiao Xu Hanyu Zhang Chaonan Cui Haiming Wu Xin Chen Mingyu Hu Hai Lin Zhen-Dong Sun Xi Wang Han-Shi Hu Jun Li Jiaxin Zheng Zhixun Luo Feng Pan Jiannian Yao Beijing National Laboratory for Molecular Sciences (BNLMS) State Key Laboratory for Structural Chemistry of Unstable and Stable Species Institute of Chemistry Chinese Academy of Sciences School of Physics Shandong University School of Advanced Materials Peking University Shenzhen Graduate School Department of Chemistry Southern University of Science and Technology University of Chinese Academy of Sciences School of Physics and Electrical Engineering Kashi University College of Science Beijing Jiaotong University Department of Chemistry and Key Laboratory of Organic Optoelectronics and Molecular Engineering of Ministry of Education Tsinghua University

Exploring stable clusters to understand structural evolution from atoms to macroscopic matter and to construct new materials is interesting yet challenging in chemistry. Utilizing our newly developed deep-ultraviolet laser ionization mass spectrometry technique, here we observe the reactions of neutral cobalt clusters with oxygen and find a very stable cluster species of Co13O8that dominates the mass distribution in the presence of a large flow rate of oxygen gas. The results of global-minimum structural search reveal a unique cubic structure and distinctive stability of the neutral Co13O8cluster that forms a new class of metal oxides that we named as ‘metalloxocubes’. Thermodynamics and kinetics calculations illustrate the structural evolution from icosahedral Co13to the metalloxocube Co13O8with decreased energy, enhanced stability and aromaticity. This class of neutral oxygen-passivated metal clusters may be an ideal candidate for genetic materials because of the cubic nature of the building blocks and the stability due to cubic aromaticity.

关键词： metalloxocube oxygen-passivated metal cluster cubic aromaticity cluster materials magnetic property

Ionization and Dissociation of Benzene and Aniline under Deep Ultraviolet Laser Irradiation

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Chinese Journal of Chemical Physics 2020年第5期33卷 583-589,I0014-I0028,I0078,I0079页

作者： lijun geng Hanyu Zhang Haiming Wu Zhendong Sun Zhixun Luo School of Physics Shandong UniversityJi'nan 250100China Beijing National Laboratory for Molecular Sciences(BNLMS) State Key Laboratory for Structural Chemistry of Unstable and Stable SpeciesInstitute of ChemistryChinese Academy of SciencesBeijing 100190China School of Physics and Electrical Engineering Kashi UniversityKashgar 844006China

We report a study on photo-ionization of benzene and aniline with incidental subsequent dissociation by the customized reflection time-of-flight mass spectrometer utilizing a deep ultraviolet 177.3 nm *** efficient ionization of benzene is observed with a weak C4H3+fragment formed by undergoing disproportional C-C bond *** comparison,a major C5H6+·fragment and a minor C6H6+·radical are produced in the ionization of aniline pertaining to the removal of CNH·and NH·radicals,***-principles calculation is employed to reveal the photo-dissociation pathways of these two molecules having a structural difference of just an amino *** is demonstrated that hydrogen atom transfer plays an important role in the cleavage of C-C or C-N bonds in benzene and aniline *** study is helpful to understand the underlying mechanisms of chemical bond fracture of benzene ring and related aromatic molecules.

关键词： Photo-dissociation Mass spectrometry Benzene Aniline Deep ultraviolet laser C-C bond activation

Co_(12)C_(12)^(-)——金属碳球烯:一种可用于储氢的幻数团簇新物种

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科学通报 2022年第36期67卷 4302-4305页

作者：耿丽君骆智训中国科学院化学研究所分子动态与稳态结构国家重点实验室北京分子科学国家实验室北京100190 中国科学院大学化学学院北京100049

金属碳化物一般具有高强度和高熔点等特点,在电子学和材料学中发挥着重要作用;同时,由于其特殊化学性质也被应用于催化合成有机金属复合物的反应中[1,2],并在储氢材料的开发中展现良好的应用前景[3].众所周知,氢气是满足不断增长的能源... 详细信息

金属碳化物一般具有高强度和高熔点等特点,在电子学和材料学中发挥着重要作用;同时,由于其特殊化学性质也被应用于催化合成有机金属复合物的反应中[1,2],并在储氢材料的开发中展现良好的应用前景[3].众所周知,氢气是满足不断增长的能源需求的可持续解决方案,是替代化石燃料的环境友好型选择.研究人员已经并继续在为开发高效储氢材料以促进氢能利用做出了巨大的努力[4],以期实现碳中和目标.

关键词：金属碳化物储氢材料化石燃料碳中和能源需求环境友好型高熔点

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国外职业教育特色与启示

当代世界 2009年第4期 59-61,64页

作者：耿立军哈尔滨职业技术学院副教授

高等职业教育在德国、瑞士等发达国家都有各自不同的发展方式和特色，其共同特征是在人才培养方面均注重技术应用与开发能力的培养，在教学方式和手段方面也具有很强的实践性。有选择地引入和借鉴国外高等职业教育的有益经验和模式，将... 详细信息

高等职业教育在德国、瑞士等发达国家都有各自不同的发展方式和特色，其共同特征是在人才培养方面均注重技术应用与开发能力的培养，在教学方式和手段方面也具有很强的实践性。有选择地引入和借鉴国外高等职业教育的有益经验和模式，将对中国高等职业教育的发展具有重要意义。

关键词：职业教育特色国外高等职业教育能力的培养发展方式发达国家技术应用人才培养

汉语方言量词重叠AAA式的韵律特征及焦点凸显

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中南大学学报（社会科学版） 2016年第5期22卷 175-181页

作者：耿丽君南京大学文学院江苏南京210046

作为一种构形重叠,量词AAA式主要分布在山东、江苏、安徽等地的胶辽官话、中原官话、江淮官话及其紧邻的吴方言,呈明显的地域类型学特征。这类重叠式是独立的载调单元,属于节奏型变调,受语流中的节奏、语调等韵律因素影响,是句法、形态... 详细信息

作为一种构形重叠,量词AAA式主要分布在山东、江苏、安徽等地的胶辽官话、中原官话、江淮官话及其紧邻的吴方言,呈明显的地域类型学特征。这类重叠式是独立的载调单元,属于节奏型变调,受语流中的节奏、语调等韵律因素影响,是句法、形态与语用互动的结果。AAA式重叠是由超音步构成的韵律词,受不同韵律规则制约,形成韵律特征各异的韵律模块。从音高和时长的凸显实验出发,探讨这类AAA式韵律词作为焦点重音的韵律实现,分析其韵律边界特征;发现其主要是由音域扩展、等时控制和(边界后)韵母段延长的方式,来实现其内部节奏和外部停延的韵律特征,音高落差和音域变化是主要边界信号。

关键词：汉语方言量词AAA式重叠节奏变调韵律单位边界信号焦点凸显