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Single-molecule imaging of dinitrogen molecule adsorption on individual iron phthalocyanine

Nano Research 2020年第9期13卷 2393-2398页

作者： Chengding Gu Jia Lin Zhang Jian Qiang Zhong Qian Shen Xiong Zhou Kaidi Yuan Shuo Sun Xu Lian Zhirui Ma Wei Chen Department of Chemistry National University of SingaporeSingapore 117543Singapore Department of Physics National University of SingaporeSingapore 117542Singapore Department of Interface Science Fritz-Haber-Institut der Max-Planck-GesellschaftBerlin 14195Germany Institute of Advanced Materials Nanjing Tech UniversityNanjing 210009China BNLMS College of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China School of Physical Science and Technology Shanghai Tech UniversityShanghai 200031China Joint School of National University of Singapore and Tianjin University International Campus of Tianjin UniversityFuzhou 350207China National University of Singapore(Suzhou)Research Institute Suzhou 215123China

Nitrogen fixation is a vital process for both nature and *** the nitrogenase can reduce nitrogen in ambient environment in nature,the industrialized Haber-Bosch process is a high temperature and high-pressure *** the discovery of the first dinitrogen complex in 1965,many dinitrogen complexes are prepared in a homogeneous solution to mimic the nitrogenase enzyme in ***,studies of the heterogeneous process on surface are rarely ***,molecular scale characterization for such dinitrogen complex is ***,we present a simple model system to investigate,at the single-molecule level,the binding of dinitrogen on a surface confined iron phthalocyanine(FePc)monolayer through the combination of in-situ low-temperature scanning tunneling microscopy(LT-STM)and X-ray photoelectron spectroscopy(XPS)*** iron center in FePc molecule deposited on Au(111)and highly oriented pyrolytic graphite(HOPG)surface can adsorb dinitrogen molecule at room temperature and low pressure.A comparative study reveals that the adsorption behaviors of FePc on these two different substrates are *** bond is formed between the dinitrogen and the Fe atom in the FePc molecule,which greatly modifies the electronic structure of *** bonding is reversible and can be manipulated by applying bias using a STM tip or by thermal annealing.

关键词： single-molecule dinitrogen iron phthalocyanine axial coordination

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Synthesis and Crystal Structure of a Ruthenium(Ⅱ) Compound of dinitrogen

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Chinese Journal of Structural Chemistry 2008年第10期27卷 1167-1170页

作者：阚剑张礼仪文惠敏施林熙陈忠宁 State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterThe Chinese Academy of Sciences

The title compound [Ru（bph）（PPh3）2（N2）]·（PF6）·1.5CH2Cl2 （bph = N-（benzoyl）- N＇-（picolinylidene）-hydrazine） has been prepared and characterized by X-ray diffraction analysis. It crystallizes in the monoclinic system, space group P21/n with a = 13.5201（6）, b = 15.5078（6）, c = 25.0656（13） A, β= 100.257（3）°, C50.50H43Cl3F6N5OP3Ru, Mr= 1150.23, V= 5171.4（4） A3, Z = 4, F（000） = 2332, Dc = 1.477 g/cm^3 and ,μ（MoKa） = 0.615 mm^-1. The structure was refined to R = 0.0524 and wR = 0.1398 for 8060 observed reflections （I 〉 2σ（I））. The Ru-N2 and N-N bond distances are 1.919（4） and 1.133（5）A, respectively.

关键词： crystal structure dinitrogen ruthenium

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dinitrogen Activation by Low-Valent Cobalt-NHC Complexes

Dinitrogen Activation by Low-Valent Cobalt-NHC Complexes

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2018年中西部地区无机化学化工学术研讨会

作者： Liang Deng Yafei Gao Shanghai Institute of Organic Chemistry Chinese Academy of Sciences

Low-valent transition-metal species that concomitantly have low coordination numbers are important reactive species proposed in inert bond-activation reactions. The knowledge on their formation, structure, and reactivity thus lays the basis for many challenging chemical transformations. Aiming to deep our understanding on dinitrogen activation by low-valent iron and cobalt species, we have initiated the study on low-valent iron and cobalt complexes with N-heterocyclic carbenes as supporting ligands. This presentation will introduce our recent studies on the synthesis, structure, and reactivity of two-and three-coordinate iron（0, I） and cobalt（-I, 0, I） complexes（see figure below）. The coordination chemistry of these low-coordinate low-valent species with dinitrogen will be discussed.

关键词： Metal Complex N-Heterocyclic Carbene dinitrogen Small Molecule Activation

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An Empirical Model for dinitrogen Gas Emission from Inland Waters

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Atmospheric and Climate Sciences 2019年第1期9卷 1-25页

作者： Elizabeth Sikar Marco Aurelio dos Santos Ednaldo Oliveira dos Santos Rua Sebastião de Moraes S&#227o Carlos Brazil Energy Planning Program/COPPE/UFRJ Centro de Tecnologia Bloco C Sala 211 Cidade Universitária Rio de Janeiro Brazil Department of Environmental Sciences Federal Rural University of Rio de Janeiro Seropédica Brazil

The motivation to calculate this empirical model resulted from often observing—at the time disconcerting—excess dinitrogen gas (N2 concentration > background concentration) in bubble-gas emission samples, collected primarily for the purpose of carbon budget research, from Brazilian rivers and reservoirs sampled during roughly 100 field surveys lasting 4 days each on average and executed between years 2000 and 2012. We model the (serendipitously) measured dinitrogen gas above environmental concentration (N2aec) escaping in bubbles from Brazilian rivers as a function of dissolved nitrogen (N) in water. To this model, we mathematically add a pre-existing model of diffusively emitted denitrified dinitrogen (also as a function of dissolved N) from streams in the United States of America (USA). The resulting model predicts denitrified dinitrogen water-air emission from inland waters in the USA, China and Germany.

关键词： dinitrogen Gas Emission Inland Waters Bubbles Diffusion Nitrogen Cycle Denitrification

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Functional customization of two-dimensional materials for photocatalytic activation and conversion of inert small molecules in the air

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National Science Open 2023年第2期2卷 46-75页

作者： Ming Cheng Lan Yang Huanhuan Zhang Jingjing Yang Chong Xiao Yi Xie Hefei National Research Center for Physical Sciences at the Microscale University of Science and Technology of ChinaHefei 230026China Institute of Energy Hefei Comprehensive National Science CenterHefei 230031China

Air has the advantage of abundance and easy availability,so it is suitable to be used as a synthetic raw material and energy ***,the triggering of inert small molecules in the air,like O_(2),N2,and CO_(2),is a kinetically complex and energetically challenging multistep *** brings hope for this challenge,but obstacles remain in many ***,aiming at the key difficulties of the photocatalytic activation and conversion of these three inert small molecules,i.e.,regulating electronic structure,active sites,charge carrier separation and mobility,and reaction energy barrier,we propose the concept of functional customization strategy of ultrathin two-dimensional materials for achieving more efficient activation and better performance,including thickness control,vacancy engineering,doping operation,single-atom site fabrication,and composite *** in-depth understanding of the functional customization will provide more profound guidance for designing photocatalysts that specialize in activating and converting inert small molecules.

关键词： inert small molecules photocatalysis functional customization dinitrogen dioxygen carbon dioxide

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