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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 industry.Whereas the nitrogenase can reduce nitrogen in ambient environment in nature,the industrialized Haber-Bosch process is a high temperature and high-pressure process.Since the discovery of the first dinitrogen complex in 1965,many dinitrogen complexes are prepared in a homogeneous solution to mimic the nitrogenase enzyme in nature.However,studies of the heterogeneous process on surface are rarely addressed.Moreover,molecular scale characterization for such dinitrogen complex is lacking.Here,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)measurements.The 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 identical.Chemical bond is formed between the dinitrogen and the Fe atom in the FePc molecule,which greatly modifies the electronic structure of FePc.The 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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Theoretical Study of Electronic Structure, Formation Mechanism and Intramolecular Sulfoxide Imidation Reactivity of iron phthalocyanine Nitrene Complex

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Chinese Journal of Structural Chemistry 2021年第4期40卷 415-423,405页

作者：袁彬彬宋金帅闫雪原肖晗李春森 State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China University of Chinese Academy of Sciences Beijing 100049China Fujian Provincial Key Laboratory of Theoretical and Computational Chemistry Xiamen 361005China

Density functional theory(DFT) calculations are performed to investigate recent experimentally studied ring-closing sulfoxide imidation catalyzed by Fe(Ⅱ)-phthalocyanine(FeⅡPc). Our results reveal that the ground state of iron phthalocyanine nitrene intermediate(PcFeNR, R =(CH_(2))_(3)(SO)Ph), which is believed to mediate the intramolecular imitation, is triplet state featuring a diradical structure. The formation of Pc Fe NR is the result of a denitrification process with a calculated high-barrier of 23.4 kcal/mol which is in good agreement with the experimentally observed high reaction temperature of 100 ℃. The generated Pc Fe NR undergoes a low-barrier intramolecular nucleophilic attack by proximal nitrogen atom on the sulfur accomplishing the cyclization of sulfoxide. This study provides theoretical insights into the mechanism-based design of useful catalysts for nitrene transfer reactions.

关键词： nitrene transfer sulfoxide cyclization iron phthalocyanine DFT reaction mechanism

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An Efficient Bio-inspired Oxygen Reduction Reaction Catalyst:MnO_(x)Nanosheets Incorporated iron phthalocyanine Functionalized Graphene

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能源与环境材料（英文） 2021年第3期4卷 474-480页

作者： Xing Wu Yi Cheng Jean-Pierre Veder San Ping Jiang Department of Environmental Engineering School of Metallurgy and EnvironmentCentral South UniversityChangsha 410083China National Engineering Technology Research Center for Control and Treatment of Heavy-metal Pollution Changsha 410083China John de Laeter Centre Curtin UniversityPerth WA 6102Australia Fuels and Energy Technology Institute Curtin UniversityPerth WA 6102Australia

Oxygen reduction reaction(ORR)catalysts play a critical role in energy storage and conversion devices and have been attracted enormous interests,and however,it remains challenging to develop highly active cheap catalysts in a simple and green route.Inspired by the heme-copper oxidases(HOCs),in which the ORR active center is originated from the incorporation of Fe-N_(4)with copper atom,we here developed a fine manganese oxide nanosheets(MnO_(x)NSs)integrated with iron phthalocyanine(FePc)anchored on highly conductive graphene(MnO_(x)/FePc-G)through a green route only involve ethanol as the reagent.The bio-inspired catalyst MnO_(x)/Fe Pc-G demonstrated high ORR activity with a half-wave potential(E_(1/2))of 0.887 V,about 57 mV more positive than that of Pt/C.And the current density(j)at 0.9 V is about 1.9 m A cm^(-2),which is three times of Pt/C and FePc-G.More importantly,the bio-inspired systems show superior stability in comparison to commercial Pt/C,showing a potential of 0.863 V to deliver a j of 3 mA cm^(-2)after 18000 s polarization,about 80 mV higher than that of 0.783 V for Pt/C.The high activity is contributed by the integration of the Fe Pc and MnO_(x)NSs that plays the role to assist the cleavage of the O_(2)bond.Our approach provides a new evidence to develop highly efficient ORR catalysts through imitate the naturally involved systems through a simple route.

关键词： bio-inspired heme-copper oxidases iron phthalocyanine MnO_(x)nanosheets oxygen reduction reaction

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Role of buffer layer in electronic structures of iron phthalocyanine molecules on Au(111)

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Chinese Physics B 2010年第9期19卷 25-30页

作者：孙家涛潘理达胡昊杜世萱高鸿钧 Nanoscale Physics and Devices Laboratory Institute of PhysicsChinese Academy of Sciences

We investigate the electronic structures of one and two monolayer iron phthalocyanine （FePc） molecules on Au（111） surfaces. The first monolayer FePc is lying flat on the Au（111） substrate, and the second monolayer FePc is tilted at -15° relative to the substrate plane along the nearest neighbour [101] direction with a lobe downward to the central hole of the unit cell in the first layer. The structural information obtained by first-principles calculations is in agreement with the experiment results. Furthermore, it is demonstrated that the electronic structures of FePc molecules in one-monolayer FePc/Au（111） system are perturbed significantly, while the electronic structures of FePc molecules in the second monolayer in two-monolayer FePc/Au（111） system remain almost unchanged due to the screening of the buffer layer on Au（111）.

关键词： iron phthalocyanine electronic structure calculations buffer layer

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Tuning the Electrochemical Property of the Ultrafine Metal-oxide Nanoclusters by iron phthalocyanine as Efficient Catalysts for Energy Storage and Conversion

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Energy & Environmental Materials 2019年第1期2卷 5-17页

作者： Yi Cheng Xing Wu Jean-Pierre Veder Lars Thomsen San Ping Jiang Shuangyin Wang Department of Environmental Engineering School of Metallurgy and EnvironmentCentral South UniversityChangsha 410083China John de Laeter Centre Curtin UniversityPerth WA 6102Australia Australian Synchrotron Clayton Vic.3168Australia Western Australian School of Mines:Minerals Energy and Chemical Engineering and Fuels and Energy Technology InstituteCurtin UniversityPerth WA 6102Australia State Key Laboratory of Chem/Bio-Sensing and Chemometrics College of Chemistry and Chemical Engineering Hunan UniversityChangsha 410082HunanChina

Nanoclusters(NCs)have been demonstrated of outstanding performance in electrochemical energy storage and conversion technologies due to their strong quantum confinement effects and strong interaction with supports.Here,we developed a class of ultrafine metal-oxide(MOx,M=Fe,Co and Ni)NCs incorporated with iron phthalocyanine(FePc),MOx/FePc-G,supported on graphene as high-performance catalysts for oxygen reduction reaction(ORR),oxygen evolution reaction(OER),and carbon dioxide reduction(CO2RR).The high activities for ORR and OER are attributed to the electron donation and accepting ability of the highly redox active of FePc-G that could tune the properties of MOx.The FeOx/FePc-G exhibits an extremely positive half-wave potential(E1/2)of 0.888 and 0.610 V for ORR in alkaline and neutral conditions,respectively,which is around 60 mV more positive than that of Pt/C.And NiOx/FePc-G shows similar OER activity with the state-of-the-art catalysts,Ir/C,and better performance than NiFeO NCs supported on graphene.Remarkably,the CoOx/FePc-G and NiOx/FePc-G show high activity and selectivity to reduce CO2 into CO with a low onset potential of-0.22 V(overpotential is 0.11 V).

关键词： CO2 reduction reaction iron phthalocyanine metal-oxide nanoclusters oxygen evolution reaction oxygen reduction reaction

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P-functionalized carbon nanotubes promote highly stable electrocatalysts based on Fe-phthalocyanines for oxygen reduction: Experimental and computational studies

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Journal of Energy Chemistry 2022年第9期31卷 276-290,I0008页

作者： Beatriz Martinez-Sanchez Diego Cazorla-Amors Emilia Morallon Departamento de Quimica Fisica and Instituto Universitario de Materiales de Alicante(IUMA)University of Alicante Ap.99.03080 AlicanteSpain Departamento de Quimica Inorganica and Instituto Universitario de Materiales de Alicante(IUMA) University of AlicanteAp.9903080 AlicanteSpain

iron(Ⅱ) phthalocyanines(FePc) supported on functionalized nanostructured carbon materials have been studied as electrocatalysts for the oxygen reduction reaction(ORR) in an alkaline medium. Herein, two types of carbon nanotubes(CNTs) have been explored as support, Single-Walled Carbon Nanotubes and Herringbone Carbon Nanotubes(SWCNTs and h CNTs, respectively), both electrochemically modified with ortho-aminophenylphosphonic acid(2APPA), which provides phosphate axial coordinating ligands for the immobilization of FePc molecules. All the catalysts were prepared via a facile incipient wetness impregnation method. Comprehensive experimental analysis together with density functional theory(DFT) calculations has demonstrated both the importance of the five-coordinated Fe macrocycles that favor the interaction between the FePc and the carbon support, as well as the effect of the CNT structure in the ORR. FePc axial coordination provides a better dispersion, leading to higher stability and a favorable electron redistribution that also tunes the ORR performance by lowering the stability of the reaction intermediates. Interestingly, such improvement occurs with a very low content of metal(~1 wt% Fe),which is especially remarkable when h CNT support is employed. This work provides a novel strategy for the development of Fe-containing complexes as precious metal-free catalysts towards the ORR.

关键词： Carbon nanotubes iron phthalocyanine Oxygen reduction Electrocatalysis Axial ligand

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Ligand centered electrocatalytic efficient CO_(2) reduction reaction at low overpotential on single-atom Ni regulated molecular catalyst

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Nano Research 2022年第7期15卷 5816-5823页

作者： Jiazhi Wang Qi Hao Haixia Zhong Kai Li Xinbo Zhang State Key Laboratory of Rare Earth Resource Utilization Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China University of Science and Technology of China Hefei 230026China Key Laboratory of Automobile Materials Ministry of EducationJilin UniversityChangchun 130022China Center for Advancing Electronics Dresden(cfaed)and Faculty of Chemistry and Food Chemistry Technische Universität DresdenDresden 01062Germany

Electrochemical CO_(2) reduction reaction(CO_(2)RR)into value-added chemicals/fuels is crucial for realizing the sustainable carbon cycle while mitigating the energy crisis.However,it is impeded by the relatively high overpotential and low energy efficiency due to the lack of efficient electrocatalysts.Herein,we develop an isolated single-atom Ni catalyst regulated strategy to activate and stabilize the iron phthalocyanine molecule(Ni SA@FePc)toward a highly efficient CO_(2)RR process at low overpotential.The well-defined and homogenous catalytic centers with unique structures confer Ni SA@FePc with a significantly enhanced CO_(2)RR performance compared to single-atom Ni catalyst and FePc molecule and afford the atomic understanding on active sites and catalytic mechanism.As expected,Ni SA@FePc exhibits a high selectivity of more significant Faraday efficiency(≥95%)over a wide potential range,a high current density of~252 mA·cm^(−2) at low overpotential(390 mV),and excellent long-term stability for CO_(2)RR to CO.X-ray absorption spectroscopy measurement and theoretical calculation indicate the formation of NiN_(4)-O_(2)-FePc heterogeneous structure for Ni SA@FePc.And CO_(2)RR prefers to occur at the raised N centers of NiN4-O_(2)-FePc heterogeneous structure for Ni SA@FePc,which enables facilitated adsorption of*COOH and desorption of CO,and thus accelerated overall reaction kinetics.

关键词： single-atom Ni iron phthalocyanine molecular catalyst carbon dioxide reduction reaction ultra-low overpotential

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电子轴向拉伸提升贫氧环境海水电池性能

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Science Bulletin 2023年第24期68卷 3172-3180,M0005页

作者：唐全骏白亮张辰孟蓉炜王莉耿传楠郭勇王飞飞刘颖馨宋贵生凌国维孙海涛翁哲杨全红 School of Marine Science and Technology Tianjin UniversityTianjin 300072China Nanoyang Group Tianjin Key Laboratory of Advanced Carbon and Electrochemical Energy StorageState Key Laboratory of Chemical EngineeringSchool of Chemical Engineering and TechnologyNational Industry-Education Integration Platform of Energy StorageCollaborative Innovation Center of Chemical Science and Engineering(Tianjin)Tianjin UniversityTianjin 300072China Haihe Laboratory of Sustainable Chemical Transformations Tianjin 300192China Marine Science and Technology College Zhejiang Ocean UniversityZhoushan 316000China Joint School of National University of Singapore and Tianjin University International Campus of Tianjin UniversityBinhai New CityFuzhou 350207China State Key Laboratory of Precision Spectroscopy School of Physics and Electronic ScienceEast China Normal UniversityShanghai 200241China Collaborative Innovation Center of Extreme Optics Shanxi UniversityTaiyuan 030006China

长寿命溶解氧海水电池是深远海观测能源网络的重要组成单元,但海水贫氧复杂环境对设计高性能氧还原催化剂提出了重要挑战.本文以酞菁铁为模型催化剂,通过理论计算与实验验证,提出了活性位点电子轴向拉伸可大幅提升催化剂在极端贫氧环境... 详细信息

长寿命溶解氧海水电池是深远海观测能源网络的重要组成单元,但海水贫氧复杂环境对设计高性能氧还原催化剂提出了重要挑战.本文以酞菁铁为模型催化剂,通过理论计算与实验验证,提出了活性位点电子轴向拉伸可大幅提升催化剂在极端贫氧环境中的氧还原活性和稳定性.该研究为构建高性能海水电池提供了材料学解决方案,同时为极端环境下催化剂的变革性设计提供了新的思路.

关键词： Seawater batteries iron phthalocyanine Axial stretching Oxygen reduction reaction Electrocatalysis

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石墨烯负载分子铁酞菁催化剂的形貌结构调控与氧还原催化应用

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Science China Materials 2023年第10期66卷 3865-3874页

作者：高曼刘静静叶龚兰赵忠坤柳建斌何观朝龚智超黄康孙洪涛费慧龙 Advanced Catalytic Engineering Research Center of the Ministry of Education State Key Laboratory for Chemo/Biosensing and Chemometricsand College of Chemistry and Chemical EngineeringHunan UniversityChangsha 410082China The Harold&Inge Marcus Department of Industrial&Manufacturing Engineering Materials Research Institute(MRI)The Pennsylvania State UniversityUniversity Park 16802PennsylvaniaUSA

分散在纳米碳基底上的分子催化剂由于具有明确的活性位点和结构可调的特点,成为了一类独特的单原子催化剂,有望代替贵金属催化剂用于电催化氧还原反应.本文中,我们开发了一种高活性氧还原催化剂,该催化剂由均匀且密集分散在泡芙状石墨... 详细信息

分散在纳米碳基底上的分子催化剂由于具有明确的活性位点和结构可调的特点,成为了一类独特的单原子催化剂,有望代替贵金属催化剂用于电催化氧还原反应.本文中,我们开发了一种高活性氧还原催化剂,该催化剂由均匀且密集分散在泡芙状石墨烯载体上的铁酞菁(FePc/PG)构成.泡芙状石墨烯载体由于具有独特的皱褶和球状形貌,具有较大的比表面积和多尺度的孔结构,有利于FePc的高密度负载、活性位点的暴露和催化过程中传质效率的提高.当用旋转圆盘电极评估性能时,FePc/PG表现出优异的半波电位,达0.909 V(相对于可逆氢电极).此外,当用作气体扩散电极时,FePc/PG在高电流密度下表现出优异的高倍率和高功率性能.这项工作为设计纳米碳材料的形貌以及高性能异相分子催化剂提供了有效的策略,有望在多种能源转换和存储技术中得到应用.

关键词： graphene single atom catalyst iron phthalocyanine morphology engineering oxygen reduction reaction

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Catalytic oxidation of cyclohexene to cyclohexanone by a triple system in acidic aqueous acetonitrile medium

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Chinese Journal of Chemistry 1997年第6期15卷 512-527页

作者： Li, HM Ye, XK Yang, XG Wu, Y Chinese Acad Sci Changchun Inst Appl Chem Changchun 130022 Jilin Peoples R China

The catalytic oxidation of cyclohexene to cyclohexanone using Pd(OAc)(2)/HQ/FePc was investigated in an acidic aqueous solution of acetonitrile. The role of each component of this system in the oxidation of cyclohexene was explored by means of UV-VIS, IR, XPS spectroscopy and. cyclic voltammetry, respectively. Based on the experimental results, the mechanism of the oxidation of cyclohexene catalyzed by Pd(OAc)(2)/HQ/FePc was elucidated.

关键词： cyclohexene oxidation cyclohexanone hydroquinone Pd(OAc)(2) iron phthalocyanine

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