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nitrogen-doped graphene nanosheets as reactive water purification membranes

Nano Research 2016年第7期9卷 1983-1993页

作者： Yanbiao Liu Ling Yu Choon Nam Ong Jianping Xie NUS Environmental Research Institute National University of Singapore 117411 Singapore Department of Chemical and Biomolecular Engineering National University of Singapore 117585 Singapore

Oxidation of organic pollutants by sulfate radicals produced via activation of persulfate has emerged as a promising advanced oxidation technology to address various challenging environmental issues. The development of an effective, environmentally-friendly, metal-free catalyst is the key to this technology. Additionally, a supported catalyst design is more advantageous than conventional suspended powder catalysts from the point of view of mass transfer and practical engineering applications （e.g. post-use separation）. In this study, a metal-free N-doped reduced graphene oxide （N-rGO） catalyst was prepared via a facile hydrothermal method. N-rGO filters were then synthesized by facile vacuum filtration, such that water can flow through nanochannels within the filters. Various advanced characterization techniques were employed to obtain structural and compositional information of the as-synthesized N-rGO filters. An optimized phenol oxidative flux of 0.036 ＋_ 0.002 mmol.h ~ was obtained by metal-flee catalytic activation of persulfate at an influent persulfate concentration of 1.0 mmol-L 1 and filter weight of 15 rag, while a N-free rGO filter demonstrated negligible phenol oxidation capability under similar conditions. Compared to a conventional batch system, the flow-through design demonstrates obviously enhanced oxidation kinetics （0.036 vs. 0.010 retool-h-I）, mainly due to the liquid flow through the filter leading to convection-enhanced transfer of the target molecule to the filter active sites. Overall, the results exemplified the advantages of organic compound removal by catalytic activation of persulfate using a metal-free catalyst in flow- through mode, and demonstrated the potential of N-rGO filters for practical environmental applications.

关键词： persulfate activation nitrogen-doped graphene phenol oxidation convective flow batch system

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CVD synthesis of nitrogen-doped graphene using urea

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Science China(Physics,Mechanics & Astronomy) 2015年第10期58卷 94-99页

作者： ZHANG CanKun LIN WeiYi ZHAO ZhiJuan ZHUANG PingPing ZHAN LinJie ZHOU YingHui CAI WeiWei Department of Physics Laboratory of Nanoscale Condense Matter Physics and State Key Laboratory of Physical Chemistry of Solid SurfacesXiamen University

This work provides an effective low-cost synthesis and in-depth mechanistic study of high quality large-area nitrogen-doped graphene(NG) films. These films were synthesized using urea as nitrogen source and methane as carbon source, and were characterized by scanning electron microscopy(SEM), Raman spectroscopy and X-ray photoelectron spectroscopy(XPS). The N doping level was determined to be 3.72 at.%, and N atoms were suggested to mainly incorporated in a pyrrolic N configuration. All distinct Raman peaks display a shift due to the nitrogen-doping and compressive strain. The increase in urea concentration broadens the D and 2D peak's Full Width at Half Maximum(FWHM), due to the decrease of mean free path of phonons. The N-doped graphene exhibited an n-type doping behavior with a considerably high carrier mobility of about 74.1 cm2/(V s), confirmed by electrical transport measurements.

关键词： nitrogen-doped graphene chemical vapor deposition Raman spectroscopy X-ray photoemission spectroscopy

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Heterogeneous single-cluster catalysts(Mn_(3),Fe_(3),Co_(3),and Mo_(3))supported on nitrogen-doped graphene for robust electrochemical nitrogen reduction

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Journal of Energy Chemistry 2021年第3期30卷 612-619页

作者： Guokui Zheng Lei Li Ziqi Tian Xingwang Zhang Liang Chen Key Laboratory of Biomass Chemical Engineering of Ministry of Education College of Chemical and Biological EngineeringZhejiang UniversityHangzhou 310027ZhejiangChina Ningbo Institute of Materials Technology and Engineering Chinese Academy of SciencesNingbo 315201ZhejiangChina University of Chinese Academy of Sciences Beijing 100049China Institute of Zhejiang University-Quzhou Quzhou 324000ZhejiangChina

Electrochemical nitrogen reduction reaction(NRR)is one of the most promising alternatives to the traditional Haber-Bosch *** efficient electrocatalysts is still *** by the recent experimental and theoretical advances on single-cluster catalysts(SCCs),we systematically investigated the catalytic performance of various triple-transition-metal-atom clusters anchored on nitrogen-doped graphene for NRR through density functional theory(DFT)*** them,Mn_(3)-N4,Fe_(3)-N4,Co_(3)-N4,and Mo_(3)-N4 were screened out as electrocatalysis systems composed of non-noble metal with high activity,selectivity,stability,and ***,the Co_(3)-N4 possesses the highest activity with a limiting potential of-0.41 V through the enzymatic *** outstanding performance of Co_(3)-N4 can be attributed to the unique electronic structure leading to strong π backdonation,which is crucial in effective N_(2) *** work not only predicts four efficient non-noble metal electrocatalysts for NRR,but also suggest the SCCs can serve as potential candidates for other important electrochemical reactions.

关键词： Single-cluster catalysts nitrogen reduction reaction nitrogen-doped graphene Density functional theory

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Zeolitic imidazolate framework-67 derived Al-Co-S hierarchical sheets bridged by nitrogen-doped graphene:Incorporation of PANI derived carbon nanorods for solid-state asymmetric supercapacitors

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Journal of Energy Chemistry 2022年第11期31卷 429-445,I0012页

作者： Emad S.Goda Bidhan Pandit Sang Eun Hong Bal Sydulu Singu Seong K.Kim Essam B.Moustafa Kuk Ro Yoon Kuk Ro Yoon Organic Nanomaterials Lab Department of ChemistryHannam UniversityDaejeon 34054Republic of Korea Gas Analysis and Fire Safety Laboratory Chemistry DivisionNational Institute for Standards136Giza 12211Egypt Department of Materials Science and Engineering and Chemical Engineering Universidad Carlos Ⅲ de MadridAvenida de La Universidad 3028911 LeganésMadridSpain Department of Chemical and Biomolecular Engineering Yonsei UniversitySeoul 03722Republic of Korea Department of Chemical Engineering Hannam University1646 Yuseongdae-roYuseong-guDaejeon 34054Republic of Korea Mechanical Engineering Department Faculty of EngineeringKing Abdulaziz UniversityP.O.Box 80204Jeddah 22254Saudi Arabia

Metal sulfides have been widely enticed as battery-type electrodes in supercapacitor devices because of their maximal theoretical ***,their lower conductivity and ion transport kinetics can largely restrict their rate performance,hence the practical usage in fields of demanding high power ***,the design of new electrodes with higher energy and power densities remains a highly challenging *** the best of our knowledge,a novel hierarchical composite of Al-CoS_(2) on nitrogendoped graphene(NG)is prepared based on a zeolite imidazole framework using a simple and scalable hydrothermal *** this hybrid,ultrathin Al-CoS_(2) nanosheet arrays are vertically orientated on the NG framework to limit self-aggregation,hence increasing the electrical property and cycle stability of *** is investigated that the Al/Co feeding ratio plays a crucial role in controlling the obtained hierarchical structure of Al-Co-S sheets and their electrode ***,Al^(3+) can influence remarkably the morphology and electrochemical property of the resultant graphene *** effective synergism is noticed between the redox Al-CoS_(2) and NG resulting in fast electron transfer and chargingdischarging ***,when the as-developed composite is utilized as a positive electrode at an applied current density of 1 A/g,a specific capacitance of 1915.8 F/g is attained with ultra-long cycle stability(96%,10,000 cycles)and an excellent retention rate(~89%).As a consequence,when a solid-state asymmetric supercapacitor(ASC)device is made by combining an Al-CoS_(2) @NG hybrid with a negative electrode made of polyaniline(PANI)derived carbon nanorods(PCNRs),it demonstrates remarkable specific capacitance(188 F/g),energy density(66.9 Wh/kg),and cyclic stability of 92%after 10,000 *** may open the pathway for the application of the next-generation supercapacitors in the future.

关键词： Hierarchical sheets MOFs Al-doped CoS_(2) nitrogen-doped graphene Solid-state supercapacitor

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nitrogen-doped graphene approach to enhance the performance of a membraneless enzymatic biofuel cell

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Frontiers in Energy 2018年第2期12卷 233-238页

作者： Alireza AHMADIAN YAZDI Jie XU Department of Mechanical and Industrial Engineering University of Illinois at ChicagoChicagoIL 60607USA

Heteroatom-doping of pristine graphene is an effective route for tailoring new characteristics in terms of catalytic performance which opens up potentials for new applications in energy conversion and storage devices. nitrogen-doped graphene （N-graphene）, for instance, has shown excellent performance in many electrochemical systems involving oxygen reduction reaction （ORR）, and more recently glucose oxidation. Owing to the excellent H2O2 sensitivity of N-graphene, the development of highly sensitive and fast-response enzymatic biosensors is made possible. However, a question that needs to be addressed is whether or not improving the anodic response to glucose detection leads to a higher overall performance of enzymatic biofuel cell （eBFC）. Thus, here we first synthesized N-graphene via a catalyst-free single-step thermal process, and made use of it as the biocatalyst support in a membraneless eBFC to identify its role in altering the performance characteristics. Our findings demonstrate that the electron accepting nitrogen sites in the graphene structure enhances the electron transfer efficiency between the mediator （redox polymer）, redox active site of the enzymes, and electrode surface. Moreover, the best performance in terms of power output and current density of eBFCs was observed when the bioanode was modified with highly doped N-graphene.

关键词： enzymatic fuel cell nitrogen-doped graphene reduced graphene oxide catalyst-free synthesis

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Design ofL-Cysteine Functionalized Au@SiO2@Fe3O4/nitrogen-doped graphene Nanocomposite and Its Application in Electrochemical Detection of Pb2＋

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Chemical Research in Chinese Universities 2017年第6期33卷 951-957页

作者： NIE Jing HE Bin CHENG Yanmei YIN Wei HOU Changjun HUO Danqun QIAN Linlin QIN Yunan FA Huanbao National-municipal Joint Engineering Laboratory for Chemical Process Intensification and Reaction College of Chemistry and Chemical Engineering Chongqing University Chongqing 400044 P. R. China Key Laboratory of Biorheology Science and Technology Ministry of Education College of Bioengineering Chongqing University Chongqing 400044 P R. China

A novel magnetic electrochemical sensor was designed for determination of lead ions based on gold na- noparticles（AuNPs）@SiO2@Fe3O4/nitrogen-doped graphene（NG） composites functionalized with L-cysteine. The Au@SiO2@Fe3O4/NG was synthesized by the electrostatic adsorption between AuNPs and SiO2-coated Fe304 NPs（SiO2@Fe304） and the amide bond between Au@SiO2@Fe3O4 and NG. L-Cysteine was successfully functionalized on the surface of Au@SiO2@Fe3O4/NG nanocomposites via the S--Au bond between L-cysteine and AuNPs. Owing to numerous active sites in L-cysteines and high conductivity of Au@SiO2@Fe3O4/NG composites, the pro- posed electrochemical sensor exhibited a well-distributed nanostructure and high responsivity toward Pb（II）. The sensor linearly responded to Pb2＋ concentration in the range of 5-80 μg/L with a detection limit of 0.6 μg/L, indicating that this L-cysteine functionalized Au@SiO2@Fe3O4/NG composite could be a promising candidate material for the detection of Pb2＋.

关键词： Electrochemical sensor Lead nitrogen-doped graphene Au@SiO2@Fe3O4 L-Cysteine

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Cuprous Oxide/nitrogen-doped graphene Nanocomposites as Electrochemical Sensors for Ofloxacin Determination

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Chemical Research in Chinese Universities 2016年第3期32卷 468-473页

作者： WU Fanghui XU Fan CHEN Le JIANG Binbin SUN Wenbin WEI Xianwen School of Chemistry and Chemical Engineering Anhui University of Technology Maanshan 243002 P. R. China

Cu2O/nitrogen-doped grapheme（NG） nanocomposite material was prepared via a facile one step chemical reduction and characterized by means of X-ray diffraction（XRD） and scanning electron microscopy（SEM）. A new electrochemical sensor was then fabricated by coating Cu2O/nitrogen-doped graphene nanocomposite with Nation on glassy carbon electrode（Cu2O/NG/Nation/GCE）. The electrochemical response of this modified electrode toward of- loxacin was examined by cyclic voltammetry. The results indicate that Cu2O/NG/Nafion composite-modified elec- trode exhibits higher catalytic activity in the electrochemical oxidation of ofloxacin compared with glassy carbon electrode（GCE）, Cu2O/Nafion modified electrode（Cu2O/Nafion/GCE）, and N-doped graphene/Nation modified electrode（NG/Nafion/GCE）. Under optimal conditions, the peak current was found to be linearly proportional to the concentration of ofloxacin in the 0.5-27.5 μmol/L and 27.5-280 μmol/L ranges with a lower detection limit of 0.34 μmol/L, higher sensitivity of 39.32 μA-L-mmoV1 and a shorter reaction time of less than 2 s. In addition, Nation can enhance the stability of the modified electrode and prevent some negative species. Thus the modified electrode exhibits good selectivity and a long working life. The Cu2O/NG/Nafion composite modified electrode shows promising application in electrochemical sensors, biosensors, and other related fields because of its excellent properties.

关键词： Cu2O nitrogen-doped graphene Ofloxacin Electrochemical method Determination

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Modified nitrogen-doped graphene Electrocatalyst for Oxygen Reduction Reaction in Alkaline Fuel Cells

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Journal of Energy and Power Engineering 2015年第10期9卷 886-895页

作者： Dureid Qazzazie Michaela Beckert Rolf Mtilhaupt Olena Yurchenko Gerald Urban Freiburg Materials Research Center University of Freiburg Freiburg D-79104 Germany Laboratory for Sensors Department of Microsystems Engineering University of Freiburg Freiburg D-79110 Germany Institute for MacromoIecular Chemistry University of Freiburg Freiburg D- 79104 Germany

We report modified nitrogen-doped graphene （CN） as electrocatalyst for ORR （oxygen reduction reaction） in alkaline medium. CN was synthesized by a novel procedure based on graphite oxide thermally treated with cyanamide suitable for facile N-doping and large-scale production, whereas cyanamide was used as N-precursor. The structure of the material was characterized by TEM （transmission electron microscopy）, SEM （scanning electron microscopy）, Raman spectroscopy and XPS （X-ray photoelectron spectroscopy）. Structural and electrochemical properties of CN were compared with those of non-modified graphene （TRGO （thermally reduced graphite oxide））. The electrochemical characterization of TRGO and CN in alkaline solution demonstrates enhanced electrocatalytic ORR activity and improved long-term stability for N-doped CN. Voltammetric studies confirmed that, oxygen reduction on CN rather follows four-electron pathway. Compared with commercial 20% PtC catalyst, CN is characterized by exceptional methanol crossover resistance and superb long-term operation stability. Owing to these factors, nitrogen-doped graphene has a great potential to be used as metal-free electrocatalyst in cathodes of alkaline fuel cells.

关键词： nitrogen-doped graphene metal-free catalysis oxygen reduction reaction alkaline fuel cells.

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Facile synthesis of nitrogen-doped graphene for measuring the releasing process of hydrogen peroxide from living cells

Facile synthesis of nitrogen-doped graphene for measuring th...

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中国化学会第28届学术年会

作者： Ping Wu,Yingdan Qian,Zhang Hui,Cai Chenxin Jiangsu Key Laboratory of New Power Batteries,Jiangsu Key Laboratory of Biofunctional Materials,College of Chemistry and Materials Science,Nanjing Normal University,Nanjing 210097,P.R.China

＜正＞Modulating the electronic characteristics of graphene is of great technological importance for improving and expanding its applications.1,2Chemical doping with other elements is a promising way to achieve this *... 详细信息

关键词： Carbon materials biotechnology electrocatalysis nitrogen-doped graphene hydrogen peroxide

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Chemical Nature of Catalytic Active Sites for the Electrochemical Redox of Acetaminophen on nitrogen-doped graphene

Chemical Nature of Catalytic Active Sites for the Electroche...

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第十三届全国电分析化学学术会议

作者： Weimeng Si Yue Cao Yuehua Zhang School of Materials Science and Engineering Shandong University of Technology School of Chemical Engineering Nanjing University of Science and Technology

nitrogen-doped graphene is one of the mostly studied doped graphene, especially since it was reported a valuable metal-free catalyst in ORR associated with alkaline fuel *** with recent intense research efforts, a variety of methods has been used in the preparation of nitrogen-doped graphene(NGE), such as annealing of graphene oxide and NH, pyrolysis of graphene oxide and urea, solvothermal with lithium nitrideand and tetrachloromethane, and so *** these, even excellent performances can be obtained, the real active sites are different to be *** the ORR, it has been generally believed that the doped nitrogen atoms(pyrrole-N, pyridine-N, graphitic-N, and pyridine-N oxide) play a key role [1].For instance, Pyridine-N doping in graphene was believed facilitating oxygen reduction reaction activity [2].Nevertheless, carbon atoms with Lewis basicity next to pyridine-N was also considered to be the real active sites for the ORR, recently [3].Besides, for its unique catalytic activities, NGE was also used in electrochemical sensors, while the real active sites are still *** instance, NGE has been used in the determination of aromatic phenol, and the dominant electro-catalysis active sites were also *** the determination of hydroquinone and catechol, pyridine-N dominant NGE showed higher electro-catalysis than the pyrrole-N dominant NGE, indicating pyridine-N the electro-catalysis active sites [4].Earlier, nitrogen-doped carbon nanotubes were devoted to the determination of acetaminophen(AP), while the main electro-active sites were not clear [5].Herein, the electro-catalysis of NGE towards the redox of AP was studied, and the quaternary-N, but not pyridine-N or pyrrole-N, may played a crucial *** enhanced electrochemical response can be obtained on NGE modified *** the superb catalysis, the NGE was employed in the determination of AP with a detection limit of 0.38μM.

关键词： nitrogen-doped graphene graphitic-N acetaminophen

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