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nitrogen vacancies enriched Ce-doped Ni_(3)N hierarchical nanosheets triggering highly-efficient urea oxidation reaction in urea-assisted energy-saving electrolysis

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Journal of Energy Chemistry 2022年第6期31卷 506-515,I0014页

作者： Meng Li Xiaodong Wu Kun Liu Yifan Zhang Xuechun Jiang Dongmei Sun Yawen Tang Kai Huang Gengtao Fu Jiangsu Key Laboratory of New Power Batteries Jiangsu Collaborative Innovation Centre of Biomedical Functional MaterialsSchool of Chemistry and Materials ScienceNanjing Normal UniversityNanjing 210023JiangsuChina School of Chemistry and Chemical Engineering Southeast UniversityNanjing 211189JiangsuChina College of Materials Science and Engineering Nanjing Tech UniversityNanjing 210009JiangsuChina

Urea oxidation reaction (UOR),which has favorable thermodynamic energy barriers compared with oxygen evolution reaction (OER),can provide more cost-effective electrons for the renewable energy systems,but is trapped by its sluggish UOR kinetics and intricate reaction intermediates formation/desorption process.Herein,we report a novel and effective electrocatalyst consisting of carbon cloth supported nitrogen vacancies-enriched Ce-doped Ni_(3)N hierarchical nanosheets (Ce-Ni_(3)N @CC) to optimize the flat-footed UOR kinetics,especially the stiff rate-determine CO_(2)desorption step of UOR.Upon the introduction of valance state variable Ce,the resultant nitrogen vacancies enriched Ce-Ni_(3)N @CC exhibits an enhanced UOR performance where the operation voltage requires only 1.31 V to deliver the current density of 10 mA cm^(-2),which is superior to that of Ni_(3)N @CC catalyst (1.36 V) and other counterparts.Density functional theory (DFT) results demonstrate that the incorporation of Ce in Ni_(3)N lowers the formation energy of nitrogen vacancies,resulting in rich nitrogen vacancies in Ce-Ni_(3)N @CC.Moreover,the nitrogen vacancies together with Ce doping optimize the local charge distribution around Ni sites,and balance the adsorption energy of CO_(2)in the rate-determining step (RDS),as well as affect the initial adsorption structure of urea,leading to the superior UOR catalytic performance of Ce-Ni_(3)N @CC.When integrating the Ce-Ni_(3)N catalyst in UOR//HER and UOR//CO_(2)R flow electrolyzer,both of them perform well with low operation voltage and robust long-term stability,proofing that the thermodynamically favorable UOR can act as a suitable substitute anodic reaction compared with that of OER.Our findings here not only provide a novel UOR catalyst but also offer a promising design strategy for the future development of energy-related devices.

关键词： Rare earth cerium Nickel nitride nitrogen vacancies Charge redistribution Urea oxidation reaction

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Regulating nitrogen vacancies within graphitic carbon nitride to boost photocatalytic hydrogen peroxide production

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SusMat 2022年第5期2卷 617-629页

作者： Yanlin Zhu Xuetao Liu Heng Liu Guangling He Jiamin Xiao Haijiao Xie Yanyan Sun Lei Han College of Materials Science and Engineering Hunan Joint International Laboratory of Advanced Materials and Technology for Clean EnergyHunan UniversityChangshaHunanChina School of Materials Science and Engineering Central South UniversityChangshaHunanChina Hangzhou Yanqu Information Technology Co.Ltd. HangzhouChina

Introducing nitrogen vacancies is an effective method to improve the catalytic performance of g-C_(3)N_(4)-based photocatalysts,whereas understanding how nitrogen vacancies types affect the catalytic performance remains unclear.Herein,two different types of nitrogen vacancies were successfully introduced into g-C_(3)N_(4)by pyrolysis of melamine under argon and ammonia atmosphere with subsequent HNO3 oxidation.The pyrolysis atmosphere is found to have a significant influence on the introduced nitrogen vacancies type,where tertiary nitrogen groups(N_(3)C)and sp2-hybridized nitrogen atoms(N_(2)C)were the preferred sites for the formation of nitrogen vacancies under ammonia and argon pyrolysis,respectively.Moreover,nitrogen vacancies from N3C are experimentally and theoretically demonstrated to facilitate the narrowed band gap and the improved oxygen absorption capability.As expected,the optimal catalyst exhibits high H_(2)O_(2)yield of 451.8µM,which is 3.8 times higher than the pristine g-C_(3)N_(4)(119.0µM)after 4 h and good stability after10 photocatalytic runs.

关键词： carbon nitride hydrogen peroxide nitrogen vacancies oxygen absorption

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Synthesis of porous few-layer carbon nitride with excellent photocatalytic nitrogen fixation

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Journal of Materiomics 2020年第1期6卷 128-137页

作者： Yanjun Xue Xiangkun Kong Yichen Guo Zhangqian Liang Hongzhi Cui Jian Tian School of Materials Science and Engineering Shandong University of Science and TechnologyQingdao266590China

The porous few-layer g-C_(3)N_(4)(PFL-g-C_(3)N_(4))is prepared by a simple molecular self-assembly method.Compared with pure g-C_(3)N_(4),the as-prepared PFL-g-C_(3)N_(4) is ultrathin,the surface is rich in pores,and the photocatalytic nitrogen fixation activity is greatly increased to 8.20 mM h^(-1) gCat^(-1).Few-layer and ultrathin nature of PFL-g-C_(3)N_(4) can provide a larger specific surface area,expose more active sites,and reduce the diffusion path of charges and protons from the inside to the surface.In addition,the porous structure can narrow the band gap,thereby increasing the light absorption range and enhancing the light absorption capability.Meanwhile,the presence of nitrogen vacancies causes PFL-g-C_(3)N_(4) to move to a more negative conductive band value.More importantly,the isotopic experiments using ^(15)N_(2) as nitrogen source confirm the ammonia production originating from N2 rather than the decomposition of g-C_(3)N_(4).Therefore,PFL-g-C_(3)N_(4) can greatly improve the efficiency of visible light photocatalytic nitrogen fixation.

关键词： Molecular self-assembly g-C_(3)N_(4) Porous structure nitrogen vacancies Photocatalytic nitrogen fixation

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Synthesis of porous few-layer carbon nitride with excellent photocatalytic nitrogen fixation

Synthesis of porous few-layer carbon nitride with excellent ...

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第七届新型太阳能电池材料科学与技术学术研讨会

作者： Yanjun Xue Xiangkun Kong Yichen Guo Zhangqian Liang Hongzhi Cui Jian Tian School of Materials Science and Engineering Shandong University of Science and Technology

The porous few-layer g-CN(PFL-g-CN) is prepared by a simple molecular self-assembly method.Compared with pure g-CN,the as-prepared PFL-g-CN is ultrathin,the surface is rich in pores,and the photocatalytic nitrogen fixation activity is greatly increased to 8.20 mM h gCat.Few-layer and ultrathin nature of PFL-g-CN can provide a larger specific surface area,expose more active sites,and reduce the diffusion path of charges and protons from the inside to the surface.In addition,the porous structure can narrow the band gap,thereby increasing the light absorption range and enhancing the light absorption capability.Meanwhile,the presence of nitrogen vacancies causes PFL-g-CN to move to a more negative conductive band value.More importantly,the isotopic experiments using 15 N as nitrogen source confirm the ammonia production originating from N rather than the decomposition of g-CN.Therefore,PFL-g-CN can greatly improve the efficiency of visible light photocatalytic nitrogen fixation.

关键词： Molecular self-assembly g-C3N4 porous structure nitrogen vacancies photocatalytic nitrogen fixation

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