Pyrogenic carbonaceous matter(PCM) catalyzes azo dye decolorization by sulfide, but the nitrogen doping catalytic mechanisms are poorly understood. In this study, we found that stagnate time of azo dye methyl orange(M...Pyrogenic carbonaceous matter(PCM) catalyzes azo dye decolorization by sulfide, but the nitrogen doping catalytic mechanisms are poorly understood. In this study, we found that stagnate time of azo dye methyl orange(MO) decolorization was reduced to 0.54-18.28 min in the presence of various nitrogen-doped graphenes(NGs), remarkably lower compared to graphene itself. Particularly, graphitic nitrogen played a critical role in NGs-catalyzed MO decolorization by sulfide. Gas chromatography-mass spectrometry and in-situ surface Raman analysis demonstrated that doping nitrogen, especially graphite one facilitated reactive intermediate polysulfides formation. This is attributed to the improved electron conductivity through graphitic nitrogen doping, and the enhanced interactions between sulfide and carbon atoms bonded to graphitic nitrogen. This study not only provides a better understanding of PCM impact on transformations and fates of organic pollutants in natural environments, but also offer a new regulation strategy for more efficient wastewater treatment processes in PCM-catalyzed engineering systems.展开更多
Nano Research volume 13,pages1704–1712(2020)Cite this article 191 Accesses Metrics details Abstract Intelligent gas sensors based on the layered transition metal dichalcogenides(TMDs)have attracted great interest in ...Nano Research volume 13,pages1704–1712(2020)Cite this article 191 Accesses Metrics details Abstract Intelligent gas sensors based on the layered transition metal dichalcogenides(TMDs)have attracted great interest in the field of gas sensing due to their multiple active sites,fast electron,mass transfer capability and large surface-to-volume ratio.However,conventional TMDs-based sensors typically work at elevated temperature in inert atmosphere,which would largely limit the corresponding practical applications.Herein,novel oxygen-doped MoSe2 hierarchical nanostructures composed of ultrathin nanosheets with large specific surface area have been designed and generated typically at 200°C in air for fast and facile gas sensing of trimethylamine(TMA),effectively.Benefited from the gas-accessible hierarchical morphology and high surface area with abundant nanochannels,highly sensitive and selective detection of trace TMA has been achieved under ambient condition,and as detected the theoretical limit of detection(LOD)is 8 ppb,which is the lowest for TMA detection under ambient condition among the reported studies.The mechanism of oxygen doping on the improved gas-sensing performance has been investigated,revealing that the oxygen doping could greatly optimize the electronic structure,thus regulate the Fermi level of MoSe2 as well as the affinity between TMA molecule and sensor surface.It is expected that the oxygen doping strategy developed for the highly efficient gas sensors based on TMDs in present work may also be applicable to other types of gas-sensing semiconductors,which could open up a new direction for the rational design of high-performance gas sensors working under ambient condition.展开更多
基金the National Natural Science Foundation of China (Nos. U19A20108, 52025101, 51821006 and 51878637) for financially supporting this study。
文摘Pyrogenic carbonaceous matter(PCM) catalyzes azo dye decolorization by sulfide, but the nitrogen doping catalytic mechanisms are poorly understood. In this study, we found that stagnate time of azo dye methyl orange(MO) decolorization was reduced to 0.54-18.28 min in the presence of various nitrogen-doped graphenes(NGs), remarkably lower compared to graphene itself. Particularly, graphitic nitrogen played a critical role in NGs-catalyzed MO decolorization by sulfide. Gas chromatography-mass spectrometry and in-situ surface Raman analysis demonstrated that doping nitrogen, especially graphite one facilitated reactive intermediate polysulfides formation. This is attributed to the improved electron conductivity through graphitic nitrogen doping, and the enhanced interactions between sulfide and carbon atoms bonded to graphitic nitrogen. This study not only provides a better understanding of PCM impact on transformations and fates of organic pollutants in natural environments, but also offer a new regulation strategy for more efficient wastewater treatment processes in PCM-catalyzed engineering systems.
基金This work was financially supported by the National Natural Science Foundation of China(Nos.U1932150 and 21571166)Anhui Provincial Natural Science Foundation(No.1908085QB72)the Fundamental Research Funds for the Central Universities(No.WK2060190099).
文摘Nano Research volume 13,pages1704–1712(2020)Cite this article 191 Accesses Metrics details Abstract Intelligent gas sensors based on the layered transition metal dichalcogenides(TMDs)have attracted great interest in the field of gas sensing due to their multiple active sites,fast electron,mass transfer capability and large surface-to-volume ratio.However,conventional TMDs-based sensors typically work at elevated temperature in inert atmosphere,which would largely limit the corresponding practical applications.Herein,novel oxygen-doped MoSe2 hierarchical nanostructures composed of ultrathin nanosheets with large specific surface area have been designed and generated typically at 200°C in air for fast and facile gas sensing of trimethylamine(TMA),effectively.Benefited from the gas-accessible hierarchical morphology and high surface area with abundant nanochannels,highly sensitive and selective detection of trace TMA has been achieved under ambient condition,and as detected the theoretical limit of detection(LOD)is 8 ppb,which is the lowest for TMA detection under ambient condition among the reported studies.The mechanism of oxygen doping on the improved gas-sensing performance has been investigated,revealing that the oxygen doping could greatly optimize the electronic structure,thus regulate the Fermi level of MoSe2 as well as the affinity between TMA molecule and sensor surface.It is expected that the oxygen doping strategy developed for the highly efficient gas sensors based on TMDs in present work may also be applicable to other types of gas-sensing semiconductors,which could open up a new direction for the rational design of high-performance gas sensors working under ambient condition.