Nitrogen-doped carbon nanotubes（NCNTs） were synthesized by chemical vapor deposition using cobaltbased oxides as catalyst and ethylenediamine（EDA） as carbon/nitrogen precursor. The influence of growth time,EDA con...Nitrogen-doped carbon nanotubes（NCNTs） were synthesized by chemical vapor deposition using cobaltbased oxides as catalyst and ethylenediamine（EDA） as carbon/nitrogen precursor. The influence of growth time,EDA concentration and growth temperature on the morphology,yield,composition,graphitization and oxidation resistance of the NCNTs was systematically investigated by using Raman spectroscopy,temperature-programmed oxidation and other techniques. The NCNT growth from ethylenediamine with a high N/C ratio involves several processes including mainly（1） catalytic growth of NCNTs,（2） homogeneous gas-phase decomposition of EDA,（3） non-catalytic deposition of pyrolytic carbon/nitrogen species and（4）surface etching of amorphous carbon or carbon at defect sites through gasification. At a later growth stage the etching process appears to be dominating,leading to the thinning of nanotubes and the decrease of yield.Moreover,the surface etching through carbon gasification strongly influences the structure and degree of graphitization of NCNTs.展开更多
RuO2 nanoparticles supported on multi-walled carbon nanotubes（CNTs） functionalized with oxygen（OCNTs） and nitrogen（NCNTs） were employed for the oxygen evolution reaction（OER） in 0.1 M KOH.The catalysts were sy...RuO2 nanoparticles supported on multi-walled carbon nanotubes（CNTs） functionalized with oxygen（OCNTs） and nitrogen（NCNTs） were employed for the oxygen evolution reaction（OER） in 0.1 M KOH.The catalysts were synthesized by metal-organic chemical vapor deposition using ruthenium carbonyl（Ru3（CO）（12）） as Ru precursor. The obtained RuO2/OCNT and RuO2/NCNT composites were characterized using TEM, H2-TPR, XRD and XPS in order probe structure–activity correlations, particularly, the effect of the different surface functional groups on the electrochemical OER performance. The electrocatalytic activity and stability of the catalysts with mean RuO2 particle sizes of 13–14 nm was evaluated by linear sweep voltammetry, cyclic voltammetry, and chronopotentiometry, showing that the generation of nitrogen-containing functional groups on CNTs was beneficial for both OER activity and stability. In the presence of RuO2, carbon corrosion was found to be significantly less severe.展开更多
Herein,Cu–Al bimetallic oxide was synthesized and mixed with mesoporous silica spheres via a simple hydrothermal method.The prepared sample was then analyzed and employed to activate potassium peroxydisulfate for bis...Herein,Cu–Al bimetallic oxide was synthesized and mixed with mesoporous silica spheres via a simple hydrothermal method.The prepared sample was then analyzed and employed to activate potassium peroxydisulfate for bisphenol A removal.Based on the results of X-ray diffraction,scanning electron microscopy,and energy dispersion spectroscopy,Cu–Al bimetallic oxide was determined as CuO-Al2O3,and mesoporous silica spheres were found around the these particles.At 30 min,a bisphenol A degradation level of 90%was achieved,and it remained at over 60%after five consecutive cycles,indicating the catalyst’s superior capacity and stability.In terms of removal performance,the radical pathway(including■OH•,and■)and singlet oxygen(■)bisphenol A,potassium peroxydisulfate,and the catalyst played a dominant role.The introduction of Al2O3 promoted the formation of surface oxygen vacancies,which improved ligand complex formation between potassium peroxydisulfate and the catalyst,thereby facilitating electron migration.Furthermore,mesoporous silica spheres augment not only enhanced bisphenol A adsorption but also alleviated Cu leaching.Overall,this work is expected to provide significant support for the rational development of catalysts with high catalytic activity for persulfate activation via surface electron migration.展开更多
基金supported by the German Federal Ministry of Education and Research(BMBF) through the Project "Carbo Elch"(Grant 03X0207C) within the scope of the Inno.CNT Alliancethe IMPRS-Sur Mat of the Max-Planck Society
文摘Nitrogen-doped carbon nanotubes（NCNTs） were synthesized by chemical vapor deposition using cobaltbased oxides as catalyst and ethylenediamine（EDA） as carbon/nitrogen precursor. The influence of growth time,EDA concentration and growth temperature on the morphology,yield,composition,graphitization and oxidation resistance of the NCNTs was systematically investigated by using Raman spectroscopy,temperature-programmed oxidation and other techniques. The NCNT growth from ethylenediamine with a high N/C ratio involves several processes including mainly（1） catalytic growth of NCNTs,（2） homogeneous gas-phase decomposition of EDA,（3） non-catalytic deposition of pyrolytic carbon/nitrogen species and（4）surface etching of amorphous carbon or carbon at defect sites through gasification. At a later growth stage the etching process appears to be dominating,leading to the thinning of nanotubes and the decrease of yield.Moreover,the surface etching through carbon gasification strongly influences the structure and degree of graphitization of NCNTs.
基金the IMPRS-Sur Mat of the Max Planck Society for a research grant
文摘RuO2 nanoparticles supported on multi-walled carbon nanotubes（CNTs） functionalized with oxygen（OCNTs） and nitrogen（NCNTs） were employed for the oxygen evolution reaction（OER） in 0.1 M KOH.The catalysts were synthesized by metal-organic chemical vapor deposition using ruthenium carbonyl（Ru3（CO）（12）） as Ru precursor. The obtained RuO2/OCNT and RuO2/NCNT composites were characterized using TEM, H2-TPR, XRD and XPS in order probe structure–activity correlations, particularly, the effect of the different surface functional groups on the electrochemical OER performance. The electrocatalytic activity and stability of the catalysts with mean RuO2 particle sizes of 13–14 nm was evaluated by linear sweep voltammetry, cyclic voltammetry, and chronopotentiometry, showing that the generation of nitrogen-containing functional groups on CNTs was beneficial for both OER activity and stability. In the presence of RuO2, carbon corrosion was found to be significantly less severe.
基金This study was financially supported by the National Natural Science Foundation of China(Grant Nos.51408295 and 41907364)National Key R&D Program of China(Grant Nos.2022YFB3805104 and 2021YFB3801400)+1 种基金Key Research and Development Project of Shandong Province(Grant Nos.2017GSF217013 and 2018GSF117007)Major Scientific and Technological Innovation Project of Shandong Province(Grant No.2021CXGC011206).
文摘Herein,Cu–Al bimetallic oxide was synthesized and mixed with mesoporous silica spheres via a simple hydrothermal method.The prepared sample was then analyzed and employed to activate potassium peroxydisulfate for bisphenol A removal.Based on the results of X-ray diffraction,scanning electron microscopy,and energy dispersion spectroscopy,Cu–Al bimetallic oxide was determined as CuO-Al2O3,and mesoporous silica spheres were found around the these particles.At 30 min,a bisphenol A degradation level of 90%was achieved,and it remained at over 60%after five consecutive cycles,indicating the catalyst’s superior capacity and stability.In terms of removal performance,the radical pathway(including■OH•,and■)and singlet oxygen(■)bisphenol A,potassium peroxydisulfate,and the catalyst played a dominant role.The introduction of Al2O3 promoted the formation of surface oxygen vacancies,which improved ligand complex formation between potassium peroxydisulfate and the catalyst,thereby facilitating electron migration.Furthermore,mesoporous silica spheres augment not only enhanced bisphenol A adsorption but also alleviated Cu leaching.Overall,this work is expected to provide significant support for the rational development of catalysts with high catalytic activity for persulfate activation via surface electron migration.
