SnS2 nanoflakes were successfully synthesized via a simple hydrothermal process. The as-prepared SnS2 samples were characterized by X-ray diffraction(XRD), scanning electron microscopy(SEM), nitrogen adsorption-de...SnS2 nanoflakes were successfully synthesized via a simple hydrothermal process. The as-prepared SnS2 samples were characterized by X-ray diffraction(XRD), scanning electron microscopy(SEM), nitrogen adsorption-desorption isotherms, and UV-vis diffuse reflectance spectroscopy(DRS). The photocatalytic activities of the as-prepared SnS2 nanoflakes under visible light irradiation(λ〉420 nm) were evaluated by the degradation of rhodamine B(Rh B). The effect of hydrothermal temperatures on the photocatalytic efficiency of as-prepared SnS2 nanoflakes was investigated. The experimental result showed that SnS2 nanoflakes synthesized at the temprature of 160 o had higher photocatalytic efficiency and good photocatalytic stability.展开更多
In the process of photocatalytic synthesis of ammonia,the kinetics of carrier separation and transport,adsorption of nitrogen,and activation of the N N triple bond are key factors that directly affect the efficiency o...In the process of photocatalytic synthesis of ammonia,the kinetics of carrier separation and transport,adsorption of nitrogen,and activation of the N N triple bond are key factors that directly affect the efficiency of converting nitro-gen to ammonia.Here,we report a new strategy for anchoring MXene quan-tum dots(MXene QDs)onto the surface of ZnIn2S4 by forming Ti-S bonds,which provide a channel for the rapid separation and transport of charge car-riers and effectively extend the lifespan of photogenerated carriers.The unique charge distribution caused by the sulfurization of the MXene QDs further enhances the performance of the photocatalysts for the adsorption and activa-tion of nitrogen.The photocatalytic ammonia synthesis efficiency of MXene QDs-ZnIn2S4 can reach up to 360.5μmol g�1 h�1.Density functional theory calculations,various in situ techniques,and ultrafast spectroscopy are used to characterize the successful construction of Ti-S bonds and the dynamic nature of excited state charge carriers in MXene QDs-ZnIn2S4,as well as their impact on nitrogen adsorption activation and photocatalytic ammonia synthesis efficiency.This study provides a new example of how to improve nitrogen adsorp-tion and activation in photocatalytic material systems and enhance charge carrier dynamics to achieve efficient photocatalytic nitrogen conversion.展开更多
Ammonia is an important chemical raw material and non-carbon-based fuel.Photocatalytic ammonia production technology as a mild alternative to the traditional Harbor–Bosch route is carried out at the air,liquid,and so...Ammonia is an important chemical raw material and non-carbon-based fuel.Photocatalytic ammonia production technology as a mild alternative to the traditional Harbor–Bosch route is carried out at the air,liquid,and solid three-phase interface.Promoting the activation of N_(2),depressing hydrogen evolution reaction(HER),and increasing the local N_(2) concentration around the catalyst surface are critical factors in achieving high conversion efficiency.In this paper,we proposed that defective TiO_(2)is surfacemodified by alkyl acids with different carbon chain lengths(C_(2),C_(5),C_(8),C_(11),and C_(14))to tune the catalyst surface properties.The defect sites greatly promote N_(2) adsorption and activation.The wettability of the catalyst can be regulated from hydrophilic to hydrophobic by the length of the alkyl chain.The hydrophobic surface enhances the N_(2) adsorption and increases the local N_(2) concentration due to its aerophile.Meanwhile,it depresses the proton adsorption and HER.Overall,the nitrogen reduction reaction(NRR)is greatly promoted.Among the series of samples,they present a systematic change and have a maximal NRR performance for n-octanoic acid-defective TiO_(2)(C8-Vo-TiO_(2);Vo=oxygen vacancy).The rate of ammonia production can be as high as 392μmol·g^(−1)·h^(−1).This work provides a new strategy for efficient ammonia synthesis at the three-phase interface using photocatalyst technology.展开更多
Harnessing solar energy by photocatalytically converting oxygen and water into high-value-added H_(2)O_(2)is a promising way of alleviating both environmental and energy issues.It is worth noting that suppressing detr...Harnessing solar energy by photocatalytically converting oxygen and water into high-value-added H_(2)O_(2)is a promising way of alleviating both environmental and energy issues.It is worth noting that suppressing detrimental side reactions,such as the generation of·O_(2)^(-),is a critical approach to enhancing H_(2)O_(2)production.Herein,a 2-fold interpenetrating 3D uranium-organic framework(YTU-W-1)was developed and introduced for photocatalytic H_(2)O_(2)production.The material demonstrates a different photocatalytic mechanism when employing uranyl as an initiator,as compared with the conventional semiconductor photocatalytic pathway involving photo-generated charge carriers.Benefiting from the strong hydrogen abstraction effect of the U≡O·and the direct one-step oxygen reduction pathway,YTU-W-1 exhibits enhanced photocatalytic performance for H_(2)O_(2)production with yield efficiency of 221μmol h^(-1)g^(-1).Furthermore,YTU-W-1 displays a high H_(2)O_(2)selectivity of 68%,confirmed by rotating ring-disk electrode(RRDE)measurement.DFTcalculations were used to elucidate the critical role of uranyl in the photocatalytic oxygen reduction reaction for H_(2)O_(2)production.This research introduces an innovative approach to photo-driven H_(2)O_(2)production,underscoring the potential for heterogeneous catalysts to engage in photocatalytic reactions independently of photogenerated charge carriers.展开更多
CdS nanowires-nitrogen doped graphene (CdS NWs-NGR) nanocomposites have been fabricated by an electrostatic self-assembly strategy followed by a hydrothermal reduction. The CdS NWs-NGR exhibits higher photoactivity ...CdS nanowires-nitrogen doped graphene (CdS NWs-NGR) nanocomposites have been fabricated by an electrostatic self-assembly strategy followed by a hydrothermal reduction. The CdS NWs-NGR exhibits higher photoactivity for selective reduction of aromatic nitro organics in water under visible light irradiation than blank CdS nanowires (CdS NWs) and CdS nanowires-reduced graphene oxide (CdS NWs-RGO) nanocomposites. The enhanced photoactivity of CdS NWs-NGR can be attributed to the improved electronic conductivity due to the introduc- tion of nitrogen atoms, which thus enhances the separation and transfer of charge carriers photogenerated from CdS NWs. Our work could provide a facile method to synthesize NGR based one-dimensional (1D) semiconductor composites for selective organic transformations, and broaden the potential applications for NGR as a cocatalyst.展开更多
This study employed microwave-assisted hydrothermal method to synthesize Ti-MCM-41,which are mesoporous materials with a high surface area and excellent photocatalytic ability. Fourier transform infrared spectroscopy...This study employed microwave-assisted hydrothermal method to synthesize Ti-MCM-41,which are mesoporous materials with a high surface area and excellent photocatalytic ability. Fourier transform infrared spectroscopy(FTIR), X-ray diffraction(XRD), X-ray photoelectron spectroscopy(XPS), transmission electron microscopy(TEM), and ultraviolet–visible spectroscopy(UV–Vis) were employed. The XRD findings showed that Ti-MCM-41 exhibited a peak at 2θ of 2.2°, which was attributed to the hexagonal MCM-41 structure. The BET(Brunauer–Emmett–Teller) results agreed with the TEM findings that Ti-MCM-41 has a pore size of about 3–5 nm and a high surface area of 883 m-2/g. FTIR results illustrated the existence of Si–O–Si and Si–O–Ti bonds in Ti-MCM-41. The appearance of Ti2 p peaks in the XPS results confirmed the FTIR findings that the Ti was successfully doped into the MCM-41 structure. Zeta(ζ)-potential results indicated that the iso-electric point(IEP) of Ti-MCM-41 was at about pH 3.02. In this study, the photocatalytic degradation of oxytetracycline(OTC) at different pH was investigated under Hg lamp irradiation(wavelength 365 nm). The rate constant(K′obs) for OTC degradation was 0.012 min-1at pH 3. Furthermore, TOC(total organic carbon) and high resolution LC–MS(liquid chromatography–mass spectrometry) analyses were conducted to elucidate the possible intermediate products and degradation pathway for OTC. The TOC removal efficiency of OTC degradation was 87.0%, 74.4% and 50.9% at pH 3, 7 and 10, respectively. LC–MS analysis results showed that the degradation products from OTC resulted from the removal of functional groups from the OTC ring.展开更多
TiO2-loaded activated carbon fibers (ACF) were prepared by a hydrothermal method. The samples were characterized by scanning electron microscopy (SEM), X-ray diffraction (XRD), Fourier transform infrared (FTIR...TiO2-loaded activated carbon fibers (ACF) were prepared by a hydrothermal method. The samples were characterized by scanning electron microscopy (SEM), X-ray diffraction (XRD), Fourier transform infrared (FTIR) spectrometry and UV-vis diffuse reflectance spectra (DRS). SEM images showed that the TiO2 nanoparticles were deposited on the surface of ACF, and the particle size and loading amount of TiO2 were varied by changing the initial concentration of tetrabutyl titanate (TBOT). The results of an ash experiment showed that the loading amounts of TiO2 were 18.4%, 43.3%, 52.5%, 75.1%, and 91.1% for initial concentrations of TBOT of 0.07,014, 0.21,0.28, and 0.35 tool/L, respectively, Physical interactions played an important role in the formation of TiO2/ACF composite fibers that absorb UV and visible light. Compared with those of ACF, improved adsorption and photocatalytic activity toward Rhodamine B (RhB) were observed for TiO2/ACF composite fiber. The Rhodamine B could be removed efficiently by TiO2/ACF composite fibers, and the TiO2 loading amount had a significant effect on the photocatalytic activity of TiO2/ACF composite fibers.展开更多
基金Funded by the National Natural Science Foundation of China(No.U1304520)the Education Department of Henan Province(2013GGJS-185)
文摘SnS2 nanoflakes were successfully synthesized via a simple hydrothermal process. The as-prepared SnS2 samples were characterized by X-ray diffraction(XRD), scanning electron microscopy(SEM), nitrogen adsorption-desorption isotherms, and UV-vis diffuse reflectance spectroscopy(DRS). The photocatalytic activities of the as-prepared SnS2 nanoflakes under visible light irradiation(λ〉420 nm) were evaluated by the degradation of rhodamine B(Rh B). The effect of hydrothermal temperatures on the photocatalytic efficiency of as-prepared SnS2 nanoflakes was investigated. The experimental result showed that SnS2 nanoflakes synthesized at the temprature of 160 o had higher photocatalytic efficiency and good photocatalytic stability.
基金financial support from the National Natural Science Foundation of China(22172021,22202170,21872022,21573039)。
文摘In the process of photocatalytic synthesis of ammonia,the kinetics of carrier separation and transport,adsorption of nitrogen,and activation of the N N triple bond are key factors that directly affect the efficiency of converting nitro-gen to ammonia.Here,we report a new strategy for anchoring MXene quan-tum dots(MXene QDs)onto the surface of ZnIn2S4 by forming Ti-S bonds,which provide a channel for the rapid separation and transport of charge car-riers and effectively extend the lifespan of photogenerated carriers.The unique charge distribution caused by the sulfurization of the MXene QDs further enhances the performance of the photocatalysts for the adsorption and activa-tion of nitrogen.The photocatalytic ammonia synthesis efficiency of MXene QDs-ZnIn2S4 can reach up to 360.5μmol g�1 h�1.Density functional theory calculations,various in situ techniques,and ultrafast spectroscopy are used to characterize the successful construction of Ti-S bonds and the dynamic nature of excited state charge carriers in MXene QDs-ZnIn2S4,as well as their impact on nitrogen adsorption activation and photocatalytic ammonia synthesis efficiency.This study provides a new example of how to improve nitrogen adsorp-tion and activation in photocatalytic material systems and enhance charge carrier dynamics to achieve efficient photocatalytic nitrogen conversion.
基金The authors would like to acknowledge the financial support of the National Natural Science Foundation of China(Nos.22272003,22172021,21872022,21573039,and 22202170).
文摘Ammonia is an important chemical raw material and non-carbon-based fuel.Photocatalytic ammonia production technology as a mild alternative to the traditional Harbor–Bosch route is carried out at the air,liquid,and solid three-phase interface.Promoting the activation of N_(2),depressing hydrogen evolution reaction(HER),and increasing the local N_(2) concentration around the catalyst surface are critical factors in achieving high conversion efficiency.In this paper,we proposed that defective TiO_(2)is surfacemodified by alkyl acids with different carbon chain lengths(C_(2),C_(5),C_(8),C_(11),and C_(14))to tune the catalyst surface properties.The defect sites greatly promote N_(2) adsorption and activation.The wettability of the catalyst can be regulated from hydrophilic to hydrophobic by the length of the alkyl chain.The hydrophobic surface enhances the N_(2) adsorption and increases the local N_(2) concentration due to its aerophile.Meanwhile,it depresses the proton adsorption and HER.Overall,the nitrogen reduction reaction(NRR)is greatly promoted.Among the series of samples,they present a systematic change and have a maximal NRR performance for n-octanoic acid-defective TiO_(2)(C8-Vo-TiO_(2);Vo=oxygen vacancy).The rate of ammonia production can be as high as 392μmol·g^(−1)·h^(−1).This work provides a new strategy for efficient ammonia synthesis at the three-phase interface using photocatalyst technology.
基金supported by the National Natural Science Foundation of China(22176163,22106117,52200204)the Natural Science Foundation of Shandong Province(ZR2020QB147,ZR2022QE032)+1 种基金the Young Taishan Scholars Program(tsqn201909082)the Interdisciplinary Basic Frontier Innovation Program of Suzhou Medical College of Soochow University(YXY2304031)。
文摘Harnessing solar energy by photocatalytically converting oxygen and water into high-value-added H_(2)O_(2)is a promising way of alleviating both environmental and energy issues.It is worth noting that suppressing detrimental side reactions,such as the generation of·O_(2)^(-),is a critical approach to enhancing H_(2)O_(2)production.Herein,a 2-fold interpenetrating 3D uranium-organic framework(YTU-W-1)was developed and introduced for photocatalytic H_(2)O_(2)production.The material demonstrates a different photocatalytic mechanism when employing uranyl as an initiator,as compared with the conventional semiconductor photocatalytic pathway involving photo-generated charge carriers.Benefiting from the strong hydrogen abstraction effect of the U≡O·and the direct one-step oxygen reduction pathway,YTU-W-1 exhibits enhanced photocatalytic performance for H_(2)O_(2)production with yield efficiency of 221μmol h^(-1)g^(-1).Furthermore,YTU-W-1 displays a high H_(2)O_(2)selectivity of 68%,confirmed by rotating ring-disk electrode(RRDE)measurement.DFTcalculations were used to elucidate the critical role of uranyl in the photocatalytic oxygen reduction reaction for H_(2)O_(2)production.This research introduces an innovative approach to photo-driven H_(2)O_(2)production,underscoring the potential for heterogeneous catalysts to engage in photocatalytic reactions independently of photogenerated charge carriers.
基金supported by the National Natural Science Foundation of China(NSFC)(20903022,20903023,21173045)the Award Program for Minjiang Scholar Professorship+2 种基金the Science and Technology Development of Foundation of Fuzhou University(2009-XQ-10)the Open Fund of Photocatalysis of Fuzhou University(0380038004)the Program for Returned High-Level Overseas Chinese Scholars of Fujian Province
文摘CdS nanowires-nitrogen doped graphene (CdS NWs-NGR) nanocomposites have been fabricated by an electrostatic self-assembly strategy followed by a hydrothermal reduction. The CdS NWs-NGR exhibits higher photoactivity for selective reduction of aromatic nitro organics in water under visible light irradiation than blank CdS nanowires (CdS NWs) and CdS nanowires-reduced graphene oxide (CdS NWs-RGO) nanocomposites. The enhanced photoactivity of CdS NWs-NGR can be attributed to the improved electronic conductivity due to the introduc- tion of nitrogen atoms, which thus enhances the separation and transfer of charge carriers photogenerated from CdS NWs. Our work could provide a facile method to synthesize NGR based one-dimensional (1D) semiconductor composites for selective organic transformations, and broaden the potential applications for NGR as a cocatalyst.
基金financial support provided by the Tunghai University Global Research and Education on Environment and Society (No. 103GREEnS 005-2)
文摘This study employed microwave-assisted hydrothermal method to synthesize Ti-MCM-41,which are mesoporous materials with a high surface area and excellent photocatalytic ability. Fourier transform infrared spectroscopy(FTIR), X-ray diffraction(XRD), X-ray photoelectron spectroscopy(XPS), transmission electron microscopy(TEM), and ultraviolet–visible spectroscopy(UV–Vis) were employed. The XRD findings showed that Ti-MCM-41 exhibited a peak at 2θ of 2.2°, which was attributed to the hexagonal MCM-41 structure. The BET(Brunauer–Emmett–Teller) results agreed with the TEM findings that Ti-MCM-41 has a pore size of about 3–5 nm and a high surface area of 883 m-2/g. FTIR results illustrated the existence of Si–O–Si and Si–O–Ti bonds in Ti-MCM-41. The appearance of Ti2 p peaks in the XPS results confirmed the FTIR findings that the Ti was successfully doped into the MCM-41 structure. Zeta(ζ)-potential results indicated that the iso-electric point(IEP) of Ti-MCM-41 was at about pH 3.02. In this study, the photocatalytic degradation of oxytetracycline(OTC) at different pH was investigated under Hg lamp irradiation(wavelength 365 nm). The rate constant(K′obs) for OTC degradation was 0.012 min-1at pH 3. Furthermore, TOC(total organic carbon) and high resolution LC–MS(liquid chromatography–mass spectrometry) analyses were conducted to elucidate the possible intermediate products and degradation pathway for OTC. The TOC removal efficiency of OTC degradation was 87.0%, 74.4% and 50.9% at pH 3, 7 and 10, respectively. LC–MS analysis results showed that the degradation products from OTC resulted from the removal of functional groups from the OTC ring.
基金financial support of the National Natural Science Foundation of China(No.21103017No.51104042)the Fundamental Research Funds for the Central Universities(No.110405007)
文摘TiO2-loaded activated carbon fibers (ACF) were prepared by a hydrothermal method. The samples were characterized by scanning electron microscopy (SEM), X-ray diffraction (XRD), Fourier transform infrared (FTIR) spectrometry and UV-vis diffuse reflectance spectra (DRS). SEM images showed that the TiO2 nanoparticles were deposited on the surface of ACF, and the particle size and loading amount of TiO2 were varied by changing the initial concentration of tetrabutyl titanate (TBOT). The results of an ash experiment showed that the loading amounts of TiO2 were 18.4%, 43.3%, 52.5%, 75.1%, and 91.1% for initial concentrations of TBOT of 0.07,014, 0.21,0.28, and 0.35 tool/L, respectively, Physical interactions played an important role in the formation of TiO2/ACF composite fibers that absorb UV and visible light. Compared with those of ACF, improved adsorption and photocatalytic activity toward Rhodamine B (RhB) were observed for TiO2/ACF composite fiber. The Rhodamine B could be removed efficiently by TiO2/ACF composite fibers, and the TiO2 loading amount had a significant effect on the photocatalytic activity of TiO2/ACF composite fibers.
基金supported by the National Natural Science Foundation of China(21833004)Taishan Scholar Program of Shandong Provincethe Natural Science Foundation of Shandong Province(ZR2020QA055)。