A novel spherical cellulose adsorbent has been prepared by homogeneous graft polymerization of N,N'-methylenebisacrylamide (MBA) onto cellulose in an ionic liquid, 1-N-butyl-3-methylimidazolium chloride (BMIMC1),...A novel spherical cellulose adsorbent has been prepared by homogeneous graft polymerization of N,N'-methylenebisacrylamide (MBA) onto cellulose in an ionic liquid, 1-N-butyl-3-methylimidazolium chloride (BMIMC1), which was then partially amine methylated through Mannich reaction to get bifunctionalized materials containing both amide and sulphinate moities. Factors affecting the attachment of functional groups were investigated. The adsorbent was characterized by Elemental Analysis (EA), Fourier Transform Infrared Spectroscopy (FTIR) and Scanning Electron Microscope (SEM). Cellulose adsorbent was then tested for its potential applications in the reduction adsorption oftrichloroacetic acid (TCAA) from aqueous solutions.展开更多
Due to the existence of water content in shale reservoir,it is quite meaningful to clarify the effect of water content on the methane adsorption capacity(MAC)of shale.However,the role of spatial configuration relation...Due to the existence of water content in shale reservoir,it is quite meaningful to clarify the effect of water content on the methane adsorption capacity(MAC)of shale.However,the role of spatial configuration relationship between organic matter(OM)and clay minerals in the MAC reduction process is still unclear.The Silurian Longmaxi Formation shale samples from the Southern Sichuan Basin in China were prepared at five relative humidity(RH)conditions(0%,16%,41%,76%,99%)and the methane adsorption experiments were conducted on these water-bearing shale samples to clarify the MAC reduction process considering the spatial configuration relationship between clay minerals and OM and establish the empirical model to fit the stages.Total organic carbon(TOC)content and mineral compositions were analyzed and the pore structures of these shale samples were characterized by field-emission scanning electron microscopy(FE-SEM),N2 adsorption and high-pressure mercury intrusion porosimetry(HPMIP).The results showed that the MAC reduction of clay minerals in OM occurred at different RH conditions from that of clay minerals outside OM.Furthermore,the amount of MAC reduction of shale samples prepared at the same RH condition was negatively related with clay content,which indicated the protection role of clay minerals for the MAC of water-bearing shale samples.The MAC reduction process was generally divided into three stages for siliceous and clayey shale samples.And the MAC of OM started to decline during stage(1)for calcareous shale sample mainly because water could enter OM pores more smoothly through hydrophobic pathway provided by carbonate minerals than through hydrophilic clay mineral pores.Overall,this study will contribute to improving the evaluation method of shale gas reserve.展开更多
Photocatalytic CO2 reduction on metal-oxide-based catalysts is promising for solving the energy and environmental crises faced by mankind. The oxygen vacancy (Vo) on metal oxides is expected to be a key factor affec...Photocatalytic CO2 reduction on metal-oxide-based catalysts is promising for solving the energy and environmental crises faced by mankind. The oxygen vacancy (Vo) on metal oxides is expected to be a key factor affecting the efficiency of photocatalytic CO2 reduction on metal-oxide-based catalysts. Yet, to date, the question of how an Vo influences photocatalytic CO2 reduction is still unanswered. Herein, we report that, on Vo-rich gallium oxide coated with Pt nanoparticles (Vo-rich Pt/Ga203), CO2 is photocatalytically reduced to CO, with a highly enhanced CO evolution rate (21.0umol.h-1) compared to those on Vo-poor Pt/Ga2O3 (3.9 gmol-h-1) and Pt/TiO2(P25) (6.7 gmol.h-1). We demonstrate that the Vo leads to improved CO2 adsorption and separation of the photoinduced charges on Pt/Ga203, thus enhancing the photocatalytic activity of Pt/Ga203. Rational fabrication of an Vo is thereby an attractive strategy for developing efficient catalysts for photocatalytic CO2 reduction.展开更多
Niobium oxide nanowire-deposited carbon fiber(CF) samples were prepared using a hydrothermal method with amorphous Nb2O5·nH2O as precursor. The physical properties of the samples were characterized by means of ...Niobium oxide nanowire-deposited carbon fiber(CF) samples were prepared using a hydrothermal method with amorphous Nb2O5·nH2O as precursor. The physical properties of the samples were characterized by means of numerous techniques, including X-ray diffraction(XRD), energy-dispersive spectroscopy(EDS), scanning electron microscopy(SEM), transmission electron microscopy(TEM), selected-area electron diffraction(SAED), UV–visible spectroscopy(UV–vis), N2 adsorption–desorption, Fourier transform infrared spectroscopy(FT-IR), and X-ray photoelectron spectroscopy. The efficiency for the removal of Cr(VI) was determined.Parameters such as pH value and initial Cr(VI) concentration could influence the Cr(VI) removal efficiency or adsorption capacity of the Nb2O5/carbon fiber sample obtained after hydrothermal treatment at 160°C for 14 hr. The maximal Cr(VI) adsorption capacity of the Nb2O5 nanowire/CF sample was 115 mg/g. This Nb2O5/CF sample also showed excellent photocatalytic activity and stability for the reduction of Cr(Ⅵ) under UV-light irradiation: the Cr(VI) removal efficiency reached 99.9% after UV-light irradiation for 1 hr and there was no significant decrease in photocatalytic performance after the use of the sample for 10 repeated cycles. Such excellent Cr(VI) adsorption capacity and photocatalytic performance was related to its high surface area,abundant surface hydroxyl groups, and good UV-light absorption ability.展开更多
Ferrihydrite is an important sink for the toxic heavy metal ions, such as Cr(Ⅵ). As ferrihydrite is thermodynamically unstable and gradually transforms into hematite and goethite, the stability of Cr(Ⅵ)-adsorbed fer...Ferrihydrite is an important sink for the toxic heavy metal ions, such as Cr(Ⅵ). As ferrihydrite is thermodynamically unstable and gradually transforms into hematite and goethite, the stability of Cr(Ⅵ)-adsorbed ferrihydrite is environmentally significant. This study investigated the phase transformation of Cr(Ⅵ)-adsorbed ferrihydrite at different pH in the presence of aqueous Mn(Ⅱ), as well as the fate of Mn(Ⅱ) and Cr(Ⅵ) in the transformation process of ferrihydrite. Among the ferrihydrite transformation products, hematite was dominant, and goethite was minor. The pre-adsorbed Cr(Ⅵ) inhibited the conversion of ferrihydrite to goethite at initial pH 3.0, whereas little amount of adsorbed Mn(Ⅱ) favored the formation of goethite at initial pH 7.0. After the aging process, Cr species in solid phase existed primarily as Cr(Ⅲ) in the presence of Mn(Ⅱ) at initial pH 7.0 and 11.0. The aqueous Mn concentration was predominantly unchanged at initial pH 3.0, whereas the aqueous Mn(Ⅱ) was adsorbed onto ferrihydrite or form Mn(OH)_(2) precipitates at initial pH 7.0 and 11.0, promoting the immobilization of Cr(Ⅵ). Moreover, the oxidation of Mn(Ⅱ) occurred at initial pH 7.0 and 11.0, forming Mn(Ⅲ/Ⅳ)(hydr)oxides.展开更多
基金Supported by the Science and Technology Project of Fujian Province Educational Department(JK2013004,JA12040)Science & Technology Development Fund of Fuzhou University(2012-XY-10,2014-XQ-11)the National Natural Science Foundation of China(41372346)
文摘A novel spherical cellulose adsorbent has been prepared by homogeneous graft polymerization of N,N'-methylenebisacrylamide (MBA) onto cellulose in an ionic liquid, 1-N-butyl-3-methylimidazolium chloride (BMIMC1), which was then partially amine methylated through Mannich reaction to get bifunctionalized materials containing both amide and sulphinate moities. Factors affecting the attachment of functional groups were investigated. The adsorbent was characterized by Elemental Analysis (EA), Fourier Transform Infrared Spectroscopy (FTIR) and Scanning Electron Microscope (SEM). Cellulose adsorbent was then tested for its potential applications in the reduction adsorption oftrichloroacetic acid (TCAA) from aqueous solutions.
基金supported by the National Science and Technology Major Project of China(No.2017ZX05035-002)the National Natural Science Foundation of China(No.41972145)the Foundation of State Key Laboratory of Petroleum Resources and Prospecting from China University of Petroleum in Beijing(Nos.PRP/indep-3-1707,PRP/indep-3-1615)。
文摘Due to the existence of water content in shale reservoir,it is quite meaningful to clarify the effect of water content on the methane adsorption capacity(MAC)of shale.However,the role of spatial configuration relationship between organic matter(OM)and clay minerals in the MAC reduction process is still unclear.The Silurian Longmaxi Formation shale samples from the Southern Sichuan Basin in China were prepared at five relative humidity(RH)conditions(0%,16%,41%,76%,99%)and the methane adsorption experiments were conducted on these water-bearing shale samples to clarify the MAC reduction process considering the spatial configuration relationship between clay minerals and OM and establish the empirical model to fit the stages.Total organic carbon(TOC)content and mineral compositions were analyzed and the pore structures of these shale samples were characterized by field-emission scanning electron microscopy(FE-SEM),N2 adsorption and high-pressure mercury intrusion porosimetry(HPMIP).The results showed that the MAC reduction of clay minerals in OM occurred at different RH conditions from that of clay minerals outside OM.Furthermore,the amount of MAC reduction of shale samples prepared at the same RH condition was negatively related with clay content,which indicated the protection role of clay minerals for the MAC of water-bearing shale samples.The MAC reduction process was generally divided into three stages for siliceous and clayey shale samples.And the MAC of OM started to decline during stage(1)for calcareous shale sample mainly because water could enter OM pores more smoothly through hydrophobic pathway provided by carbonate minerals than through hydrophilic clay mineral pores.Overall,this study will contribute to improving the evaluation method of shale gas reserve.
文摘Photocatalytic CO2 reduction on metal-oxide-based catalysts is promising for solving the energy and environmental crises faced by mankind. The oxygen vacancy (Vo) on metal oxides is expected to be a key factor affecting the efficiency of photocatalytic CO2 reduction on metal-oxide-based catalysts. Yet, to date, the question of how an Vo influences photocatalytic CO2 reduction is still unanswered. Herein, we report that, on Vo-rich gallium oxide coated with Pt nanoparticles (Vo-rich Pt/Ga203), CO2 is photocatalytically reduced to CO, with a highly enhanced CO evolution rate (21.0umol.h-1) compared to those on Vo-poor Pt/Ga2O3 (3.9 gmol-h-1) and Pt/TiO2(P25) (6.7 gmol.h-1). We demonstrate that the Vo leads to improved CO2 adsorption and separation of the photoinduced charges on Pt/Ga203, thus enhancing the photocatalytic activity of Pt/Ga203. Rational fabrication of an Vo is thereby an attractive strategy for developing efficient catalysts for photocatalytic CO2 reduction.
基金financially supported by the major Project of the national science and technology of China (No. SQ2017YFGX010248)the Beijing Natural Science Foundation (No. 2172011)
文摘Niobium oxide nanowire-deposited carbon fiber(CF) samples were prepared using a hydrothermal method with amorphous Nb2O5·nH2O as precursor. The physical properties of the samples were characterized by means of numerous techniques, including X-ray diffraction(XRD), energy-dispersive spectroscopy(EDS), scanning electron microscopy(SEM), transmission electron microscopy(TEM), selected-area electron diffraction(SAED), UV–visible spectroscopy(UV–vis), N2 adsorption–desorption, Fourier transform infrared spectroscopy(FT-IR), and X-ray photoelectron spectroscopy. The efficiency for the removal of Cr(VI) was determined.Parameters such as pH value and initial Cr(VI) concentration could influence the Cr(VI) removal efficiency or adsorption capacity of the Nb2O5/carbon fiber sample obtained after hydrothermal treatment at 160°C for 14 hr. The maximal Cr(VI) adsorption capacity of the Nb2O5 nanowire/CF sample was 115 mg/g. This Nb2O5/CF sample also showed excellent photocatalytic activity and stability for the reduction of Cr(Ⅵ) under UV-light irradiation: the Cr(VI) removal efficiency reached 99.9% after UV-light irradiation for 1 hr and there was no significant decrease in photocatalytic performance after the use of the sample for 10 repeated cycles. Such excellent Cr(VI) adsorption capacity and photocatalytic performance was related to its high surface area,abundant surface hydroxyl groups, and good UV-light absorption ability.
基金This research was supported by the National Natural Science Foundation of China(No.51978174)the Natural Science Foundation of Guangdong Province(No.2018A030313099).
文摘Ferrihydrite is an important sink for the toxic heavy metal ions, such as Cr(Ⅵ). As ferrihydrite is thermodynamically unstable and gradually transforms into hematite and goethite, the stability of Cr(Ⅵ)-adsorbed ferrihydrite is environmentally significant. This study investigated the phase transformation of Cr(Ⅵ)-adsorbed ferrihydrite at different pH in the presence of aqueous Mn(Ⅱ), as well as the fate of Mn(Ⅱ) and Cr(Ⅵ) in the transformation process of ferrihydrite. Among the ferrihydrite transformation products, hematite was dominant, and goethite was minor. The pre-adsorbed Cr(Ⅵ) inhibited the conversion of ferrihydrite to goethite at initial pH 3.0, whereas little amount of adsorbed Mn(Ⅱ) favored the formation of goethite at initial pH 7.0. After the aging process, Cr species in solid phase existed primarily as Cr(Ⅲ) in the presence of Mn(Ⅱ) at initial pH 7.0 and 11.0. The aqueous Mn concentration was predominantly unchanged at initial pH 3.0, whereas the aqueous Mn(Ⅱ) was adsorbed onto ferrihydrite or form Mn(OH)_(2) precipitates at initial pH 7.0 and 11.0, promoting the immobilization of Cr(Ⅵ). Moreover, the oxidation of Mn(Ⅱ) occurred at initial pH 7.0 and 11.0, forming Mn(Ⅲ/Ⅳ)(hydr)oxides.