CO_(2) mineralization plays a critical role in the storage and utilization of CO_(2).Coal fly ash(CFA)and red mud(RM)are widely utilized as CO_(2) mineralizers.However,the inert calcium species in CFA limit its carbon...CO_(2) mineralization plays a critical role in the storage and utilization of CO_(2).Coal fly ash(CFA)and red mud(RM)are widely utilized as CO_(2) mineralizers.However,the inert calcium species in CFA limit its carbonation capacity,meanwhile the substantial Ca^(2+)releasing of RM is hindered by a covering layer of calcium carbonate.In this study,CO_(2) mineralization in a composite system of CFA and RM was investigated to enhance the carbonation capacity.Multiple analyzers were employed to characterize the raw materials and resulting mineralization products.The results demonstrated that a synergistic effect existed in the composite system of CFA and RM,resulting in improving CO_(2) mineralization rate and efficiency.The produced calcium carbonate was ectopically attached the surface of CFA in the composite system,thus slowing down its coverage on the surface of RM.This phenomenon facilitated further releasing Ca^(2+)from the internal RM,thereby enhancing CO_(2) mineralization efficiency.Meanwhile,the inclusion of RM significantly improved the alkalinity of the composite system,which not only promoted the dissolution of Ca^(2+)of the inert CaSO_(4)(H_(2)O)_(2) in CFA,but also accelerated CO_(2) mineralization rate.The investigation would be beneficial to CO_(2) mineralization using industrial solid wastes.展开更多
Mineral matter in a residue(RC G)from coal gasification(CG)was removed by two-stage acid leaching.Hierarchical activated carbon(HAC)was prepared by activating RC Gwith CO2.The performance of HAC on removing methylene ...Mineral matter in a residue(RC G)from coal gasification(CG)was removed by two-stage acid leaching.Hierarchical activated carbon(HAC)was prepared by activating RC Gwith CO2.The performance of HAC on removing methylene blue(MB)from an aqueous solution was investigated.HAC was characterized by N2 adsorption–desorption isotherm,Fourier transform infrared spectroscopy,and scanning electron microscopy.The results show that HAC exhibits hierarchical pore structure with high specific surface area(862.76 m2·g-1)and total pore volume(0.684 cm3·g-1),and abundant organic functional groups.The adsorption equilibrium data of MB on HAC are best fitted to the Redlich-Peterson.The kinetic data show that the pseudo-first-order model is more suitable at low MB concentration,while the advantages of the pseudo-second-orderand the Elovich models are more obvious as the concentration increases.According to the thermodynamic parameters,the HAC-MB adsorption process is spontaneous and endothermic.展开更多
Phosphorus-doped carbon nanospheres without any metal residues were synthesized and characterized. The results revealed that the doping phosphorus atoms could significantly improve the electrocatalytic activity of gra...Phosphorus-doped carbon nanospheres without any metal residues were synthesized and characterized. The results revealed that the doping phosphorus atoms could significantly improve the electrocatalytic activity of graphitic carbon for the oxygen-reduction reaction (ORR) both in acidic and alkaline media, and the materials exhibited high electrocatalytic activity, long-term stability, and excellent tolerance to crossover effects especially in alkaline media. Quantum mechanics calculations with the density functional theory demonstrated that the changes in charge density and energetic characteristics of frontier orbitals for the P-doped graphene sheet could facilitate the ORR.展开更多
Soluble portions(SPs) 1-4(SP1-SP4) were afforded from sequentially dissolution and alkanolyses of Baiyinhua lignite(BL) in cyclohexane,CH3OH,CH3CH2OH,and(CH3)2CHOH at 300℃.They were analyzed with a gas chromatograph/...Soluble portions(SPs) 1-4(SP1-SP4) were afforded from sequentially dissolution and alkanolyses of Baiyinhua lignite(BL) in cyclohexane,CH3OH,CH3CH2OH,and(CH3)2CHOH at 300℃.They were analyzed with a gas chromatograph/mass spectrometer and quadrupole exactive orbitrap mass spectrometer(QEOTMS) with an atmosphere pressure chemical ionization source in positive-ion mode,while BL was characterized with an X-ray photoelectron spectrometer(XRPES).The results show that the yields of SP2 and SP3 are much higher than those of SP1 and SP4,and the total SP yield is ca.39.0%.According to the analysis with XRPES,pyrrolic nitrogen atoms are the most abundant nitrogen existing forms in BL.Thousands of nitrogen-containing aromatics(NCAs) were resolved with QEOTMS and their molecular masses are mainly in the range of 200-450 u.The main NCAs are N1O1 and N1O2 class species with double bond equivalent values of 4-18 and carbon numbers of 7-30.The nitrogen atoms appear in pyridine s,quinolines,benzoquinolines or acridine,and dibenzoquinolines or naphthoquinolines,while the oxygen atoms exist in methoxy and furan rings.展开更多
Fushun oil shale(FOS) was subjected to thermal dissolution(TD) under different conditions. The results show that the optimal solvent, temperature, time, and ratio of solvent to FOS are ethanol, 300 °C, 2 h, and 5...Fushun oil shale(FOS) was subjected to thermal dissolution(TD) under different conditions. The results show that the optimal solvent, temperature, time, and ratio of solvent to FOS are ethanol, 300 °C, 2 h, and 5 ml·g^(-1),respectively and the corresponding yield of the soluble portion(SP) is 32.2%(daf), which is much higher than the oil content of FOS(ca. 6%), suggesting that TD in ethanol is an excellent way to extract organics from FOS.According to 3 direct analyses, aliphatic moieties in FOS are the most abundant followed by C\\O-containing moieties and each cluster in FOS has 3 conjugated aromatic rings on average with fewer substituents. According to the analysis with a gas chromatograph/mass spectrometer, alkanes are predominant in all the SPs. A number of alkenes were identified in the SPs from the TD, while none of the alkenes were detected in acetone-SP obtained at room temperature, implying that the TD can destroy the π-π and intertwining interactions between alkenes and macromolecular structures in FOS. Moreover, a small amount of alkyl-substituted phenols and alkoxysubstituted phenols were detected in ethanol-SP from the TD, which could be the products from ethanolyzing the macromolecular moiety of FOS.展开更多
A series of Pd/γ-Al_(2)O_(3) hybrid catalysts were prepared by impregnation and subsequent calcination under microwave irradiation.The catalysts were used for direct synthesis of dimethylether(DME)from syngas.The res...A series of Pd/γ-Al_(2)O_(3) hybrid catalysts were prepared by impregnation and subsequent calcination under microwave irradiation.The catalysts were used for direct synthesis of dimethylether(DME)from syngas.The results show that calcination under microwave irradiation improved both the activity and selectivity of the catalysts for DME synthesis.The optimum power of the microwave was determined to be 420 W.Under such optimum conditions,CO conversion,DME selectivity and time space yield of DME were 60.1%,67.0%,and 21.5 mmol$mL-1$h^(-1),respectively.Based on various characterizations such as nitrogen physisorption,X-ray diffraction,COtemperature-programmed desorption,and Fourier transform infrared spectral analysis,the promotional effect of the microwave irradiation on the catalytic property was mainly attributed to both the higher dispersion of Pd and the significant increase in the adsorption on the CO-bridge of Pd.Microwave irradiation with very high power led to the increase in CO-bridge adsorption and thereby decreased the catalytic activity,whereas the coverage by metallic Pd of the active sites on acidicγ-Al_(2)O_(3) significantly occurred under microwave irradiation with very low power,resulting in a decrease in the selectivity to DME.展开更多
基金National Natural Science Foundation of China(21706172)Shanxi Province Natural Science Foundation(202203021221069 and 20210302123167).
文摘CO_(2) mineralization plays a critical role in the storage and utilization of CO_(2).Coal fly ash(CFA)and red mud(RM)are widely utilized as CO_(2) mineralizers.However,the inert calcium species in CFA limit its carbonation capacity,meanwhile the substantial Ca^(2+)releasing of RM is hindered by a covering layer of calcium carbonate.In this study,CO_(2) mineralization in a composite system of CFA and RM was investigated to enhance the carbonation capacity.Multiple analyzers were employed to characterize the raw materials and resulting mineralization products.The results demonstrated that a synergistic effect existed in the composite system of CFA and RM,resulting in improving CO_(2) mineralization rate and efficiency.The produced calcium carbonate was ectopically attached the surface of CFA in the composite system,thus slowing down its coverage on the surface of RM.This phenomenon facilitated further releasing Ca^(2+)from the internal RM,thereby enhancing CO_(2) mineralization efficiency.Meanwhile,the inclusion of RM significantly improved the alkalinity of the composite system,which not only promoted the dissolution of Ca^(2+)of the inert CaSO_(4)(H_(2)O)_(2) in CFA,but also accelerated CO_(2) mineralization rate.The investigation would be beneficial to CO_(2) mineralization using industrial solid wastes.
基金financial support from the National Natural Science Foundation of China(51762042)the(2019PT-18)+1 种基金the Science and Technology Program of Shaanxi Province(2017GY-136,2018GY-086)the Shaanxi Province Education Department Key Scientific Research Project(18JS123)。
文摘Mineral matter in a residue(RC G)from coal gasification(CG)was removed by two-stage acid leaching.Hierarchical activated carbon(HAC)was prepared by activating RC Gwith CO2.The performance of HAC on removing methylene blue(MB)from an aqueous solution was investigated.HAC was characterized by N2 adsorption–desorption isotherm,Fourier transform infrared spectroscopy,and scanning electron microscopy.The results show that HAC exhibits hierarchical pore structure with high specific surface area(862.76 m2·g-1)and total pore volume(0.684 cm3·g-1),and abundant organic functional groups.The adsorption equilibrium data of MB on HAC are best fitted to the Redlich-Peterson.The kinetic data show that the pseudo-first-order model is more suitable at low MB concentration,while the advantages of the pseudo-second-orderand the Elovich models are more obvious as the concentration increases.According to the thermodynamic parameters,the HAC-MB adsorption process is spontaneous and endothermic.
基金supported by the Guangdong Provincial Science and Technology Project of China (2011B010400016)China Postdoctoral Science Foundation (No. 20110490878)
文摘Phosphorus-doped carbon nanospheres without any metal residues were synthesized and characterized. The results revealed that the doping phosphorus atoms could significantly improve the electrocatalytic activity of graphitic carbon for the oxygen-reduction reaction (ORR) both in acidic and alkaline media, and the materials exhibited high electrocatalytic activity, long-term stability, and excellent tolerance to crossover effects especially in alkaline media. Quantum mechanics calculations with the density functional theory demonstrated that the changes in charge density and energetic characteristics of frontier orbitals for the P-doped graphene sheet could facilitate the ORR.
基金Supported by the Key Project of Joint Fund from National Natural Science Foundation of China and the Government of Xinjiang Uygur Autonomous Region(U1503293)the National Key Research and Development Program of China(2018YFB0604602)the Priority Academic Program Development of Jiangsu Higher Education Institutions.
文摘Soluble portions(SPs) 1-4(SP1-SP4) were afforded from sequentially dissolution and alkanolyses of Baiyinhua lignite(BL) in cyclohexane,CH3OH,CH3CH2OH,and(CH3)2CHOH at 300℃.They were analyzed with a gas chromatograph/mass spectrometer and quadrupole exactive orbitrap mass spectrometer(QEOTMS) with an atmosphere pressure chemical ionization source in positive-ion mode,while BL was characterized with an X-ray photoelectron spectrometer(XRPES).The results show that the yields of SP2 and SP3 are much higher than those of SP1 and SP4,and the total SP yield is ca.39.0%.According to the analysis with XRPES,pyrrolic nitrogen atoms are the most abundant nitrogen existing forms in BL.Thousands of nitrogen-containing aromatics(NCAs) were resolved with QEOTMS and their molecular masses are mainly in the range of 200-450 u.The main NCAs are N1O1 and N1O2 class species with double bond equivalent values of 4-18 and carbon numbers of 7-30.The nitrogen atoms appear in pyridine s,quinolines,benzoquinolines or acridine,and dibenzoquinolines or naphthoquinolines,while the oxygen atoms exist in methoxy and furan rings.
基金Supported by the Fundamental Research Funds for the Central Universities(2017BSCXB27)the Research and the Postgraduate Research&Practice Innovation Program of Jiangsu Province(KYCX17_1507)
文摘Fushun oil shale(FOS) was subjected to thermal dissolution(TD) under different conditions. The results show that the optimal solvent, temperature, time, and ratio of solvent to FOS are ethanol, 300 °C, 2 h, and 5 ml·g^(-1),respectively and the corresponding yield of the soluble portion(SP) is 32.2%(daf), which is much higher than the oil content of FOS(ca. 6%), suggesting that TD in ethanol is an excellent way to extract organics from FOS.According to 3 direct analyses, aliphatic moieties in FOS are the most abundant followed by C\\O-containing moieties and each cluster in FOS has 3 conjugated aromatic rings on average with fewer substituents. According to the analysis with a gas chromatograph/mass spectrometer, alkanes are predominant in all the SPs. A number of alkenes were identified in the SPs from the TD, while none of the alkenes were detected in acetone-SP obtained at room temperature, implying that the TD can destroy the π-π and intertwining interactions between alkenes and macromolecular structures in FOS. Moreover, a small amount of alkyl-substituted phenols and alkoxysubstituted phenols were detected in ethanol-SP from the TD, which could be the products from ethanolyzing the macromolecular moiety of FOS.
基金supported by the Special Fund for Major State Basic Research Project(Grant 2005CB221204-G)the Fund from the Natural Science Foundation of China for Innovative Research Group(Grant 50921002)+1 种基金the Research Fund from Key Laboratory of Coal Processing&Efficient Utilization,Ministry of Education(Grant CPEUKF08-09)Yong Teacher Research Foundation from China University of Mining&Technology(Grant OH080254).
文摘A series of Pd/γ-Al_(2)O_(3) hybrid catalysts were prepared by impregnation and subsequent calcination under microwave irradiation.The catalysts were used for direct synthesis of dimethylether(DME)from syngas.The results show that calcination under microwave irradiation improved both the activity and selectivity of the catalysts for DME synthesis.The optimum power of the microwave was determined to be 420 W.Under such optimum conditions,CO conversion,DME selectivity and time space yield of DME were 60.1%,67.0%,and 21.5 mmol$mL-1$h^(-1),respectively.Based on various characterizations such as nitrogen physisorption,X-ray diffraction,COtemperature-programmed desorption,and Fourier transform infrared spectral analysis,the promotional effect of the microwave irradiation on the catalytic property was mainly attributed to both the higher dispersion of Pd and the significant increase in the adsorption on the CO-bridge of Pd.Microwave irradiation with very high power led to the increase in CO-bridge adsorption and thereby decreased the catalytic activity,whereas the coverage by metallic Pd of the active sites on acidicγ-Al_(2)O_(3) significantly occurred under microwave irradiation with very low power,resulting in a decrease in the selectivity to DME.