Crystallined hybrid carbon was synthesized by the catalytic carbonization of biomass (Pinus kesiya sawdust) at 1100 ℃ and in-situ growth of carbon nanofibers (CNFs) at 750 ℃ from acetylene. The microstructure of...Crystallined hybrid carbon was synthesized by the catalytic carbonization of biomass (Pinus kesiya sawdust) at 1100 ℃ and in-situ growth of carbon nanofibers (CNFs) at 750 ℃ from acetylene. The microstructure of the composite was characterized by scanning electron microscopy (SEM), X-ray diffraction (XRD), transmission electron microscopy (TEM) and high-resolution transmission electron microscopy (HRTEM). It was found that highly crystallined carbon composed of well-aligned graph℃ene layers with interlayer spacing of 0.34 nm can be formed by catalytic carbonization of biomass. However, the structure of the in-situ growing CNFs is lessaligned. Based on the results of the investigation, the formation mechanism of the crystallined hybrid carbon was discussed. Owning to synergistic effect of the highly crystallined carbon and the conductive network formed by CNFs, the crystallined hybrid carbon shows 32.6% lower electrical resistivity than biocarbon. When being used as anode material of lithium-ion batteries (LIBs), the crystallined hybrid carbon and the biocarbon have nearly the same first coulombic efficiencies (CEs), however, the former has a discharge capacity of 67% higher than the latter since the second cycle.展开更多
Through our newly-developed "chemical vapor deposition integrated process (ISVD-IP)'" using carbon OlOXlae (t..u2) as me raw matenal and only carbon source introduced, CO2 could be catalytically activated and c...Through our newly-developed "chemical vapor deposition integrated process (ISVD-IP)'" using carbon OlOXlae (t..u2) as me raw matenal and only carbon source introduced, CO2 could be catalytically activated and converted to a new solid-form product, i.e., carbon nanotubes (CO2-derived) at a quite high yield (the single-pass carbon yield in the solid-form carbon-product produced from CO2 catalytic capture and conversion was more than 30% at a single-pass carbon-base). For comparison, when only pure carbon dioxide was introduced using the conventional CVD method without integrated process, no solid-form carbon-material product could be formed. In the addition of saturated steam at room temperature in the feed for CVD, there were much more end-opening carbon nano-tubes produced, at a slightly higher carbon yield. These inspiring works opened a remarkable and alternative new approach for carbon dioxide catalytic capture to solid-form product, comparing with that of CO2 sequestration (CCS) or CO2 mineralization (solidification), etc. As a result, there was much less body volume and almost no greenhouse effect for this solid-form carbon-material than those of primitive carbon dioxide.展开更多
To improve the denitrification performance of carbon-based materials for sintering flue gas,we prepared a composite catalyst comprising coconut shell activated carbon(AC)modified by thermal oxidation air.The microstru...To improve the denitrification performance of carbon-based materials for sintering flue gas,we prepared a composite catalyst comprising coconut shell activated carbon(AC)modified by thermal oxidation air.The microstructure,the specific surface area,the pore volume,the crystal structure,and functional groups presented in the prepared Cu2O/AC catalysts were thoroughly characterized.By using scanning electron microscopy(SEM),nitrogen adsorption/desorption isotherms,Fourier-transform infrared(FTIR)spectroscopy and X-ray diffractometry(XRD),the effects of Cu2O loading and calcination temperature on Cu2O/AC catalysts were investigated at low temperature(150℃).The research shows that Cu on the Cu2O/AC catalyst is in the form of Cu2O with good crystalline performance and is spherical and uniformly dispersed on the AC surface.The loading of Cu2O increases the active sites and the specific surface area of the reaction gas contact,which is conducive to the rapid progress of the carbon monoxide selective catalytic reduction(CO-SCR)reaction.When the loading of Cu2O was 8%and the calcination temperature was 500℃,the removal rate of NOx facilitated by the Cu2O/AC catalyst reached 97.9%.These findings provide a theoretical basis for understanding the denitrification of sintering flue gas.展开更多
The development of efficient catalytic electrode toward oxygen reduction reaction(ORR)is still a great challenge for the wide use of zinc–air batteries.Herein,Co_(2)N nanoparticles(NPs)anchored on N-doped carbon from...The development of efficient catalytic electrode toward oxygen reduction reaction(ORR)is still a great challenge for the wide use of zinc–air batteries.Herein,Co_(2)N nanoparticles(NPs)anchored on N-doped carbon from cattail were verified with excellent catalytic performances for ORR.The onset and half-wave potentials over the optimal catalyst reach to 0.96 V and 0.84 V,respectively.Current retention rates of 96.8%after 22-h test and 98.8%after running 1600 s were obtained in 1 M methanol solution.Density functional theory simulation proposes an apparently increased electronic states of Co_(2)N in N-doped carbon layer close to the Fermi level.Higher charge density,favorable adsorption,and charge transfer of intermediates originate from the coexistence of Co_(2)N NPs and N atoms in carbon skeleton.The superior catalytic activity of composites also was confirmed in zinc–air batteries.This novel catalytic property and controllable preparation approach of Co_(2)Ncarbon composites provide a promising avenue to fabricate metal-containing catalytically active carbon from biomass.展开更多
Commercial spherical activated carbon(SAC) was modified by impregnation to enhance the catalytic properties of SAC in acetylene hydrochlorination through melamine modification. Different modification conditions for ...Commercial spherical activated carbon(SAC) was modified by impregnation to enhance the catalytic properties of SAC in acetylene hydrochlorination through melamine modification. Different modification conditions for SAC with nitrogen were compared by changing the SAC-Melamine ratios. The effect of carbonization temperature on the modification was also investigated. Surface chemistry and adsorption properties of the modified and unmodified SACs were studied by scanning electron microscope(SEM), X-ray photoelectron spectroscopy(XPS), elementary analysis, BET, and temperature-programmed desorption(TPD). Moreover, the catalytic properties of SAC in acetylene hydrochlorination under differently modified conditions were also investigated. Elemental analysis showed that the nitrogen content of the modified SAC was greatly improved. XPS revealed that nitrogen mainly exists in Pyrrole nitrogen and Pyridine nitrogen. TPD showed that desorption of C2H2 was changed by modification. The conversion rate of acetylene was up to 70% under the following reaction conditions: temperature, 150 ℃; C2H2 hourly space velocity(GHSV), 36 h-1; feed volume ratio V(HCl)/V(C2H2) = 1.15. The catalytic properties of SAC were improved significantly via melamine modification.展开更多
There are abundant bitumens and oil seepages stored in vugs in a Lower-Triassic Daye formation(T_1d)marlite in Ni'erguan village in the Southern Guizhou Depression. However, the source of those oil seepages has no...There are abundant bitumens and oil seepages stored in vugs in a Lower-Triassic Daye formation(T_1d)marlite in Ni'erguan village in the Southern Guizhou Depression. However, the source of those oil seepages has not been determined to date. Multiple suites of source rocks of different ages exist in the depression. Both the oil seepages and potential source rocks have undergone complicated secondary alterations, which have added to the difficulty of an oil-source correlation. For example, the main source rock, a Lower-Cambrian Niutitang Formation"(∈_1n) mudstone, is over mature, and other potential source rocks, both from the Permian and the Triassic, are still in the oil window. In addition, the T_1d oil seepages underwent a large amount of biodegradation. To minimize the influence of biodegradation and thermal maturation, special methods were employed in this oil-source correlation study. These methods included catalytic hydropyrolysis, to release covalently bound biomarkers from the over mature"kerogen of ∈_1n mudstone, sequential extraction, to obtain chloroform bitumen A and chloroform bitumen C from the T_1d marlite, and anhydrous pyrolysis, to release pyrolysates from the kerogen of T_1d marlite. Using the methods above, the biomarkers and n-alkanes releasedfrom the oil samples and source rocks were analysed by GC–MS and GC-C-IRMS. The oil-source correlation indicated that the T_1d oil seepage primarily originated from"the ∈_1n mudstone and was partially mixed with oil generated from the T_1d marlite. Furthermore, the seepage also demonstrated that the above methods were effective for the complicated oil-source correlation in the Southern Guizhou Depression.展开更多
The reduction of low-concentration carbon dioxide with water to organic fuels is still a huge challenge. In this study, we successfully designed the partially oxidized cobalt nanoparticles coated by the nitrogendoped ...The reduction of low-concentration carbon dioxide with water to organic fuels is still a huge challenge. In this study, we successfully designed the partially oxidized cobalt nanoparticles coated by the nitrogendoped carbon layer(Co@NC) of 2-8 nm via a facile method and then interspersed with different amount of Pt nanoparticles. The Co@NC decorated with 1 wt% Pt exhibits the best ability for COreduction to CHand a CHproduction rate of 14.4 μmol·g·his achieved. It is worth noting that the system is carried out under low-concentration CO(400 ppm) circumstance without any sacrificial agent, which could be meaningful to the design of catalysts for atmospheric COreduction.展开更多
The properties of the porous granules produced by agglomeration of catalytically grown carbon nanofibers were investigated in this work. The single pellet crushing strength of the granules is high, e.g., 1.6-2.5 MPa. ...The properties of the porous granules produced by agglomeration of catalytically grown carbon nanofibers were investigated in this work. The single pellet crushing strength of the granules is high, e.g., 1.6-2.5 MPa. They have high specific surface areas, averaging 72-141 m^2·g^-1, and the majority of their pores are mesopores or macropores. The adsorption at 298 K of benzene or phenol on the granules is much lower than that on activated carbon and depends not only on the specific surface area of the carbon material but also on the sewing structure of the granules and the morphology of the carbon nanofibers. Treatment in dilute nitric acid appreciably reduces such adsorption.展开更多
Ozonation of oxalate in aqueous phase was performed with a commercial activated carbon(AC)in this work. The effect of AC dosage and solution pH on the contribution of hydroxyl radicals(HOU) in bulk solution and ox...Ozonation of oxalate in aqueous phase was performed with a commercial activated carbon(AC)in this work. The effect of AC dosage and solution pH on the contribution of hydroxyl radicals(HOU) in bulk solution and oxidation on the AC surface to the removal of oxalate was studied. We found that the removal of oxalate was reduced by tert-butyl alcohol(tBA) with low dosages of AC,while it was hardly affected by tBA when the AC dosage was greater than 0.3 g/L. tBA also inhibited ozone decomposition when the AC dosage was no more than 0.05 g/L, but it did not work when the AC dosage was no less than 0.1 g/L. These observations indicate that HOUin bulk solution and oxidation on the AC surface both contribute to the removal of oxalate. HOU oxidation in bulk solution is significant when the dosage of AC is low, whereas surface oxidation is dominant when the dosage of AC is high. The oxalate removal decreased with increasing pH of the solution with an AC dosage of 0.5 g/L. The degradation of oxalate occurs mainly through surface oxidation in acid and neutral solution, but through HOUoxidation in basic bulk solution. A mechanism involving both HOUoxidation in bulk solution and surface oxidation was proposed for AC enhanced ozonation of oxalate.展开更多
Carbon nanotube (CNT) arrays were fabricated on Ct-Me-N-(O) alloys with content of Ct in the range of 6-40 at.% by chemical vapour deposition. The Ct was a catalytic metal from the group of the following elements...Carbon nanotube (CNT) arrays were fabricated on Ct-Me-N-(O) alloys with content of Ct in the range of 6-40 at.% by chemical vapour deposition. The Ct was a catalytic metal from the group of the following elements: Ni, Co, Fe, Pd, while Me was a transition metal from the group of IV-VII of the periodic table (where Me=Ti, V, Cr, Zr, Nb, Mo, Ta, W, Re). Carbon nanotubes were found to grow efficiently on the alloy surface with its composition containing Ti, V, Cr, Zr, Hf, Nb or Ta. The growth of CNTs was not observed when the alloy contained W or Re. Additions of oxygen and nitrogen in the alloy facilitated the formation of oxynitrides and catalyst extrusion on the alloy surface. Replacement of the metals in alloy composition affected the diameter of the resulting CNTs. The obtained results showed that the alloy films of varying thickness (10-500 nm) may be used for the CNTs growth. The resulting CNT material was highly homogenous and its synthesis reproducible.展开更多
基金supported by the National Natural Science Foundation of China(No.51264016)the Natural Science Foundation of Yunnan Province of China(No.2009ZC006X)+1 种基金the Scientific Research Foundation of Kunming University of Science and Technology,China(No.2009-027)the Analysis and Testing Foundation of Kunming University of Science and Technology,China(No.2011458)
文摘Crystallined hybrid carbon was synthesized by the catalytic carbonization of biomass (Pinus kesiya sawdust) at 1100 ℃ and in-situ growth of carbon nanofibers (CNFs) at 750 ℃ from acetylene. The microstructure of the composite was characterized by scanning electron microscopy (SEM), X-ray diffraction (XRD), transmission electron microscopy (TEM) and high-resolution transmission electron microscopy (HRTEM). It was found that highly crystallined carbon composed of well-aligned graph℃ene layers with interlayer spacing of 0.34 nm can be formed by catalytic carbonization of biomass. However, the structure of the in-situ growing CNFs is lessaligned. Based on the results of the investigation, the formation mechanism of the crystallined hybrid carbon was discussed. Owning to synergistic effect of the highly crystallined carbon and the conductive network formed by CNFs, the crystallined hybrid carbon shows 32.6% lower electrical resistivity than biocarbon. When being used as anode material of lithium-ion batteries (LIBs), the crystallined hybrid carbon and the biocarbon have nearly the same first coulombic efficiencies (CEs), however, the former has a discharge capacity of 67% higher than the latter since the second cycle.
基金the National 973 Program of Ministry of Sciences and Technologies of China(2011CB201202)the National Natural Science Foundation of China(20776089)
文摘Through our newly-developed "chemical vapor deposition integrated process (ISVD-IP)'" using carbon OlOXlae (t..u2) as me raw matenal and only carbon source introduced, CO2 could be catalytically activated and converted to a new solid-form product, i.e., carbon nanotubes (CO2-derived) at a quite high yield (the single-pass carbon yield in the solid-form carbon-product produced from CO2 catalytic capture and conversion was more than 30% at a single-pass carbon-base). For comparison, when only pure carbon dioxide was introduced using the conventional CVD method without integrated process, no solid-form carbon-material product could be formed. In the addition of saturated steam at room temperature in the feed for CVD, there were much more end-opening carbon nano-tubes produced, at a slightly higher carbon yield. These inspiring works opened a remarkable and alternative new approach for carbon dioxide catalytic capture to solid-form product, comparing with that of CO2 sequestration (CCS) or CO2 mineralization (solidification), etc. As a result, there was much less body volume and almost no greenhouse effect for this solid-form carbon-material than those of primitive carbon dioxide.
基金Open Fund of Key Laboratory of Ministry of Education for Metallurgical Emission Reduction and Comprehensive Utilization of Resources,China(No.JKF19-08)General Project of Science and Technology Plan of Yunnan Science and Technology Department,China(No.2019FB077)+1 种基金Industrialization Cultivation Project of Scientific Research Fund of Yunnan Provincial Department of Education,China(No.2016CYH07)Top Young Talents of Yunnan Ten Thousand Talents Plan,China(No.YNWR-QNBJ-2019-263)。
文摘To improve the denitrification performance of carbon-based materials for sintering flue gas,we prepared a composite catalyst comprising coconut shell activated carbon(AC)modified by thermal oxidation air.The microstructure,the specific surface area,the pore volume,the crystal structure,and functional groups presented in the prepared Cu2O/AC catalysts were thoroughly characterized.By using scanning electron microscopy(SEM),nitrogen adsorption/desorption isotherms,Fourier-transform infrared(FTIR)spectroscopy and X-ray diffractometry(XRD),the effects of Cu2O loading and calcination temperature on Cu2O/AC catalysts were investigated at low temperature(150℃).The research shows that Cu on the Cu2O/AC catalyst is in the form of Cu2O with good crystalline performance and is spherical and uniformly dispersed on the AC surface.The loading of Cu2O increases the active sites and the specific surface area of the reaction gas contact,which is conducive to the rapid progress of the carbon monoxide selective catalytic reduction(CO-SCR)reaction.When the loading of Cu2O was 8%and the calcination temperature was 500℃,the removal rate of NOx facilitated by the Cu2O/AC catalyst reached 97.9%.These findings provide a theoretical basis for understanding the denitrification of sintering flue gas.
基金Financial supports from the National Natural Science Foundation of China(no.31901272,no.22075254)the Jiangsu Province Key Laboratory of Biomass Energy and Materials(no.JSBEM-S-201906)。
文摘The development of efficient catalytic electrode toward oxygen reduction reaction(ORR)is still a great challenge for the wide use of zinc–air batteries.Herein,Co_(2)N nanoparticles(NPs)anchored on N-doped carbon from cattail were verified with excellent catalytic performances for ORR.The onset and half-wave potentials over the optimal catalyst reach to 0.96 V and 0.84 V,respectively.Current retention rates of 96.8%after 22-h test and 98.8%after running 1600 s were obtained in 1 M methanol solution.Density functional theory simulation proposes an apparently increased electronic states of Co_(2)N in N-doped carbon layer close to the Fermi level.Higher charge density,favorable adsorption,and charge transfer of intermediates originate from the coexistence of Co_(2)N NPs and N atoms in carbon skeleton.The superior catalytic activity of composites also was confirmed in zinc–air batteries.This novel catalytic property and controllable preparation approach of Co_(2)Ncarbon composites provide a promising avenue to fabricate metal-containing catalytically active carbon from biomass.
基金Funded by the National Basic Research Program of China(973 Program,2012CB720302)the Program for Changjiang Scholars and Innovative Research Team in University(No.IRT1161)the Corps Science and Technology Innovation Team Scheme(2011CC001)
文摘Commercial spherical activated carbon(SAC) was modified by impregnation to enhance the catalytic properties of SAC in acetylene hydrochlorination through melamine modification. Different modification conditions for SAC with nitrogen were compared by changing the SAC-Melamine ratios. The effect of carbonization temperature on the modification was also investigated. Surface chemistry and adsorption properties of the modified and unmodified SACs were studied by scanning electron microscope(SEM), X-ray photoelectron spectroscopy(XPS), elementary analysis, BET, and temperature-programmed desorption(TPD). Moreover, the catalytic properties of SAC in acetylene hydrochlorination under differently modified conditions were also investigated. Elemental analysis showed that the nitrogen content of the modified SAC was greatly improved. XPS revealed that nitrogen mainly exists in Pyrrole nitrogen and Pyridine nitrogen. TPD showed that desorption of C2H2 was changed by modification. The conversion rate of acetylene was up to 70% under the following reaction conditions: temperature, 150 ℃; C2H2 hourly space velocity(GHSV), 36 h-1; feed volume ratio V(HCl)/V(C2H2) = 1.15. The catalytic properties of SAC were improved significantly via melamine modification.
基金supported jointly by the National Science and Technology Major Project of China (Grant Nos: 2011ZX05008002 and 2011ZX05005-001)
文摘There are abundant bitumens and oil seepages stored in vugs in a Lower-Triassic Daye formation(T_1d)marlite in Ni'erguan village in the Southern Guizhou Depression. However, the source of those oil seepages has not been determined to date. Multiple suites of source rocks of different ages exist in the depression. Both the oil seepages and potential source rocks have undergone complicated secondary alterations, which have added to the difficulty of an oil-source correlation. For example, the main source rock, a Lower-Cambrian Niutitang Formation"(∈_1n) mudstone, is over mature, and other potential source rocks, both from the Permian and the Triassic, are still in the oil window. In addition, the T_1d oil seepages underwent a large amount of biodegradation. To minimize the influence of biodegradation and thermal maturation, special methods were employed in this oil-source correlation study. These methods included catalytic hydropyrolysis, to release covalently bound biomarkers from the over mature"kerogen of ∈_1n mudstone, sequential extraction, to obtain chloroform bitumen A and chloroform bitumen C from the T_1d marlite, and anhydrous pyrolysis, to release pyrolysates from the kerogen of T_1d marlite. Using the methods above, the biomarkers and n-alkanes releasedfrom the oil samples and source rocks were analysed by GC–MS and GC-C-IRMS. The oil-source correlation indicated that the T_1d oil seepage primarily originated from"the ∈_1n mudstone and was partially mixed with oil generated from the T_1d marlite. Furthermore, the seepage also demonstrated that the above methods were effective for the complicated oil-source correlation in the Southern Guizhou Depression.
基金financially supported by the National Natural Science Foundation of China(Nos.51772312 and 51472260)the Environmental Functional Materials Innovation Team of Ministry of Education(IRT 16R49)the International Joint Laboratory on Resource Chemistry(IJLRC)
文摘The reduction of low-concentration carbon dioxide with water to organic fuels is still a huge challenge. In this study, we successfully designed the partially oxidized cobalt nanoparticles coated by the nitrogendoped carbon layer(Co@NC) of 2-8 nm via a facile method and then interspersed with different amount of Pt nanoparticles. The Co@NC decorated with 1 wt% Pt exhibits the best ability for COreduction to CHand a CHproduction rate of 14.4 μmol·g·his achieved. It is worth noting that the system is carried out under low-concentration CO(400 ppm) circumstance without any sacrificial agent, which could be meaningful to the design of catalysts for atmospheric COreduction.
基金The authors thank National Science Foundation of ChinaNingxia Natural Gas Conversion Key Lab for financial supports under contract No.20006012 and No.2004008.
文摘The properties of the porous granules produced by agglomeration of catalytically grown carbon nanofibers were investigated in this work. The single pellet crushing strength of the granules is high, e.g., 1.6-2.5 MPa. They have high specific surface areas, averaging 72-141 m^2·g^-1, and the majority of their pores are mesopores or macropores. The adsorption at 298 K of benzene or phenol on the granules is much lower than that on activated carbon and depends not only on the specific surface area of the carbon material but also on the sewing structure of the granules and the morphology of the carbon nanofibers. Treatment in dilute nitric acid appreciably reduces such adsorption.
基金supported by the National Natural Science Foundation of China (No. 21177130)the National Key Technology R&D Program (No. 2011BAC06B09)the Chinese Academy of Sciences Visiting Professorships for Senior International Scientists (No. 2009G2-28)
文摘Ozonation of oxalate in aqueous phase was performed with a commercial activated carbon(AC)in this work. The effect of AC dosage and solution pH on the contribution of hydroxyl radicals(HOU) in bulk solution and oxidation on the AC surface to the removal of oxalate was studied. We found that the removal of oxalate was reduced by tert-butyl alcohol(tBA) with low dosages of AC,while it was hardly affected by tBA when the AC dosage was greater than 0.3 g/L. tBA also inhibited ozone decomposition when the AC dosage was no more than 0.05 g/L, but it did not work when the AC dosage was no less than 0.1 g/L. These observations indicate that HOUin bulk solution and oxidation on the AC surface both contribute to the removal of oxalate. HOU oxidation in bulk solution is significant when the dosage of AC is low, whereas surface oxidation is dominant when the dosage of AC is high. The oxalate removal decreased with increasing pH of the solution with an AC dosage of 0.5 g/L. The degradation of oxalate occurs mainly through surface oxidation in acid and neutral solution, but through HOUoxidation in basic bulk solution. A mechanism involving both HOUoxidation in bulk solution and surface oxidation was proposed for AC enhanced ozonation of oxalate.
基金financially supported by the Russian Science Foundation(No.16-19-10625)
文摘Carbon nanotube (CNT) arrays were fabricated on Ct-Me-N-(O) alloys with content of Ct in the range of 6-40 at.% by chemical vapour deposition. The Ct was a catalytic metal from the group of the following elements: Ni, Co, Fe, Pd, while Me was a transition metal from the group of IV-VII of the periodic table (where Me=Ti, V, Cr, Zr, Nb, Mo, Ta, W, Re). Carbon nanotubes were found to grow efficiently on the alloy surface with its composition containing Ti, V, Cr, Zr, Hf, Nb or Ta. The growth of CNTs was not observed when the alloy contained W or Re. Additions of oxygen and nitrogen in the alloy facilitated the formation of oxynitrides and catalyst extrusion on the alloy surface. Replacement of the metals in alloy composition affected the diameter of the resulting CNTs. The obtained results showed that the alloy films of varying thickness (10-500 nm) may be used for the CNTs growth. The resulting CNT material was highly homogenous and its synthesis reproducible.