Photocatalytic decomposition of sugars is a promising way of providing H_(2),CO,and HCOOH as sus-tainable energy vectors.However,the production of C_(1) chemicals requires the cleavage of robust C−C bonds in sugars wi...Photocatalytic decomposition of sugars is a promising way of providing H_(2),CO,and HCOOH as sus-tainable energy vectors.However,the production of C_(1) chemicals requires the cleavage of robust C−C bonds in sugars with concurrent production of H_(2),which remains challenging.Here,the photo-catalytic activity for glucose decomposition to HCOOH,CO(C_(1) chemicals),and H_(2) on Cu/TiO_(2)was enhanced by nitrogen doping.Owing to nitrogen doping,atomically dispersed and stable Cu sites resistant to light irradiation are formed on Cu/TiO_(2).The electronic interaction between Cu and nitrogen ions originates valence band structure and defect levels composed of N 2p orbit,distinct from undoped Cu/TiO_(2).Therefore,the lifetime of charge carriers is prolonged,resulting in the pro-duction of C_(1) chemicals and H_(2) with productivities 1.7 and 2.1 folds that of Cu/TiO_(2).This work pro-vides a strategy to design coordinatively stable Cu ions for photocatalytic biomass conversion.展开更多
Carbonaceous gold mines are important refractory gold ores. The previous results demonstrate that the carbonaceous matter is mainly composed of elemental carbon, organic acid and hydrocarbons. The dissolved aurocyanid...Carbonaceous gold mines are important refractory gold ores. The previous results demonstrate that the carbonaceous matter is mainly composed of elemental carbon, organic acid and hydrocarbons. The dissolved aurocyanide complex is robbed by adsorption of carbonaceous matter, which is similar to activated carbon in cyanide leaching of gold. The pretreatment methods of carbonaceous gold ores were introduced, including high temperature roasting, bio-oxidation, chemical oxidation, competitive adsorption, barrier inhibition and microwave roasting. Recently, bio-oxidation was developed rapidly due to its advantages such as mild conditions, simple processes, low energy consumption and friendly environment. The known microorganisms related with bio-oxidation pretreatment mainly are chemolithotroph bacteria such as Thiobacillus ferrooxidans, Thiobacillus thiooxidans and Leptospirillum ferrooxidans. The researches on decomposing and passivating carbonaceous matter were commenced by Phanerochaete chrysosporium, Pseudomonadaceae and Streptomyces setonii. Finally, the main problems were analyzed and the application prospect of this technique was looked forward.展开更多
We reports an efficient approach for production of hydrogen from crude bio-oil and biomass char in the dual fixed-bed system by using the electrochemical catalytic reforming method. The maximal absolute hydrogen yield...We reports an efficient approach for production of hydrogen from crude bio-oil and biomass char in the dual fixed-bed system by using the electrochemical catalytic reforming method. The maximal absolute hydrogen yield reached 110.9 g H2/kg dry biomass. The product gas was a mixed gas containing 72%H2, 26%CO2, 1.9%CO, and a trace amount of CH4. It was observed that adding biomass char （a by-product of pyrolysis of biomass） could remarkably increase the absolute H2 yield （about 20%-50%）. The higher reforming temperature could enhance the steam reforming reaction of organic compounds in crude bio-oil and the reaction of CO and H20. In addition, the CuZn-Al2O3 catalyst in the water-gas shift bed could also increase the absolute H2 yield via shifting CO to CO2.展开更多
Highly efficient synthesis of clean biofuels using the bio-syngas obtained from biomass gasi- fication was performed over Fel.5CulZnlAllK0.117 catalyst. The maximum biofuel yield from the bio-syngas reaches about 1.59...Highly efficient synthesis of clean biofuels using the bio-syngas obtained from biomass gasi- fication was performed over Fel.5CulZnlAllK0.117 catalyst. The maximum biofuel yield from the bio-syngas reaches about 1.59 kg biofuels/（kgcat·rh） with a contribution of 0.57 kg alcohols/（kgcat·rh） and 1.02 kg liquid hydrocarbons/（kgcat·rh）. The alcohol products in the resulting biofuels were dominated by the C2＋ alcohols （mainly C2-C6 alcohols） with a content of 73.55%-89.98%. The selectivity .of the liquid hydrocarbons （C5＋） in the hydrocarbon products ranges from 60.37% to 70.94%. The synthesis biofuels also possess a higher heat value of 40.53-41.49 MJ/kg. The effects of the synthesis conditions, including temperature, pressure, and gas hourly space velocity, on the biofuel synthesis were investigated in detail. The catalyst features were characterized by inductively coupled plasma and atomic emission spectroscopy, X-ray diffraction, temperature programmed reduction, and the N2 adsorption-desorption isotherms measurements. The present biofuel synthesis with a higher biofuel yield and a higher selectivity of liquid hydrocarbons and C2＋ alcohols may be a potentially useful route to produce clean biofuels and chemicals from biomass.展开更多
On basis of analysis on agroforestry-animal husbandry ecosystem characters, the research explored nutrient flow model of material cycle and carbon cycle and agroforestry-animal husbandry mutualism model and supporting...On basis of analysis on agroforestry-animal husbandry ecosystem characters, the research explored nutrient flow model of material cycle and carbon cycle and agroforestry-animal husbandry mutualism model and supporting technology in Yangtze-Huaihe Region, taking Robinia pseudoacacia stand and rubber garden as an example.展开更多
The oxygen reduction reaction(ORR)is a vitally important process in fuel cells.The development of high‐performance and low‐cost ORR electrocatalysts with outstanding stability is essential for the commercialization ...The oxygen reduction reaction(ORR)is a vitally important process in fuel cells.The development of high‐performance and low‐cost ORR electrocatalysts with outstanding stability is essential for the commercialization of the electrochemical energy technology.Herein,we report a facile synthesis of cobalt(Co)and nitrogen(N)co‐doped carbon nanotube@porous carbon(Co/N/CNT@PC‐800)electrocatalyst through a one‐step pyrolysis of waste paper,dicyandiamide,and cobalt(II)acetylacetonate.The surface of the hierarchical porous carbon supported a large number of carbon nanotubes(CNTs),which were derived from dicyandiamide through the catalysis of Co.The addition of Co resulted in the formation of a hierarchical micro/mesoporous structure,which was beneficial for the exposure of active sites and rapid transportation of ORR‐relevant species(O2,H+,OH?,and H2O).The doped N and Co formed more active sites to enhance the ORR activity of the electrocatalyst.The Co/N/CNT@PC‐800 material exhibited optimal ORR performance with an onset potential of 0.005 V vs.Ag/AgCl and a half‐wave potential of?0.173 V vs.Ag/AgCl.Meanwhile,the electrocatalyst showed an excellent methanol tolerance and a long‐term operational durability than that of Pt/C,as well as a quasi‐four‐electron reaction pathway.The low‐cost and simple synthesis approach makes the Co/N/CNT@PC‐800 a prospective electrocatalyst for the ORR.Furthermore,this work provides an alternative approach for exploring the use of biomass‐derived electrocatalysts for renewable energy applications.展开更多
The scarcity and weak durability of metal,especially precious metal catalysts are big obstacles for their large-scale application in many reactions.The state-of-the-art of the catalytic science prefers such type of ca...The scarcity and weak durability of metal,especially precious metal catalysts are big obstacles for their large-scale application in many reactions.The state-of-the-art of the catalytic science prefers such type of catalysts,which can replace metal-based catalysts to alleviate energy and environmental crises and exhibit catalytic performance comparable to or even exceeding these metal catalysts.Herein,we report that N-doped porous carbon(NKC)derived from cheap and abundant radish can be employed as versatile and efficient bifunctional catalysts in both the catalytic reduction of 4-nitrophenol(NRR)and oxidation of styrene(SOR).The series of NKC catalysts were prepared with a simple and facile one-pot strategy by coupling the N-doping,carbonization and KOH activation processes.These catalysts show hierarchical porosity,with the specific surface area,total pore volume and N-doping content ranging from 918.9-3062.7 m^2 g^-1,1.01-2.04 cm^3 g^-1 and 1.29-15.3 at%,respectively.Interestingly,our finding suggests that the catalytic performance is not directly related to these parameters but correlates positively with the content of graphitic N dopants,which is the dominant contributor for impelling both the NRR and SOR.Another intriguing finding is that for both reactions,the optimal catalyst was found to be the NKC-3-800 which possesses the highest graphitic N content of 3.13 at%.In addition,to gain insight into the catalytic behavior,analyses of kinetics and thermodynamics were performed,and the catalytic mechanisms were postulated.This work paves the way for the construction of biomass-derived N-doped carbon catalysts for bi-or even multi-functional applications in various organic reactions.展开更多
100%green carbon foam from the fibrous fruits of Platanus Orientalis-L(Plane)along with the tar oil as binder has been prepared using a powder molding technique.The objective was to develop a porous monolithic carbon ...100%green carbon foam from the fibrous fruits of Platanus Orientalis-L(Plane)along with the tar oil as binder has been prepared using a powder molding technique.The objective was to develop a porous monolithic carbon from biomaterials with a considerable strength necessary for various physical,thermal and electromagnetic shielding applications.Fast carbonization was carried out at1000°C under the cover of Plane tree pyrolyzed seeds without using any external protective gas.For comparative analysis,some samples were mixed with5%(mass fraction)iron chloride during the molding process.Iron chloride being a graphitization catalyst and activating agent helped in increasing the specific surface area from88to294m2/g with a25%decrease in flexural strength.Thermal stability was improved due to the incorporation of more graphitic phases in the sample resulting in a little higher thermal conductivity from0.22to0.67W/(m·K).The catalytic carbon foam exhibited shielding effectiveness of more than20dB over the X-band frequency.Absorption was dominant with only8.26%?10.33%reflectance,indicating an absorption dominant shielding mechanism.The new material is quite suitable for high temperature thermal insulation being lightweight,highly porous with interconnected porous morphology most of which is preserved from the original biomaterial.展开更多
文摘Photocatalytic decomposition of sugars is a promising way of providing H_(2),CO,and HCOOH as sus-tainable energy vectors.However,the production of C_(1) chemicals requires the cleavage of robust C−C bonds in sugars with concurrent production of H_(2),which remains challenging.Here,the photo-catalytic activity for glucose decomposition to HCOOH,CO(C_(1) chemicals),and H_(2) on Cu/TiO_(2)was enhanced by nitrogen doping.Owing to nitrogen doping,atomically dispersed and stable Cu sites resistant to light irradiation are formed on Cu/TiO_(2).The electronic interaction between Cu and nitrogen ions originates valence band structure and defect levels composed of N 2p orbit,distinct from undoped Cu/TiO_(2).Therefore,the lifetime of charge carriers is prolonged,resulting in the pro-duction of C_(1) chemicals and H_(2) with productivities 1.7 and 2.1 folds that of Cu/TiO_(2).This work pro-vides a strategy to design coordinatively stable Cu ions for photocatalytic biomass conversion.
基金Projects(51174062,51104036)supported by the National Natural Science Foundation of ChinaProject(2012BAE06B05)supported by the National Science and Technology Support Program of China during the 12th Five-Year Plan Period+1 种基金Projects(2012AA061502,2012AA061501)supported by the National High-Tech Research and Development Program of ChinaProjects(N120602006,N110302002,N110602005)supported by Fundamental Research Funds for the Central Universities of China
文摘Carbonaceous gold mines are important refractory gold ores. The previous results demonstrate that the carbonaceous matter is mainly composed of elemental carbon, organic acid and hydrocarbons. The dissolved aurocyanide complex is robbed by adsorption of carbonaceous matter, which is similar to activated carbon in cyanide leaching of gold. The pretreatment methods of carbonaceous gold ores were introduced, including high temperature roasting, bio-oxidation, chemical oxidation, competitive adsorption, barrier inhibition and microwave roasting. Recently, bio-oxidation was developed rapidly due to its advantages such as mild conditions, simple processes, low energy consumption and friendly environment. The known microorganisms related with bio-oxidation pretreatment mainly are chemolithotroph bacteria such as Thiobacillus ferrooxidans, Thiobacillus thiooxidans and Leptospirillum ferrooxidans. The researches on decomposing and passivating carbonaceous matter were commenced by Phanerochaete chrysosporium, Pseudomonadaceae and Streptomyces setonii. Finally, the main problems were analyzed and the application prospect of this technique was looked forward.
基金This work was supported by the National Basic Research Program of Ministry of Science and Technology of China （No.2007CB210206）, the National High Tech Research and Development Program （No.2009AA05Z435）, and the National Natural Science Foundation of China （No.50772107）.
文摘We reports an efficient approach for production of hydrogen from crude bio-oil and biomass char in the dual fixed-bed system by using the electrochemical catalytic reforming method. The maximal absolute hydrogen yield reached 110.9 g H2/kg dry biomass. The product gas was a mixed gas containing 72%H2, 26%CO2, 1.9%CO, and a trace amount of CH4. It was observed that adding biomass char （a by-product of pyrolysis of biomass） could remarkably increase the absolute H2 yield （about 20%-50%）. The higher reforming temperature could enhance the steam reforming reaction of organic compounds in crude bio-oil and the reaction of CO and H20. In addition, the CuZn-Al2O3 catalyst in the water-gas shift bed could also increase the absolute H2 yield via shifting CO to CO2.
基金This work was supported by the National Basic Research Program of Ministry of Science and Technology of China （No.2007CB210206）, the National High Tech Research and Development Program （No.2009AA05Z435）, and the National Natural Science Foundation of China （No.50772107）.
文摘Highly efficient synthesis of clean biofuels using the bio-syngas obtained from biomass gasi- fication was performed over Fel.5CulZnlAllK0.117 catalyst. The maximum biofuel yield from the bio-syngas reaches about 1.59 kg biofuels/（kgcat·rh） with a contribution of 0.57 kg alcohols/（kgcat·rh） and 1.02 kg liquid hydrocarbons/（kgcat·rh）. The alcohol products in the resulting biofuels were dominated by the C2＋ alcohols （mainly C2-C6 alcohols） with a content of 73.55%-89.98%. The selectivity .of the liquid hydrocarbons （C5＋） in the hydrocarbon products ranges from 60.37% to 70.94%. The synthesis biofuels also possess a higher heat value of 40.53-41.49 MJ/kg. The effects of the synthesis conditions, including temperature, pressure, and gas hourly space velocity, on the biofuel synthesis were investigated in detail. The catalyst features were characterized by inductively coupled plasma and atomic emission spectroscopy, X-ray diffraction, temperature programmed reduction, and the N2 adsorption-desorption isotherms measurements. The present biofuel synthesis with a higher biofuel yield and a higher selectivity of liquid hydrocarbons and C2＋ alcohols may be a potentially useful route to produce clean biofuels and chemicals from biomass.
基金Supported by the National S&T Support Program during the Twelfth Five-year Pla Period(2012BAD14B13)~~
文摘On basis of analysis on agroforestry-animal husbandry ecosystem characters, the research explored nutrient flow model of material cycle and carbon cycle and agroforestry-animal husbandry mutualism model and supporting technology in Yangtze-Huaihe Region, taking Robinia pseudoacacia stand and rubber garden as an example.
基金supported by the National Nature Science Foundation of China(21476098,21471069,21576123)International Postdoctoral Exchange Fellowship Program of China Postdoctoral Council(20150060)~~
文摘The oxygen reduction reaction(ORR)is a vitally important process in fuel cells.The development of high‐performance and low‐cost ORR electrocatalysts with outstanding stability is essential for the commercialization of the electrochemical energy technology.Herein,we report a facile synthesis of cobalt(Co)and nitrogen(N)co‐doped carbon nanotube@porous carbon(Co/N/CNT@PC‐800)electrocatalyst through a one‐step pyrolysis of waste paper,dicyandiamide,and cobalt(II)acetylacetonate.The surface of the hierarchical porous carbon supported a large number of carbon nanotubes(CNTs),which were derived from dicyandiamide through the catalysis of Co.The addition of Co resulted in the formation of a hierarchical micro/mesoporous structure,which was beneficial for the exposure of active sites and rapid transportation of ORR‐relevant species(O2,H+,OH?,and H2O).The doped N and Co formed more active sites to enhance the ORR activity of the electrocatalyst.The Co/N/CNT@PC‐800 material exhibited optimal ORR performance with an onset potential of 0.005 V vs.Ag/AgCl and a half‐wave potential of?0.173 V vs.Ag/AgCl.Meanwhile,the electrocatalyst showed an excellent methanol tolerance and a long‐term operational durability than that of Pt/C,as well as a quasi‐four‐electron reaction pathway.The low‐cost and simple synthesis approach makes the Co/N/CNT@PC‐800 a prospective electrocatalyst for the ORR.Furthermore,this work provides an alternative approach for exploring the use of biomass‐derived electrocatalysts for renewable energy applications.
文摘The scarcity and weak durability of metal,especially precious metal catalysts are big obstacles for their large-scale application in many reactions.The state-of-the-art of the catalytic science prefers such type of catalysts,which can replace metal-based catalysts to alleviate energy and environmental crises and exhibit catalytic performance comparable to or even exceeding these metal catalysts.Herein,we report that N-doped porous carbon(NKC)derived from cheap and abundant radish can be employed as versatile and efficient bifunctional catalysts in both the catalytic reduction of 4-nitrophenol(NRR)and oxidation of styrene(SOR).The series of NKC catalysts were prepared with a simple and facile one-pot strategy by coupling the N-doping,carbonization and KOH activation processes.These catalysts show hierarchical porosity,with the specific surface area,total pore volume and N-doping content ranging from 918.9-3062.7 m^2 g^-1,1.01-2.04 cm^3 g^-1 and 1.29-15.3 at%,respectively.Interestingly,our finding suggests that the catalytic performance is not directly related to these parameters but correlates positively with the content of graphitic N dopants,which is the dominant contributor for impelling both the NRR and SOR.Another intriguing finding is that for both reactions,the optimal catalyst was found to be the NKC-3-800 which possesses the highest graphitic N content of 3.13 at%.In addition,to gain insight into the catalytic behavior,analyses of kinetics and thermodynamics were performed,and the catalytic mechanisms were postulated.This work paves the way for the construction of biomass-derived N-doped carbon catalysts for bi-or even multi-functional applications in various organic reactions.
基金Project(CX201627) supported by the Innovation Foundation for Doctor Dissertation of Northwestern Polytechnical University,China
文摘100%green carbon foam from the fibrous fruits of Platanus Orientalis-L(Plane)along with the tar oil as binder has been prepared using a powder molding technique.The objective was to develop a porous monolithic carbon from biomaterials with a considerable strength necessary for various physical,thermal and electromagnetic shielding applications.Fast carbonization was carried out at1000°C under the cover of Plane tree pyrolyzed seeds without using any external protective gas.For comparative analysis,some samples were mixed with5%(mass fraction)iron chloride during the molding process.Iron chloride being a graphitization catalyst and activating agent helped in increasing the specific surface area from88to294m2/g with a25%decrease in flexural strength.Thermal stability was improved due to the incorporation of more graphitic phases in the sample resulting in a little higher thermal conductivity from0.22to0.67W/(m·K).The catalytic carbon foam exhibited shielding effectiveness of more than20dB over the X-band frequency.Absorption was dominant with only8.26%?10.33%reflectance,indicating an absorption dominant shielding mechanism.The new material is quite suitable for high temperature thermal insulation being lightweight,highly porous with interconnected porous morphology most of which is preserved from the original biomaterial.
