The objective of this study was to evaluate the performance of an in-chamber tar cracking and syngas reforming unit.This unit was composed of a two-stage tubular reactor placed within the combustion zone of an updraft...The objective of this study was to evaluate the performance of an in-chamber tar cracking and syngas reforming unit.This unit was composed of a two-stage tubular reactor placed within the combustion zone of an updraft biomass gasifier.Heat generated in the exothermic combustion reactions of biomass gasification drove tar cracking and syngas reforming in the tubes,eliminating the need of external heating.The performance of the unit was evaluated using char-supported NiO catalysts and was found to be very effective in tar removal and syngas composition enhancement.A tar removal rate of 95% was achieved at 0.3 s residence time and 10%nickel loading.This condition also gave syngas high-heating value increment of 36%(to 7.3 MJ/m^(3)).The effect of gas residence time and Ni loading on tar removal and syngas composition of the unit was also studied.Gas residence of 0.2-0.3 s and Ni loading of 5%-10% were found appropriate to produce clean syngas with tar content appropriate for industrial applications(<0.6 g/m^(3))in an updraft biomass gasifier without external heating.展开更多
B3LYP/6-31G(d,p) method was used to investigate the catalytic cracking mechanism of biomass tar model compound.Phenol,toluene and benzene were selected as the tar model compounds and CaO was selected as the catalyst.T...B3LYP/6-31G(d,p) method was used to investigate the catalytic cracking mechanism of biomass tar model compound.Phenol,toluene and benzene were selected as the tar model compounds and CaO was selected as the catalyst.The pathways of tar compound radical absorbed by CaO were determined firstly through comparing enthalpy changes of the absorption,and then Mulliken population changes were analyzed.The results show that the absorption of tar model compound radical and CaO is an exothermic reaction.Formation of C—O—Ca is more easily than that of C—Ca—O and formation of Caromatic—Caromatic—Ca—O is more easily than that of Caromatic—C(O)—Ca—O.The C—C bond Mulliken populations in tar model compound radicals are reduced by 11.9%,10.5% and 15.5% in the case of a hydrogen atom removed,and those are 15.7%,14.3% and 16.3% in the case of two hydrogen atoms removed through the absorption of CaO.Catalytic ability of CaO acting on the tar model compound is in an order of phenol>benzene>toluene.展开更多
Catalysts, such as HZSM-5(Si/Al=50), HZSM-5(25), zeolite 5A, CaHZSM-5(50), ZnHZSM-5(50), and Kaolin were used in upgrading of crude biomass oil from pyrolysis in a fixed-bed reactor under atmospheric pressure, in orde...Catalysts, such as HZSM-5(Si/Al=50), HZSM-5(25), zeolite 5A, CaHZSM-5(50), ZnHZSM-5(50), and Kaolin were used in upgrading of crude biomass oil from pyrolysis in a fixed-bed reactor under atmospheric pressure, in order to investigate the effects of catalyst type on the yield of desired product. A blank test was carried out in a bed of inert packings to determine the extent of non-catalytical thermal cracking. The gas produced in the reaction was analyzed by the chemical absorption method. Among those catalysts, HZSM-5(50) gave the highest yield of the desired organic distillate while Kaolin gave the least formation of coke. Regeneration of deactivated HZSM-5(50) was studied. In terms of yield of organic distillate and formation rate of coke, the catalytic activity did not change much during the first 3 times of regeneration.展开更多
Pyrolysis-gas chromatography/mass spectrometry (Py-GC/MS) was employed to achieve fast pyrolysis of biomass and on-line analysis of the pyrolysis vapors. Four biomass materials (poplar wood, fir wood, cotton straw and...Pyrolysis-gas chromatography/mass spectrometry (Py-GC/MS) was employed to achieve fast pyrolysis of biomass and on-line analysis of the pyrolysis vapors. Four biomass materials (poplar wood, fir wood, cotton straw and rice husk) were pyrolyzed to reveal the difference among their products. Moreover, catalytic cracking of the pyrolysis vapors from cotton straw was performed by using five catalysts, including two microporous zeolites (HZSM-5 and HY) and three mesoporous catalysts (ZrO2&TiO2, SBA-15 and Al/SBA-15). The results showed that the distribution of the pyrolytic products from the four materials differed a little from each other, while catalytic cracking could significantly alter the pyrolytic products. Those important primary pyrolytic products such as levoglucosan, hydroxyacetaldehyde and 1-hydroxy-2-propanone were decreased greatly after catalysis. The two microporous zeolites were ef-fective to generate high yields of hydrocarbons, while the three mesoporous materials favored the formation of furan, furfural and other furan compounds, as well as acetic acid.展开更多
基于定温热重实验,建立了甲烷催化裂解反应动力学模型和催化剂表面积炭失活动力学模型。其中,甲烷催化裂解动力学模型将初始产氢速率视为催化剂未积炭条件下的动力学基础数据;催化剂表面积炭失活动力学则基于甲烷催化裂解速率的降低。...基于定温热重实验,建立了甲烷催化裂解反应动力学模型和催化剂表面积炭失活动力学模型。其中,甲烷催化裂解动力学模型将初始产氢速率视为催化剂未积炭条件下的动力学基础数据;催化剂表面积炭失活动力学则基于甲烷催化裂解速率的降低。实验使用Ni-Mg复合催化剂,分别在535、585、635℃,甲烷分压10~4、2×10~4、3×10~4Pa条件下展开甲烷催化裂解动力学特性研究。结果表明,甲烷催化裂解的反应级数为0.5,活化能为82 k J/mol;Ni-Mg复合催化剂反应失活级数为0.5,催化剂失活活化能为118 k J/mol。实验条件下均制得了多壁碳纳米管。展开更多
基金supported by the U.S.Department of Agriculture and Sun Grant(Award No.2010-38502-21836 and Subaward No.AB-5-67630.KSU11)the startup fund of North Carolina State Universitypartially supported by the scholarship program of IFARHU-SENACYT from the Government of Panama.
文摘The objective of this study was to evaluate the performance of an in-chamber tar cracking and syngas reforming unit.This unit was composed of a two-stage tubular reactor placed within the combustion zone of an updraft biomass gasifier.Heat generated in the exothermic combustion reactions of biomass gasification drove tar cracking and syngas reforming in the tubes,eliminating the need of external heating.The performance of the unit was evaluated using char-supported NiO catalysts and was found to be very effective in tar removal and syngas composition enhancement.A tar removal rate of 95% was achieved at 0.3 s residence time and 10%nickel loading.This condition also gave syngas high-heating value increment of 36%(to 7.3 MJ/m^(3)).The effect of gas residence time and Ni loading on tar removal and syngas composition of the unit was also studied.Gas residence of 0.2-0.3 s and Ni loading of 5%-10% were found appropriate to produce clean syngas with tar content appropriate for industrial applications(<0.6 g/m^(3))in an updraft biomass gasifier without external heating.
基金Project(51276023)supported by the National Natural Science Foundation of China
文摘B3LYP/6-31G(d,p) method was used to investigate the catalytic cracking mechanism of biomass tar model compound.Phenol,toluene and benzene were selected as the tar model compounds and CaO was selected as the catalyst.The pathways of tar compound radical absorbed by CaO were determined firstly through comparing enthalpy changes of the absorption,and then Mulliken population changes were analyzed.The results show that the absorption of tar model compound radical and CaO is an exothermic reaction.Formation of C—O—Ca is more easily than that of C—Ca—O and formation of Caromatic—Caromatic—Ca—O is more easily than that of Caromatic—C(O)—Ca—O.The C—C bond Mulliken populations in tar model compound radicals are reduced by 11.9%,10.5% and 15.5% in the case of a hydrogen atom removed,and those are 15.7%,14.3% and 16.3% in the case of two hydrogen atoms removed through the absorption of CaO.Catalytic ability of CaO acting on the tar model compound is in an order of phenol>benzene>toluene.
基金Supported by 863 National High Technology Development Program of China(No. 2001AA514021)
文摘Catalysts, such as HZSM-5(Si/Al=50), HZSM-5(25), zeolite 5A, CaHZSM-5(50), ZnHZSM-5(50), and Kaolin were used in upgrading of crude biomass oil from pyrolysis in a fixed-bed reactor under atmospheric pressure, in order to investigate the effects of catalyst type on the yield of desired product. A blank test was carried out in a bed of inert packings to determine the extent of non-catalytical thermal cracking. The gas produced in the reaction was analyzed by the chemical absorption method. Among those catalysts, HZSM-5(50) gave the highest yield of the desired organic distillate while Kaolin gave the least formation of coke. Regeneration of deactivated HZSM-5(50) was studied. In terms of yield of organic distillate and formation rate of coke, the catalytic activity did not change much during the first 3 times of regeneration.
基金Supported by the National Basic Research Program of China (Grant No. 2007CB210203)National Key Technologies R&D Program of China (Grant No. 2007BAD34B02)Knowledge Innovation Program of Chinese Academy of Sci-ences (Grant No. KGCX2-YW-330)
文摘Pyrolysis-gas chromatography/mass spectrometry (Py-GC/MS) was employed to achieve fast pyrolysis of biomass and on-line analysis of the pyrolysis vapors. Four biomass materials (poplar wood, fir wood, cotton straw and rice husk) were pyrolyzed to reveal the difference among their products. Moreover, catalytic cracking of the pyrolysis vapors from cotton straw was performed by using five catalysts, including two microporous zeolites (HZSM-5 and HY) and three mesoporous catalysts (ZrO2&TiO2, SBA-15 and Al/SBA-15). The results showed that the distribution of the pyrolytic products from the four materials differed a little from each other, while catalytic cracking could significantly alter the pyrolytic products. Those important primary pyrolytic products such as levoglucosan, hydroxyacetaldehyde and 1-hydroxy-2-propanone were decreased greatly after catalysis. The two microporous zeolites were ef-fective to generate high yields of hydrocarbons, while the three mesoporous materials favored the formation of furan, furfural and other furan compounds, as well as acetic acid.
文摘基于定温热重实验,建立了甲烷催化裂解反应动力学模型和催化剂表面积炭失活动力学模型。其中,甲烷催化裂解动力学模型将初始产氢速率视为催化剂未积炭条件下的动力学基础数据;催化剂表面积炭失活动力学则基于甲烷催化裂解速率的降低。实验使用Ni-Mg复合催化剂,分别在535、585、635℃,甲烷分压10~4、2×10~4、3×10~4Pa条件下展开甲烷催化裂解动力学特性研究。结果表明,甲烷催化裂解的反应级数为0.5,活化能为82 k J/mol;Ni-Mg复合催化剂反应失活级数为0.5,催化剂失活活化能为118 k J/mol。实验条件下均制得了多壁碳纳米管。
