水洗法回收高铝煤焦催化气化催化剂的实验研究
|
摘要
采用水洗法回收孙家壕(SJH)高铝煤焦Na_2CO_3催化气化灰渣中的钠催化剂,结合ICP和XRD表征方法,研究了高铝煤焦气化催化剂的失活规律和回收特性。在高铝煤焦催化气化过程中,Na_2CO_3与煤中矿物质发生反应生成NaAlSiO_4是造成Na_2CO_3催化剂失活的原因。以水为溶剂回收不同Na_2CO_3负载量的煤焦气化灰渣中的钠催化剂时,钠催化剂的回收率随着Na_2CO_3负载量的增大而增大。当用盐酸回收时,钠催化剂的回收率显著增加,表明相当一部分钠生成不溶于水但可溶于盐酸的NaAlSiO_4。钠催化剂的最大失活量相当于9%Na_2CO_3负载量。
The deactivation mechanism and recovery characteristics of gasification catalyst are investigated through the recovery of sodium-based catalyst from Na_2CO_3-catalyzed gasification residues of Sunjiahao(SJH) high-aluminum coal char with water leaching method combined with ICP and XRD characterization.Na_2CO_3 reacts with the minerals in coal char to form NaAlSiO_4 during the catalytic gasification process of high-aluminum coal char,leading to the deactivation of Na_2CO_3 catalyst. The recovery rate of sodium-based catalyst increases with the increment of Na_2CO_3 loading amount in gasification process when water is used as recovery solvent to recover sodium-based catalyst from ash residues generated in the catalytic gasification of SJH char with different Na_2CO_3 loading amount. The recovery rate is remarkably higher when diluted hydrochloric acid is used as extraction agent,suggesting that substantial sodium forms NaAlSiO_4 that is water insoluble but soluble in hydrochloric acid. Moreover,the deactivation amount of sodium catalyst reaches saturation level when the catalyst loading amount is 9% on the basis of the dry char mass.
The deactivation mechanism and recovery characteristics of gasification catalyst are investigated through the recovery of sodium-based catalyst from Na_2CO_3-catalyzed gasification residues of Sunjiahao(SJH) high-aluminum coal char with water leaching method combined with ICP and XRD characterization.Na_2CO_3 reacts with the minerals in coal char to form NaAlSiO_4 during the catalytic gasification process of high-aluminum coal char,leading to the deactivation of Na_2CO_3 catalyst. The recovery rate of sodium-based catalyst increases with the increment of Na_2CO_3 loading amount in gasification process when water is used as recovery solvent to recover sodium-based catalyst from ash residues generated in the catalytic gasification of SJH char with different Na_2CO_3 loading amount. The recovery rate is remarkably higher when diluted hydrochloric acid is used as extraction agent,suggesting that substantial sodium forms NaAlSiO_4 that is water insoluble but soluble in hydrochloric acid. Moreover,the deactivation amount of sodium catalyst reaches saturation level when the catalyst loading amount is 9% on the basis of the dry char mass.
引文
[1]Kopyscinski J,Schildhauer T J,Biollaz S M A. Production of synthetic natural gas(SNG)from coal and dry biomass-A technology review from 1950 to 2009[J].Fuel,2010,89:1763-1783.
[2]Hirsch R L,Gallagher J E,Lessard R R,et al.Catalytic coal gasification:An emerging technology[J].Science,1982,215:121-127.
[3]Wood B J,Sancier K M.The mechanism of the catalytic gasification of coal char:A critical review[J].Cat Rev-Sci Eng,1984,26:233-279.
[4]Vuthalurua H B,Domazetis G,Wall T F,et al. Reducing fly ash deposition by pretreatment of brown coal:Effect of aluminium on ash character[J].Fuel Process Technol,1996,46:117-132.
[5]Kosminski A,Ross D P,Agnew J B.Reactions between sodium and kaolin during gasification of a low-rank coal[J].Fuel Process Technol,2006,87(12):1051-1062.
[6]Kosminski A,Ross D P,Agnew J B.Reactions between sodium and silica during gasification of a low-rank coal[J].Fuel Process Technol,2006,87(12):1037-1049.
[7]Wang X,Zhu H,Wang X,et al.Transformation and reactivity of a potassium catalyst during coal-steam catalytic pyrolysis and gasification[J].Energy Technol,2014,2(7):598-603.
[8]王兴军,陈凡敏,刘海峰,等.煤水蒸气气化过程中钾催化剂与矿物质的相互作用[J].燃料化学学报,2013,41(1):9-13.
[9]Zhang J,Zhang L,Yang Z,et al.Effect of bauxite additives on ash sintering characteristics during the K2CO3-catalyzed steam gasification of lignite[J].RSC Adv,2015,5(9):6720-6727.
[10]Sheth A C,Sastry C,Yeboah Y D,et al.Catalytic gasification of coal using eutectic salts:Recovery,regeneration,and recycle of spent eutectic catalysts[J].J Air Waste Manage Assoc,2003,53(4):451-460.
[11]Zhang Y,Ashizawa M,Kajitani S,et al.A new approach to catalytic coal gasification:The recovery and reuse of calcium using biomass derived crude vinegars[J].Fuel,2010,89(2):417-422.
[12]Nahas N C. Exxon catalytic coal gasif ication process[J]. Fuel,1983,62:238-240.
[13]陈杰,陈凡敏,王兴军,等.煤催化气化过程中钾催化剂回收的实验研究[J].化学工程,2012,40(6):68-71.
[14]Yuan X,Fan S,Zhao L,et al.Investigations of both catalytic steam gasification of indonesian lanna coal and potassium catalyst recovery using K2CO3as a catalyst[J].Energy Fuels,2016,30:2492-2502.
[15]Yuan X,Fan S,Choi S W,et al.Potassium catalyst recovery process and performance evaluation of the recovered catalyst in the K2CO3-catalyzed steam gasification system[J]. Appl Energy,2017,195:850-860.
[16]Yuan X,Zhao L,Namkung H,et al.Lab-scale investigations on catalyst recovery of gasified residue collected from the potassium-catalyzed steam gasification process[J]. Fuel Process Technol,2016,141:44-53.
[17]Kim Y K,Park J I,Jung D,et al.Low-temperature catalytic conversion of lignite:2.Recovery and reuse of potassium carbonate supported on perovskite oxide in steam gasification[J].J Ind Eng Chem,2014,20(1):194-201.
[18]Wang Y,Wang Z,Huang J,et al.Investigation into the characteristics of Na2CO3-catalyzed steam gasification for a high-aluminum coal char[J].J Therm Anal Calorim,2018,131(2):1213-1220.
[19]Wang Y,Wang Z,Huang J,et al. Catalytic gasification activity of Na2CO3and comparison with K2CO3for a high-aluminum coal char[J].Energy Fuels,2015,29(10):6988-6998.
[20]Wu S,Huang S,Wu Y,et al.Characteristics and catalytic actions of inorganic constituents from entrained-flow coal gasification slag[J].J Energy Inst,2015,88(1):93-103.
[2]Hirsch R L,Gallagher J E,Lessard R R,et al.Catalytic coal gasification:An emerging technology[J].Science,1982,215:121-127.
[3]Wood B J,Sancier K M.The mechanism of the catalytic gasification of coal char:A critical review[J].Cat Rev-Sci Eng,1984,26:233-279.
[4]Vuthalurua H B,Domazetis G,Wall T F,et al. Reducing fly ash deposition by pretreatment of brown coal:Effect of aluminium on ash character[J].Fuel Process Technol,1996,46:117-132.
[5]Kosminski A,Ross D P,Agnew J B.Reactions between sodium and kaolin during gasification of a low-rank coal[J].Fuel Process Technol,2006,87(12):1051-1062.
[6]Kosminski A,Ross D P,Agnew J B.Reactions between sodium and silica during gasification of a low-rank coal[J].Fuel Process Technol,2006,87(12):1037-1049.
[7]Wang X,Zhu H,Wang X,et al.Transformation and reactivity of a potassium catalyst during coal-steam catalytic pyrolysis and gasification[J].Energy Technol,2014,2(7):598-603.
[8]王兴军,陈凡敏,刘海峰,等.煤水蒸气气化过程中钾催化剂与矿物质的相互作用[J].燃料化学学报,2013,41(1):9-13.
[9]Zhang J,Zhang L,Yang Z,et al.Effect of bauxite additives on ash sintering characteristics during the K2CO3-catalyzed steam gasification of lignite[J].RSC Adv,2015,5(9):6720-6727.
[10]Sheth A C,Sastry C,Yeboah Y D,et al.Catalytic gasification of coal using eutectic salts:Recovery,regeneration,and recycle of spent eutectic catalysts[J].J Air Waste Manage Assoc,2003,53(4):451-460.
[11]Zhang Y,Ashizawa M,Kajitani S,et al.A new approach to catalytic coal gasification:The recovery and reuse of calcium using biomass derived crude vinegars[J].Fuel,2010,89(2):417-422.
[12]Nahas N C. Exxon catalytic coal gasif ication process[J]. Fuel,1983,62:238-240.
[13]陈杰,陈凡敏,王兴军,等.煤催化气化过程中钾催化剂回收的实验研究[J].化学工程,2012,40(6):68-71.
[14]Yuan X,Fan S,Zhao L,et al.Investigations of both catalytic steam gasification of indonesian lanna coal and potassium catalyst recovery using K2CO3as a catalyst[J].Energy Fuels,2016,30:2492-2502.
[15]Yuan X,Fan S,Choi S W,et al.Potassium catalyst recovery process and performance evaluation of the recovered catalyst in the K2CO3-catalyzed steam gasification system[J]. Appl Energy,2017,195:850-860.
[16]Yuan X,Zhao L,Namkung H,et al.Lab-scale investigations on catalyst recovery of gasified residue collected from the potassium-catalyzed steam gasification process[J]. Fuel Process Technol,2016,141:44-53.
[17]Kim Y K,Park J I,Jung D,et al.Low-temperature catalytic conversion of lignite:2.Recovery and reuse of potassium carbonate supported on perovskite oxide in steam gasification[J].J Ind Eng Chem,2014,20(1):194-201.
[18]Wang Y,Wang Z,Huang J,et al.Investigation into the characteristics of Na2CO3-catalyzed steam gasification for a high-aluminum coal char[J].J Therm Anal Calorim,2018,131(2):1213-1220.
[19]Wang Y,Wang Z,Huang J,et al. Catalytic gasification activity of Na2CO3and comparison with K2CO3for a high-aluminum coal char[J].Energy Fuels,2015,29(10):6988-6998.
[20]Wu S,Huang S,Wu Y,et al.Characteristics and catalytic actions of inorganic constituents from entrained-flow coal gasification slag[J].J Energy Inst,2015,88(1):93-103.