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熱鉀堿溶液脫除沼氣中CO2反應機制與相際傳質(zhì)研究
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國家自然科學基金重點項目(U1609214)、浙江省重點研發(fā)計劃項目(2017C03010)和浙江省廢棄生物質(zhì)循環(huán)利用與生態(tài)處理技術重點實驗室開放基金項目(2016REWB13)


Reaction Mechanism and Interphase Mass Transfer of CO2 from Biogas by Hot Potassium Carbonate Solvent
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    摘要:

    對CO2氣液吸收過程進行了化學平衡熱力學研究,計算了吸收反應體系的獨立反應數(shù),提出了4獨立反應理論。根據(jù)對獨立反應平衡常數(shù)的計算,認為H2CO3電離為H+和HCO-3,雖然其平衡常數(shù)僅為6.0189×10-7,但由于溶液中CO2-3離子的大量存在,使得H+濃度很低,因此H2CO3電離度不可忽略。在此基礎上,提出了CO2氣液吸收過程串并聯(lián)復雜反應機理,認為CO2吸收速率是由其分別與H2O和OH-兩條平行反應路線共同決定的。分析了CO2-3離子的關鍵作用:該離子與H+作用直接促進了CO2吸收過程;由于溶液中H+離子濃度很低,導致OH-離子濃度升高,從而間接加快了CO2與OH-離子之間的反應速率。應用雙驅(qū)動反應器,采取H2O-CO2體系對氣液相際傳質(zhì)過程進行了研究,當氣相攪拌轉(zhuǎn)速達到140r/min以上時,氣膜傳質(zhì)阻力可忽略不計;通過線性回歸分析,關聯(lián)了液相傳質(zhì)系數(shù)與液相攪拌轉(zhuǎn)速之間的關系,得到了回歸關聯(lián)式,計算誤差最大值為11.312%,認為關聯(lián)式真實可靠。

    Abstract:

    Through chemical equilibrium thermodynamics analysis of CO2 gas-liquid absorption process, the number of independent reactions in the absorption reaction system was calculated and a fourindependent reaction hypothesis was presented. According to the calculation of the independent reaction equilibrium constants, ionization of H2CO3 into H+ and HCO-3 was postulated. Although the equilibrium constant was 6.0189×10-7, the concentration of H+ ions was still very low due to the large presence of CO2-3 ions in the solution, such that the ionization degree of H2CO3 can not be ignored. Moreover, it was proposed that the reaction mechanism of CO2 gas-liquid absorption was a serialparallel complex. The absorption rate of CO2 was believed to be determined by its parallel reactions with H2O and OH-. Meanwhile, the critical roles of CO2-3 ions were analyzed in great detail. Firstly, the interaction between H+ and CO2-3 directly promoted the absorption of CO2;secondly, the concentration of OH- ions in solution was increased as the decrease of concentration of H+ ions. The latter indirectly accelerated the reaction rate between CO2 and OH- ions. A dualdrive reactor was used to study the gasliquid mass transfer process in H2O-CO2 system and the main conclusions were as following: when the gas phase stirring rate reached above 140r/min, the mass transfer resistance of the gas film can be negligible;based on the linear regression analysis, the relationship between the liquid mass transfer coefficient and the speed of liquid phase stirring paddle was verified and the regression correlation was obtained. By calculating the residual, the maximum value was 11.312%,and the correlation was considered to be robust.

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張良佺,鄭貓英,毛琰昊,蓋希坤,楊瑞芹,單勝道.熱鉀堿溶液脫除沼氣中CO2反應機制與相際傳質(zhì)研究[J].農(nóng)業(yè)機械學報,2019,50(4):283-289. ZHANG Liangquan, ZHENG Maoying, MAO Yanhao, GAI Xikun, YANG Ruiqin, SHAN Shengdao. Reaction Mechanism and Interphase Mass Transfer of CO2 from Biogas by Hot Potassium Carbonate Solvent[J]. Transactions of the Chinese Society for Agricultural Machinery,2019,50(4):283-289.

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  • 收稿日期:2018-09-29
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  • 在線發(fā)布日期: 2019-04-10
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