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熱鉀堿溶液脫除沼氣中CO2的反應(yīng)動力學(xué)
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國家自然科學(xué)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(shù)重點實驗室開放基金項目(2016REWB13)


Reaction Kinetics of CO2 Removal from Biogas Using Hot Potassium Carbonate Solvent
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    摘要:

    根據(jù)CO2吸收過程串并聯(lián)反應(yīng)機理,建立了本征動力學(xué)方程;基于雙膜擴散理論,建立了CO2吸收反應(yīng)的宏觀動力學(xué)方程,并結(jié)合溶液的非理想性,對速率方程中的濃度效應(yīng)進行了修正,獲得了8個修正模型。通過實驗設(shè)計,測定并進行了模型參數(shù)估值,分別計算了各模型的殘差。通過比較殘差大小及其分布,對模型進行了篩選,〖JP2〗選取模型4為理想模型。其動力學(xué)參數(shù)為:表觀活化能1938394J/mol,表觀指前因子3.0429×10-5mol/(m2·s·Pa)。在此基礎(chǔ)上,通過理論推導(dǎo)獲得了熱鉀堿吸收CO2的本征動力學(xué)方程,其模型參數(shù)為:本征反應(yīng)活化能54.47kJ/mol,指前因子3.2228×109m3/(mol·s)。計算了膜內(nèi)轉(zhuǎn)化系數(shù)γ,該值大于2,表明CO2吸收為快速反應(yīng)過程,反應(yīng)主要在膜內(nèi)完成。

    Abstract:

    Following the mechanism of seriesparallel reaction in CO2 absorption process, the intrinsic kinetic equation was established. A macroscopic kinetic equation of CO2 absorption reaction was established based on the theory of double membrane diffusion. Considering the noneideal solution, the concentration effect in the rate equation was corrected differently to obtain eight correction models. Through the orthogonal experiment design, the experimental factors were reaction temperature, initial concentration of potassium carbonate, reaction time and mixture of methane and carbon dioxide, and the level of each factor was 3. The experimental data were measured in a doubledrive reactor and the model parameters were estimated. The residual values of each model were calculated respectively. The models were contrasted by comparing the residual value sizes and distributions, and the model 4 was considered as the ideal with kinetic parameters as follows: apparent activation energy Eob was 1938394J/mol, apparent anterior factor k(0)ob was 3.0429×10-5mol/(m2·s·Pa). Through theoretical derivation based on these model parameters, the intrinsic kinetic equation of CO2 absorption by hot potash was obtained with following model parameters: the intrinsic reaction activation energy E was 5447kJ/mol, the anterior factor k0 was 3.2228×109m3/(mol〖DK〗·s). The conversion coefficient γ was calculated to be a value much greater than 2, which indicated that the CO2 absorption was a rapid reaction process that mainly happened in the membrane. 

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張良佺,歐陽書情,毛琰昊,蓋希坤,楊瑞芹,單勝道.熱鉀堿溶液脫除沼氣中CO2的反應(yīng)動力學(xué)[J].農(nóng)業(yè)機械學(xué)報,2019,50(5):362-369. ZHANG Liangquan, OUYANG Shuqing, MAO Yanhao, GAI Xikun, YANG Ruiqin, SHAN Shengdao. Reaction Kinetics of CO2 Removal from Biogas Using Hot Potassium Carbonate Solvent[J]. Transactions of the Chinese Society for Agricultural Machinery,2019,50(5):362-369.

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  • 收稿日期:2018-09-29
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  • 在線發(fā)布日期: 2019-05-10
  • 出版日期: 2019-05-10
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