摘要
水合物法捕集和封存二氧化碳(CO_(2))具有储气量高和成本低等优点,但生成CO_(2)水合物(简称“水合物”)的诱导时间长、生成速率缓慢限制了该方法的应用。为促进水合物的生成,采用恒容法研究了纳米氧化锌(ZnO)和十二烷基硫酸钠(SDS)对水合物生成的影响。结果表明,在一定条件下增大初始压力和引入机械搅拌可以促进水合物生成,并且单独添加纳米ZnO或SDS均能显著缩短诱导时间。其中,在ZnO质量分数为0.06%和275.65 K的条件下,确定了初始压力和搅拌速率的最优值分别为4.5 MPa和500 r/min。在3.5 MPa、275.65 K和300 r/min的条件下,加入质量分数为0.10%、粒径为50 nm的纳米ZnO(ZnO-50)体系的诱导时间为41.6 min,较纯水体系的诱导时间(487.4 min)缩短了91.5%。体系中ZnO-50的质量分数为0.06%时,气体消耗总量为0.903 mol,较纯水体系的气体消耗总量(0.444 mol)提高了103.4%。提高SDS的质量分数对气体消耗总量的促进效果逐渐增强,当体系中SDS的质量分数为0.10%时,气体消耗总量达到最大(1.027 mol),比纯水体系的气体消耗总量提高了131.3%。以质量分数为0.10%的SDS与质量分数为0.02%的ZnO-50构建协同体系,其气体消耗总量(1.045 mol)受相平衡压力的影响变化不大,但可以显著加快水合物生成速率,实验半程(反应5 h)的气体消耗量可达0.924 mol,占实验全程(反应10 h)气体消耗总量的88.4%,明显高于单独使用质量分数为0.02%的ZnO-50和质量分数为0.10%的SDS体系的相应数据(分别为63.7%和48.5%)。相关研究结果可为应用水合物技术进行CO_(2)捕集和封存提供一定的理论指导。
The hydrate method for capturing and storing carbon dioxide(CO_(2))has the advantages of high gas storage capacity and low cost,but the long induction time and slow formation rate of CO_(2) hydrate(“hydrate”for short)limit its application.To promote hydrate formation,the effects of nano zinc oxide(ZnO)and sodium dodecyl sulfate(SDS)on hydrate formation were investigated by constant volume method.The results indicate that under certain conditions,increasing the initial pressure and introducing mechanical stirring can promote hydrate formation.Additionally,the addition of either nano ZnO or SDS alone can significantly reduce the induction time.Specifically,under the conditions of ZnO mass fraction of 0.06% and 275.65 K,the optimal values of initial pressure and stirring rate are determined to be 4.5 MPa and 500 r/min,respectively.Under the conditions of 3.5 MPa,275.65 K and 300 r/min,the induction time of the system adding nano ZnO with the mass fraction of 0.10% and particle size of 50 nm(ZnO-50)is 41.6 min,which is 91.5% shorter than that of the pure water system(487.4 min).When the mass fraction of ZnO-50 in the system is 0.06%,the total gas consumption is 0.903 mol,which is 103.4%higher than that of the pure water system(0.444 mol).The promotion effect of increasing SDS mass fraction on total gas consumption gradually increases,reaching a maximum(1.027 mol)when the mass fraction of SDS in the system is 0.10%,which is 131.3% higher than that of the pure water system.Constructing a synergistic system with the mass fraction of 0.10% SDS and 0.02% ZnO-50,the total gas consumption(1.045 mol)remains relatively constant under equilibrium pressure,but the hydrate formation rate can be significantly accelerated.The gas consumption at half-time of the experiment(reaction for 5 h)reaches 0.924 mol,accounting for 88.4% of the total gas consumption over the entire experiment(reaction for 10 h),which is significantly higher than the corresponding data(63.7% and 48.5%,respectively)when using ZnO-50 with mass fraction of 0
作者
崔茂
辛公明
李德祥
CUI Mao;XIN Gongming;LI Dexiang(School of Energy and Power Engineering,Shandong University,Jinan 250061,Shandong,China)
出处
《低碳化学与化工》
CAS
北大核心
2024年第6期129-140,共12页
Low-Carbon Chemistry and Chemical Engineering
基金
国家自然科学基金(52304032)。
