摘要
本研究采用密度泛函理论,研究含吡咯氮生物质炭(CN5)及其耦合不同金属氧化物(ZnO、CaO、Na_(2)O)对CO_(2)吸附特性的影响机理。计算CO_(2)在不同金属氧化物耦合含吡咯氮生物质炭(CN5@MOx∶CN5@ZnO、CaO、Na_(2)O)上的吸附量,并结合吸附热对吸附量差异进行分析,发现CO_(2)在CN5@Na_(2)O表面发生多层吸附,相较于CN5@ZnO及CN5@CaO,CO_(2)在CN5@Na_(2)O上吸附热与吸附量均较高,100 kPa、20℃时达到6.11 mmol/g,相互作用更强,更有利于吸附。进一步考察了CN5@MOx吸附能,计算结果表明,CN5@Na_(2)O对CO_(2)吸附能高于CN5@CaO和CN5@ZnO,与吸附量一致。然后对其开展电荷差分密度及态密度分析,电荷差分密度表明CN5@Na_(2)O吸附能高是由于Na_(2)O中Na参与吸附,与CO_(2)中O之间发生电荷转移,态密度分析结果表明CO_(2)在CN5@Na_(2)O表面吸附更稳定。
In this study,density functional theory was used to study the influence mechanism of pyrroleaze-containing biochar(CN5)and its coupling of different metal oxides(ZnO,CaO,Na_(2)O)on the adsorption characteristics of CO_(2).Calculating the adsorption capacity of CO_(2) on different metal oxides coupled with pyrrole nitrogen-containing biochar(CN5@MOx∶CN5@ZnO,CN5@CaO,CN5@Na_(2)O),and analyzing the difference in adsorption capacity combined with adsorption heat,it was found that CO_(2) multi-layer adsorption occurred on the CN5@Na_(2)O surface,compared with CN5@ZnO and CN5@CaO,CO_(2) adsorption heat and adsorption capacity on CN5@Na_(2)O were higher,reaching 6.11 mmol/g at 100 kPa and 20℃,with stronger interaction and more utilization of adsorption.The CN5@MOx adsorption energy was further investigated,and the calculation results showed that the CN5@Na_(2)O adsorption energy for CO_(2) was higher than that of CN5@CaO and CN5@ZnO,which was consistent with the adsorption capacity.The charge differential density and state density analysis were carried out,and the charge differential density showed that due to the participation of Na in Na_(2)O in adsorption,charge transfer occurred between O in CO_(2),and the state density analysis showed that CO_(2) was more stable adsorption on the CN5@Na_(2)O surface.
作者
汪辉春
顾明言
陈萍
王莹
葛振凌
汪一
WANG Hui-chun;GU Ming-yan;CHEN Ping;WANG Ying;GE Zhen-ling;WANG Yi(School of Energy and Environment,Anhui University of Technology,Ma'anshan,243002,China;State Key Laboratory of Energy Coal Combustion,Huazhong University of Science and Technology,Wuhan 430074,China)
出处
《燃料化学学报（中英文）》
EI
CAS
CSCD
北大核心
2023年第8期1182-1192,共11页
Journal of Fuel Chemistry and Technology
基金
国家自然科学基金青年项目(52206129)
安徽省自然科学基金青年项目(2208085QE158)
煤燃烧国家重点实验室开放基金(FSKLCCA2206)
2022年安徽工业大学“大学生创新创业训练计划”(S202210360403)资助。
