摘要
为了提高铜基氧载体的释氧性能,采用溶胶凝胶-燃烧法制备了一系列锆掺杂的铜基氧载体并进行了实验研究。通过XRD、SEM、BET、固定床实验等手段研究了锆掺杂对铜基氧载体物相结构、表面形貌、释氧性能和循环反应性能的影响。实验结果表明:锆离子能够进入氧载体晶格形成固溶体;掺杂锆能提高铜基氧载体的比表面积,细化其晶粒;掺杂锆的铜基氧载体,释氧量和释氧性能得到提高;掺杂8%Zr的铜基氧载体在多次循环实验中表现出较好的稳定性。量子化学的密度泛函理论计算结果表明:Zr掺杂能有效降低氧化铜释氧反应的活化能垒,提高其释氧能力,与实验结果吻合。
To enhance the performance of Cu-based oxygen carriers, a series of Zr-doped Cu-based oxygen carriers were prepared by the sol-gel combustion method and studied by experiments. The effects of doping Zr on surface topography, phase structure and oxygen desorption were investigated by XRD, SEM, BET, and fixed bed experiment. The experimental results indicate that Zr ion can enter the crystal lattice of oxygen carrier to form a solid solution. The addition of Zr enlarges the specific surface area and refines the grains. The Zr-doped Cu-based oxygen carriers have high oxygen release capacity and oxygen desorption reaction rates. The 8% Zr-doped Cu-based oxygen carriers have high cyclic stability in cyclic operation. Density functional theoretical calculation shows that the Zr-doped CuO has lower energy barrier for oxygen desorption compared with the pure CuO, thus facilitating the oxygen release of CuO, which agrees with the experimental results. © 2015, China Coal Society. All right reserved.
出处
《煤炭学报》
EI
CAS
CSCD
北大核心
2015年第11期2727-2732,共6页
Journal of China Coal Society
基金
国家重点基础研究发展计划(973)资助项目(2011CB707301)
湖北省自然科学基金资助项目(2015CFA046)
关键词
铜基氧载体
锆掺杂
化学链氧解耦
密度泛函理论
Density functional theory
Desorption
Oxygen
Phase structure
Reaction rates
Sol
gels
Surface topography
