原子与分子物理学报
原子與分子物理學報
원자여분자물이학보
CHINESE JOURNAL OF ATOMIC AND MOLECULAR PHYSICS
2015年
3期
492-498
,共7页
Gd掺杂CeO2%表面储释氧能力%第一性原理
Gd摻雜CeO2%錶麵儲釋氧能力%第一性原理
Gd참잡CeO2%표면저석양능력%제일성원리
Gd doped CeO2%Surface oxygen storage/release capacity%First principles
本文采用第一性原理平面波超软赝势方法，研究了Gd掺杂CeO2改性材料应用于固体氧化物电池电解质时的表面储释氧性能.对比研究了三种表面覆盖率Ce1－xGdxO2（x＝0，0.10，0.15）下掺杂元素Gd对CeO2的晶体结构、电子结构、氧缺陷形成过程以及表面积碳过程的影响.计算给出了相应掺杂比例下的氧缺陷形成能以及晶体表面吸附石墨烯的吸附能；结果表明：随着掺杂量的增大，氧缺陷形成能减小，晶体表面对石墨烯的吸附能增大；分析掺杂前后改性催化材料的电子结构的变化；说明Gd掺杂会导致CeO2晶体表面结构畸变收缩，有效活化表面氧，同时利用化学平衡原理证明了Gd掺杂后的催化材料可以有效抑制表面碳沉积.从理论的角度解释了Gd掺杂CeO2改性材料在固体氧化物电解质应用中的优势.
本文採用第一性原理平麵波超軟贗勢方法，研究瞭Gd摻雜CeO2改性材料應用于固體氧化物電池電解質時的錶麵儲釋氧性能.對比研究瞭三種錶麵覆蓋率Ce1－xGdxO2（x＝0，0.10，0.15）下摻雜元素Gd對CeO2的晶體結構、電子結構、氧缺陷形成過程以及錶麵積碳過程的影響.計算給齣瞭相應摻雜比例下的氧缺陷形成能以及晶體錶麵吸附石墨烯的吸附能；結果錶明：隨著摻雜量的增大，氧缺陷形成能減小，晶體錶麵對石墨烯的吸附能增大；分析摻雜前後改性催化材料的電子結構的變化；說明Gd摻雜會導緻CeO2晶體錶麵結構畸變收縮，有效活化錶麵氧，同時利用化學平衡原理證明瞭Gd摻雜後的催化材料可以有效抑製錶麵碳沉積.從理論的角度解釋瞭Gd摻雜CeO2改性材料在固體氧化物電解質應用中的優勢.
본문채용제일성원리평면파초연안세방법，연구료Gd참잡CeO2개성재료응용우고체양화물전지전해질시적표면저석양성능.대비연구료삼충표면복개솔Ce1－xGdxO2（x＝0，0.10，0.15）하참잡원소Gd대CeO2적정체결구、전자결구、양결함형성과정이급표면적탄과정적영향.계산급출료상응참잡비례하적양결함형성능이급정체표면흡부석묵희적흡부능；결과표명：수착참잡량적증대，양결함형성능감소，정체표면대석묵희적흡부능증대；분석참잡전후개성최화재료적전자결구적변화；설명Gd참잡회도치CeO2정체표면결구기변수축，유효활화표면양，동시이용화학평형원리증명료Gd참잡후적최화재료가이유효억제표면탄침적.종이론적각도해석료Gd참잡CeO2개성재료재고체양화물전해질응용중적우세.
A first-principles plane-wave pseudopotential method was used to investigate the Oxygen Storage/Re-lease Properties of a new type of modified catalytic materials-Gd doped CeO2 for applications in the Solid oxide fuel cells.A comparative study was carried out using three differently doped materials, Ce1-x Gdx O2 ( x =0, 0.10, 0.15.The effects of doped element Gd on ceria 111 surface.Such as electronic structure, crystal struc-ture, formation of oxygen defect, and surface carbon deposition were studied.The energies of oxygen defect for-mation and adsorption on graphene surface under different doping ratios were obtained through calculation.The results indicate that the energy of oxygen defect formation decreased with the doping ratio increasing, while the energy of the crystal surface adsorbing graphene increases with the increase in doping ratio.While the energy of adsorption on graphene surface increase with the increase in doping ratio.According to the variation in the elec-tronic and atomic structures before and after the doping Gd, the doping caused the distortion and contraction of crystal surface structure.Resulting in the efficient activation of surface oxygen atoms.Simultaneously, the Gd-doped catalytic materials effectively restrained the surface carbon deposition, as explained by the principle of chemical equilibrium.Thus, Gd-doped CeO2 materials are advantageous as an electrolyte in solid oxide fuel cells.
