王清云,佟永纯,徐新建,王永成.石墨烯中的Stone-wales缺陷对铂原子催化解离氧分子的影响[J].分子催化,2016,30(1):80-87
石墨烯中的Stone-wales缺陷对铂原子催化解离氧分子的影响
The influence of the Stone-wales defect in graphene on the platinum catalyzed dissociation of oxygen
投稿时间:2015-12-03  修订日期:2015-12-15
DOI:
中文关键词:  Stone-wales缺陷石墨烯  催化  密度泛函理论
英文关键词:Wang, Qingyuna Tong, Yongchuna* Xu, Xinjiana Wang, Yongchengb
基金项目:甘肃省高等学校科研项目NO.2015A-140
作者单位E-mail
王清云 河西学院化学化工学院 w_qingyun@163.com 
佟永纯* 河西学院化学化工学院 w_qingyun@163.com, tongjia12@163.com 
徐新建 河西学院化学化工学院 80735604@qq.com 
王永成 西北师范大学化学化工学院 w11111@163.com 
摘要点击次数: 1514
全文下载次数: 3443
中文摘要:
      采用密度泛函理论中的UB3LYP方法,研究了石墨烯中的Stone-wales缺陷对铂原子催化解离氧气分子的影响。通过计算发现,氧气分子在以Stone-wales缺陷石墨烯片为载体的铂上(Pt-SW)形成三种吸附结构,通过四条路径,最终生成两种产物。氧气分子最易通过 [2+1]环加成作用,吸附在以Stone-wales缺陷石墨烯片为载体的Pt的表面上,吸附能(Eads)为-0.64 eV。由于石墨烯片上的Stone-wales缺陷的存在,氧气分子在Pt-SW上解离的四条路径中最有利的解离路径中的决速步能垒都明显高于氧气在以完美石墨烯为载体的Pt(Pt/Graphene)上解离的能垒(1.51 eV vs 1.35 eV),相应吸收的热量也高于在Pt/Graphene上吸收的热量(0.79eV vs 0.15eV)。
英文摘要:
      The influence of the Stone-wales defect in graphene on the platinum catalyzed dissociation of oxygen has been studied by density functional theory calculation. By calculation, we find that the oxygen can form three absorption structures on the platinum catalyst which is supported by the graphene with Stone-wales defect (Pt-SW), and it forms two products through four reaction pathways. Firstly, the oxygen molecule is adsorbed on the Pt-SW by [2 + 1] cycloaddition, with the adsorption energy (Eads) of −0.64 eV. In the most favorable reaction pathway (R2→TS4→IM2→TS5→IM3→TS6→P2), because of the existing Stone-Wales defect of graphene, the dissociation barrier of O2 in rate-determining step is higer than the oxygen molecule dissociation on the platinum catalyst (Pt/Graphene) supported the pristine graphene(1.51 eV vs 1.35 eV). Correspondingly, the endothermic of the most favorable reaction pathway is 0.79 eV higher the oxygen molecule dissociation on the Pt/Graphene (0.79eV vs 0.15eV).
HTML  查看全文  查看/发表评论  下载PDF阅读器