Pd 掺杂对ZnO(1120 ) 面上水解离的影响.PDF

2012 Chinese Journal of Catalysis Vol. 33 No. 8 文章编号: 0253-9837(2012)08-1427-05 DOI : 10.3724/SP.J.1088.2012.20526 研究论文: 1427~1431 Pd 掺杂对 ZnO( 1120 ) 面上水解离的影响 顾向奎, 丁戊辰, 黄传奇, 李微雪* 中国科学院大连化学物理研究所催化基础国家重点实验室, 辽宁大连 116023 摘要: 采用密度泛函理论计算研究了清洁的以及 Pd 掺杂的 ZnO( 1120 ) 面上水分子的吸附和解离. 结果表明, 在清洁 ZnO( 1120 ) 上, 水分子倾向于分子吸附, 解离吸附较为困难. 在 Pd 掺杂的 ZnO 上, 水分子仍倾向吸附在 Zn 原子上, 且吸附能 与其在清洁 ZnO 表面的相当. 然而, Pd 的掺杂可增强水解离产物 OH 和 H 的吸附, 从而显著提高了水的解离活性, 相应的水 解离能垒为 0.36 eV, 放热 0.21 eV. 关键词: 钯; 掺杂; 氧化锌; 水; 解离; 密度泛函理论 中图分类号: O643 文献标识码: A 收稿日期: 2012-05-15. 接受日期: 2012-05-30. *通讯联系人. 电话/传真: (0411 电子信箱: wxli@ 基金来源: 国家自然科学基金 . Effect of Pd Doping on Water Dissociation on ZnO( 1120 ) Surface * GU Xiangkui, DING Wuchen, HUANG Chuanqi, LI Weixue State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, Liaoning, China Abstract: Water monomer adsorption and dissociation on clean and Pd-doped ZnO( 1120 ) surface were investigated by using density func- tional theory calculations. It was found that water monomer on clean ZnO( 1120 ) prefers the molecular adsorption rather than dissociation. However, its dissociation on Pd-doped ZnO became exothermic with reaction energy of -0.21 eV and kinetically facile with barrier of 0.36 eV, due to enhanced bonding strength of the product OH and H. Key words: palladium; doping; zinc oxide; water; dissociation; density functional theory Received 15 May 2012. Accepted 30 May 2012. *Corresponding author: Tel/Fax: +86-411 E-mail: wxli@ This work wa