| 傅钢,吕鑫,徐昕,万惠霖.CO2在金属表面活化的能学方法研究[J].分子催化,2001,(6):484-486 |
| CO2在金属表面活化的能学方法研究 |
| Energetics Study of CO2 Activation on Metal Surface |
| |
| DOI： |
| 中文关键词: CO2 UBI－QEP方法 活化 甲醇 合成 二氧化碳 金属表面 吸附 活化能 能学方法 催化转化 |
| 英文关键词:CO 2,UBI QEP energetics methods,Activation,Methanol synthesis |
| 基金项目:国家自然科学基金，国家重点基础研究发展计划(973计划)，20973031，G1999022408，， |
| 傅钢 吕鑫 徐昕 万惠霖 |
| 厦门大学,化学系, |
| 摘要点击次数: 936 |
| 全文下载次数: 34 |
| 中文摘要: |
| 应用UBI-QEP方法, 估算了CO2-在金属表面的吸附热, 并计算了CO2在Cu(111)、Pd(111)、Fe(111)、Ni(111)表面的各种反应途径的活化能垒. 结果表明, CO2-在4种过渡金属表面相对的稳定性和CO2解离吸附的活性顺序一致,均为Fe>Ni>Cu>Pd. 说明CO2-可能是CO2解离吸附的关键中间体. 在Cu、Pd、Ni表面上, CO2解离吸附的最终产物是CO,而在Fe表面其最终会解离成C和O. 在Cu、Fe、Ni表面, CO2加氢活化是一种有效模式, 而在Pd上则不容易进行. 在Cu和Pd表面,碳酸盐物种也可能是CO2活化的重要中间体. |
| 英文摘要: |
| The adsorption energy of CO 2 - and the energy barrier of various pathways of CO 2 activation on Cu(111), Pd(111), Fe(111) surfaces were predicted using UBI QEP energetics method. The theoretical results show that the stability of adsorbed CO 2 and the reactivity of CO 2 toward dissociation on the above four transition metal surfaces follow the same order: Fe(111)>Ni(111)>Cu(111)>Pd(111). This suggests that CO 2\+- is a pivotal intermediate in the process of CO 2 dissociation. The final products of CO 2 dissociation are CO(a) and O(a) on the Cu, Pd, Ni surfaces and C(a) and O(a) on Fe surface, respectively. The hydrogenation of CO 2 is an effective mode for CO 2 activation on Cu, Ni, and Fe surfaces, but is unfavorable on Pd surface. On Cu and Pd surfaces, carbonate species would also be a important intermediate for CO 2 activation. |
| HTML 查看全文 查看/发表评论 下载PDF阅读器 |
|
|
|
