| 律佳媛,任瑞鹏,吕永康.NixCuy-B24N28催化CO2氧化C3H8速控步骤的反应机理研究[J].分子催化,2022,36(2):137-144 |
| NixCuy-B24N28催化CO2氧化C3H8速控步骤的反应机理研究 |
| The Study of the Mechanism of the Rate-Controlling Step of C3H8 by CO2 on the NixCuy-B24N28 Surface |
| 投稿时间：2022-01-05 修订日期：2022-02-10 |
| DOI：10.16084/j.issn1001-3555.2022.02.005 |
| 中文关键词: NixCuy-B24N28 丙烷 二氧化碳 初步氧化 密度泛函理论 |
| 英文关键词:NixCuy-B24N28 C3H8 CO2 preliminary oxidation DFT |
| 基金项目:国家自然科学基金资助项目(22078226);山西浙大新材料与化工研究院项目(2021SX-AT004和2021SX-FR001) |
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| 中文摘要: |
| 采用密度泛函理论(DFT)研究了C3H8和CO2在NixCuy-B24N28(x+y=4, x=1、2、3、4)表面吸附及速控步骤反应机理.计算了C3H8、CO2和相应中间体在NixCuy-B24N28表面的吸附能以及6条可能路径下的反应热和活化能.计算结果表明, C3H8和CO2在NixCuy-B24N28表面是物理吸附, C3H8+CO2→CH3CHCH3+OCOH是最有利的路径,其在不同催化剂表面的活化能顺序是NiCu3-B24N28(1.42 eV)、Ni2Cu2-B24N28(1.57 eV)、Ni3Cu-B24N28(1.62 eV)、Ni4-B24N28(1.75 eV).由此可知,在NixCuy-B24N28催化CO2氧化C3H8的体系中, Cu含量直接影响其催化活性,即NiCu3-B24N28用于催化CO2氧化C3H8有一定优势. |
| 英文摘要: |
| Density functional theory(DFT) was used to study the adsorption and the mechanism of the rate-controlling step of C3H8 and CO2 on the surface of NixCuy-B24N28(x+y=4,x=1,2,3,4).We calculated the adsorption energy of C3H8,CO2 and other corresponding intermediates on the surface of NixCuy-B24N28,and calculated the relevant reaction heat and activation energy under the six possible paths.The calculation results showed that C3H8 and CO2 are physically adsorbed on the surface of NixCuy-B24N28,C3H8+CO2→ CH3CHCH3+OCOH was the most favorable path,and its activation energy sequence on the different catalyst surfaces was NiCu3-B24N28(1.42 eV),Ni2Cu2-B24N28(1.57 eV),Ni3Cu-B24N28(1.62 eV),Ni4-B24N28(1.75 eV).It is concluded that the NixCuy-B24N28 catalytic system used for the oxidation reaction of C3H8 by CO2,the content of Cu directly affects its catalytic activity,that is,NiCu3-B24N28 is more advantageous for catalyzing the oxidation of C3H8 by CO2. |
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