DFT Study of CO2 Adsorption and Hydrogenation on the In2O3 Surface
DFT Study of CO2 Adsorption and Hydrogenation on the In2O3 Surface
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DOI：
10.1021/jp3004773
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发表时间：
2012-03
影响因子：
3.7
通讯作者：
Jingyun Ye;Chang‐jun Liu;Q. Ge
中科院分区：
文献类型：
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作者：
Jingyun Ye;Chang‐jun Liu;Q. Ge
二氧化碳催化转化为液体燃料或有价值的化学物质是地质封存的一个有吸引力的替代方案。在本研究中，我们应用密度泛函理论平板计算研究了CO2在In2O3（110）表面的吸附和加氢。结果表明，吸附后的CO2被活化，与表面氧结合形成表面碳酸盐，吸附能为- 1.25 eV。H2的异解离吸附导致H的表面羟基与表面O位点结合，H的表面氢化物与in位点结合。氢从In位迁移到相邻的O位在能量上是有利的，但具有1.32 eV的显著激活势垒。水可以分子吸附或解离吸附在表面，吸附能分别为- 0.83 eV和- 1.19 eV。从CO2与H附原子在In2O3表面的共吸附开始，我们研究了CO2的两种可能的转化途径：(a) CO2…
Catalytic conversion of CO2 to liquid fuels or valuable chemicals is an attractive alternative to geological sequestration. In the present study, we applied density functional theory slab calculations in the investigation of the adsorption and hydrogenation of CO2 on the (110) surface of In2O3. Our results indicate that the adsorbed CO2 is activated, forming a surface carbonate species by combining with surface oxygen, and has an adsorption energy of −1.25 eV. Heterolytic dissociative adsorption of H2 results in a surface hydroxyl from H binding the surface O site and a hydride from H binding the In site. The migration of H from the In site to the neighboring O site is energetically favorable but has a significant activation barrier of 1.32 eV. Water may adsorb on the surface either molecularly or dissociatively, with adsorption energy of −0.83 eV and −1.19 eV, respectively. Starting from CO2 coadsorbed with the H adatoms on the In2O3 surface, we examined two possible conversion pathways for CO2: (a) CO2 ...