利用第一性原理研究氧化铟在甲醇水蒸气重整反应中的催化作用(英文)

First-principle insights into the catalytic role of indium oxide in methanol steam reforming

基于第一性原理方法,证明了甲醛在In2O3(110)表面可以选择性地转化为CO2.水分解得到的OH物种有利于甲醛脱氢得到CHO,后者不易直接脱氢,其H原子被周围的OH捕获生成CO和H2O.最后,相比较其从表面直接脱附,CO更容易获得一个晶格氧生成CO2.计算结果表明,在没有PdIn合金参与催化的甲醇水蒸气重整反应过程中,In2O3确实扮演着非常重要的角色,进而从理论上证实了甲醇在氧化铟表面选择性生成CO2的实验结果.

Using first-principle methods,we have shown that formaldehyde can be selectively converted to CO2 over In2 O3(110).The OH generated from the splitting of water was found to assist in the dehydrogenation of formaldehyde to give the corresponding formyl(CHO) species.Rather than direct dehydrogenation,a hydrogen atom from the CHO was then removed by a neighboring OH to produce CO.Finally,in favoring of desorption,the CO seized a lattice O atom to yield CO2.Our calculation results indicate that In2 O3 plays an important role in terms of selectivity during the methanol steam reforming reaction without the participation of the PdIn alloy,confirming the experimentally observed selectivity towards CO2.