School of Energy and Power Engineering, Chongqing University
Key Laboratory of Low-Grade Energy Utilization Technologies and Systems,Ministry of Education of PRC, Chongqing University

CO 作为常见的气态污染物之一,严重影响人类健康生活和经济绿色发展。 大量研究表明,负载型金属氧化物催化剂可对 CO 进行高效催化氧化。 但如何从众多氧化物中筛选获得高 CO氧化性能的催化剂以及从微观层面揭示影响 CO 氧化活性的关键因素一直是研究人员关注的热点。 本文利用密度泛函理论(DFT) 计算,研究了一系列负载型过渡金属氧化物 MxOyHz / TiO2催化剂表面的 CO 氧化反应,分析得到影响催化剂表面进行 CO 氧化反应的关键因素,计算和预测了部分负载型氧化物的 CO 氧化活性。 结果表明:CO 分子在催化剂表面的吸附能(Eads)和活性位点中氧的空位形成能(Eov)大小共同决定了催化剂的 CO 氧化活性;CuO/ TiO2催化剂的 CO 催化氧化活性最高,VO3H、CrOH3、ZrO2、WO3 / TiO2的活性最低,其余催化剂的活性介于两者之间;活性测试的实验结果与 DFT 计算结果一致。

As one of the common gaseous pollutants, CO has seriously affected human healthy life andgreen economic development. Extensive research has shown that the supported metal oxide catalysts canperform efficient catalytic oxidation of CO. However, how to obtain catalysts with high CO oxidationperformance from numerous oxides and to reveal the key factors impacting CO oxidation activity frommicroscopic aspects have been the topical concerns of researchers. In this paper, we investigated theCO oxidation reactions on the surface of a series of supported transition metal oxide MxOyHz / TiO2 cata⁃lysts using density functional theory (DFT) calculations, and analyzed the key factors influencing theCO oxidation reactions conducted on the catalyst surface. Then the CO oxidation activity of partiallysupported oxides was calculated and predicted. The results showed that the adsorption energy (Eads) ofCO molecules on the catalyst surface and the oxygen vacancy formation energy (Eov) of the active sitejointly determine the CO oxidation activity of the catalyst. The CuO/ TiO2 catalyst exhibited the highestCO catalytic oxidation activity; VO3 H, CrOH3, ZrO2, and WO3 / TiO2 displayed the lowest activity;the remaining catalysts were intermediate in activity. Then activity testing experiments were carried outand the results were found to be consistent with the DFT calculations.

国家重点研发计划政府间国际科技创新合作专项目(2021YFE0110800)

0 引 言
1 实验方法
1.1 计算细节
1.2 实验细节
2 结果和讨论
2.1 CO分子在催化剂表面的吸附
2.2 CO分子在催化剂表面反应的氧化机理
2.3 吸附能(Eads)、氧空位形成能(Evf)与催化剂CO氧化活性的关系
3 活性验证
4 结 论

陈坤露, 杜学森, 王星, 等. 基于密度泛函理论的负载型氧化物催化剂 CO 氧化的研究[J]. 能源环境保护, 2023, 37(3): 155-162.

CHEN Kunlu, DU Xuesen, WANG Xing, et al. Research of CO oxidation on supported oxide catalysts based ondensity functional theory[J]. Energy Environmental Protection, 2023, 37(3): 155-162.