Department of Chemistry, University of Kerala, Kariavattom Campus, Thiruvananthapuram, Kerala, 695 581 India.
Environ Sci Technol. 2013 Mar 19;47(6):2746-53. doi: 10.1021/es303992j. Epub 2013 Feb 28.
We synthesized MnCo(2)O(4) catalyst with very high porosity on the surface of dealuminated zeolite molecular sieves (DAZMS) for CO oxidation under actual automobile conditions. The MnCo(2)O(4) catalyst was selected on the basis of preliminary DFT study using the software ADF BAND. The MnCo(2)O(4) catalyst had comparatively higher CO adsorption energy and very low oxygen vacancy formation energy. The synthesized MnCo(2)O(4)/DAZMS catalyst was characterized by XRD, XRF, BET, SEM, and Confocal Microscopy. The Confocal microscopic analysis revealed that porosity of the dealuminated zeolite surface was significantly enhanced after the catalyst loading process. The completely precious metal free and DAZMS-supported catalyst exhibited excellent CO oxidation ability with renewed activity for seven months under actual automobile conditions with reference to normal and cold start conditions. The synthesized MnCo(2)O(4)/DAZMS not only exhibited surprisingly high catalytic activity for CO oxidation at a temperature resembling a cold start period but was also sufficiently stable/active under actual automobile conditions and ambient conditions containing large amounts of CO,H(2)O,CO(2), and NO(x) at 155-715 °C. These significant results revealed the flexible use of the present catalyst system for a wide variety of automobiles from a small gasoline-fuelled vehicle to a large diesel-fuelled vehicle that may produce high CO-content exhaust.
我们在脱铝沸石分子筛(DAZMS)表面合成了具有极高孔隙率的 MnCo(2)O(4)催化剂,用于实际汽车条件下的 CO 氧化。MnCo(2)O(4)催化剂是基于使用 ADF BAND 软件的初步 DFT 研究选择的。MnCo(2)O(4)催化剂具有相对较高的 CO 吸附能和非常低的氧空位形成能。合成的 MnCo(2)O(4)/DAZMS 催化剂通过 XRD、XRF、BET、SEM 和共聚焦显微镜进行了表征。共聚焦显微镜分析表明,催化剂负载后,脱铝沸石表面的孔隙率显著增强。完全不含贵金属且负载在 DAZMS 上的催化剂在实际汽车条件下(参照正常和冷启动条件)具有出色的 CO 氧化能力,经过七个月的更新后仍具有活性。合成的 MnCo(2)O(4)/DAZMS 不仅在类似于冷启动期的温度下对 CO 氧化表现出惊人的高催化活性,而且在实际汽车条件和含有大量 CO、H(2)O、CO(2)和 NO(x)的环境条件下在 155-715°C 下也具有足够的稳定性/活性。这些显著的结果表明,本催化剂体系可灵活应用于从小型汽油车到大型柴油车等各种汽车,这些汽车可能会产生高含量 CO 的废气。