State Key Laboratory of Environmental Criteria and Risk Assessment and Key Laboratory of Eco-Industry of the Ministry of Environmental Protection, Chinese Research Academy of Environmental Sciences , Beijing 100012, China.
Particles and Catalysis Research Group, School of Chemical Engineering, University of New South Wales , Sydney, NSW 2052, Australia.
Environ Sci Technol. 2016 Mar 1;50(5):2635-40. doi: 10.1021/acs.est.5b03342. Epub 2016 Feb 15.
Three-dimensional (3D) ordered mesoporous Ag/MnO2 catalyst was prepared by impregnation method based on 3D-MnO2 and used for catalytic oxidation of HCHO. Ag nanoparticles are uniformly distributed on the polycrystalline wall of 3D-MnO2. The addition of Ag does not change the 3D ordered mesoporous structure of the Ag/MnO2, but does reduce the pore size and surface area. Ag nanoparticles provide sufficient active site for the oxidation reaction of HCHO, and Ag (111) crystal facets in the Ag/MnO2 are active faces. The 8.9% Ag/MnO2 catalyst shows a higher normalized rate (10.1 nmol·s(-1)·m(-2) at 110 °C) and TOF (0.007 s(-1) at 110 °C) under 1300 ppm of HCHO and 150 000 h(-1) of GHSV, and its apparent activation energy of the reaction is the lowest (39.1 kJ/mol). More Ag active sites, higher low-temperature reducibility, more abundant surface lattice oxygen species, oxygen vacancies, and lattice defects generated from interaction Ag with MnO2 are responsible for the excellent catalytic performance of HCHO oxidation on the 8.9% Ag/MnO2 catalyst. The 8.9% Ag/MnO2 catalyst remained highly active and stable under space velocity increasing from 60 000 to 150 000 h(-1), under initial HCHO concentration increasing from 500 to 1300 ppm, and under the presence of humidity, respectively.
三维(3D)有序介孔 Ag/MnO2 催化剂通过浸渍法基于 3D-MnO2 制备,并用于 HCHO 的催化氧化。Ag 纳米颗粒均匀分布在 3D-MnO2 的多晶壁上。Ag 的添加并未改变 Ag/MnO2 的 3D 有序介孔结构,但降低了孔径和比表面积。Ag 纳米颗粒为 HCHO 的氧化反应提供了充足的活性位,Ag/MnO2 中的 Ag(111)晶面是活性面。在 1300 ppm 的 HCHO 和 150000 h-1 的 GHSV 条件下,8.9%Ag/MnO2 催化剂表现出更高的归一化速率(110°C 时为 10.1 nmol·s-1·m-2)和 TOF(110°C 时为 0.007 s-1),其反应的表观活化能最低(39.1 kJ/mol)。更多的 Ag 活性位、更高的低温还原性、更丰富的表面晶格氧物种、氧空位和由 Ag 与 MnO2 相互作用产生的晶格缺陷是 8.9%Ag/MnO2 催化剂在 HCHO 氧化反应中表现出优异催化性能的原因。在空速从 60000 增加到 150000 h-1、初始 HCHO 浓度从 500 增加到 1300 ppm 以及湿度存在的情况下,8.9%Ag/MnO2 催化剂仍保持高活性和稳定性。