Zhu Chen, Guan Shengnan, Li Wenzhi, Ogunbiyi Ajibola T, Chen Kun, Zhang Qi
Laboratory of Basic Research in Biomass Conversion and Utilization, Department of Thermal Science and Energy Engineering, University of Science and Technology of China, Hefei 230026, China.
CAS Key Laboratory of Renewable Energy, Guangzhou Institute of Energy Conversion, Chinese Academy of Sciences, Guangzhou 510640, PR China.
ACS Omega. 2021 Dec 14;6(51):35404-35415. doi: 10.1021/acsomega.1c04769. eCollection 2021 Dec 28.
Here, we prepare a MnO/CeO hollow sphere catalyst using the carbon sphere as a self-sacrificing template for formaldehyde (HCHO) removal. In the feed gas of 20 ppm of HCHO (balanced by N) + 20 vol % O, a HCHO removal efficiency of 70% was achieved at 20 °C and full conversion was reached at around 47 °C at GHSV = 50,000 mL (g h) for MnO/CeO hollow spheres. The catalytic performance and structural and chemical properties of MnO/CeO hollow spheres for the removal of core carbon spheres were explored, and the influence of using the carbon sphere as a self-sacrificing template was proved by comparing with carbon@MnO/CeO (a core carbon sphere with a MnO/CeO shell) and nonmorphologic MnO/CeO. The properties of the MnO/CeO hollow spheres are significantly improved compared to carbon@MnO/CeO (removal efficiency of 45% at 150 °C) and MnO/CeO (removal efficiency of 46% at 20 °C) as a result of an evolution in the interaction between Mn/Ce and carbon. This increase in the interaction strength seems to (i) increase the oxygen vacancy, (ii) promote the oxygen species mobility, and (iii) improve the chemical stability of the MnO/CeO hollow spheres. We believe that these results are beneficial to the fabrication of binary transition metal oxides and applications of them in HCHO removal.
在此,我们以碳球作为自牺牲模板制备了MnO/CeO空心球催化剂用于去除甲醛(HCHO)。在含有20 ppm HCHO(以N平衡)+ 20 vol% O的原料气中,MnO/CeO空心球在20 °C时的HCHO去除效率达到70%,在约47 °C、气体时空速(GHSV)= 50,000 mL/(g h)时实现完全转化。我们探究了MnO/CeO空心球去除核心碳球时的催化性能以及结构和化学性质,并通过与碳@MnO/CeO(具有MnO/CeO壳层的核心碳球)和无定形MnO/CeO进行比较,证明了使用碳球作为自牺牲模板的影响。由于Mn/Ce与碳之间相互作用的演变,MnO/CeO空心球的性能相较于碳@MnO/CeO(150 °C时去除效率为45%)和MnO/CeO(20 °C时去除效率为46%)有显著提高。这种相互作用强度的增加似乎(i)增加了氧空位,(ii)促进了氧物种的迁移率,以及(iii)提高了MnO/CeO空心球的化学稳定性。我们认为这些结果有利于二元过渡金属氧化物的制备及其在HCHO去除中的应用。