Journal
CHEMICAL ENGINEERING JOURNAL
Volume 380, Issue -, Pages -Publisher
ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2019.122498
Keywords
Catalytic oxidation of HCHO; Interfacial electrons transfer; Activation barrier; C-H dissociation; ZrO2 phase-junctions
Categories
Funding
- National Key Research and Development Program of China, China [2016YFA0203000]
- National Science Foundation of China, China [51708537, 41401567, 41573138]
- China Postdoctoral Science Foundation, China [2017M613237]
- Open foundation of State Key Laboratory of Loess and Quaternary Geology, China [SKLLQG1638, SKLLQGPY1605]
- Key Projects of Chinese Academy of Sciences, China [ZDRW-ZS-2017-6]
- Strategic Priority Research Program of the Chinese Academy of Sciences, China [XDA23010300, XDA23010000]
- Key Project of International Cooperation of the Chinese Academy of Sciences, China [GJHZ1543]
- Research Grants Council of Hong Kong, China [PolyU 152083/14E]
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The room temperature catalytic efficiency of formaldehyde (HCHO) is determined by interfacial electrons transfer properties, gas adsorption configuration and reactivity of catalysts. The phase-junctions with lattice planes of high matching degree and abundant active sites may do better in the above three aspects than traditional catalysts and their heterojunctions. In this work, tetragonal-monoclinic nano-zirconia (ZrO2 ) phase-junctions (TMZ) were synthesized for the first time. The highest conversion efficiency of HCHO into CO2 was around 81% at 25 degrees C exceeded the value for pure ZrO2. Density functional theory calculations and in-situ diffuse reflectance infrared Fourier transform spectroscopy measurements revealed that the adsorption enhancement of rich zirconium sites and single electron activation at TMZ interface caused C-H dissociation of HCHO and hydrogenation of O-2 (D-H), significantly lowering the activation barrier of catalytic oxidation of HCHO. Our findings can facilitate further design of more active catalyst for room temperature removal of HCHO.
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