期刊
SMALL
卷 17, 期 51, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/smll.202102970
关键词
Co-CoO interface; hydrogen production; lattice strain modulation; oxygen vacancies; reforming of formaldehyde
类别
资金
- National Natural Science Foundation of China [21872123, 22172143]
- Zhejiang Provincial Natural Science Foundation of China [LY18B030007]
- Excellent Postgraduate Thesis Program of Zhejiang Sci-Tech University [2019D05]
- National Research Foundation of Singapore under its Campus for Research Excellence and Technological Enterprise (CREATE) program
Lattice strain modulation and vacancy engineering were found to be effective in controlling the catalytic properties of Co@CoO heterointerface catalysts. The bifunctional nature of oxygen-vacancy-rich Co-CoO interfaces was elucidated, with Co and CoO sites responsible for different catalytic reactions. The study also demonstrated that the sample reduced at 350 degrees C, Co@CoO-350, exhibited optimal catalytic activity with the highest turnover frequency for the aqueous phase reforming of formaldehyde to produce hydrogen.
Lattice strain modulation and vacancy engineering are both effective approaches to control the catalytic properties of heterogeneous catalysts. Here, Co@CoO heterointerface catalysts are prepared via the controlled reduction of CoO nanosheets. The experimental quantifications of lattice strain and oxygen vacancy concentration on CoO, as well as the charge transfer across the Co-CoO interface are all linearly correlated to the catalytic activity toward the aqueous phase reforming of formaldehyde to produce hydrogen. Mechanistic investigations by spectroscopic measurements and density functional theory calculations elucidate the bifunctional nature of the oxygen-vacancy-rich Co-CoO interfaces, where the Co and the CoO sites are responsible for C-H bond cleavage and O-H activation, respectively. Optimal catalytic activity is achieved by the sample reduced at 350 degrees C, Co@CoO-350 which exhibits the maximum concentration of Co-CoO interfaces, the maximum concentration of oxygen vacancies, a lattice strain of 5.2% in CoO, and the highest aqueous phase formaldehyde reforming turnover frequency of 50.4 h(-1) at room temperature. This work provides not only new insights into the strain-vacancy-activity relationship at bifunctional catalytic interfaces, but also a facile synthetic approach to prepare heterostructures with highly tunable catalytic activities.
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