Source abstract
Abstract
Ag-based catalysts have been extensively investigated in HCHO oxidation on account of the low price of the Ag precursor and their considerable low-temperature activity. It is known that H 2 pretreatment has a remarkable promotion effect on Pt- and Pd- catalysts for HCHO oxidation, whereas the effect of H 2 reduction on Ag-based catalysts has been rarely reported, probably due to the coexistence of multiple states of Ag species resulting from the high Ag loading. Herein, we prepared a 1% Ag/Al 2 O 3 (Ag/Al-fresh) catalyst with Ag species in a uniform state and then reduced Ag/Al-fresh with H 2 at 600 °C to obtain the Ag/Al-600H 2 catalyst. We observed that H 2 reduction had a significant influence on the performance of Ag/Al 2 O 3 nanocatalysts in HCHO oxidation. In a dry reaction atmosphere, Ag/Al-fresh and Ag/Al-600H 2 exhibited comparable HCHO conversion levels, but Ag/Al-600H 2 showed much higher CO 2 selectivity than Ag/Al-fresh. The presence of water vapor severely suppressed the HCHO conversion of the Ag/Al-fresh catalyst, while Ag/Al-600H 2 showed high water resistance, maintaining high HCHO conversion and CO 2 selectivity at 35% RH. Characterization results showed that the Ag species on Ag/Al-fresh and Ag/Al-600H 2 were single-atom cationic Ag and metallic Ag nanoparticles, respectively. It was revealed that the Ag 0 nanoparticles were more conducive than single-atom Ag + to formate decomposition, as well as O 2 and H 2 O activation, thus accelerating the conversion of HCOO – and CO intermediates to CO 2 and contributing to the higher activity and water resistance of the Ag/Al-600H 2 catalyst.
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Affiliations
State Key Joint Laboratory of Environment Simulation and Pollution Control, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing 100085, China
School of Materials Science and Engineering, Qilu University of Technology (Shandong Academy of Sciences), Jinan 250353, China
Hebei Chemical and Pharmaceutical College, Shijiazhuang 050026, China
Bayin Guoleng Vocational and Technical College, Korla 841002, China
University of Chinese Academy of Sciences, Beijing 100049, China
Weifang Research Institute of Materials and Technology for Eco-environmental Protection, Weifang, Shandong 261300, China
Funding
National Natural Science Foundation of China