Effect of gold addition by the recharge method on silver supported catalysts in the catalytic wet air oxidation (CWAO) of phenol

Catalysts Ag/ZrO 2 -CeO 2 and Au/ZrO 2 -CeO 2 were synthesized by a deposition-precipitation method and Ag-Au/ZrO 2 -CeO 2 was prepared using a recharge method for the second metal (Au). The materials were characterized by physisorption of N 2 , XRD, ICP, UV-vis RDS, H2-TPR, XPS and TEM. The results...

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Veröffentlicht in:RSC advances 2019-04, Vol.9 (2), p.11123-11134
Hauptverfasser: Silahua-Pavón, Adib A, Torres-Torres, Gilberto, Arévalo-Pérez, Juan Carlos, Cervantes-Uribe, Adrián, Guerra-Que, Zenaida, Cordero-García, Adrián, Espinosa de los Monteros, Alejandra, Beltramini, Jorge N
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Sprache:eng
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Zusammenfassung:Catalysts Ag/ZrO 2 -CeO 2 and Au/ZrO 2 -CeO 2 were synthesized by a deposition-precipitation method and Ag-Au/ZrO 2 -CeO 2 was prepared using a recharge method for the second metal (Au). The materials were characterized by physisorption of N 2 , XRD, ICP, UV-vis RDS, H2-TPR, XPS and TEM. The results obtained show that the specific areas for monometallic materials were 29-37 m 2 g −1 and 27-74 m 2 g −1 for bimetallics. The tetragonal crystal phase of ZrO 2 stabilizes when CeO 2 quantity increases. Using XPS an increment in Ce 3+ species abundance was determined for bimetallic catalysts in contrast to the monometallic ones; according to the Ag 3d region, this metal oxidation was observed when augmenting the content of CeO 2 in the materials, and with Au the opposite effect was produced. It was determined by TEM, that the average size of the metallic particles was smaller at bimetallic catalysts due the preparation method. Catalytic activity was evaluated by CWAO of phenol, the Ag-Au/ZrO 2 -CeO 2 catalyst with 20% wt of cerium reached a degradation of 100% within an hour, being the most active catalyst. Maleic, formic and oxalic acid were identified as reaction intermediates; and at the end of the reaction acetic acid was identified as the main by-product, because it is the most refractory and the conditions for oxidation must be more severe. Addition of gold changed the properties of silver monometallic catalysts by inhibiting the low formation of intermediates and changed of reaction route by formic acid to CO 2 and water. Furthermore, the bimetallic catalyst showed in the reuse cycles the better stability in CWAO of phenol.
ISSN:2046-2069
2046-2069
DOI:10.1039/c9ra00540d