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通过再充电法添加金对苯酚催化湿式空气氧化（CWAO）中银负载催化剂的影响。

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

作者信息

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

机构信息

Universidad Juárez Autónoma de Tabasco, Laboratorio de Nanomateriales Catalíticos Aplicados al Desarrollo de Fuentes de Energìa y de Remediaciòn Ambiental, Centro de Investigación de Ciencia y Tecnología Aplicada de Tabasco (CICTAT), DACB Km. 1 Carretera Cunduacán-Jalpa de Méndez AP. 24, C.P. 86690, Cunduacán Tabasco Mexico

Instituto Tecnológico de Villahermosa Km. 3.5 Carretera, Villahermosa - Frontera, Cd. Industrial 86010 Villahermosa Tabasco Mexico.

出版信息

RSC Adv. 2019 Apr 9;9(20):11123-11134. doi: 10.1039/c9ra00540d.

DOI:10.1039/c9ra00540d
PMID:35520247
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC9063395/
Abstract

Catalysts Ag/ZrO-CeO and Au/ZrO-CeO were synthesized by a deposition-precipitation method and Ag-Au/ZrO-CeO was prepared using a recharge method for the second metal (Au). The materials were characterized by physisorption of N, 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 g and 27-74 m g for bimetallics. The tetragonal crystal phase of ZrO stabilizes when CeO quantity increases. Using XPS an increment in Ce 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 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-CeO 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.

摘要

采用沉积沉淀法合成了催化剂Ag/ZrO-CeO和Au/ZrO-CeO，并使用第二种金属（Au）的再充电方法制备了Ag-Au/ZrO-CeO。通过N的物理吸附、XRD、ICP、UV-vis RDS、H2-TPR、XPS和TEM对材料进行了表征。结果表明，单金属材料的比表面积为29-37 m²/g，双金属材料的比表面积为27-74 m²/g。当CeO含量增加时，ZrO的四方晶相稳定。使用XPS测定，与单金属催化剂相比，双金属催化剂中Ce物种的丰度有所增加；根据Ag 3d区域，当材料中CeO含量增加时，观察到这种金属的氧化，而对于Au则产生相反的效果。通过TEM测定，由于制备方法的原因，双金属催化剂中金属颗粒的平均尺寸较小。通过苯酚的催化湿式空气氧化（CWAO）评估催化活性，含20%重量铈的Ag-Au/ZrO-CeO催化剂在一小时内达到了100%的降解率，是活性最高的催化剂。马来酸、甲酸和草酸被鉴定为反应中间体；在反应结束时，乙酸被鉴定为主要副产物，因为它最难降解，氧化条件必须更苛刻。

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