回流合成体相的和稀释的青铜型W-Nb-O混合氧化物用于短链含氧化合物混合水溶液的定值化反应

doi:10.1016/S1872-2067(19)63419-4

催化学报 ›› 2019, Vol. 40 ›› Issue (11): 1778-1787.DOI: 10.1016/S1872-2067(19)63419-4

回流合成体相的和稀释的青铜型W-Nb-O混合氧化物用于短链含氧化合物混合水溶液的定值化反应

D. Delgado, A. Fernández-Arroyo, N. La Salvia, M. E. Domine, Jose M. López Nieto

瓦莱尼亚理工大学化学技术研究所-高级科学研究理事会, 橘子大道 46022, 瓦伦西亚, 西班牙

收稿日期:2019-03-13 修回日期:2019-06-01 出版日期:2019-11-18 发布日期:2019-09-06
通讯作者: Jose M. López Nieto, M. E. Domine
基金资助:
西班牙政府（RTI2018-099668-B-C21，PGC2018-097277-B-100和SEV-2016-0683）

Reflux-synthesized bulk and diluted W-Nb-O mixed oxide bronzes for the valorization of short-chain oxygenates aqueous mixtures

D. Delgado, A. Fernández-Arroyo, N. La Salvia, M. E. Domine, Jose M. López Nieto

Instituto de Tecnología Química, Universitat Politècnica de València-Consejo Superior de Investigaciones Científicas, Avenida de los Naranjos s/n, 46022, Valencia, Spain

Received:2019-03-13 Revised:2019-06-01 Online:2019-11-18 Published:2019-09-06
Contact: Jose M. López Nieto, M. E. Domine
Supported by:
Financial support by the Spanish Government (RTI2018-099668-B-C21, PGC2018-097277-B-100, and SEV-2016-0683) is gratefully acknowledged. DD and AF-A thank the Severo Ochoa Excellence Program (SVP-2014-068669) and the "La Caixa-Severo Ochoa" Foundation, respectively, for their fellowships. NS thanks "Conselho Nacional de Desenvolvimento Científico y Tecnológico (CNPq)" in Brasil. Authors are also grateful to the Electron Microscopy Service (Universitat Politècnica de València) for facilities.

摘要/Abstract

摘要： 本文报道了用回流法制备体相的和KIT-6稀释的青铜型W-Nb-O混合氧化物.研究了铌和介孔硅胶的掺入对催化剂物化性质的影响.Nb的加入有利于形成单相青铜结构氧化物，并改善了Lewis酸性；而KIT-6的加入使混合金属氧化物颗粒在稀释剂上分散得很好.这些稀释的W-Nb-O催化剂的比表面积和中孔体积增加.通过C-C键形成反应，对材料进行了模型混合水溶液（丙酮/丙醛/乙醇/乙酸/水重量比为5/25/10/30/30）的定值化试验.表面Lewis酸性的增加是反应过程中总有机产率达最大的关键（C5-C10产物）.最好的催化剂在连续使用五次后仍保持其催化性能.

关键词: KIT-6, W-Nb-O氧化物, 含氧物水溶液, 生物质原料, C-C键形成

Abstract: This work reports the preparation of bulk and KIT-6-diluted W-Nb-O mixed oxide bronzes by a reflux method. The influence of the incorporation of Nb and a mesoporous silica on the physico-chemical features of the catalysts is studied. The addition of Nb favors the formation of single-phase oxide bronze structure, with improved Lewis acidity; while the incorporation of KIT-6 gives rise to well-dispersed mixed metal oxide particles on the diluter. These diluted W-Nb-O catalysts present enhanced surface areas and mesopore volumes. The materials have been tested in the valorization of an aqueous model mixture (acetol/propanal/ethanol/acetic acid/water weight ratio of 5/25/10/30/30), through C-C bond formation reactions. The increase in the Lewis nature of surface acid sites stands as the key point to maximize the total organic yield during the reaction (C₅-C₁₀ products). The best catalysts maintain their catalytic behavior after five consecutive uses.

Key words: KIT-6, W-Nb-O oxides, Aqueous oxygenates, Biomass feedstocks, C-C bond formation

D. Delgado, A. Fernández-Arroyo, N. La Salvia, M. E. Domine, Jose M. López Nieto. 回流合成体相的和稀释的青铜型W-Nb-O混合氧化物用于短链含氧化合物混合水溶液的定值化反应[J]. 催化学报, 2019, 40(11): 1778-1787.

D. Delgado, A. Fernández-Arroyo, N. La Salvia, M. E. Domine, Jose M. López Nieto. Reflux-synthesized bulk and diluted W-Nb-O mixed oxide bronzes for the valorization of short-chain oxygenates aqueous mixtures[J]. Chinese Journal of Catalysis, 2019, 40(11): 1778-1787.

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回流合成体相的和稀释的青铜型W-Nb-O混合氧化物用于短链含氧化合物混合水溶液的定值化反应

Reflux-synthesized bulk and diluted W-Nb-O mixed oxide bronzes for the valorization of short-chain oxygenates aqueous mixtures

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