Catalysts based on nickel salt heteropolytungstates for selective oxidation of diphenyl sulfide

IF 3.8 4区工程技术 Q2 CHEMISTRY, MULTIDISCIPLINARY

Green Processing and Synthesis Pub Date : 2023-01-01 DOI:10.1515/gps-2023-0026

M. Muñoz, Matthieu Greber, K. B. Tayeb, C. Lamonier, C. Cabello, G. Romanelli

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Abstract

Abstract Nickel salts of Keggin heteropolytungstates with the general formula Ni x A y W12−y O39or40 (A = Si/P) were synthesized and studied as bulk catalytic materials or supported ones by deposition on modified and functionalized clay minerals (pillared layered clay and porous clay heterostructure). Characterizations by Raman, 31P and 29Si-NMR, and ESEM-EDS techniques showed that pure and supported systems preserved the Ni/W ratio and the expected structural properties of heteropolyanions. These materials were evaluated as catalysts in the selective oxidation of sulfides to sulfoxides or sulfones, using aqueous hydrogen peroxide and mild reaction conditions. The bulk materials, with a higher content of Ni, displayed a remarkable catalytic behavior in the oxidation of diphenyl sulfide (Ni3PW11NiO40H, 90% conversion in 15 min at 75°C, 100% sulfone selectivity in 3 h). Supported catalysts, particularly the non-functionalized PCH (Ni2SW12O40/PCH), showed excellent activity, with also being selective in the oxidation of sulfide to sulfoxide (87% conversion, 88.9% sulfoxide selectivity). The reuse of these materials was studied in the optimum reaction conditions, resulting in similar activity and selectivity. Graphical abstract Selective oxidation reaction of DPS to DPSO2 with hydrogen peroxide as oxidant in presence of nickel salts of Keggin heteropolytungstates as catalysts

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镍盐杂多钨酸盐选择性氧化二苯基硫化物催化剂

摘要通过在改性和功能化的粘土矿物（柱撑层状粘土和多孔粘土异质结构）上沉积，合成了通式为Ni x A y W12−y O39or40（A=Si/P）的Keggin杂多钨酸镍盐，并将其作为本体催化材料或负载材料进行了研究。拉曼光谱、31P和29Si NMR以及ESEM-EDS技术的表征表明，纯的和负载的体系保持了杂多酸的Ni/W比和预期的结构性质。这些材料被评价为使用过氧化氢水溶液和温和反应条件将硫化物选择性氧化为亚砜或砜的催化剂。镍含量较高的大块材料在氧化二苯硫醚（Ni3PW11NiO40H，15 75°C时最小，3分钟内100%砜选择性 h）。负载型催化剂，特别是非官能化的PCH（Ni2SW12O40/PCH），表现出优异的活性，在硫化物氧化为亚砜方面也具有选择性（87%的转化率，88.9%的亚砜选择性）。在最佳反应条件下研究了这些材料的再利用，得到了相似的活性和选择性。在Keggin杂多酸镍盐催化下，过氧化氢作为氧化剂将DPS选择性氧化为DPSO2

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来源期刊

Green Processing and Synthesis CHEMISTRY, MULTIDISCIPLINARY-ENGINEERING, CHEMICAL

CiteScore

6.70

自引率

9.30%

发文量

审稿时长

7 weeks

期刊介绍： Green Processing and Synthesis is a bimonthly, peer-reviewed journal that provides up-to-date research both on fundamental as well as applied aspects of innovative green process development and chemical synthesis, giving an appropriate share to industrial views. The contributions are cutting edge, high-impact, authoritative, and provide both pros and cons of potential technologies. Green Processing and Synthesis provides a platform for scientists and engineers, especially chemists and chemical engineers, but is also open for interdisciplinary research from other areas such as physics, materials science, or catalysis.