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Integrating hydrogen production with anodic selective oxidation of sulfides over a CoFe layered double hydroxide electrode
Chemical Science ( IF 8.4 ) Pub Date : 2020-11-11 , DOI: 10.1039/d0sc05499b
Lina Ma 1 , Hua Zhou 2 , Ming Xu 1 , Peipei Hao 1 , Xianggui Kong 1 , Haohong Duan 2
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Replacing the sluggish oxygen evolution reaction (OER) with oxidation reactions for the synthesis of complex pharmaceutical molecules coupled with enhanced hydrogen evolution reaction (HER) is highly attractive, but it is rarely explored. Here, we report an electrochemical protocol for selective oxidation of sulfides to sulfoxides over a CoFe layered double hydroxide (CoFe-LDH) anode in an aqueous-MeCN electrolyte, coupled with 2-fold promoted cathodic H2 productivity. This protocol displays high activity (85–96% yields), catalyst stability (10 cycles), and generality (12 examples) in selective sulfide oxidation. We demonstrate its applicability in the synthesis of four important pharmaceutical related sulfoxide compounds with scalability (up to 1.79 g). X-ray spectroscopy investigations reveal that the CoFe-LDH material evolved into amorphous CoFe-oxyhydroxide under catalytic conditions. This work may pave the way towards sustainable organic synthesis of valuable pharmaceuticals coupled with H2 production.

中文翻译:

在 CoFe 层状双氢氧化物电极上将制氢与硫化物的阳极选择性氧化相结合

用氧化反应代替缓慢的析氧反应 (OER) 来合成复杂的药物分子并结合增强的析氢反应 (HER) 是非常有吸引力的,但它很少被探索。在这里,我们报告了一种电化学方案,用于在水性-MeCN 电解质中的 CoFe 层状双氢氧化物 (CoFe-LDH) 阳极上将硫化物选择性氧化为亚砜,再加上 2 倍促进的阴极 H 2生产率。该协议在选择性硫化物氧化中表现出高活性(85–96% 产率)、催化剂稳定性(10 个循环)和通用性(12 个示例)。我们证明了它在合成四种重要的药物相关亚砜化合物中的适用性,具有可扩展性(高达 1.79 g)。X 射线光谱研究表明,CoFe-LDH 材料在催化条件下演变为无定形 CoFe-羟基氧化物。这项工作可能为有价值药物的可持续有机合成以及 H 2生产铺平道路。
更新日期:2020-11-19
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