In order to prevent metal leaching in aqueous-phase hydrogenolysis of a carboxylic acid, metallic particles were encapsulated inside porous silica nanoparticles by coating silica onto the surface of metal–polyvinylpyrrolidone (PVP) colloids. Four catalysts prepared were denoted as M@SiO₂ and Re-M@SiO₂ (M = Pd and Ru), where Re signifies a rhenium promoter. They were characterized with SEM, TEM, nitrogen and n-butylamine adsorption/desorption, XRD, TPR and were used for catalyzing the aqueous-phase hydrogenolysis of succinic acid (SA, which can be produced from food waste via fermentation) to γ-butyrolactone (GBL), tetrahydrofuran (THF) and 1,4-butanediol (BDO) in a batch reactor. 84.7% GBL yield (93.8% selectivity) and 29% BDO yield were obtained with Pd@SiO₂ and Ru@SiO₂, respectively. Catalyst acidity, activity and product selectivity were changed significantly with the Re addition. 52.7% THF yield and 42.6% BDO yield were produced using Re-Pd@SiO₂ and Re-Ru@SiO₂, respectively. Kinetic studies indicated that succinic acid disappearance rate was first-order with respect to succinic acid concentration and activation energy decreased significantly with Re addition. XRD, TPR and reuse studies indicated that little metal leaching occurred during the aqueous-phase hydrogenolysis.

Graphic abstract

Re-M@SiO₂ (M = Pd and Ru)

C₂H₄(COOH)₂ + H₂ → γ-butyrolactone(GBL), tetrahydrofuran(THF), 1,4-butanediol(BDO)

中文翻译：

---

琥珀酸在包裹在多孔二氧化硅纳米粒子中的 Ru 和 Pd 催化剂上的氢解

为了防止羧酸水相氢解中的金属浸出，通过将二氧化硅涂覆在金属-聚乙烯吡咯烷酮 (PVP) 胶体的表面上，将金属颗粒封装在多孔二氧化硅纳米颗粒中。制备的四种催化剂表示为 M@SiO ₂和 Re-M@SiO ₂（M = Pd 和 Ru），其中 Re 表示铼助催化剂。它们通过扫描电镜、透射电镜、氮气和正丁胺吸附/解吸、XRD、TPR 进行表征，并用于催化琥珀酸（SA，可通过发酵从食物垃圾中获得）水相氢解为 γ-丁内酯(GBL)、四氢呋喃 (THF) 和 1,4-丁二醇 (BDO) 在间歇式反应器中。使用 Pd@SiO ₂获得 84.7% GBL 产率（93.8% 选择性）和 29% BDO 产率和 Ru@SiO ₂。随着 Re 的加入，催化剂的酸度、活性和产物选择性发生了显着变化。使用 Re-Pd@SiO ₂和 Re-Ru@SiO ₂分别产生了 52.7% 的 THF 产率和 42.6% 的 BDO 产率。动力学研究表明，琥珀酸的消失率与琥珀酸浓度有关，活化能随着 Re 的加入显着降低。XRD、TPR 和再利用研究表明，在水相氢解过程中几乎没有发生金属浸出。

图形摘要

Re-M@SiO ₂ (M = Pd 和 Ru)

C ₂ H ₄ (COOH) ₂  + H ₂  → γ-丁内酯(GBL)、四氢呋喃(THF)、1,4-丁二醇(BDO)