催化作用
材料科学
化学
纤维
碳纤维
苯甲酸
化学工程
有机化学
复合数
复合材料
工程类
作者
Aiqun Kong,Menghui Liu,Houjun Zhang,Zifan Cao,Jinli Zhang,Wei Li,You Han,Yan Fu
标识
DOI:10.1016/j.cej.2022.136719
摘要
The superior ECH performance of Pt/C/CFP for BA is achieved by the graphitization degree of carbon fiber optimizing electrons around the Pt regions, further altering the adsorption strength of BA. • Highly selective conversion of BA into CCA was achieved via ECH. • The Pt/C/CFP electrode exhibites ECH performance with 100% selectivity and conversion. • The Pt/C/CFP electrode possesses outstanding stability after 10 ECH cycles. • Carbon fiber with different defect degrees can regulate the electron density of Pt. • In situ Raman and DFT results revealed the adsorption strength of BA on Pt. Cyclohexanecarboxylic acid (CCA), an important chemical and pharmaceutical intermediate, is commonly produced from thermal catalytic hydrogenation of benzoic acid (BA) under high temperature and pressure. Herein, electrocatalytic hydrogenation (ECH) for highly selective conversion of BA into CCA using carbon fibers with different graphitization degree (carbon fiber paper (CFP), carbon fiber cloth (CFC)) supported commercial platinum carbon (Pt/C) electrode was reported for the first time without using external H 2 . Our experimental results show that, at room temperature and 1 atm, the BA conversion and the CCA selectivity are both as high as 100% in 0.05 M H 2 SO 4 over carbon fiber paper (CFP)-supported Pt/C (Pt/C/CFP). Meanwhile, Pt/C/CFP electrode still maintains outstanding stability after 10 reaction cycles. In situ Raman results and theoretical calculations reveal that the adsorption strength of BA over Pt/C/carbon fibers electrode varies with the graphitization degree of carbon fibers along with the applied potential. The superior ECH performance of the Pt/C/CFP is mainly attributed to the high dispersity of Pt/C catalysts on CFP as well as unique electronic interaction, which improved the adsorption and activation of BA. Typically, CFP with few defects can induce the accumulation of electrons around the Pt regions and enhance the electron-deficient aromatic adsorption thus improving the ECH performance of Pt/C/CFP, which is the opposite for CFC with more defects.
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