Journal
CHEMICAL ENGINEERING JOURNAL
Volume 445, Issue -, Pages -Publisher
ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2022.136719
Keywords
Electrocatalytic hydrogenation; Selectivity; Carbon fiber; Cyclohexanecarboxylic acid; Benzoic acid
Categories
Funding
- National Key Research and Development Program [2021YFB4000303]
- NSFC [22090034, U20A20151]
- Haihe Laboratory of Sustainable Chemical Transformations [CYZC202108]
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In this study, electrocatalytic hydrogenation was used to convert benzoic acid into cyclohexanecarboxylic acid. Carbon fibers with different degrees of graphitization were used as the support for commercial platinum carbon electrode without external hydrogen. The results showed that the conversion of benzoic acid and the selectivity of cyclohexanecarboxylic acid reached 100% using carbon fiber paper (CFP)-supported Pt/C electrode at room temperature and 1 atm pressure in 0.05 M H2SO4 solution.
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 H2. 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 H2SO4 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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