Graphene-Immobilized fac-Re(bipy)(CO)3Cl for Syngas Generation from Carbon Dioxide

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• 作者：Xin Zhou ; Daniel Micheroni ; Zekai Lin ; Christopher Poon ; Zhong Li ; Wenbin Lin
• 刊名：ACS Applied Materials & Interfaces
• 出版年：2016
• 出版时间：February 17, 2016
• 年：2016
• 卷：8
• 期：6
• 页码：4192-4198
• 全文大小：386K
• ISSN：1944-8252

文摘

We report the synthesis of fac-M(4-amino-bipy)(CO)₃X (M = Mn and X = Br or M = Re and X = Cl, with bipy = 2,2′-bipyridine), their immobilization on graphene oxide (GrO) via diazonium grafting, and the use of Re-functionalized GrO for electrocatalytic syngas production. Infrared (IR) spectroscopy, X-ray absorption fine structure (XAFS) spectroscopy, and electrocatalysis indicated successful grafting of the Re catalyst onto GrO. Re-functionalized GrO was then deposited onto a glassy carbon electrode (GCE) for CO₂ reduction. Investigation of the Re-functionalized GCE for syngas production was performed in a CO₂-saturated acetonitrile solution with 3.1 M H₂O as the proton source and 0.1 M tetrabutylammonium hexafluorophosphate (TBAPF₆) as the supporting electrolyte. Cyclic voltammetry (CV), controlled potential electrolysis (CPE), and gas chromatography (GC) were employed to determine its CO₂-to-CO conversion performance. The Re catalyst shows a turnover frequency (TOF) for generating CO up to 4.44 s^–1 with a CO/H₂ ratio of 7:5.