Thermodynamically driven self-formation of copper-embedded nitrogen-doped carbon nanofiber catalysts for a cascade electroreduction of carbon dioxide to ethylene. Issue 23 (3rd June 2020)

• Record Type: Journal Article
• Authors: Lee, Jae-Chan; Kim, Ji-Yong; Joo, Won-Hyo; Hong, Deokgi; Oh, Sang-Ho; Kim, Beomil; Lee, Gun-Do; Kim, Miyoung; Oh, Jihun; Joo, Young-Chang
• Is Part Of: Journal of materials chemistry. Volume 8:Issue 23(2020)
• Page Start: 11632
• Page End: 11641
• Publication Date: 2020-06-03
• Subjects: Materials -- Research -- Periodicals; Chemistry, Analytic -- Periodicals; Environmental sciences -- Research -- Periodicals; 543.0284
• DOI: 10.1039/d0ta03322g
• Languages: English
• ISSNs: 2050-7488

Abstract

Abstract : Cu acetate/PAN nanofibers were transformed into porous C nanofibers with doped N and Cu particles, via O2 partial pressure-controlled calcination. N atoms next to Cu trigger the CO2 RR by increasing the amount of CO* on the Cu, lowering the energy needed for CO dimerization. Abstract : Electrocatalysts for CO2 electroreduction require not only high-performance active materials to control the series reaction but also conductive and durable supports to ensure long-term stability under harsh operating conditions. Instead of conventional heterogeneous catalysts made by attaching metal on supports, we manufactured a self-formed tandem catalyst designed for a cascade electroreduction of CO2 to C2 H4 . Using oxygen partial pressure-controlled calcination, electrospun copper acetate/polyacrylonitrile nanofibers were successfully transformed into porous carbon nanofibers consisting of doped N and metallic Cu particles. Doped nitrogen atoms adjacent to Cu atoms trigger the reaction by increasing the amount of CO* on the Cu surfaces, which lowers the energy required for CO dimerization that is used for C2 H4 production. The Cu-embedded N-doped carbon nanofibers exhibit a C2 H4 faradaic efficiency of 62% at a potential of −0.57 V vs. RHE with high current density of 600 mA cm −2 and excellent long-term stability. DFT calculations suggest that the lowered overpotential originates from the decreased CO dimerization energy barrier due to the doped N triggering CO production around the Cu particles.