Electrochemical Fragmentation of Cu 2 O Nanoparticles Enhancing Selective C-C Coupling from CO 2 Reduction Reaction

Hyejin Jung, Si Young Lee, Chan Woo Lee, Min Kyung Cho, Da Hye Won, Cheonghee Kim, Hyung Suk Oh, Byoung Koun Min, Yun Jeong Hwang

Research output: Contribution to journalArticle

4 Citations (Scopus)

Abstract

In this study, we demonstrate that the initial morphology of nanoparticles can be transformed into small fragmented nanoparticles, which were densely contacted to each other, during electrochemical CO 2 reduction reaction (CO 2 RR). Cu-based nanoparticles were directly grown on a carbon support by using cysteamine immobilization agent, and the synthesized nanoparticle catalyst showed increasing activity during initial CO 2 RR, doubling Faradaic efficiency of C 2 H 4 production from 27% to 57.3%. The increased C 2 H 4 production activity was related to the morphological transformation over reaction time. Twenty nm cubic Cu 2 O crystalline particles gradually experienced in situ electrochemical fragmentation into 2-4 nm small particles under the negative potential, and the fragmentation was found to be initiated from the surface of the nanocrystal. Compared to Cu@CuO nanoparticle/C or bulk Cu foil, the fragmented Cu-based NP/C catalyst achieved enhanced C 2+ production selectivity, accounting 87% of the total CO 2 RR products, and suppressed H 2 production. In-situ X-ray absorption near edge structure studies showed metallic Cu 0 state was observed under CO 2 RR, but the fragmented nanoparticles were more readily reoxidized at open circuit potential inside of the electrolyte, allowing labile Cu states. The unique morphology, small nanoparticles stacked upon on another, is proposed to promote C-C coupling reaction selectivity from CO 2 RR by suppressing HER.

Original languageEnglish
Pages (from-to)4624-4633
Number of pages10
JournalJournal of the American Chemical Society
Volume141
Issue number11
DOIs
Publication statusPublished - 2019 Mar 20

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Carbon Monoxide
Nanoparticles
Cysteamine
Catalysts
Catalyst selectivity
X ray absorption
Reaction products
Nanocrystals
Metal foil
Electrolytes
Immobilization
Carbon
Crystalline materials
X-Rays
Networks (circuits)

ASJC Scopus subject areas

  • Catalysis
  • Chemistry(all)
  • Biochemistry
  • Colloid and Surface Chemistry

Cite this

Electrochemical Fragmentation of Cu 2 O Nanoparticles Enhancing Selective C-C Coupling from CO 2 Reduction Reaction . / Jung, Hyejin; Lee, Si Young; Lee, Chan Woo; Cho, Min Kyung; Won, Da Hye; Kim, Cheonghee; Oh, Hyung Suk; Min, Byoung Koun; Hwang, Yun Jeong.

In: Journal of the American Chemical Society, Vol. 141, No. 11, 20.03.2019, p. 4624-4633.

Research output: Contribution to journalArticle

Jung, Hyejin ; Lee, Si Young ; Lee, Chan Woo ; Cho, Min Kyung ; Won, Da Hye ; Kim, Cheonghee ; Oh, Hyung Suk ; Min, Byoung Koun ; Hwang, Yun Jeong. / Electrochemical Fragmentation of Cu 2 O Nanoparticles Enhancing Selective C-C Coupling from CO 2 Reduction Reaction In: Journal of the American Chemical Society. 2019 ; Vol. 141, No. 11. pp. 4624-4633.
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abstract = "In this study, we demonstrate that the initial morphology of nanoparticles can be transformed into small fragmented nanoparticles, which were densely contacted to each other, during electrochemical CO 2 reduction reaction (CO 2 RR). Cu-based nanoparticles were directly grown on a carbon support by using cysteamine immobilization agent, and the synthesized nanoparticle catalyst showed increasing activity during initial CO 2 RR, doubling Faradaic efficiency of C 2 H 4 production from 27{\%} to 57.3{\%}. The increased C 2 H 4 production activity was related to the morphological transformation over reaction time. Twenty nm cubic Cu 2 O crystalline particles gradually experienced in situ electrochemical fragmentation into 2-4 nm small particles under the negative potential, and the fragmentation was found to be initiated from the surface of the nanocrystal. Compared to Cu@CuO nanoparticle/C or bulk Cu foil, the fragmented Cu-based NP/C catalyst achieved enhanced C 2+ production selectivity, accounting 87{\%} of the total CO 2 RR products, and suppressed H 2 production. In-situ X-ray absorption near edge structure studies showed metallic Cu 0 state was observed under CO 2 RR, but the fragmented nanoparticles were more readily reoxidized at open circuit potential inside of the electrolyte, allowing labile Cu states. The unique morphology, small nanoparticles stacked upon on another, is proposed to promote C-C coupling reaction selectivity from CO 2 RR by suppressing HER.",
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