Synthesis of monocarboxylic acids via direct CO2conversion over Ni-Zn intermetallic catalysts

Malayil Gopalan Sibi, Deepak Verma, Handi Cayadi Setiyadi, Muhammad Kashif Khan, Neha Karanwal, Sang Kyu Kwak, Kyung Yoon Chung, Jae Ho Park, Daseul Han, Kyung Wan Nam, Jaehoon Kim

Research output: Contribution to journalArticlepeer-review

48 Scopus citations

Abstract

The direct conversion of CO2 to methane, gasoline-to-diesel range fuels, methanol, and light olefins using sustainable hydrogen sources is considered a promising approach for mitigating global warming. Nevertheless, the direct conversion of CO2 to high value-added chemicals, such as acetic acid and propionic acid (AA and PA, respectively), has not been explored to date. Herein, we report a Ni-Zn intermetallic/Zn-rich NixZnyO catalyst that directly converted CO2 to AA and PA with an overall selectivity of 77.1% at a CO2 conversion of 13.4% at 325 °C. The surface restructuring of the ZnO and NiO phases during calcination and subsequent reduction led to the formation of a Ni-Zn intermetallic on the Zn-rich NixZnyO phase. Surface-adsorbed (∗CHx)n species were formed via the reverse water gas shift reaction and subsequent CO hydrogenation. Afterward, monocarboxylic acids were produced via the direct insertion of CO2 into the (∗CHx)n species and subsequent hydrogenation. The synthesis of monocarboxylic acid was highly stable up to 216 h on-stream over the Ni-Zn intermetallic catalyst, and the catalyst maintained its phase structure and morphology during long-term CO2 hydrogenation. The high selectivity toward monocarboxylic acids and high stability of the Ni-Zn intermetallic demonstrated its high potential for the conversion of CO2 into value-added chemicals.

Original languageEnglish
Pages (from-to)8382-8398
Number of pages17
JournalACS Catalysis
Volume11
DOIs
StatePublished - 2021

Keywords

  • Acetic acid
  • CO
  • Hydrogenation
  • Intermetallic phase
  • Ni-Zn
  • Propionic acid

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