Carbon Nanosphere-Encapsulated Fe Core–Shell Structures for Catalytic CO2 Hydrogenation

Weber, Daniel; Rui, Ning; Zhang, Feng; Zhang, Heng; Vovchok, Dimitriy; Wildy, Michael; Arizapana, Kevin; Saporita, Alexa; Zhang, Jin Zhong; Senanayake, Sanjaya D.; Lu, Ping; Zhang, Cheng

doi:10.1021/acsanm.2c02602

Title: Carbon Nanosphere-Encapsulated Fe Core–Shell Structures for Catalytic CO₂ Hydrogenation

Journal Article · 01 August 2022 · ACS Applied Nano Materials

DOI: https://doi.org/10.1021/acsanm.2c02602 · OSTI ID:1893764

Weber, Daniel ^[1];

^[2]; Zhang, Feng ^[2]; Zhang, Heng ^[3];

^[2]; Wildy, Michael ^[4];

^[4]; Saporita, Alexa ^[1];

^[3];

^[2]; Lu, Ping ^[4];

^[1]

Long Island University, Brookville, NY (United States)
Brookhaven National Lab. (BNL), Upton, NY (United States)
Univ. of California, Santa Cruz, CA (United States)
Rowan Univ., Glassboro, NJ (United States)

In this work, we synthesized a unique carbon nanosphere (CNS)-encapsulated Fe core–shell catalyst (CNS–Fe) for CO₂ hydrogenation. The synthesized CNS–Fe catalyst exhibited a core–shell structure with a core of ca. 40 nm containing iron species and a shell thickness of ca. 10 nm composed of mainly graphitic carbon. X-ray diffraction, X-ray photoelectron spectroscopy, Raman spectroscopy, and thermogravimetric analysis were used to characterize the fresh and spent CNS–Fe catalysts and reveal a mixture of Fe₃O₄, metallic Fe, and Fe₅C₂ in the core and graphitic carbon as the shell with defect sites. Hydrogen temperature-programmed reduction, X-ray absorption near-edge structure, and extended X-ray absorption fine structure for the fresh CNS–Fe confirmed the composition of the iron species encapsulated in the CNS. The catalytic performance of CNS–Fe was investigated at ambient pressure for CO2 hydrogenation with hydrocarbons (CH₄, C₂–C₄⁼, C₂–C₄⁰), and CO was observed as the main product.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Workforce Development for Teachers and Scientists (WDTS)

Grant/Contract Number:: SC0012704

OSTI ID:: 1893764

Report Number(s):: BNL-223591-2022-JAAM

Journal Information:: ACS Applied Nano Materials, Journal Name: ACS Applied Nano Materials Journal Issue: 8 Vol. 5; ISSN 2574-0970

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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36 MATERIALS SCIENCE
CO2 hydrogenation
carbon nanosphere encapsulated iron
core-shell structure
light olefins
nano-reactor

Title: Carbon Nanosphere-Encapsulated Fe Core–Shell Structures for Catalytic CO2 Hydrogenation

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Title: Carbon Nanosphere-Encapsulated Fe Core–Shell Structures for Catalytic CO₂ Hydrogenation