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Title: The Preparation and Characterization of Co–Ni Nanoparticles and the Testing of a Heterogenized Co–Ni/Alumina Catalyst for CO Hydrogenation

Abstract

Samples of well-controlled nanoparticles consisting of alloys of cobalt and nickel of different atomic ratios were synthesized using wet chemical methods with oleylamine as the solvent and the reducing agent. These materials were characterized by a variety of techniques, including high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM), X-ray energy dispersive spectroscopy (EDS), and X-ray diffraction (XRD). Small amounts of heterogenized catalysts were prepared using alumina as the support. However, the potential for use of Co–Ni catalysts in CO hydrogenation was explored using a larger amount of Co–Ni/alumina catalyst prepared from standard aqueous impregnation methods and tested in a continuously stirred tank reactor (CSTR) for Fischer–Tropsch synthesis (FTS). Results are compared to a reference catalyst containing only cobalt. The heterogenized catalysts were characterized using synchrotron methods, including temperature programmed reduction with extended X-ray absorption fine structure spectroscopy and X-ray absorption near edge spectroscopy (TPR-EXAFS/XANES). The characterization results support intimate contact between Co and Ni, strongly suggesting alloy formation. In FTS testing, drawbacks of Ni addition included decreased CO conversion on a per gram catalyst basis, although Ni did not significantly impact the turnover number of cobalt, and produced slightly higher light gas selectivity. Benefits of Ni addition included an invertedmore » induction period relative to undoped Co/Al2O3, where CO conversion increased with time on-stream in the initial period, and the stabilization of cobalt nanoparticles at a lower weight % of Co.« less

Authors:
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [2];  [3];  [4];  [5];  [5];  [5];  [3]
  1. Univ. of Texas at San Antonio, TX (United States); Univ. Michoacana de San Nicolás de Hidalgo, Morelia, (Mexico)
  2. Univ. Nacional Autónoma de México (Mexico)
  3. Univ. of Texas at San Antonio, TX (United States)
  4. Univ. of Kentucky, Lexington, KY (United States)
  5. Argonne National Lab. (ANL), Argonne, IL (United States)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Fossil Energy (FE); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Contributing Org.:
[Consejo Nacional de Ciencia y Tecnologia (CONACYT)]
OSTI Identifier:
1600464
Grant/Contract Number:  
[AC02-06CH11357]
Resource Type:
Accepted Manuscript
Journal Name:
Catalysts
Additional Journal Information:
[ Journal Volume: 10; Journal Issue: 1]; Journal ID: ISSN 2073-4344
Publisher:
MDPI
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; CO hydrogenation; CSTR; Fischer–Tropsch synthesis; HAADF-STEM; TPR-EXAFS/XANES; alumina; cobalt; cobalt–nickel alloys; cobalt–nickel nanoparticles; nickel

Citation Formats

López-Tinoco, Julián, Mendoza-Cruz, Rubén, Bazán-Díaz, Lourdes, Karuturi, Sai Charan, Martinelli, Michela, Cronauer, Donald C., Kropf, A. Jeremy, Marshall, Christopher L., and Jacobs, Gary. The Preparation and Characterization of Co–Ni Nanoparticles and the Testing of a Heterogenized Co–Ni/Alumina Catalyst for CO Hydrogenation. United States: N. p., 2019. Web. doi:10.3390/catal10010018.
López-Tinoco, Julián, Mendoza-Cruz, Rubén, Bazán-Díaz, Lourdes, Karuturi, Sai Charan, Martinelli, Michela, Cronauer, Donald C., Kropf, A. Jeremy, Marshall, Christopher L., & Jacobs, Gary. The Preparation and Characterization of Co–Ni Nanoparticles and the Testing of a Heterogenized Co–Ni/Alumina Catalyst for CO Hydrogenation. United States. doi:10.3390/catal10010018.
López-Tinoco, Julián, Mendoza-Cruz, Rubén, Bazán-Díaz, Lourdes, Karuturi, Sai Charan, Martinelli, Michela, Cronauer, Donald C., Kropf, A. Jeremy, Marshall, Christopher L., and Jacobs, Gary. Sat . "The Preparation and Characterization of Co–Ni Nanoparticles and the Testing of a Heterogenized Co–Ni/Alumina Catalyst for CO Hydrogenation". United States. doi:10.3390/catal10010018. https://www.osti.gov/servlets/purl/1600464.
@article{osti_1600464,
title = {The Preparation and Characterization of Co–Ni Nanoparticles and the Testing of a Heterogenized Co–Ni/Alumina Catalyst for CO Hydrogenation},
author = {López-Tinoco, Julián and Mendoza-Cruz, Rubén and Bazán-Díaz, Lourdes and Karuturi, Sai Charan and Martinelli, Michela and Cronauer, Donald C. and Kropf, A. Jeremy and Marshall, Christopher L. and Jacobs, Gary},
abstractNote = {Samples of well-controlled nanoparticles consisting of alloys of cobalt and nickel of different atomic ratios were synthesized using wet chemical methods with oleylamine as the solvent and the reducing agent. These materials were characterized by a variety of techniques, including high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM), X-ray energy dispersive spectroscopy (EDS), and X-ray diffraction (XRD). Small amounts of heterogenized catalysts were prepared using alumina as the support. However, the potential for use of Co–Ni catalysts in CO hydrogenation was explored using a larger amount of Co–Ni/alumina catalyst prepared from standard aqueous impregnation methods and tested in a continuously stirred tank reactor (CSTR) for Fischer–Tropsch synthesis (FTS). Results are compared to a reference catalyst containing only cobalt. The heterogenized catalysts were characterized using synchrotron methods, including temperature programmed reduction with extended X-ray absorption fine structure spectroscopy and X-ray absorption near edge spectroscopy (TPR-EXAFS/XANES). The characterization results support intimate contact between Co and Ni, strongly suggesting alloy formation. In FTS testing, drawbacks of Ni addition included decreased CO conversion on a per gram catalyst basis, although Ni did not significantly impact the turnover number of cobalt, and produced slightly higher light gas selectivity. Benefits of Ni addition included an inverted induction period relative to undoped Co/Al2O3, where CO conversion increased with time on-stream in the initial period, and the stabilization of cobalt nanoparticles at a lower weight % of Co.},
doi = {10.3390/catal10010018},
journal = {Catalysts},
number = [1],
volume = [10],
place = {United States},
year = {2019},
month = {12}
}

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