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Title: State of Supported Nickel Nanoparticles during Catalysis in Aqueous Media

Abstract

The state of Ni supported on HZSM-5 zeolite, silica, and sulfonated carbon was determined during aqueous phase catalysis of phenol hydrodeoxygenation using in situ extended X-ray absorption fine structure spectroscopy (EXAFS). On sulfonated carbon and HZSM-5 supports, the NiO and Ni(OH)2 were readily reduced to Ni(0) under reaction conditions (~35 bar H2 in aqueous phenol solutions containing up to 0.5 wt. % phosphoric acid at 473 K). On the silica support, less than 70% of the Ni was converted to Ni(0) under reaction conditions, which is attributed to the formation of Ni phyllosilicates. Over a broad range of reaction conditions there was no leaching of Ni from the supports. In contrast, rapid leaching of the Ni(II) from HZSM-5 was observed, when 15 wt. % aqueous acetic acid was substituted for the aqueous phenol solution. Once the metallic state of Ni was established there was no leaching in 15 wt. % acetic acid at 473 K and 35 bar H2. This work was supported by the U.S. Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences (BES), Division of Chemical Sciences, Geosciences & Biosciences. The STEM was supported under the Laboratory Directed Research and Development Program: Chemical Imagingmore » Initiative at Pacific Northwest National Laboratory (PNNL), a multi-program national laboratory operated for DOE by Battelle under Contract DE-AC05-76RL01830. STEM was performed at EMSL, a DOE Office of Science user facility sponsored by the Office of Biological and Environmental Research and located at PNNL.« less

Authors:
; ; ; ; ; ; ; ; ;
Publication Date:
Research Org.:
Pacific Northwest National Laboratory (PNNL), Richland, WA (US), Environmental Molecular Sciences Laboratory (EMSL)
Sponsoring Org.:
USDOE
OSTI Identifier:
1233763
Report Number(s):
PNNL-SA-107104
Journal ID: ISSN 1521-3765; 48810; KC0302010
DOE Contract Number:  
AC05-76RL01830
Resource Type:
Journal Article
Journal Name:
Chemistry - A European Journal (Online)
Additional Journal Information:
Journal Volume: 21; Journal Issue: 46; Journal ID: ISSN 1521-3765
Publisher:
ChemPubSoc Europe
Country of Publication:
United States
Language:
English
Subject:
in situ EXAFS; hydrogenation; nanoparticles; XANES; nickel silicate; Environmental Molecular Sciences Laboratory

Citation Formats

Chase, Zizwe, Kasakov, Stanislav, Shi, Hui, Vjunov, Aleksei, Fulton, John L., Camaioni, Donald M., Balasubramanian, Mahalingam, Zhao, Chen, Wang, Yong, and Lercher, Johannes A. State of Supported Nickel Nanoparticles during Catalysis in Aqueous Media. United States: N. p., 2015. Web. doi:10.1002/chem.201502723.
Chase, Zizwe, Kasakov, Stanislav, Shi, Hui, Vjunov, Aleksei, Fulton, John L., Camaioni, Donald M., Balasubramanian, Mahalingam, Zhao, Chen, Wang, Yong, & Lercher, Johannes A. State of Supported Nickel Nanoparticles during Catalysis in Aqueous Media. United States. doi:10.1002/chem.201502723.
Chase, Zizwe, Kasakov, Stanislav, Shi, Hui, Vjunov, Aleksei, Fulton, John L., Camaioni, Donald M., Balasubramanian, Mahalingam, Zhao, Chen, Wang, Yong, and Lercher, Johannes A. Mon . "State of Supported Nickel Nanoparticles during Catalysis in Aqueous Media". United States. doi:10.1002/chem.201502723.
@article{osti_1233763,
title = {State of Supported Nickel Nanoparticles during Catalysis in Aqueous Media},
author = {Chase, Zizwe and Kasakov, Stanislav and Shi, Hui and Vjunov, Aleksei and Fulton, John L. and Camaioni, Donald M. and Balasubramanian, Mahalingam and Zhao, Chen and Wang, Yong and Lercher, Johannes A.},
abstractNote = {The state of Ni supported on HZSM-5 zeolite, silica, and sulfonated carbon was determined during aqueous phase catalysis of phenol hydrodeoxygenation using in situ extended X-ray absorption fine structure spectroscopy (EXAFS). On sulfonated carbon and HZSM-5 supports, the NiO and Ni(OH)2 were readily reduced to Ni(0) under reaction conditions (~35 bar H2 in aqueous phenol solutions containing up to 0.5 wt. % phosphoric acid at 473 K). On the silica support, less than 70% of the Ni was converted to Ni(0) under reaction conditions, which is attributed to the formation of Ni phyllosilicates. Over a broad range of reaction conditions there was no leaching of Ni from the supports. In contrast, rapid leaching of the Ni(II) from HZSM-5 was observed, when 15 wt. % aqueous acetic acid was substituted for the aqueous phenol solution. Once the metallic state of Ni was established there was no leaching in 15 wt. % acetic acid at 473 K and 35 bar H2. This work was supported by the U.S. Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences (BES), Division of Chemical Sciences, Geosciences & Biosciences. The STEM was supported under the Laboratory Directed Research and Development Program: Chemical Imaging Initiative at Pacific Northwest National Laboratory (PNNL), a multi-program national laboratory operated for DOE by Battelle under Contract DE-AC05-76RL01830. STEM was performed at EMSL, a DOE Office of Science user facility sponsored by the Office of Biological and Environmental Research and located at PNNL.},
doi = {10.1002/chem.201502723},
journal = {Chemistry - A European Journal (Online)},
issn = {1521-3765},
number = 46,
volume = 21,
place = {United States},
year = {2015},
month = {11}
}