Promotional effect of Au on reduction of Ni(II) to form Au-Ni alloy catalysts for hydrogenolysis of benzylic alcohols

Hiroaki Nishikawa, Daisuke Kawamoto, Yusuke Yamamoto, Tamao Ishida, Hironori Ohashi, Tomoki Akita, Tetsuo Honma, Hiroshi Oji, Yasuhiro Kobayashi, Akiyuki Hamasaki, Takushi Yokoyama, Makoto Tokunaga

Research output: Contribution to journalArticle

18 Citations (Scopus)

Abstract

Gold-nickel bimetallic catalysts were prepared from Au/NiO and Au(OH) 3-Ni(OH)2-NiCO3 coprecipitates by treatment with hydrogen. Gold promoted the reduction of Ni(II) to Ni(0) at relatively low temperatures in the range of 100-150 C, which was confirmed by H2-TPR and in situ XAFS measurements, whereas NiO without Au was not fully reduced even at 300 C. The obtained catalysts were characterized by XRD, HAADF-STEM, XAFS, and 197Au Mössbauer, and these analyses revealed the formation of Au-Ni alloy components in the obtained catalysts. Au existed as Au nanoparticles together with Au-Ni alloy components in Au-Ni-1 prepared from Au/NiO by H2 treatment. When Au(OH)3-Ni(OH) 2-NiCO3 was treated in a flow of H2 to produce Au-Ni-2, the formation of Au NPs was not clearly observed, thereby meaning that Au atoms were highly dispersed as a single atom and/or small clusters in the obtained catalysts. Moreover, most of the Au atoms were alloyed with Ni atoms for Au-Ni-2. The obtained Au-Ni-1 and Au-Ni-2 exhibited superior catalytic activities for the selective hydrogenolysis of benzylic alcohols into alkylbenzene derivatives in terms of reaction rates normalized by catalyst surface area. Accordingly, Au-Ni-1 and Au-Ni-2 recorded the reaction rates of 4.79 and 9.79 mmol L-1 h-1 m-2, respectively. These values were greater than that obtained for Raney Ni (0.14 mmol L -1 h-1 m-2). In addition, Au-Ni-2, which contains higher Au-Ni alloy content, showed greater reaction rates when compared to Au-Ni-1. Since Au/TiO2 showed poor catalytic activity for the hydrogenolysis, Au-Ni alloy enhanced the catalytic activities of Ni(0).

Original languageEnglish
Pages (from-to)254-264
Number of pages11
JournalJournal of Catalysis
Volume307
DOIs
Publication statusPublished - Sep 11 2013

Fingerprint

hydrogenolysis
Hydrogenolysis
alcohols
Alcohols
catalysts
Catalysts
Reaction rates
catalytic activity
Catalyst activity
Atoms
reaction kinetics
Gold
atoms
gold
in situ measurement
Nickel
Hydrogen
nickel
Nanoparticles
Derivatives

All Science Journal Classification (ASJC) codes

  • Catalysis
  • Physical and Theoretical Chemistry

Cite this

Promotional effect of Au on reduction of Ni(II) to form Au-Ni alloy catalysts for hydrogenolysis of benzylic alcohols. / Nishikawa, Hiroaki; Kawamoto, Daisuke; Yamamoto, Yusuke; Ishida, Tamao; Ohashi, Hironori; Akita, Tomoki; Honma, Tetsuo; Oji, Hiroshi; Kobayashi, Yasuhiro; Hamasaki, Akiyuki; Yokoyama, Takushi; Tokunaga, Makoto.

In: Journal of Catalysis, Vol. 307, 11.09.2013, p. 254-264.

Research output: Contribution to journalArticle

Nishikawa, H, Kawamoto, D, Yamamoto, Y, Ishida, T, Ohashi, H, Akita, T, Honma, T, Oji, H, Kobayashi, Y, Hamasaki, A, Yokoyama, T & Tokunaga, M 2013, 'Promotional effect of Au on reduction of Ni(II) to form Au-Ni alloy catalysts for hydrogenolysis of benzylic alcohols', Journal of Catalysis, vol. 307, pp. 254-264. https://doi.org/10.1016/j.jcat.2013.07.027
Nishikawa, Hiroaki ; Kawamoto, Daisuke ; Yamamoto, Yusuke ; Ishida, Tamao ; Ohashi, Hironori ; Akita, Tomoki ; Honma, Tetsuo ; Oji, Hiroshi ; Kobayashi, Yasuhiro ; Hamasaki, Akiyuki ; Yokoyama, Takushi ; Tokunaga, Makoto. / Promotional effect of Au on reduction of Ni(II) to form Au-Ni alloy catalysts for hydrogenolysis of benzylic alcohols. In: Journal of Catalysis. 2013 ; Vol. 307. pp. 254-264.
@article{58a990fde47e493ebd01492a359d002e,
title = "Promotional effect of Au on reduction of Ni(II) to form Au-Ni alloy catalysts for hydrogenolysis of benzylic alcohols",
abstract = "Gold-nickel bimetallic catalysts were prepared from Au/NiO and Au(OH) 3-Ni(OH)2-NiCO3 coprecipitates by treatment with hydrogen. Gold promoted the reduction of Ni(II) to Ni(0) at relatively low temperatures in the range of 100-150 C, which was confirmed by H2-TPR and in situ XAFS measurements, whereas NiO without Au was not fully reduced even at 300 C. The obtained catalysts were characterized by XRD, HAADF-STEM, XAFS, and 197Au M{\"o}ssbauer, and these analyses revealed the formation of Au-Ni alloy components in the obtained catalysts. Au existed as Au nanoparticles together with Au-Ni alloy components in Au-Ni-1 prepared from Au/NiO by H2 treatment. When Au(OH)3-Ni(OH) 2-NiCO3 was treated in a flow of H2 to produce Au-Ni-2, the formation of Au NPs was not clearly observed, thereby meaning that Au atoms were highly dispersed as a single atom and/or small clusters in the obtained catalysts. Moreover, most of the Au atoms were alloyed with Ni atoms for Au-Ni-2. The obtained Au-Ni-1 and Au-Ni-2 exhibited superior catalytic activities for the selective hydrogenolysis of benzylic alcohols into alkylbenzene derivatives in terms of reaction rates normalized by catalyst surface area. Accordingly, Au-Ni-1 and Au-Ni-2 recorded the reaction rates of 4.79 and 9.79 mmol L-1 h-1 m-2, respectively. These values were greater than that obtained for Raney Ni (0.14 mmol L -1 h-1 m-2). In addition, Au-Ni-2, which contains higher Au-Ni alloy content, showed greater reaction rates when compared to Au-Ni-1. Since Au/TiO2 showed poor catalytic activity for the hydrogenolysis, Au-Ni alloy enhanced the catalytic activities of Ni(0).",
author = "Hiroaki Nishikawa and Daisuke Kawamoto and Yusuke Yamamoto and Tamao Ishida and Hironori Ohashi and Tomoki Akita and Tetsuo Honma and Hiroshi Oji and Yasuhiro Kobayashi and Akiyuki Hamasaki and Takushi Yokoyama and Makoto Tokunaga",
year = "2013",
month = "9",
day = "11",
doi = "10.1016/j.jcat.2013.07.027",
language = "English",
volume = "307",
pages = "254--264",
journal = "Journal of Catalysis",
issn = "0021-9517",
publisher = "Academic Press Inc.",

}

TY - JOUR

T1 - Promotional effect of Au on reduction of Ni(II) to form Au-Ni alloy catalysts for hydrogenolysis of benzylic alcohols

AU - Nishikawa, Hiroaki

AU - Kawamoto, Daisuke

AU - Yamamoto, Yusuke

AU - Ishida, Tamao

AU - Ohashi, Hironori

AU - Akita, Tomoki

AU - Honma, Tetsuo

AU - Oji, Hiroshi

AU - Kobayashi, Yasuhiro

AU - Hamasaki, Akiyuki

AU - Yokoyama, Takushi

AU - Tokunaga, Makoto

PY - 2013/9/11

Y1 - 2013/9/11

N2 - Gold-nickel bimetallic catalysts were prepared from Au/NiO and Au(OH) 3-Ni(OH)2-NiCO3 coprecipitates by treatment with hydrogen. Gold promoted the reduction of Ni(II) to Ni(0) at relatively low temperatures in the range of 100-150 C, which was confirmed by H2-TPR and in situ XAFS measurements, whereas NiO without Au was not fully reduced even at 300 C. The obtained catalysts were characterized by XRD, HAADF-STEM, XAFS, and 197Au Mössbauer, and these analyses revealed the formation of Au-Ni alloy components in the obtained catalysts. Au existed as Au nanoparticles together with Au-Ni alloy components in Au-Ni-1 prepared from Au/NiO by H2 treatment. When Au(OH)3-Ni(OH) 2-NiCO3 was treated in a flow of H2 to produce Au-Ni-2, the formation of Au NPs was not clearly observed, thereby meaning that Au atoms were highly dispersed as a single atom and/or small clusters in the obtained catalysts. Moreover, most of the Au atoms were alloyed with Ni atoms for Au-Ni-2. The obtained Au-Ni-1 and Au-Ni-2 exhibited superior catalytic activities for the selective hydrogenolysis of benzylic alcohols into alkylbenzene derivatives in terms of reaction rates normalized by catalyst surface area. Accordingly, Au-Ni-1 and Au-Ni-2 recorded the reaction rates of 4.79 and 9.79 mmol L-1 h-1 m-2, respectively. These values were greater than that obtained for Raney Ni (0.14 mmol L -1 h-1 m-2). In addition, Au-Ni-2, which contains higher Au-Ni alloy content, showed greater reaction rates when compared to Au-Ni-1. Since Au/TiO2 showed poor catalytic activity for the hydrogenolysis, Au-Ni alloy enhanced the catalytic activities of Ni(0).

AB - Gold-nickel bimetallic catalysts were prepared from Au/NiO and Au(OH) 3-Ni(OH)2-NiCO3 coprecipitates by treatment with hydrogen. Gold promoted the reduction of Ni(II) to Ni(0) at relatively low temperatures in the range of 100-150 C, which was confirmed by H2-TPR and in situ XAFS measurements, whereas NiO without Au was not fully reduced even at 300 C. The obtained catalysts were characterized by XRD, HAADF-STEM, XAFS, and 197Au Mössbauer, and these analyses revealed the formation of Au-Ni alloy components in the obtained catalysts. Au existed as Au nanoparticles together with Au-Ni alloy components in Au-Ni-1 prepared from Au/NiO by H2 treatment. When Au(OH)3-Ni(OH) 2-NiCO3 was treated in a flow of H2 to produce Au-Ni-2, the formation of Au NPs was not clearly observed, thereby meaning that Au atoms were highly dispersed as a single atom and/or small clusters in the obtained catalysts. Moreover, most of the Au atoms were alloyed with Ni atoms for Au-Ni-2. The obtained Au-Ni-1 and Au-Ni-2 exhibited superior catalytic activities for the selective hydrogenolysis of benzylic alcohols into alkylbenzene derivatives in terms of reaction rates normalized by catalyst surface area. Accordingly, Au-Ni-1 and Au-Ni-2 recorded the reaction rates of 4.79 and 9.79 mmol L-1 h-1 m-2, respectively. These values were greater than that obtained for Raney Ni (0.14 mmol L -1 h-1 m-2). In addition, Au-Ni-2, which contains higher Au-Ni alloy content, showed greater reaction rates when compared to Au-Ni-1. Since Au/TiO2 showed poor catalytic activity for the hydrogenolysis, Au-Ni alloy enhanced the catalytic activities of Ni(0).

UR - http://www.scopus.com/inward/record.url?scp=84883511211&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=84883511211&partnerID=8YFLogxK

U2 - 10.1016/j.jcat.2013.07.027

DO - 10.1016/j.jcat.2013.07.027

M3 - Article

AN - SCOPUS:84883511211

VL - 307

SP - 254

EP - 264

JO - Journal of Catalysis

JF - Journal of Catalysis

SN - 0021-9517

ER -