Bimetallic Pt-Re Nanoporous Networks: Synthesis, Characterization, and Catalytic Reactivity

Sally Nijem; Shahar Dery; Mazal Carmiel; Gal Horesh; Jan Garrevoet; Kathryn Spiers; Gerald Falkenberg; Carlo Marini; Elad Gross

doi:10.1021/acs.jpcc.8b07863

Bimetallic Pt-Re Nanoporous Networks: Synthesis, Characterization, and Catalytic Reactivity

Sally Nijem, Shahar Dery, Mazal Carmiel, Gal Horesh, Jan Garrevoet, Kathryn Spiers, Gerald Falkenberg, Carlo Marini, Elad Gross^*

^*Corresponding author for this work

Institute of Chemistry

Research output: Contribution to journal › Article › peer-review

13 Scopus citations

Abstract

The preparation of bimetallic nanoporous networks (BNNs) that combine the high surface area and thermal stability of inorganic nanostructures with the unique catalytic properties of bimetallic systems is highly desirable. Here we show a simple and highly versatile approach for synthesis of Pt-Re BNN and demonstrate the influence of preparation conditions on the BNN structure, composition, and catalytic reactivity. Pt-Re BNN was prepared by reduction of double complex [Pt(NH₃)₄][Re(Cl₆)] salt crystals, in which two oppositely charged metal complexes are evenly distributed in each unit cell in a 1:1 ratio. Exposure of the salt crystals to reducing conditions induced the evaporation of the inorganic ligands, collapse of the salt structure, and reduction of the metal ions for the formation of high-surface-area Pt-Re BNNs. Single-particle X-ray fluorescence tomography and various ensemble-based spectroscopy measurements (X-ray photoelectron spectroscopy and X-ray absorption near edge spectroscopy) identified that the bulk and surface compositions of the bimetallic structure and the oxidation state of the two metals can be tuned by adjusting the reduction temperature of the bimetallic salt. Pt-Re BNN showed reactivity in deoxydehydration reaction of glycerol toward the selective formation of allyl alcohol. Combination of reactivity and spectroscopic measurements revealed that enhanced reactivity was correlated to the presence of highly oxidized Re species (mostly Re⁷⁺) and equal distribution of Pt and Re on the BNN surface.

Original language	American English
Pages (from-to)	24801-24808
Number of pages	8
Journal	Journal of Physical Chemistry C
Volume	122
Issue number	43
DOIs	https://doi.org/10.1021/acs.jpcc.8b07863
State	Published - 1 Nov 2018

Bibliographical note

Funding Information:
X-ray tomography measurements were carried out on beamline P06 at Petra III at DESY, a member of the Helmholtz Association (HGF). X-ray absorption experiments were performed at CLAESS beamline at ALBA Synchrotron. S.D. acknowledges the Israeli Ministry of Energy and the Rudin fellowship for their financial support. Avishai Barnoy is acknowledged for his assistance in analysis of the X-ray tomography images.

Publisher Copyright:
Copyright © 2018 American Chemical Society.

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@article{0e2870e9829c4f3bb81f305334a7a66c,

title = "Bimetallic Pt-Re Nanoporous Networks: Synthesis, Characterization, and Catalytic Reactivity",

abstract = "The preparation of bimetallic nanoporous networks (BNNs) that combine the high surface area and thermal stability of inorganic nanostructures with the unique catalytic properties of bimetallic systems is highly desirable. Here we show a simple and highly versatile approach for synthesis of Pt-Re BNN and demonstrate the influence of preparation conditions on the BNN structure, composition, and catalytic reactivity. Pt-Re BNN was prepared by reduction of double complex [Pt(NH3)4][Re(Cl6)] salt crystals, in which two oppositely charged metal complexes are evenly distributed in each unit cell in a 1:1 ratio. Exposure of the salt crystals to reducing conditions induced the evaporation of the inorganic ligands, collapse of the salt structure, and reduction of the metal ions for the formation of high-surface-area Pt-Re BNNs. Single-particle X-ray fluorescence tomography and various ensemble-based spectroscopy measurements (X-ray photoelectron spectroscopy and X-ray absorption near edge spectroscopy) identified that the bulk and surface compositions of the bimetallic structure and the oxidation state of the two metals can be tuned by adjusting the reduction temperature of the bimetallic salt. Pt-Re BNN showed reactivity in deoxydehydration reaction of glycerol toward the selective formation of allyl alcohol. Combination of reactivity and spectroscopic measurements revealed that enhanced reactivity was correlated to the presence of highly oxidized Re species (mostly Re7+) and equal distribution of Pt and Re on the BNN surface.",

author = "Sally Nijem and Shahar Dery and Mazal Carmiel and Gal Horesh and Jan Garrevoet and Kathryn Spiers and Gerald Falkenberg and Carlo Marini and Elad Gross",

note = "Funding Information: X-ray tomography measurements were carried out on beamline P06 at Petra III at DESY, a member of the Helmholtz Association (HGF). X-ray absorption experiments were performed at CLAESS beamline at ALBA Synchrotron. S.D. acknowledges the Israeli Ministry of Energy and the Rudin fellowship for their financial support. Avishai Barnoy is acknowledged for his assistance in analysis of the X-ray tomography images. Publisher Copyright: Copyright {\textcopyright} 2018 American Chemical Society.",

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doi = "10.1021/acs.jpcc.8b07863",

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AU - Nijem, Sally

AU - Dery, Shahar

AU - Carmiel, Mazal

AU - Horesh, Gal

AU - Garrevoet, Jan

AU - Spiers, Kathryn

AU - Falkenberg, Gerald

AU - Marini, Carlo

AU - Gross, Elad

N1 - Funding Information: X-ray tomography measurements were carried out on beamline P06 at Petra III at DESY, a member of the Helmholtz Association (HGF). X-ray absorption experiments were performed at CLAESS beamline at ALBA Synchrotron. S.D. acknowledges the Israeli Ministry of Energy and the Rudin fellowship for their financial support. Avishai Barnoy is acknowledged for his assistance in analysis of the X-ray tomography images. Publisher Copyright: Copyright © 2018 American Chemical Society.

PY - 2018/11/1

Y1 - 2018/11/1

N2 - The preparation of bimetallic nanoporous networks (BNNs) that combine the high surface area and thermal stability of inorganic nanostructures with the unique catalytic properties of bimetallic systems is highly desirable. Here we show a simple and highly versatile approach for synthesis of Pt-Re BNN and demonstrate the influence of preparation conditions on the BNN structure, composition, and catalytic reactivity. Pt-Re BNN was prepared by reduction of double complex [Pt(NH3)4][Re(Cl6)] salt crystals, in which two oppositely charged metal complexes are evenly distributed in each unit cell in a 1:1 ratio. Exposure of the salt crystals to reducing conditions induced the evaporation of the inorganic ligands, collapse of the salt structure, and reduction of the metal ions for the formation of high-surface-area Pt-Re BNNs. Single-particle X-ray fluorescence tomography and various ensemble-based spectroscopy measurements (X-ray photoelectron spectroscopy and X-ray absorption near edge spectroscopy) identified that the bulk and surface compositions of the bimetallic structure and the oxidation state of the two metals can be tuned by adjusting the reduction temperature of the bimetallic salt. Pt-Re BNN showed reactivity in deoxydehydration reaction of glycerol toward the selective formation of allyl alcohol. Combination of reactivity and spectroscopic measurements revealed that enhanced reactivity was correlated to the presence of highly oxidized Re species (mostly Re7+) and equal distribution of Pt and Re on the BNN surface.

AB - The preparation of bimetallic nanoporous networks (BNNs) that combine the high surface area and thermal stability of inorganic nanostructures with the unique catalytic properties of bimetallic systems is highly desirable. Here we show a simple and highly versatile approach for synthesis of Pt-Re BNN and demonstrate the influence of preparation conditions on the BNN structure, composition, and catalytic reactivity. Pt-Re BNN was prepared by reduction of double complex [Pt(NH3)4][Re(Cl6)] salt crystals, in which two oppositely charged metal complexes are evenly distributed in each unit cell in a 1:1 ratio. Exposure of the salt crystals to reducing conditions induced the evaporation of the inorganic ligands, collapse of the salt structure, and reduction of the metal ions for the formation of high-surface-area Pt-Re BNNs. Single-particle X-ray fluorescence tomography and various ensemble-based spectroscopy measurements (X-ray photoelectron spectroscopy and X-ray absorption near edge spectroscopy) identified that the bulk and surface compositions of the bimetallic structure and the oxidation state of the two metals can be tuned by adjusting the reduction temperature of the bimetallic salt. Pt-Re BNN showed reactivity in deoxydehydration reaction of glycerol toward the selective formation of allyl alcohol. Combination of reactivity and spectroscopic measurements revealed that enhanced reactivity was correlated to the presence of highly oxidized Re species (mostly Re7+) and equal distribution of Pt and Re on the BNN surface.

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DO - 10.1021/acs.jpcc.8b07863

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EP - 24808

JO - Journal of Physical Chemistry C

JF - Journal of Physical Chemistry C

IS - 43

ER -

Bimetallic Pt-Re Nanoporous Networks: Synthesis, Characterization, and Catalytic Reactivity

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