Porous Nanocrystalline Silicon Supported Bimetallic Pd-Au Catalysts: Preparation, Characterization, and Direct Hydrogen Peroxide Synthesis
Full article
| Общее |
Language:
Английский,
Genre:
Full article,
Status:
Published,
Source type:
Original
|
| Journal |
Frontiers in Chemistry
ISSN: 2296-2646
|
| Output data |
Year: 2018,
Volume: 6,
Article number
: 85,
Pages count
: 13
DOI:
10.3389/fchem.2018.00085
|
| Tags |
Alloy nanoparticles, Bimetallic nanoparticles, Direct H2O2 synthesis, Direct hydrogen peroxide synthesis, Double complex salts, Gold-palladium catalysts, Pd-Au catalysts, Porous silicon |
| Authors |
Potemkin Dmitriy I.
1,2
,
Maslov Dmitry K.
2
,
Loponov Konstantin
3
,
Snytnikov Pavel V.
1,2
,
Shubin Yuri V.
1,4
,
Plyusnin Pavel E.
1,4
,
Svintsitskiy Dmitry A.
1,2
,
Sobyanin Vladimir A.
2
,
Lapkin Alexei A.
3,5
|
| Affiliations |
| 1 |
Laboratory of the Energy-Efficient Catalytic Processes, Novosibirsk State University, Novosibirsk, Russia
|
| 2 |
Department of Heterogeneous Catalysis, Boreskov Institute of Catalysis, Novosibirsk, Russia
|
| 3 |
Department of Chemical Engineering and Biotechnology, University of Cambridge, Cambridge, United Kingdom
|
| 4 |
Laboratory of the Rare Platinum Metals Chemistry, Nikolaev Institute of Inorganic Chemistry, Novosibirsk, Russia
|
| 5 |
Cambridge Centre for Advanced Research and Education in Singapore Ltd., Singapore, Singapore
|
|
Funding (2)
|
1
|
Russian Foundation for Basic Research
|
16-33-60106
|
|
2
|
National Research Foundation of Singapore
|
|
Bimetallic Pd-Au catalysts were prepared on the porous nanocrystalline silicon (PSi) for the first time. The catalysts were tested in the reaction of direct hydrogen peroxide synthesis and characterized by standard structural and chemical techniques. It was shown that the Pd-Au/PSi catalyst prepared from conventional H-2[PdCl4] and H[AuCl4] precursors contains monometallic Pd and a range of different Pd-Au alloy nanoparticles over the oxidized PSi surface. The PdAu2/PSi catalyst prepared from the {Pd(NH3)(4)]{AuCl4](2) double complex salt (DCS) single-source precursor predominantly contains bimetallic Pd-Au alloy nanoparticles. For both catalysts the surface of bimetallic nanoparticles is Pd-enriched and contains palladium in Pd-0 and Pd2+ states. Among the catalysts studied, the PdAu2/PSi catalyst was the most active and selective in the direct H2O2 synthesis with H2O2 productivity of 0.5mol g(Pd)(-1) h(-1) at selectivity of 50% and H2O2 concentration of 0.023M in 0.03M H2SO4-methanol solution after 5 h on stream at -10 degrees C and atmospheric pressure. This performance is due to high activity in the H2O2 synthesis reaction and low activities in the undesirable H2O2 decomposition and hydrogenation reactions. Good performance of the PdAu2/PSi catalyst was associated with the major part of Pd in the catalyst being in the form of the bimetallic Pd-Au nanoparticles. Porous silicon was concluded to be a promising catalytic support for direct hydrogen peroxide synthesis due to its inertness with respect to undesirable side reactions, high thermal stability, and conductivity, possibility of safe operation at high temperatures and pressures and a well-established manufacturing process.