Platinum(IV) Carbonato Complexes: Formation via the Addition of CO2 to the [Pt(OH)6]2– Anion and Generation of Platinum(IV) Oxide Nanoparticles for the Preparation of Catalysts Full article
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Inorganic Chemistry
ISSN: 0020-1669 , E-ISSN: 1520-510X |
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| Output data | Year: 2023, Volume: 62, Number: 64, Pages: 9732–9748 Pages count : 17 DOI: 10.1021/acs.inorgchem.3c01320 | ||||||
| Tags | DENSITY-FUNCTIONAL THEORY; HYDROGEN GENERATION; CORRELATION-ENERGY; DFT CALCULATIONS; CHEMICAL-SHIFTS; BASIS-SETS; NMR; DIOXIDE; APPROXIMATION; CHEMISTRY | ||||||
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Funding (1)
| 1 | Russian Science Foundation | 21-73-10038 (121071400043-3) |
Abstract:
A combination of multinuclear nuclear magnetic resonance spectroscopy and theoretical calculation based on density functional theory was used for a speciation study of Pt in solutions prepared either by the interaction of [Pt(OH)6]2– with gaseous CO2 in an alkaline solution of platinum(IV) hydroxide ([Pt(OH)4(H2O)2]) or by the dissolution of [Pt(OH)4(H2O)2] in an aqueous KHCO3 solution. The formed solutions contained coexisting Pt(IV) carbonato complexes with κ1- and κ2-coordination modes. The gradual condensation of mononuclear Pt species in such bicarbonate solutions resulted in the formation of PtO2 nanoparticles aggregating into a solid precipitate on prolonged aging. The deposition of PtO2 particles from bicarbonate solutions was adapted for the preparation of Pt-containing heterogeneous catalysts: bimetallic Pt–Ni catalysts were prepared using various supporting materials (CeO2, SiO2, and g-C3N4) and tested for the activity in hydrazine-hydrate decomposition. All prepared materials showed high selectivity with respect to H2 production from the hydrazine-hydrate with PtNi/CeO2 showing the highest rate of H2 evolution. In the long-range evaluation, the PtNi/CeO2 catalyst operating at 50 °C showed an exceptional turnover number value of 4600 producing hydrogen at a 97% selectivity level and with a mean turnover frequency value of about 470 h–1. In the case of the PtNi/g-C3N4 catalyst, for the first time, the photodriven decomposition of hydrazine-hydrate was shown to enhance the productivity of the catalyst by 40%.
Cite:
Vasilchenko D.
, Tkachev S.
, Tkachenko P.
, Berdyugin S.
, Popovetskiy P.
, Gerasimov E.
, Zhurenok A.
, Kozlova E.
Platinum(IV) Carbonato Complexes: Formation via the Addition of CO2 to the [Pt(OH)6]2– Anion and Generation of Platinum(IV) Oxide Nanoparticles for the Preparation of Catalysts
Inorganic Chemistry. 2023. V.62. N64. P.9732–9748. DOI: 10.1021/acs.inorgchem.3c01320 WOS Scopus РИНЦ ANCAN PMID OpenAlex
Platinum(IV) Carbonato Complexes: Formation via the Addition of CO2 to the [Pt(OH)6]2– Anion and Generation of Platinum(IV) Oxide Nanoparticles for the Preparation of Catalysts
Inorganic Chemistry. 2023. V.62. N64. P.9732–9748. DOI: 10.1021/acs.inorgchem.3c01320 WOS Scopus РИНЦ ANCAN PMID OpenAlex
Dates:
| Submitted: | Apr 24, 2023 |
| Published online: | Jun 8, 2023 |
| Published print: | Jun 19, 2023 |
Identifiers:
| Web of science: | WOS:001006168800001 |
| Scopus: | 2-s2.0-85163729265 |
| Elibrary: | 54146928 |
| Chemical Abstracts: | 2023:1169766 |
| Chemical Abstracts (print): | 183:230379 |
| PMID: | 37291758 |
| OpenAlex: | W4379967228 |