Engineering of the N-doped carbon support for improved performance of supported Pd catalysts in hydrogen production from gas-phase formic acid

Golub, Fedor S.; Gerasimov, Evgeny Yu.; Prosvirin, Igor P.; Plyusnin, P. E.; Болотов, В. А.; Parmon, Valentin N.; Bulushev, Dmitri A.

doi:10.1016/j.ijhydene.2023.03.042

Cited by 6 publications

(7 citation statements)

References 52 publications

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“…At the same time, the TOF for Pd/hatnCTF was by a factor of 1.5 lower than the TOF for the 1 wt % Pd catalyst prepared on the N-doped carbon through heating of a mixture of melamine with mesoporous carbon at 673 K and containing single-atom Pd sites and nanoparticles with the mean size of 1.6 nm . Even higher values were reported by Podyacheva et al for formic acid decomposition in gas phase over a Pd catalyst supported on N-doped carbon nanotubes.…”

Section: Resultsmentioning

confidence: 69%

“…The electronic state and surface contents of elements were determined using XPS. A SPECS photoelectron spectrometer equipped with a PHOIBOS-150-MCD-9 hemispherical analyzer and a FOCUS-500 X-ray monochromator (AlKα radiation, h ν = 1486.74 eV, 200 W) and a VG-Microtech Multilab 3000 spectrometer equipped with a semispherical electron analyzer and a Mg Kα ( h ν = 1253.6 eV) with a 300 W X-ray source were used. , …”

Section: Methodsmentioning

confidence: 99%

“…Supported Pd catalysts were prepared by impregnation with palladium acetylacetonate [Pd(acac) 2 , Sigma-Aldrich] solution in acetone . 28 The amount of Pd(acac) 2 was calculated to obtain 1 wt % Pd catalysts (see Supporting Information file). Every sample was pretreated in a flow of formic acid/Ar mixture at 573 K for 30 min before any measurement.…”

Section: Methodsmentioning

confidence: 99%

“…The necessary gases were supplied by a flow setup (Figure S1). 28 A bubbler filled with liquid formic acid was used to saturate an Ar flow with gaseous formic acid at 303 K. The flow was diluted with Ar to reach the necessary concentration of formic acid equal to 2.5 vol %. The total flow rate and catalyst loading were constant and corresponded to 67 mL min −1 and 16 mg, respectively, for obtaining temperature-conversion dependences.…”

Section: Catalytic Measurementsmentioning

confidence: 99%

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Pd Active Sites on Covalent Triazine Frameworks for Catalytic Hydrogen Production from Formic Acid

Bulushev

Golub

Трубина

et al. 2023

ACS Appl. Nano Mater.

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Covalent triazine frameworks (CTF) have been recently applied as supports for metal catalysts for different reactions. Varying the nature of the CTF support could improve catalytic properties due to a change in the nature of metal active sites presented in the form of single atoms and dispersed nanoparticles. To understand these changes, for the first time, 1 wt % Pd catalysts supported on hatnCTF and acacCTF prepared from hexaazatrinaphthylene-tricarbonitrile and malonyldibenzonitrile, respectively, were tested in formic acid decomposition in the gas phase. The results were compared with those obtained for a Pd/g-C 3 N 4 catalyst. The catalysts were characterized by high-angle annular dark-field/scanning transmission electron microscopy, X-ray absorption near edge structure/extended X-ray absorption fine structure and Xray photoelectron spectroscopy. The activity of the Pd/hatnCTF catalyst was significantly higher than those for Pd/acacCTF and Pd/g-C 3 N 4 , providing the reaction at a lower temperature by ∼60 K. The high performance of this catalyst was attributed to single-atom Pd 2+ −C 1 N 3 sites, which are the main active Pd species in this sample. The Pd/acacCTF sample contained single-atom Pd 2+ −O 4 sites and metallic Pd nanoparticles, while the Pd/g-C 3 N 4 sample contained mainly metallic Pd nanoparticles. The selectivity toward H 2 was high (>98%) for all catalysts even at 573 K. The obtained results could be useful for the development of different applications of CTF materials.

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Section: Resultsmentioning

confidence: 69%

Section: Methodsmentioning

confidence: 99%

Section: Methodsmentioning

confidence: 99%

Section: Catalytic Measurementsmentioning

confidence: 99%

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Pd Active Sites on Covalent Triazine Frameworks for Catalytic Hydrogen Production from Formic Acid

Bulushev

Golub

Трубина

et al. 2023

ACS Appl. Nano Mater.

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“…Subsequent studies found that introducing a heteroatom N into the carbon structure could improve the catalytic performance of Pd/C catalysts for hydrogen production from FA. N atoms were thought to enhance the physical and chemical properties of carbon supports, regulate the pore structure and surface properties, promote the dispersion of Pd nanoparticles, and regulate the electronic structure of the Pd active center. , More specifically, N atoms located between C atoms can also break the electroneutrality of C and generate more adsorption sites to stabilize Pd . In addition, the enriched N can provide abundant FA adsorption sites to make the catalyst more effective with the reactants, and the electronic effect between N atoms and Pd nanoparticles promotes the cleavage of C–H bonds in FA …”

Section: Introductionmentioning

confidence: 99%

Efficient Dehydrogenation of Formic Acid at Room Temperature Using a Pd/Chitosan-Derived Nitrogen-Doped Carbon Catalyst: Synthesis, Characterization, and Kinetic Study

Geng,

Johnravindar,

Xue

et al. 2023

Ind. Eng. Chem. Res.

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Formic acid (FA) can serve as a hydrogen carrier and is easy to store and transport. However, the decomposition of FA requires the use of a catalyst to accelerate the reaction rate and improve the hydrogen yield, which is of great significance for promoting the development of hydrogen energy technology and achieving sustainable development goals. Herein, chitosan-derived nitrogen-doped biochar-supporting palladium nanoparticles were synthesized and used as catalysts for formic acid dehydrogenation, showing excellent catalytic performance. The initial TOF of the Pd 9.2 /C−N catalyst reached 615 mol H 2 mol Pd −1 h −1 and the activation energy was 39.15 kJ mol −1 . The good catalytic performance of the catalyst was attributed to the well-distributed ultrafine palladium nanoparticles with a size of 2.2−2.6 nm and proper metal-carrier interaction, which enhanced the capability of the palladium nanoparticles in the cleavage of the C−H bond of FA. Parameters, such as palladium loading and reaction time, were investigated along with an improved and comprehensive kinetic study, which provides new insights into the field of FA dehydrogenation.

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The influence of carbon nanomaterials on catalytic decomposition of formic acid

Chesnokov,

Prosvirin,

Gerasimov

et al. 2024

International Journal of Hydrogen Energy

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Engineering of the N-doped carbon support for improved performance of supported Pd catalysts in hydrogen production from gas-phase formic acid

Cited by 6 publications

References 52 publications

Pd Active Sites on Covalent Triazine Frameworks for Catalytic Hydrogen Production from Formic Acid

Pd Active Sites on Covalent Triazine Frameworks for Catalytic Hydrogen Production from Formic Acid

Efficient Dehydrogenation of Formic Acid at Room Temperature Using a Pd/Chitosan-Derived Nitrogen-Doped Carbon Catalyst: Synthesis, Characterization, and Kinetic Study

The influence of carbon nanomaterials on catalytic decomposition of formic acid

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