Role of the Metal‐Oxide Support in the Catalytic Activity of Pd Nanoparticles for Ethanol Electrooxidation in Alkaline Media

Monyoncho, Evans A.; Ntais, Spyridon; Brazeau, Nicolas; Wu, Jhing-Jhou; Sun, Chia‐Liang; Baranova, Elena A.

doi:10.1002/celc.201500432

Cited by 74 publications

(59 citation statements)

References 66 publications

(45 reference statements)

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“…In order to quantitative comparison of electrocatalytic active sites, the electrochemical surface area (ECSA) was analyzed on the basis of the PdO reduction coulombic charge. [20] The computed ECSA of Pd/BC-2 is 67.0 m 2 g À 1 , which is higher than that of Pd/BC-1 (62.7 m 2 g À 1 ) and Pd/BC-3 (47.8 m 2 g À 1 ) and is about 2.5 times as large as commercial Pd/C (27.0 m 2 g À 1 ).…”

Section: Electrocatalytic Property Of Eormentioning

confidence: 82%

“…The vertical coordinates of current density are standardized via the Pd chemical mass loading. [20] Furthermore, the ratio of j f /jr can be expressed to evaluate the poisoning tolerance of carbonaceous species for as produced catalysts. One is the peak current density in the forward anodic scan (j f ) and another is the peak current density in the backward scan (j r ).…”

Section: Electrocatalytic Property Of Eormentioning

confidence: 99%

“…[8][9] Therefore, the development of other novel catalysts with high electrocatalytic activity and stability for ethanol oxidation reaction (EOR) has aroused sustained attentions. [17][18][19][20][21] For palladium based catalysts, it is imperative to explore other electrocatalyst carriers with specific structure and component characteristic. [10][11][12][13][14][15][16] The stabilities and performance to EOR principally relay on carriers and active components of electrocatalysts.…”

Section: Introductionmentioning

confidence: 99%

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Palladium Nanoparticles Supported on B‐Doped Carbon Nanocage as Electrocatalyst toward Ethanol Oxidation Reaction

Yao

Zhang

et al. 2019

ChemElectroChem

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Boron-doped carbon nanocage (BC-2) was used as carrier to anchor palladium nanoparticles and enhanced the catalytic performance for the ethanol oxidation reaction. The BC-2 was synthesized via thermal treatment the predesigned compound containing cobalt and boron at 900°C with the help of hydrogen and acid washing process. Palladium nanoparticles can be loaded on the BC-2 supports (Pd/BC-2) for ethanol oxide reaction (EOR). The BC-2 support has the following character-istics: (i) The hollow structure contains highly order nanoporous to offer more channel and space in catalysis process; (ii) borondoped carbon structures can supply abundant activity sites for stabilizing palladium nanoparticles; (iii) the unique three-dimensional architecture can prevent the agglomeration and inactivation of metal catalysts. The Pd/BC-2 catalyst displays higher catalytic activities 3614.11 mA mg À 1 toward the peak current density compared to that of Pd/C (804.39 mA mg À 1 ).

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Section: Electrocatalytic Property Of Eormentioning

confidence: 82%

Section: Electrocatalytic Property Of Eormentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Palladium Nanoparticles Supported on B‐Doped Carbon Nanocage as Electrocatalyst toward Ethanol Oxidation Reaction

Yao

Zhang

et al. 2019

ChemElectroChem

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“…Herein, the spectra for the species on the electrode surface and spectra of the sum species in the thin cavity will be referred to as "surface" and "bulk solution" species, respectively. 67 Prior to the measurement of ethanol electro-oxidation species spectra, it is important to ensure that there is no atmospheric CO 2 and water vapor in the optical path, which would not only decrease the infrared (IR) intensity but also would contribute to observed spectra features. The presence of CO 2 is especially critical, because it is one of the anticipated ethanol oxidation products.…”

Section: Acs Catalysismentioning

confidence: 99%

Ethanol Electro-oxidation on Palladium Revisited Using Polarization Modulation Infrared Reflection Absorption Spectroscopy (PM-IRRAS) and Density Functional Theory (DFT): Why Is It Difficult To Break the C–C Bond?

et al. 2016

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International audienceInsights into the ethanol electro-oxidation reaction mechanism on palladium in alkaline media are presented combining polarization modulation infrared reflec- tion absorption spectroscopy (PM-IRRAS) and density functional theory (DFT) calculations. The synergy between PM-IRRAS and DFT calculations helps to explain why the C− C bond is not broken during ethanol electro-oxidation, and the reaction stops at acetate. Coupling chronoamperometry (CA) with in situ PM-IRRAS enables us to simultaneously identify ethanol electro-oxidation products on the catalyst surface and in the bulk solution. We show that, at lower potential, it is possible to break the C−C bond on Pd/C in alkaline media to form CO2. However, the selectivity is poor, because of competition with the formation of acetate and other side products, which gets worse at higher potentials. DFT computations complete the picture using the computational hydrogen electrode approach. The computations highlight the pivotal role of the CH3CO intermediate that can either undergo a C−C bond scission yielding CO and then CO2 or that can be oxidized toward CH3COO−. The latter is a dead end in the reaction scheme toward CO2 production, since it cannot be easily oxidized nor broken into C1 fragments. However, CH3CO is not the most favored intermediate formed from ethanol electro-oxidation on Pd, hence limiting the production of CO2

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“…and the use of alternative catalyst supports (CeO 2 , TiO 2 , SnO 2 , etc.) 22,23 that show metal-support interaction (MSI) effects, 24,25 we have screened for bimetallics and metal oxides from a database of more than 600 entries.…”

Section: Introductionmentioning

confidence: 99%

Computational screening for selective catalysts: Cleaving the C C bond during ethanol electro-oxidation reaction

Monyoncho

Steinmann

Sautet

et al. 2018

Electrochimica Acta

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The efficiency of direct ethanol fuel cells suffers from the partial oxidation of ethanol into acetic acid as opposed to the complete oxidation of this fuel to CO 2 . Herein, we support the quest for a selective catalyst for ethanol electro-oxidation to CO 2 , building on our previous mechanistic hypothesis based on experimental insight and DFT computations. We derive a simple descriptor of the expected selectivity towards full oxidation, Ω, as a function of the adsorption energy of atomic C and O. Three different families of catalyst surfaces are screened using this descriptor: monometallics, bimetallics and conducting metal oxides, totaling to 600 surfaces. In agreement with available experimental data, no single metal surface is more selective for total oxidation than platinum and palladium. While the selected conducting oxides were not predicted to be selective towards splitting the C-C bond, structurally-controlled monometallics (such as Pd (100)) or some bimetallics (Pd 3 Ag) are found to be competitive with the most stable facet, (111), of Pd and Pt. Despite this very extensive screening, no very promising catalyst has been identified. This highlights the need to identify catalysts for acetate oxidation or to exploit support effects and electrolyte engineering to profit from the full power of direct ethanol fuel cells.

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Role of the Metal‐Oxide Support in the Catalytic Activity of Pd Nanoparticles for Ethanol Electrooxidation in Alkaline Media

Cited by 74 publications

References 66 publications

Palladium Nanoparticles Supported on B‐Doped Carbon Nanocage as Electrocatalyst toward Ethanol Oxidation Reaction

Palladium Nanoparticles Supported on B‐Doped Carbon Nanocage as Electrocatalyst toward Ethanol Oxidation Reaction

Ethanol Electro-oxidation on Palladium Revisited Using Polarization Modulation Infrared Reflection Absorption Spectroscopy (PM-IRRAS) and Density Functional Theory (DFT): Why Is It Difficult To Break the C–C Bond?

Computational screening for selective catalysts: Cleaving the C C bond during ethanol electro-oxidation reaction

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