Role of the Three-Phase Boundary of the Platinum–Support Interface in Catalysis: A Model Catalyst Kinetic Study

Papaioannou, Evangelos I.; Bachmann, Christoph; Neumeier, Jonas J; Frankel, Daniel; Over, Herbert; Janek, Jürgen; Metcalfe, Ian S.

doi:10.1021/acscatal.6b00829

Cited by 15 publications

(18 citation statements)

References 43 publications

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“…The effect of electrode microstructure on ammonia production is also essential since porosity, particle size, TPB length, and tortuosity play key role on the accessibility of activated nitrogen and hydrogen species on the reactive sites. Correlation of the microstructural characteristic with ammonia production can only be realized with structured electrode [69]. In future work, these possibilities will be investigated experimentally and combined with plasma modeling for the particular reactor geometry under study here.…”

Section: Table Of Contentsmentioning

confidence: 99%

“…Correlation of the microstructural characteristic with ammonia production can only be realized with structured electrode. 69 In future work, these possibilities will be investigated experimentally and combined with plasma modeling for the particular reactor geometry under study here.…”

Section: Acs Energy Lettersmentioning

confidence: 99%

“…Moreover, a Pt cathode electrocatalyst has been used, which is highly active for HER kinetics. − Recent theoretical studies have suggested that a more selective catalyst for nitrogen reduction reaction or with lower hydrogen evolution activity, such as Co, Ni, and Ru, respectively, could significantly improve the NH 3 formation rate. , The effect of electrode microstructure on ammonia production is also essential since porosity, particle size, TPB length, and tortuosity play a key role on the accessibility of activated nitrogen and hydrogen species on the reactive sites. Correlation of the microstructural characteristic with ammonia production can only be realized with structured electrode . In future work, these possibilities will be investigated experimentally and combined with plasma modeling for the particular reactor geometry under study here.…”

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Plasma Activated Electrochemical Ammonia Synthesis from Nitrogen and Water

et al. 2020

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Ammonia is an important precursor of fertilizers, as well as a potential carbon-free energy carrier. Nowadays, ammonia is synthesized via the Haber-Bosch process which is capital-and energyintensive process with an immense CO 2 footprint. Thus, alternative processes for the sustainable and decentralized ammonia production from N2 and H2O using renewable electricity are required.The key challenges for the realization of such processes are the efficient activation of the N2 bond and selectivity towards NH3. In this contribution, we report an all-electric method for sustainable ammonia production from nitrogen and water using a plasma-activated proton conducting solid oxide electrolyser. Hydrogen species produced by water oxidation over the anode are transported through the proton conducting membrane to the cathode where they react with the plasmaactivated nitrogen towards ammonia. Ammonia production rates and faradaic efficiencies up to of 26.8 nmol NH3/s/cm 2 and 88%, respectively, were achieved.H-B process, as they prevent the possibility of lowering capital costs [16], decentralization and small-scale ammonia production at the level of local communities. Moreover, the world's hydrogen, which is also a key reactant in ammonia production, is produced primarily from the steam reforming of methane, emitting huge amounts of CO2 that account for 1.6% of global emissions per year [2, 15]. Therefore, alternative technologies need to be explored for ammonia synthesis, which occur under more moderate conditions [17], require less carbon input [18], or can be powered by intermittent renewable energy sources [19].Nowadays, plasma technology has attracted a lot of attention as an alternative method of clean ammonia synthesis, including a renewable pathway that coupled this technology with other renewable energy approaches. At low temperature, plasmas are reported as one of the most efficient approaches for rupturing the triple nitrogen bond [20][21][22][23][24], which is the fundamental requirement for the ammonia synthesis. Most of the studies on plasma-assisted ammonia synthesis are based on atmospheric pressure dielectric barrier discharge plasma over various catalytic systems, with nitrogen conversion between 0.2-7.8% in N2/H2 mixtures [25][26][27][28][29][30]. There are also approaches in which plasma activation of nitrogen and water vapor (as a hydrogen source) have been investigated for ammonia synthesis offering promising results in terms of selectivity [31][32][33][34].However, there are a few studies on the synthesis of ammonia from nitrogen−hydrogen using low pressure (0.01−10 Torr) discharges [35][36][37][38][39][40]. In fact, low pressure nitrogen discharges are wellknown for efficiently producing vibrationally excited molecules that can further generate atomic nitrogen via a vibrational dissociation channel [41][42][43]. Despite the potential benefits of plasma technologies, such as localized and environmentally friendly energy storage through chemical conversion, the two most critical challenges for upscaling ...

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Section: Table Of Contentsmentioning

confidence: 99%

Section: Acs Energy Lettersmentioning

confidence: 99%

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confidence: 99%

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Plasma Activated Electrochemical Ammonia Synthesis from Nitrogen and Water

et al. 2020

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“…When the relative humidity gets higher than 40%, it becomes impossible to attain uniform fiber from the polymeric solution. After collecting the fiber from 600 cm [2] central area on the aluminum foil, the electrospun fiber was later calcined at 600 °C for 3 h or 6 h with a heating rate of 1 °C min −1 in the air to burn off PVP and obtain oxide nanofibers. Fiber outside the 600 cm 2 central region had non-uniform texture, so it was not calcined for further use.…”

Section: Electrospinningmentioning

confidence: 99%

“…CO oxidation is a representative model oxidation reaction in heterogeneous catalysis [1]. When studying model catalysts such as three-phase boundary (TPB) controlled platinum-YSZ (yttria stabilized zirconia) or single crystal platinum, CO oxidation was chosen to be the reaction of interest [2,3]. CO is a well-known environmental pollutant, and the molecule strongly binds to the surface of precious metal catalysts blocking other desired reactants from the available surface sites [4].…”

Section: Introductionmentioning

confidence: 99%

Low temperature CO oxidation by doped cerium oxide electrospun fibers

Sim

Wang

2020

Nano Convergence

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We investigated CO oxidation behavior of doped cerium oxide fibers. Electrospinning technique was used to fabricate the inorganic fibers after burning off polymer component at 600 °C in air. Cu, Ni, Co, Mn, Fe, and La were doped at 10 and 30 mol% by dissolving metal salts into the polymeric electrospinning solution. 10 mol% Cu-doped ceria fiber showed excellent catalytic activity for low temperature CO oxidation with 50% CO conversion at just 52 °C. This 10 mol% Cu-doped sample showed unexpected regeneration behavior under simple ambient air annealing at 400 °C. From the CO oxidation behavior of the 12 samples, we conclude that absolute oxygen vacancy concentration estimated by Raman spectroscopy is not a good indicator for low temperature CO oxidation catalysts unless extra care is taken such that the Raman signal reflects oxide surface status. The experimental trend over the six dopants showed limited agreement with theoretically calculated oxygen vacancy formation energy in the literature.

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phase‐boundary catalysis

Cornils¹

2020

Catalysis From a to Z

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Role of the Three-Phase Boundary of the Platinum–Support Interface in Catalysis: A Model Catalyst Kinetic Study

Cited by 15 publications

References 43 publications

Plasma Activated Electrochemical Ammonia Synthesis from Nitrogen and Water

Plasma Activated Electrochemical Ammonia Synthesis from Nitrogen and Water

Low temperature CO oxidation by doped cerium oxide electrospun fibers

phase‐boundary catalysis

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