Bifunctionally faceted Pt/Ru nanoparticles for preferential oxidation of CO in H2

Du, Xudong; Lang, Yun; Cao, Kun; Yang, Jixing; Cai, Jing; Shan, Bin; Chen, Rong

doi:10.1016/j.jcat.2021.02.010

Cited by 17 publications

(16 citation statements)

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“…Besides the above CO oxidation process, the obtained catalysts also showed potential application in proton-exchange-membrane fuel cells (PEMFCs), as the CO was required to be timely removed from reformate hydrogen to avoid the Pt anode poisoning [46][47][48]. As shown in Fig.…”

Section: Atomic-level Structural Characterizationmentioning

confidence: 99%

Optimizing the Pt‐FeO_x Interaction over Atomic Pt/FeO_x/CeO₂ Catalysts for Improved CO Oxidation Activity

Wang

Luo

Chu

et al. 2022

Chemie Ingenieur Technik

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The metal‐supported CeO2 catalysts (such as Pt/CeO2) have been considered as the most promising exhaust‐treatment catalyst to meet the future emission standard. However, the Pt‐O‐Ce interface on Pt/CeO2 system seems to over‐stabilize the Pt sites to cause low activity for CO oxidation. In this work, by adding Fe oxides, the enhanced Pt‐FeOx interaction was formed with the disappearance of the Pt‐O‐Ce interface, facilitating the electron transfer from the support to the atomically dispersed Pt on the Pt‐FeOx interface for the dramatically CO (preferential) oxidation performance. The single‐atom Pt/1.5FeOx/CeO2 performed the best catalytic activity with a reaction rate of 0.58 s−1 at 144 °C (T100). Such strategy in resorting the special metal‐support interaction to tune the active sites can be extended to other metal‐oxide systems for further optimized catalysis.

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Section: Atomic-level Structural Characterizationmentioning

confidence: 99%

Optimizing the Pt‐FeO_x Interaction over Atomic Pt/FeO_x/CeO₂ Catalysts for Improved CO Oxidation Activity

Wang

Luo

Chu

et al. 2022

Chemie Ingenieur Technik

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“… 8 − 10 Previous studies have shown that metals such as Pt, Rh, Au, and Ru show high CO conversion performance and selectivity. 9 − 19 In particular, Ru exhibits high PROX performance over a wide temperature range and is relatively inexpensive compared with other noble metals 8 , 9 Therefore, although several potential non-noble metal-based PROX catalysts have been reported, 20 − 28 Ru is still widely used as a PROX catalyst. 6 , 11 …”

Section: Introductionmentioning

confidence: 99%

“…In domestic PEFC systems, CO is removed from the hydrogen-rich reformate by a two-stage process: first, the majority of the CO is removed by conversion to hydrogen and carbon dioxide via the water–gas shift reaction, and then the remaining CO is oxidized with air via preferential oxidation (PROX). PROX catalysts for use in domestic PEFC systems must have high activity, high selectivity for CO oxidation in the presence of excess hydrogen, and high durability against impurities, and they should be able to catalyze the oxidation reaction at low temperatures. − Previous studies have shown that metals such as Pt, Rh, Au, and Ru show high CO conversion performance and selectivity. − In particular, Ru exhibits high PROX performance over a wide temperature range and is relatively inexpensive compared with other noble metals , Therefore, although several potential non-noble metal-based PROX catalysts have been reported, − Ru is still widely used as a PROX catalyst. , …”

Section: Introductionmentioning

confidence: 99%

Operando Spectroscopic Study of the Dynamics of Ru Catalyst during Preferential Oxidation of CO and the Prevention of Ammonia Poisoning by Pt

Sato

Zaitsu

Kitayama

et al. 2022

JACS Au

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Hydrogen is a promising clean energy source. In domestic polymer electrolyte fuel cell systems, hydrogen is produced by reforming of natural gas; however, the reformate contains carbon monoxide (CO) as a major impurity. This CO is removed from the reformate by a combination of the water–gas shift reaction and preferential oxidation of CO (PROX). Currently, Ru-based catalysts are the most common type of PROX catalyst; however, their durability against ammonia (NH 3 ) as an impurity produced in situ from trace amounts of nitrogen also contained in the reformate is an important issue. Previously, we found that addition of Pt to an Ru catalyst inhibited deactivation by NH 3 . Here, we conducted operando XAFS and FT-IR spectroscopic analyses with simultaneous gas analysis to investigate the cause of the deactivation of an Ru-based PROX catalyst (Ru/α-Al 2 O 3 ) by NH 3 and the mechanism of suppression of the deactivation by adding Pt (Pt/Ru/α-Al 2 O 3 ). We found that nitric oxide (NO) produced by oxidation of NH 3 induces oxidation of the Ru nanoparticle surface, which deactivates the catalyst via a three-step process: First, NO directly adsorbs on Ru 0 to form NO-Ru δ+ , which then induces the formation of O-Ru n + by oxidation of the surrounding Ru 0 . Then, O-Ru m + is formed by oxidation of Ru 0 starting from the O-Ru n + nuclei and spreading across the surface of the nanoparticle. Pt inhibits this process by alloying with Ru and inducing the decomposition of adsorbed NO, which keeps the Ru in a metallic state.

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“…Hydrogen (H 2 ) is widely considered as the fuel of the future in terms of meeting sustainability and carbon emissions reduction goals, renewable energy storage potential, and supporting various end-uses in industrial and transport sectors. At present, the global H 2 production capacity is still dominated by fossil fuel resources [1]. During the transition from fossil-based H 2 to renewable 'green' H 2 energy, there are certain requirements that pertain to H 2 purity.…”

Section: Introductionmentioning

confidence: 99%

“…On the other hand, the design of PSA purification units is fairly complex; it involves the use of high compression ratios and multicolumn adsorption systems. CO preferential oxidation (CO PROX) has been identified as a cost-effective CO abatement technology [1]. Arzamendi et al [7] suggested that CO PROX is a simple process, supporting compact reactor technologies, and it could be used to convert CO in a H 2 -rich gas stream in small-scale fuel processors and in on-board applications.…”

Section: Introductionmentioning

confidence: 99%

CO Preferential Oxidation in a Microchannel Reactor Using a Ru-Cs/Al2O3 Catalyst: Experimentation and CFD Modelling

et al. 2021

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This work presents an experimental and modelling evaluation of the preferential oxidation of CO (CO PROX) from a H2-rich gas stream typically produced from fossil fuels and ultimately intended for hydrogen fuel cell applications. A microchannel reactor containing a washcoated 8.5 wt.% Ru/Al2O3 catalyst was used to preferentially oxidise CO to form CO2 in a gas stream containing (by vol.%): 1.4% CO, 10% CO2, 18% N2, 68.6% H2, and 2% added O2. CO concentrations in the product gas were as low as 42 ppm (99.7% CO conversion) at reaction temperatures in the range 120–140 °C and space velocities in the range 65.2–97.8 NL gcat−1 h−1. For these conditions, less than 4% of the H2 feed was consumed via its oxidation and reverse water-gas shift. Furthermore, a computational fluid dynamic (CFD) model describing the microchannel reactor for CO PROX was developed. With kinetic parameter estimation and goodness of fit calculations, it was determined that the model described the reactor with a confidence interval far greater than 95%. In the temperature range 100–200 °C, the model yielded CO PROX reaction rate profiles, with associated mass transport properties, within the axial dimension of the microchannels––not quantifiable during the experimental investigation. This work demonstrates that microchannel reactor technology, supporting an active catalyst for CO PROX, is well suited for CO abatement in a H2-rich gas stream at moderate reaction temperatures and high space velocities.

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Bifunctionally faceted Pt/Ru nanoparticles for preferential oxidation of CO in H2

Cited by 17 publications

References 50 publications

Optimizing the Pt‐FeO_x Interaction over Atomic Pt/FeO_x/CeO₂ Catalysts for Improved CO Oxidation Activity

Optimizing the Pt‐FeO_x Interaction over Atomic Pt/FeO_x/CeO₂ Catalysts for Improved CO Oxidation Activity

Operando Spectroscopic Study of the Dynamics of Ru Catalyst during Preferential Oxidation of CO and the Prevention of Ammonia Poisoning by Pt

CO Preferential Oxidation in a Microchannel Reactor Using a Ru-Cs/Al2O3 Catalyst: Experimentation and CFD Modelling

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Bifunctionally faceted Pt/Ru nanoparticles for preferential oxidation of CO in H2

Cited by 17 publications

References 50 publications

Optimizing the Pt‐FeOx Interaction over Atomic Pt/FeOx/CeO2 Catalysts for Improved CO Oxidation Activity

Optimizing the Pt‐FeOx Interaction over Atomic Pt/FeOx/CeO2 Catalysts for Improved CO Oxidation Activity

Operando Spectroscopic Study of the Dynamics of Ru Catalyst during Preferential Oxidation of CO and the Prevention of Ammonia Poisoning by Pt

CO Preferential Oxidation in a Microchannel Reactor Using a Ru-Cs/Al2O3 Catalyst: Experimentation and CFD Modelling

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Optimizing the Pt‐FeO_x Interaction over Atomic Pt/FeO_x/CeO₂ Catalysts for Improved CO Oxidation Activity

Optimizing the Pt‐FeO_x Interaction over Atomic Pt/FeO_x/CeO₂ Catalysts for Improved CO Oxidation Activity