Unknown

Dataset Information

0

In situ spectroscopy-guided engineering of rhodium single-atom catalysts for CO oxidation.

ABSTRACT: Single-atom catalysts have recently been applied in many applications such as CO oxidation. Experimental in situ investigations into this reaction, however, are limited. Hereby, we present a suite of operando/in situ spectroscopic experiments for structurally well-defined atomically dispersed Rh on phosphotungstic acid during CO oxidation. The identification of several key intermediates and the steady-state catalyst structure indicate that the reactions follow an unconventional Mars-van Krevelen mechanism and that the activation of O2 is rate-limiting. In situ XPS confirms the contribution of the heteropoly acid support while in situ DRIFT spectroscopy consolidates the oxidation state and CO adsorption of Rh. As such, direct observation of three key components, i.e., metal center, support and substrate, is achieved, providing a clearer picture on CO oxidation on atomically dispersed Rh sites. The obtained information are used to engineer structurally similar catalysts that exhibit T20 values up to 130?°C below the previously reported Rh1/NPTA.

SUBMITTER: Hulsey MJ 

PROVIDER: S-EPMC6430772 | biostudies-literature | 2019 Mar

REPOSITORIES: biostudies-literature

Json Xml
altmetric image

Publications

In situ spectroscopy-guided engineering of rhodium single-atom catalysts for CO oxidation.

Hülsey Max J MJ   Zhang Bin B   Ma Zhirui Z   Asakura Hiroyuki H   Do David A DA   Chen Wei W   Tanaka Tsunehiro T   Zhang Peng P   Wu Zili Z   Yan Ning N  

Nature communications 20190322 1

Single-atom catalysts have recently been applied in many applications such as CO oxidation. Experimental in situ investigations into this reaction, however, are limited. Hereby, we present a suite of operando/in situ spectroscopic experiments for structurally well-defined atomically dispersed Rh on phosphotungstic acid during CO oxidation. The identification of several key intermediates and the steady-state catalyst structure indicate that the reactions follow an unconventional Mars-van Krevelen  ...[more]

Similar Datasets

Unknown Control over Electrochemical CO<sub>2</sub> Reduction Selectivity by Coordination Engineering of Tin Single-Atom Catalysts.
| S-EPMC8655193 | biostudies-literature
Unknown Ni Single Atom Catalysts for CO<sub>2</sub> Activation.
| S-EPMC6728101 | biostudies-literature
Unknown Universal-Descriptors-Guided Design of Single Atom Catalysts toward Oxidation of Li<sub>2</sub> S in Lithium-Sulfur Batteries.
| S-EPMC8655168 | biostudies-literature
Unknown Water enables mild oxidation of methane to methanol on gold single-atom catalysts.
| S-EPMC7900127 | biostudies-literature
Unknown Time-resolved, in situ DRIFTS/EDE/MS studies on alumina-supported rhodium catalysts: effects of ceriation and zirconiation on rhodium-CO interactions.
| S-EPMC4529662 | biostudies-literature
Unknown Understanding the Impact of Defects on Catalytic CO Oxidation of LaFeO<sub>3</sub>-Supported Rh, Pd, and Pt Single-Atom Catalysts.
| S-EPMC6443215 | biostudies-literature
Unknown Linear Activation Energy-Reaction Energy Relations for LaBO<sub>3</sub> (B = Mn, Fe, Co, Ni) Supported Single-Atom Platinum Group Metal Catalysts for CO Oxidation.
| S-EPMC7493305 | biostudies-literature
Unknown Thermally stable single atom Pt/m-Al2O3 for selective hydrogenation and CO oxidation.
| S-EPMC5537564 | biostudies-literature
Unknown Single-atom catalysts for CO<sub>2</sub> electroreduction with significant activity and selectivity improvements.
| S-EPMC5369399 | biostudies-literature
Unknown Directing reaction pathways via in situ control of active site geometries in PdAu single-atom alloy catalysts.
| S-EPMC7943817 | biostudies-literature