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Surfactant-Mediated One-Pot Method To Prepare Pd-CeO₂ Colloidal Assembled Spheres and Their Enhanced Catalytic Performance for CO Oxidation.

ABSTRACT: A simple, one-pot method to fabricate ordered, monodispersed Pd-CeO₂ colloidal assembled spheres (CASs) was developed using the surfactant-mediated solvothermal approach, which involves a tunable self-assembled process by carefully controlling different chemical reactions. The evolution process and formation mechanism of the CASs were thoroughly investigated by time-controlled and component-controlled experiments. For CO oxidation, this CAS nanocatalyst exhibited much higher catalytic activity and thermal stability than Pd/CeO₂ prepared by an impregnation method, and its complete CO conversion temperature is ?120 °C. The enhanced catalytic performance for CO oxidation could be attributed to the synergistic effect of highly dispersed PdO species and Pd²⁺ ions incorporated into the CeO₂ lattice. For this CAS catalyst, each sphere can be viewed as a single reactor, and its catalytic performance can be further improved after being supported on alumina, which is obviously higher than results previously reported. Furthermore, this method was used to successfully prepare M-CeO₂ CASs (M = Pt, Cu, Mn, Co), showing further that this is a new and ideal approach for fabricating active and stable ceria-based materials.

SUBMITTER: Du C

PROVIDER: S-EPMC6640731 | biostudies-literature | 2016 Jul

REPOSITORIES: biostudies-literature

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Surfactant-Mediated One-Pot Method To Prepare Pd-CeO<sub>2</sub> Colloidal Assembled Spheres and Their Enhanced Catalytic Performance for CO Oxidation.

Du Chenhao C Lu Guanzhong G Guo Yun Y Guo Yanglong Y Gong Xue-Qing XQ

ACS omega 20160719 1

A simple, one-pot method to fabricate ordered, monodispersed Pd-CeO<sub>2</sub> colloidal assembled spheres (CASs) was developed using the surfactant-mediated solvothermal approach, which involves a tunable self-assembled process by carefully controlling different chemical reactions. The evolution process and formation mechanism of the CASs were thoroughly investigated by time-controlled and component-controlled experiments. For CO oxidation, this CAS nanocatalyst exhibited much higher catalytic ...[more]

PMID: 31457119

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Project description:CO elimination through oxidation over highly active and cost-effective catalysts is a way forward for many processes of industrial and environmental importance. In this study, doped CeO2 with transition metals (TM = Cu, Co, Mn, Fe, Ni, Zr, and Zn) at a level of 20 at. % was tested for CO oxidation. The oxides were prepared using microwave-assisted sol-gel synthesis to improve catalyst's performance for the reaction of interest. The effect of heteroatoms on the physicochemical properties (structure, morphology, porosity, and reducibility) of the binary oxides M-Ce-O was meticulously investigated and correlated to their CO oxidation activity. It was found that the catalytic activity (per gram basis or TOF, s-1) follows the order Cu-Ce-O > Ce-Co-O > Ni-Ce-O > Mn-Ce-O > Fe-Ce-O > Ce-Zn-O > CeO2. Participation of mobile lattice oxygen species in the CO/O2 reaction does occur, the extent of which is heteroatom-dependent. For that, state-of-the-art transient isotopic 18O-labeled experiments involving 16O/18O exchange followed by step-gas CO/Ar or CO/O2/Ar switches were used to quantify the contribution of lattice oxygen to the reaction. SSITKA-DRIFTS studies probed the formation of carbonates while validating the Mars-van Krevelen (MvK) mechanism. Scanning transmission electron microscopy-high-angle annular dark field imaging coupled with energy-dispersive spectroscopy proved that the elemental composition of dopants in the individual nanoparticle of ceria is less than their composition at a larger scale, allowing the assessment of the doping efficacy. Despite the similar structural features of the catalysts, a clear difference in the Olattice mobility was also found as well as its participation (as expressed with the α descriptor) in the reaction, following the order αCu > αCo> αMn > αZn. Kinetic studies showed that it is rather the pre-exponential (entropic) factor and not the lowering of activation energy that justifies the order of activity of the solids. DFT calculations showed that the adsorption of CO on the Cu-doped CeO2 surface is more favorable (-16.63 eV), followed by Co, Mn, Zn (-14.46, -4.90, and -4.24 eV, respectively), and pure CeO2 (-0.63 eV). Also, copper compensates almost three times more charge (0.37e-) compared to Co and Mn, ca. 0.13e- and 0.10e-, respectively, corroborating for its tendency to be reduced. Surface analysis (X-ray photoelectron spectroscopy), apart from the oxidation state of the elements, revealed a heteroatom-ceria surface interaction (Oa species) of different extents and of different populations of Oa species.

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Surfactant-Mediated One-Pot Method To Prepare Pd-CeO₂ Colloidal Assembled Spheres and Their Enhanced Catalytic Performance for CO Oxidation.

Publications

Surfactant-Mediated One-Pot Method To Prepare Pd-CeO<sub>2</sub> Colloidal Assembled Spheres and Their Enhanced Catalytic Performance for CO Oxidation.

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Surfactant-Mediated One-Pot Method To Prepare Pd-CeO2 Colloidal Assembled Spheres and Their Enhanced Catalytic Performance for CO Oxidation.

Publications

Surfactant-Mediated One-Pot Method To Prepare Pd-CeO<sub>2</sub> Colloidal Assembled Spheres and Their Enhanced Catalytic Performance for CO Oxidation.

Similar Datasets

OmicsDI is part of the ELIXIR infrastructure

Tweets

Surfactant-Mediated One-Pot Method To Prepare Pd-CeO₂ Colloidal Assembled Spheres and Their Enhanced Catalytic Performance for CO Oxidation.