Dataset Information

Complex Three-Dimensional Co?O? Nano-Raspberry: Highly Stable and Active Low-temperature CO Oxidation Catalyst.

ABSTRACT: Highly stable and active low-temperature CO oxidation catalysts without noble metals are desirable to achieve a sustainable society. While zero-dimensional to three-dimensional Co?O? nanoparticles show high catalytic activity, simple-structured nanocrystals easily self-aggregate and become sintered during catalytic reaction. Thus, complex three-dimensional nanostructures with high stability are of considerable interest. However, the controlled synthesis of complex nanoscale shapes remains a great challenge as no synthesis theory has been established. In this study, 100 nm raspberry-shaped nanoparticles composed of 7?8 nm Co?O? nanoparticles were synthesized by hydrothermally treating cobalt glycolate solution with sodium sulfate. Surface single nanometer-scale structures with large surface areas of 89 m²·g^-1 and abundant oxygen vacancies were produced. The sulfate ions functioned as bridging ligands to promote self-assembly and suppress particle growth. The Co?O? nano-raspberry was highly stable under catalytic tests at 350 °C and achieved nearly 100% CO conversion at room temperature. The addition of bridging ligands is an effective method to control the formation of complex but ordered three-dimensional nanostructures that possessed extreme thermal and chemical stability and exhibited high performance.

SUBMITTER: Fuchigami T

PROVIDER: S-EPMC6164048 | biostudies-literature | 2018 Aug

REPOSITORIES: biostudies-literature

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Complex Three-Dimensional Co₃O₄ Nano-Raspberry: Highly Stable and Active Low-temperature CO Oxidation Catalyst.

Fuchigami Teruaki T Kimata Ryosuke R Haneda Masaaki M Kakimoto Ken-Ichi KI

Nanomaterials (Basel, Switzerland) 20180826 9

Highly stable and active low-temperature CO oxidation catalysts without noble metals are desirable to achieve a sustainable society. While zero-dimensional to three-dimensional Co₃O₄ nanoparticles show high catalytic activity, simple-structured nanocrystals easily self-aggregate and become sintered during catalytic reaction. Thus, complex three-dimensional nanostructures with high stability are of considerable interest. However, the controlled synthesis of complex nanoscale shapes remains a grea ...[more]

PMID: 30149672

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Project description:The desire for a carbon-free society and the continuously increasing demand for clean energy make it valuable to exploit green ammonia (NH3) synthesis that proceeds via the electrolysis driven Haber-Bosch (eHB) process. The key for successful operation is to develop advanced catalysts that can operate under mild conditions with efficacy. The main bottleneck of NH3 synthesis under mild conditions is the known scaling relation in which the feasibility of N2 dissociative adsorption of a catalyst is inversely related to that of the desorption of surface N-containing intermediate species, which leads to the dilemma that NH3 synthesis could not be catalyzed effectively under mild conditions. The present work offers a new strategy via introducing atomically dispersed Ru onto a single Co atom coordinated with pyrrolic N, which forms RuCo dual single-atom active sites. In this system the d-band centers of Ru and Co were both regulated to decouple the scaling relation. Detailed experimental and theoretical investigations demonstrate that the d-bands of Ru and Co both become narrow, and there is a significant overlapping of t2g and eg orbitals as well as the formation of a nearly uniform Co 3d ligand field, making the electronic structure of the Co atom resemble that of a "free-atom". The "free-Co-atom" acts as a bridge to facilitate electron transfer from pyrrolic N to surface Ru single atoms, which enables the Ru atom to donate electrons to the antibonding π* orbitals of N2, thus resulting in promoted N2 adsorption and activation. Meanwhile, H2 adsorbs dissociatively on the Co center to form a hydride, which can transfer to the Ru site to cause the hydrogenation of the activated N2 to generate N2H x (x = 1-4) intermediates. The narrow d-band centers of this RuCo catalyst facilitate desorption of surface *NH3 intermediates even at 50 °C. The cooperativity of the RuCo system decouples the sites for the activation of N2 from those for the desorption of *NH3 and *N2H x intermediates, giving rise to a favorable pathway for efficient NH3 synthesis under mild conditions.

Dataset Information

Complex Three-Dimensional Co?O? Nano-Raspberry: Highly Stable and Active Low-temperature CO Oxidation Catalyst.

Publications

Complex Three-Dimensional Co₃O₄ Nano-Raspberry: Highly Stable and Active Low-temperature CO Oxidation Catalyst.

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