Dataset Information

Enhanced oxygen reduction with single-atomic-site iron catalysts for a zinc-air battery and hydrogen-air fuel cell.

ABSTRACT: Efficient, durable and inexpensive electrocatalysts that accelerate sluggish oxygen reduction reaction kinetics and achieve high-performance are highly desirable. Here we develop a strategy to fabricate a catalyst comprised of single iron atomic sites supported on a nitrogen, phosphorus and sulfur co-doped hollow carbon polyhedron from a metal-organic framework@polymer composite. The polymer-based coating facilitates the construction of a hollow structure via the Kirkendall effect and electronic modulation of an active metal center by long-range interaction with sulfur and phosphorus. Benefiting from structure functionalities and electronic control of a single-atom iron active center, the catalyst shows a remarkable performance with enhanced kinetics and activity for oxygen reduction in both alkaline and acid media. Moreover, the catalyst shows promise for substitution of expensive platinum to drive the cathodic oxygen reduction reaction in zinc-air batteries and hydrogen-air fuel cells.

SUBMITTER: Chen Y

PROVIDER: S-EPMC6303331 | biostudies-literature | 2018 Dec

REPOSITORIES: biostudies-literature

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Enhanced oxygen reduction with single-atomic-site iron catalysts for a zinc-air battery and hydrogen-air fuel cell.

Chen Yuanjun Y Ji Shufang S Zhao Shu S Chen Wenxing W Dong Juncai J Cheong Weng-Chon WC Shen Rongan R Wen Xiaodong X Zheng Lirong L Rykov Alexandre I AI Cai Shichang S Tang Haolin H Zhuang Zhongbin Z Chen Chen C Peng Qing Q Wang Dingsheng D Li Yadong Y

Nature communications 20181221 1

Efficient, durable and inexpensive electrocatalysts that accelerate sluggish oxygen reduction reaction kinetics and achieve high-performance are highly desirable. Here we develop a strategy to fabricate a catalyst comprised of single iron atomic sites supported on a nitrogen, phosphorus and sulfur co-doped hollow carbon polyhedron from a metal-organic framework@polymer composite. The polymer-based coating facilitates the construction of a hollow structure via the Kirkendall effect and electronic ...[more]

PMID: 30575726

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Project description:Recently Debe et al. reported that Pt3Ni7 leads to extraordinary Oxygen Reduction Reaction (ORR) activity. However, several reports show that hardly any Ni remains in the layers of the catalysts close to the surface ("Pt-skin effect"). This paradox that Ni is essential to the high catalytic activity with the peak ORR activity at Pt3Ni7 while little or no Ni remains close to the surface is explained here using large-scale first-principles-based simulations. We make the radical assumption that processing Pt-Ni catalysts under ORR conditions would leach out all Ni accessible to the solvent. To simulate this process we use the ReaxFF reactive force field, starting with random alloy particles ranging from 50% Ni to 90% Ni and containing up to ?300?000 atoms, deleting the Ni atoms, and equilibrating the resulting structures. We find that the Pt3Ni7 case and a final particle radius around 7.5 nm lead to internal voids in communication with the exterior, doubling the external surface footprint, in fair agreement with experiment. Then we examine the surface character of these nanoporous systems and find that a prominent feature in the surface of the de-alloyed particles is a rhombic structure involving 4 surface atoms which is crystalline-like but under-coordinated. Using density-functional theory, we calculate the energy barriers of ORR steps on Pt nanoporous catalysts, focusing on the Oad-hydration reaction (Oad + H2Oad ? OHad + OHad) but including the barriers of O2 dissociation (O2ad ? Oad + Oad) and water formation (OHad + Had ? H2Oad). We find that the reaction barrier for the Oad-hydration rate-determining-step is reduced significantly on the de-alloyed surface sites compared to Pt(111). Moreover we find that these active sites are prevalent on the surface of particles de-alloyed from a Pt-Ni 30?:?70 initial composition. These simulations explain the peak in surface reactivity at Pt3Ni7, and provide a rational guide to use for further optimization of improved catalytic and nanoporous materials.

Dataset Information

Enhanced oxygen reduction with single-atomic-site iron catalysts for a zinc-air battery and hydrogen-air fuel cell.

Publications

Enhanced oxygen reduction with single-atomic-site iron catalysts for a zinc-air battery and hydrogen-air fuel cell.

Similar Datasets

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