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具有密集上区顶面暴露面的各向异性N-石墨烯扩散CoO纳米晶体作为高效氧还原反应电催化剂。

Anisotropic N-Graphene-diffused CoO nanocrystals with dense upper-zone top-on-plane exposure facets as effective ORR electrocatalysts.

作者信息

Hassen D, Shenashen M A, El-Safty A R, Elmarakbi A, El-Safty S A

机构信息

National Institute for Materials Science (NIMS), Research Center for Strategic Materials, 1-2-1 Sengen, Tsukuba-shi, Ibaraki-ken, 305-0047, Japan.

Faculty of Engineering and Advanced and Manufacturing, University of Sunderland, St Peter's Campus, Sunderland, SR6 0DD, UK.

出版信息

Sci Rep. 2018 Feb 27;8(1):3740. doi: 10.1038/s41598-018-21878-w.

DOI:10.1038/s41598-018-21878-w
PMID:29487302
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC5829235/
Abstract

We provide strong evidence of the effectiveness of homogenously self-propelled particle-in-particle diffusion, interaction and growth protocol. This technique was used for one-pot synthesis of novel nitrogen-graphene oxide (N-GO)/CoO nanocrystals with cuboid rectangular prism-shaped nanorods (NRs) along {110}-plane and truncated polyhedrons with densely-exposed, multi-facet sites along {311} and {111} planes. These hierarchal nanocrystals create electrode catalyst patterns with vast-range accessibility to active Co sites, a vascular system for the transport and retention of captured O molecule interiorly, and low adsorption energy and dense electron configuration surfaces during the oxygen reduction reaction (ORR). The superior electrocatalytic ORR activity of the N-GO/CoO polyhedron nanocrystals in terms of electrochemical selectivity, durability and stability compared with NRs or commercial Pt/C catalysts confirms the synergetic contribution of multi-functional, dense-exposed, and actively topographic facets of polyhedrons to significantly activate the catalytic nature of the catalyst. Our findings show real evidence, for the first time that not only the large number of catalytically active Co cations at the top surface layer but also the dense location of active Co sites on the upper-zone top-on-plane exposure, and the electron density configuration and distribution around the Co sites were important for effective ORR.

摘要

我们提供了关于均匀自推进颗粒内扩散、相互作用和生长协议有效性的有力证据。该技术用于一锅法合成新型氮氧化石墨烯(N-GO)/CoO纳米晶体,其具有沿{110}平面的长方体矩形棱柱形纳米棒(NRs)以及沿{311}和{111}平面具有密集暴露的多面位点的截顶多面体。这些分级纳米晶体形成了电极催化剂图案,在氧还原反应(ORR)过程中,对活性Co位点具有广泛的可及性,具有用于在内部运输和保留捕获的O分子的血管系统,以及低吸附能和致密电子构型表面。与NRs或商业Pt/C催化剂相比,N-GO/CoO多面体纳米晶体在电化学选择性、耐久性和稳定性方面具有优异的电催化ORR活性,这证实了多面体的多功能、密集暴露和活跃的形貌面的协同作用,可显著激活催化剂的催化性质。我们的研究结果首次表明,不仅顶层表面大量具有催化活性的Co阳离子,而且活性Co位点在上层区域顶面暴露上的密集位置,以及Co位点周围的电子密度构型和分布对于有效的ORR都很重要。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/14ac/5829235/f6e6bcbd9e54/41598_2018_21878_Fig6_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/14ac/5829235/580f57a7d267/41598_2018_21878_Fig1_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/14ac/5829235/7c6a58300468/41598_2018_21878_Fig2_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/14ac/5829235/b80f9e700b3a/41598_2018_21878_Fig3_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/14ac/5829235/8b57bc3bbdf7/41598_2018_21878_Fig4_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/14ac/5829235/65829b7dd1b5/41598_2018_21878_Fig5_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/14ac/5829235/f6e6bcbd9e54/41598_2018_21878_Fig6_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/14ac/5829235/580f57a7d267/41598_2018_21878_Fig1_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/14ac/5829235/7c6a58300468/41598_2018_21878_Fig2_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/14ac/5829235/b80f9e700b3a/41598_2018_21878_Fig3_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/14ac/5829235/8b57bc3bbdf7/41598_2018_21878_Fig4_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/14ac/5829235/65829b7dd1b5/41598_2018_21878_Fig5_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/14ac/5829235/f6e6bcbd9e54/41598_2018_21878_Fig6_HTML.jpg

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