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揭示铁双(三联吡啶)配合物在精确开发用于促进氧还原反应的铁氮碳电催化剂方面的潜力。

Unveiling the Potential of an Fe Bis(terpyridine) Complex for Precise Development of an Fe-N-C Electrocatalyst to Promote the Oxygen Reduction Reaction.

作者信息

Sarkar Subhajit, Biswas Ashmita, Kamboj Navpreet, Dey Ramendra Sundar

机构信息

Institute of Nano Science and Technology, Mohali 160062, Punjab, India.

出版信息

Inorg Chem. 2020 Sep 21;59(18):13453-13464. doi: 10.1021/acs.inorgchem.0c01879. Epub 2020 Sep 10.

DOI:10.1021/acs.inorgchem.0c01879
PMID:32909753
Abstract

Improvements in highly efficient precious-metal-free electrocatalysts for the oxygen reduction reaction (ORR) are extremely important but still a significant challenge. Herein, we report a novel catalyst design strategy integrating a bis(terpyridine) (hexadentate chelating ligand) with Fe which acts as nitrogen, a self-supporting carbon source, and a potent metal-ligand active site binding structure (Fe-btpy) and promotes the formation of Fe-N/C active sites, bypassing the complications induced during Fe-N-C catalyst synthesis. The resulting Fe-N/C electrocatalyst shows a very high ORR onset () and half-wave potential () of 1.05 and 0.89 V (vs reversible hydrogen electrode), respectively, outperforming the commercial Pt/C catalyst in alkaline medium. Most importantly, the Fe-N/C catalyst displays decent stability and remarkable methanol tolerance in comparison to the Pt/C catalyst. A fabricated rechargeable zinc-air battery with an Fe-N/C cathode catalyst demonstrated an excellent peak power density of 225 mW cm at a current density of 240 mA cm, in comparison to the Pt/C cathode catalyst. This work illuminates blueprints utilizing a new long-chain one-dimensional macromolecule that could be viable to produce Fe-N/C-based carbon electrocatalysts toward energy conversion applications.

摘要

开发高效的无贵金属氧还原反应(ORR)电催化剂具有极其重要的意义,但仍是一项重大挑战。在此,我们报道了一种新颖的催化剂设计策略,即将双(三联吡啶)(六齿螯合配体)与作为氮源的铁、自支撑碳源以及强大的金属 - 配体活性位点结合结构(Fe - btpy)相结合,促进Fe - N/C活性位点的形成,避免了Fe - N - C催化剂合成过程中产生的复杂问题。所得的Fe - N/C电催化剂在碱性介质中表现出非常高的ORR起始电位()和半波电位(),分别为1.05和0.89 V(相对于可逆氢电极),优于商业Pt/C催化剂。最重要的是,与Pt/C催化剂相比,Fe - N/C催化剂具有良好的稳定性和出色的甲醇耐受性。使用Fe - N/C阴极催化剂制备的可充电锌空气电池在电流密度为240 mA cm时表现出225 mW cm的优异峰值功率密度,相比之下Pt/C阴极催化剂则较低。这项工作为利用新型长链一维大分子生产用于能量转换应用的Fe - N/C基碳电催化剂提供了蓝图。

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