Sarkar Subhajit, Biswas Ashmita, Kamboj Navpreet, Dey Ramendra Sundar
Institute of Nano Science and Technology, Mohali 160062, Punjab, India.
Inorg Chem. 2020 Sep 21;59(18):13453-13464. doi: 10.1021/acs.inorgchem.0c01879. Epub 2020 Sep 10.
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.
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。