Sanad Mohamed Fathi, Franklin Hannah M, Ali Basant A, Puente Santiago Alain R, Nair Aruna N, Chava Venkata S N, Fernandez-Delgado Olivia, Allam Nageh K, Stevenson Steven, Sreenivasan Sreeprasad T, Echegoyen Luis
Department of Chemistry and Biochemistry and Environmental Sciences and Engineering, The University of Texas at El Paso, 500 W. University Avenue, El Paso, TX 79968, USA.
Department of Chemistry, Purdue University, Fort Wayne, IN 46805, USA.
Angew Chem Int Ed Engl. 2022 May 16;61(21):e202116727. doi: 10.1002/anie.202116727. Epub 2022 Mar 23.
A new isolation protocol was recently reported for highly purified metallic Fullertubes D -C , D -C , and D -C which exhibit unique electronic features. Here, we report the oxygen reduction electrocatalytic behavior of C , C (spheroidal fullerenes), and C , C , and C (tubular fullerenes) using a combination of experimental and theoretical approaches. C (a metal-free catalyst) displayed remarkable oxygen reduction reaction (ORR) activity, with an onset potential of 0.85 V and a halfway potential of 0.75 V, which are close to the state-of-the-art Pt/C benchmark catalyst values. We achieved an excellent power density of 0.75 W cm using C as a modified cathode in a proton-exchange membrane fuel cell, comparable to other recently reported efficient metal-free catalysts. Combined band structure (experimentally calculated) and free-energy (DFT) investigations show that both favorable energy-level alignment active catalytic sites on the carbon cage are responsible for the superior activity of C .
最近报道了一种用于高度纯化的金属富勒管D -C、D -C和D -C的新分离协议，这些富勒管具有独特的电子特性。在此，我们结合实验和理论方法报告了C、C（球形富勒烯）以及C、C和C（管状富勒烯）的氧还原电催化行为。C（一种无金属催化剂）表现出显著的氧还原反应（ORR）活性，起始电位为0.85 V，半波电位为0.75 V，接近最先进的Pt/C基准催化剂值。在质子交换膜燃料电池中，我们使用C作为改性阴极实现了0.75 W cm的优异功率密度，与其他最近报道的高效无金属催化剂相当。结合能带结构（实验计算）和自由能（DFT）研究表明，碳笼上有利的能级排列和活性催化位点共同导致了C的优异活性。
