Cylindrical C96 Fullertubes: A Highly Active Metal Free O2-Reduction Electrocatalyst
Cylindrical C96 Fullertubes: A Highly Active Metal Free O2-Reduction Electrocatalyst
复制标题
圆柱形 C96 Fullertubes：高活性无金属 O2 还原电催化剂
DOI：
10.1002/e202116727
复制
发表时间：
2022
影响因子：
--
通讯作者：
Sreeprasad T. Sreenivasan
中科院分区：
文献类型：
--
作者：
Mohamed Fathi Sanad;Hannah M. Franklin;Basant A Ali;Alain R. Puente Santiago;Aruna N Nair;Venkata S.N. Chava;Olivia Fernandez-Delgado;Nageh K. Allam;Steven Stevenson;Sreeprasad T. Sreenivasan
最近报道了一种新的分离方案，用于高度纯化的金属富勒烯管D5 h-C90，D3 d-C96和D5 d-C100，它们具有独特的电子特性。在这里，我们报告的C60，C70（球状富勒烯），C90，C96和C100（管状富勒烯）的氧还原电催化行为，使用实验和理论相结合的方法。C96（无金属催化剂）显示出显著的氧还原反应（ORR）活性，起始电位为0.85 V，中间电位为0.75 V，接近最新技术水平的Pt/C基准催化剂值。 我们使用C96作为质子交换膜燃料电池的改性阴极，实现了0.75 W cm− 2的优异功率密度，与最近报道的其他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，碳笼上的两个有利的能级排列活性催化位点是C96具有优异上级活性的原因。
A new isolation protocol was recently reported for highly purified metallic FullertubesD5h‐C90,D3d‐C96, andD5d‐C100,which exhibit unique electronic features. Here, we report the oxygen reduction electrocatalytic behavior of C60, C70(spheroidal fullerenes), and C90, C96, and C100(tubular fullerenes) using a combination of experimental and theoretical approaches. C96(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−2using C96as 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 C96.