Beijing Key Laboratory of Green Chemical Reaction Engineering and Technology, Department of Chemical Engineering, Tsinghua University, Beijing, 100084, P. R. China.
Adv Mater. 2017 Apr;29(13). doi: 10.1002/adma.201604103. Epub 2017 Jan 9.
The oxygen reduction reaction (ORR) is the cornerstone of various sustainable energy-conversion technologies. Metal-free nanocarbon electrocatalysts with competitive activity, enhanced durability, and satisfactory cost, have been proposed as the most promising substitute for precious-metal catalysts. However, their further development is still primarily based on trial-and-error approaches due to the controversial knowledge of critical active sites and mechanisms. Herein, the activity origins of nanocarbon-based ORR electro-catalysts are comprehensively reviewed and correlated, considering the dopants, edges, and defects. Analogously, they can effectively modify the charge/spin distribution on the sp -conjugated carbon matrix, leading to optimized intermediate chemisorption and facilitated electron transfer. Specific doping at defective edges is expected to render practical applications for metal-free nanocarbon electrocatalysts.
氧还原反应(ORR)是各种可持续能源转换技术的基石。具有竞争力的活性、增强的耐久性和令人满意的成本的无金属纳米碳电催化剂已被提议作为贵金属催化剂的最有前途的替代品。然而,由于对关键活性位和机制的争议性认识,其进一步的发展仍然主要基于试错方法。在此,考虑掺杂剂、边缘和缺陷,全面综述和关联了基于纳米碳的 ORR 电催化剂的活性起源。类似地,它们可以有效地修饰 sp 共轭碳基质上的电荷/自旋分布,从而优化中间化学吸附并促进电子转移。在有缺陷的边缘进行特定掺杂有望为无金属纳米碳电催化剂提供实际应用。