Department of Chemistry, Tsinghua University, Beijing, 100084, China.
Beijing Synchrotron Radiation Facility, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing, China.
Angew Chem Int Ed Engl. 2017 Jun 6;56(24):6937-6941. doi: 10.1002/anie.201702473. Epub 2017 Apr 12.
The development of low-cost, efficient, and stable electrocatalysts for the oxygen reduction reaction (ORR) is desirable but remains a great challenge. Herein, we made a highly reactive and stable isolated single-atom Fe/N-doped porous carbon (ISA Fe/CN) catalyst with Fe loading up to 2.16 wt %. The catalyst showed excellent ORR performance with a half-wave potential (E ) of 0.900 V, which outperformed commercial Pt/C and most non-precious-metal catalysts reported to date. Besides exceptionally high kinetic current density (J ) of 37.83 mV cm at 0.85 V, it also had a good methanol tolerance and outstanding stability. Experiments demonstrated that maintaining the Fe as isolated atoms and incorporating nitrogen was essential to deliver the high performance. First principle calculations further attributed the high reactivity to the high efficiency of the single Fe atoms in transporting electrons to the adsorbed OH species.
开发低成本、高效、稳定的氧还原反应（ORR）电催化剂是可取的，但仍然是一个巨大的挑战。在此，我们制备了一种具有高达 2.16wt%负载量的高反应性和稳定性的孤立单原子 Fe/N 掺杂多孔碳（ISA Fe/CN）催化剂。该催化剂表现出优异的 ORR 性能，半波电位（E ）为 0.900V，优于商业 Pt/C 和迄今为止报道的大多数非贵金属催化剂。除了在 0.85V 时具有异常高的动力学电流密度（J ）37.83mVcm 外，它还具有良好的甲醇耐受性和出色的稳定性。实验表明，保持 Fe 作为孤立原子并掺入氮对于提供高性能是至关重要的。第一性原理计算进一步表明，单个 Fe 原子将电子高效地传递到吸附的 OH 物种是高反应性的原因。
