Two-dimensional iron-phthalocyanine (Fe-Pc) monolayer as a promising single-atom-catalyst for oxygen reduction reaction: a computational study
Two-dimensional iron-phthalocyanine (Fe-Pc) monolayer as a promising single-atom-catalyst for oxygen reduction reaction: a computational study
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二维铁酞菁（Fe-Pc）单层作为氧还原反应的有前途的单原子催化剂：一项计算研究
DOI：
10.1039/c5nr00302d
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发表时间：
2015
期刊：
影响因子：
6.7
通讯作者：
Chen Zhongfang
中科院分区：
文献类型：
--
作者：
Wang Yu;Yuan Hao;Li Yafei;Chen Zhongfang
寻找低成本的非铂催化剂用于氧还原反应（ORR）已成为燃料电池发展的关键科学问题。本文通过密度泛函理论的综合计算，系统地探索了利用具有精确控制铁原子分布的二维Fe-酞菁（Fe- pc）单层作为ORR催化剂的潜力。计算结果表明，O2分子在Fe-Pc单层表面可以被充分激活，并且后续的ORR步骤更倾向于通过更有效的4e途径在Fe-Pc单层上进行，其极限电位为0.68 V。特别是Fe-Pc单层在酸性介质中比Fe-Pc分子更稳定，对ORR轴向配体的加成具有良好的催化性能。因此，Fe-Pc单层膜是一种很有前途的高效燃料电池ORR单原子催化剂。
Searching for low-cost non-Pt catalysts for oxygen reduction reaction (ORR) has been a key scientific issue in the development of fuel cells. In this work, the potential of utilizing the experimentally available two-dimensional (2D) Fe-phthalocyanine (Fe-Pc) monolayer with precisely-controlled distribution of Fe atoms as a catalyst of ORR was systematically explored by means of comprehensive density functional theory computations. The computations revealed that O2 molecules can be sufficiently activated on the surface of the Fe-Pc monolayer, and the subsequent ORR steps prefer to proceed on the Fe-Pc monolayer through a more efficient 4e pathway with a considerable limiting potential of 0.68 V. Especially, the Fe-Pc monolayer is more stable than the Fe-Pc molecule in acidic medium, and can present good catalytic performance for ORR on the addition of axial ligands. Therefore, the Fe-Pc monolayer is quite a promising single-atom-catalyst with high efficiency for ORR in fuel cells.