Bottom-Up Construction of Active Sites in a Cu–N4–C Catalyst for Highly Efficient Oxygen Reduction Reaction,ACS Nano

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Bottom-Up Construction of Active Sites in a Cu–N4–C Catalyst for Highly Efficient Oxygen Reduction Reaction
ACS Nano ( IF 15.8 ) Pub Date : 2019-03-01 00:00:00 , DOI: 10.1021/acsnano.8b08692
Wei Li _{1,

2} , Chungang Min ₂ , Feng Tan _{1,

2} , Zhanping Li ₃ , Bingsen Zhang ₄ , Rui Si ₅ , Mingli Xu ₆ , Weiping Liu ₁ , Liexing Zhou ₂ , Qingmao Wei _{1,

2} , Yuzhen Zhang _{1,

2} , Xikun Yang _{1,

2}

Affiliation

Bottom-up construction of efficient active sites in transition metal–nitrogen–carbon (M–N–C) catalysts for oxygen reduction reaction (ORR) from single molecular building blocks remains one of the most difficult challenges. Herein, we report a bottom-up approach to produce a highly active Cu–N₄–C catalyst with well-defined Cu–N₄ coordination sites derived from a small molecular copper complex containing Cu–N₄ moieties. The Cu–N₄ moieties were found to be covalently integrated into graphene sheets to create the Cu–N₄ active sites for ORR. Furthermore, the activity was boosted by tuning the structure of active sites. We find that the high ORR activity of the Cu–N₄–C catalyst is related to the Cu–N₄ center linked to edges of the graphene sheets, where the electronic structure of the Cu center has the right symmetry for the degenerate π* orbital of the O₂ molecule. These findings point out the direction for the synthesis of the M–N–C catalysts at the molecular level.

中文翻译：

Cu-N ₄ -C催化剂中活性位的自下而上构建，可实现高效氧还原反应

自底向上构造过渡金属–氮–碳（MC–N–C）催化剂中有效的活性位点以从单个分子结构单元进行氧还原反应（ORR）仍然是最困难的挑战之一。在本文中，我们报告了一种自下而上的方法，该方法用于生产具有明确定义的Cu-N ₄配位点的高活性Cu–N ₄ –C催化剂，该催化剂源自包含Cu–N ₄部分的小分子铜络合物。发现Cu–N ₄部分被共价整合到石墨烯片中，从而形成ORR的Cu–N ₄活性位。此外，通过调节活性位点的结构来促进活性。我们发现Cu–N ₄的高ORR活性–C催化剂与连接到石墨烯片边缘的Cu–N ₄中心有关，其中Cu中心的电子结构对O ₂分子的简并π*轨道具有正确的对称性。这些发现指出了在分子水平上合成M–N–C催化剂的方向。

更新日期：2019-03-01

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