Selectively nitrogen-doped carbon materials as superior metal-free catalysts for oxygen reduction.
Selectively nitrogen-doped carbon materials as superior metal-free catalysts for oxygen reduction.
复制标题
选择性氮掺杂碳材料作为氧还原的优质无金属催化剂
DOI：
10.1038/s41467-018-05878-y
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发表时间：
2018-08-23
影响因子：
16.6
通讯作者：
Li Y
中科院分区：
文献类型：
--
作者：
Lv Q;Si W;He J;Sun L;Zhang C;Wang N;Yang Z;Li X;Wang X;Deng W;Long Y;Huang C;Li Y
用吡啶氮原子掺杂已知是提高碳基催化剂用于氧还原反应的活性的有效策略。然而，吡啶氮原子更喜欢占据在碳材料的边缘或缺陷位置。在此，命名为氢取代石墨二炔的碳骨架为吡啶氮掺杂提供了合适的碳基质。在氢取代的石墨二炔中，苯环中的三个碳原子与氢键合并用作活性位点，如常规碳材料的边缘或缺陷位置，在其上可以选择性地掺杂吡啶氮。所合成的吡啶氮掺杂氢取代石墨二炔在碱性介质中对氧还原反应表现出比商业铂基催化剂更好的电催化性能，在酸性介质中表现出相当的活性。密度泛函理论计算表明，吡啶氮掺杂的氢取代石墨二炔比吡啶氮掺杂的石墨烯更有效地用于氧还原。
Doping with pyridinic nitrogen atoms is known as an effective strategy to improve the activity of carbon-based catalysts for the oxygen reduction reaction. However, pyridinic nitrogen atoms prefer to occupy at the edge or defect sites of carbon materials. Here, a carbon framework named as hydrogen-substituted graphdiyne provides a suitable carbon matrix for pyridinic nitrogen doping. In hydrogen-substituted graphdiyne, three of the carbon atoms in a benzene ring are bonded to hydrogen and serve as active sites, like the edge or defect positions of conventional carbon materials, on which pyridinic nitrogen can be selectively doped. The as-synthesized pyridinic nitrogen-doped hydrogen-substituted graphdiyne shows much better electrocatalytic performance for the oxygen reduction reaction than that of the commercial platinum-based catalyst in alkaline media and comparable activity in acidic media. Density functional theory calculations demonstrate that the pyridinic nitrogen-doped hydrogen-substituted graphdiyne is more effective than pyridinic nitrogen-doped graphene for oxygen reduction.
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影响因子：
17.1
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