Electrochemical oxygen reduction catalysed by Ni3(hexaiminotriphenylene)2.
Electrochemical oxygen reduction catalysed by Ni3(hexaiminotriphenylene)2.
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DOI：
10.1038/ncomms10942
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发表时间：
2016-03-08
影响因子：
16.6
通讯作者：
Dincă M
中科院分区：
文献类型：
--
作者：
Miner EM;Fukushima T;Sheberla D;Sun L;Surendranath Y;Dincă M
对多相催化剂的结构和电子性质的控制在用于氧还原反应的活性和稳定的非铂族金属电催化剂的有针对性的设计中构成了主要障碍。在这里，我们介绍了Ni 3（HITP）2（HITP=2，3，6，7，10，11-hexaminotriphenylene）作为一个本质上导电的金属有机框架，其功能作为一个明确的，可调的氧还原电催化剂在碱性溶液中。Ni 3（HITP）2表现出与最具活性的非铂族金属电催化剂竞争的氧还原活性和在延长的极化期间的稳定性。正方形平面Ni-N4位点在结构上使人联想到含有M-N4单元的高活性和广泛研究的非铂族金属电催化剂。Ni 3（HITP）2及其类似物联合收割机了金属有机骨架的高结晶度、石墨材料的物理耐久性和导电性以及分子种类的多样但良好控制的合成可及性。这样的性质可以实现作为用于可再生能源应用的燃料电池和电解槽的组分的氧还原电催化剂的目标合成和系统优化。 存在许多非均相氧还原反应催化剂，尽管在这些材料中合成可调谐性是罕见的。在这里，作者报告说，导电金属有机框架作为一个明确的，可调的电催化剂的氧气还原反应在碱性溶液中。
Control over the architectural and electronic properties of heterogeneous catalysts poses a major obstacle in the targeted design of active and stable non-platinum group metal electrocatalysts for the oxygen reduction reaction. Here we introduce Ni3(HITP)2 (HITP=2, 3, 6, 7, 10, 11-hexaiminotriphenylene) as an intrinsically conductive metal-organic framework which functions as a well-defined, tunable oxygen reduction electrocatalyst in alkaline solution. Ni3(HITP)2 exhibits oxygen reduction activity competitive with the most active non-platinum group metal electrocatalysts and stability during extended polarization. The square planar Ni-N4 sites are structurally reminiscent of the highly active and widely studied non-platinum group metal electrocatalysts containing M-N4 units. Ni3(HITP)2 and analogues thereof combine the high crystallinity of metal-organic frameworks, the physical durability and electrical conductivity of graphitic materials, and the diverse yet well-controlled synthetic accessibility of molecular species. Such properties may enable the targeted synthesis and systematic optimization of oxygen reduction electrocatalysts as components of fuel cells and electrolysers for renewable energy applications. There are numerous heterogeneous oxygen reduction reaction catalysts, although synthetic tunability is rare among these materials. Here, the authors report that a conductive metal-organic framework functions as a well-defined, tunable electrocatalyst for the oxygen reduction reaction in alkaline solution.