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cfhxmc木虫 (正式写手)
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ABSTRACT: Organometallic complexes with metal− nitrogen/carbon (M−N/C) coordination are the most important alternatives to precious metal catalysts for oxygen reduction and evolution reactions (ORR and OER) in energy conversion devices. Here, we designed and developed a range of molecule-level graphitic carbon nitride (g-C3N4) coordinated transition metals (M−C3N4) as a new generation of M−N/C catalysts for these oxygen electrode reactions. As a proof-of-concept example, we conducted theoretical evaluation and experimental validation on a cobalt−C 3N4 catalyst with a desired molecular configuration, which possesses comparable electrocatalytic activity to that of precious metal benchmarks for the ORR and OER in alkaline media. The correlation of experimental and computational results confirms that this high activity originates from the precise M−N2 coordination in the g-C3N4 matrix. Moreover, the reversible ORR/ OER activity trend for a wide variety of M−C3N4 complexes has been constructed to provide guidance for the molecular design of this promising class of catalysts. |
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redwang8181
至尊木虫 (职业作家)
- 应助: 16 (小学生)
- 金币: 12250.8
- 散金: 300
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- 虫号: 600394
- 注册: 2008-09-12
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- 专业: 元素化学
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感谢参与，应助指数 +1
cfhxmc: 金币+30, ★有帮助 2017-03-15 23:18:11
感谢参与，应助指数 +1
cfhxmc: 金币+30, ★有帮助 2017-03-15 23:18:11
| 在能量转换的装置中，能够替代氧气还原反应（ORR）和氧气析出反应中（OER）的贵金属催化剂最重要的产品是带有碳/氮元素配位（M-N/C）的有机金属复合物。本文我们开发了一种分子水平的石墨-碳化氮和过渡金属配位的M-N/C新一代催化剂产品作为氧气电极反应的催化剂。以产品开发初期的概念证明阶段为例，我们对带有一个理想分子结构的钴-碳化氮催化剂做了理论评论和试验验证，得出他的电催化活性可以和在碱性介质中对ORR和OER起作用的贵金属催化剂相媲美。试验结果和计算模拟结果的关系确认了其高活性是源于在石墨-碳化氮矩阵中的贵金属和氮气的配位。另外，多种类的金属-碳化氮配位化合物在可逆的ORR/OER反应中使用的趋势为最有希望的一类催化剂的分子设计提供了指导。 |
2楼2017-03-14 17:03:27