Understanding the Roles of Nitrogen Configurations in Hydrogen Evolution: Trace Atomic Cobalt Boosts the Activity of Planar Nitrogen-Doped Graphene
Understanding the Roles of Nitrogen Configurations in Hydrogen Evolution: Trace Atomic Cobalt Boosts the Activity of Planar Nitrogen-Doped Graphene
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了解氮构型在析氢中的作用：微量原子钴增强平面氮掺杂石墨烯的活性
DOI：
10.1021/acsenergylett.8b00522
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发表时间：
2018
影响因子：
22
通讯作者：
Wei Zidong
中科院分区：
文献类型：
--
作者：
Wang Huaixin;Yang Na;Li Wei;Ding Wei;Chen Ke;Li Jing;Li Li;Wang Jianchuan;Jiang Jinxia;Jia Fengqiu;Wei Zidong
揭示氮掺杂石墨烯（NG）中氮构型的确切作用以及氮构型的精确控制对于实现其在清洁能源技术中的先进功能至关重要。在此，我们第一次建立了NG的析氢反应（HER）活性显示一定的趋势，由于其氮的配置，这是选择性地产生通过使用具有不同层间距和功能的层状结构的蒙脱土（MMT）调制的Co 2+，Ni 2+，Na+，和H+离子。我们发现，在三种类型的N，即，吡啶、吡咯和季铵N的催化活性最高，而引入微量钴原子后，平面（吡啶和吡咯）N的催化活性最高。相比之下，当涉及痕量原子Ni以取代Co时，前者导致NG催化剂的HER活性严重降低。密度泛函理论计算进一步提高了...
Revealing the exact roles of nitrogen configurations and precise control of the nitrogen configuration in nitrogen-doped graphene (NG) are extremely important for realizing its advanced functions in clean energy technologies. Herein, for the first time, we established that the hydrogen evolution reaction (HER) activities of NG display definite trends due to its nitrogen configurations, which were selectively generated by using layer-structured montmorillonite (MMT) with different layer distances and functions modulated by Co2+, Ni2+, Na+, and H+ ions. We found that among the three types of N, i.e., pyridine, pyrrolic, and quaternary N, quaternary N is the most active one for HER in a metal-free NG catalyst, whereas with an introduction of trace atomic cobalt, the planar (pyridine and pyrrolic) N becomes the better one. In contrast, when trace atomic Ni is involved to replace the Co, the former results in heavily depressed HER activities for the NG catalyst. Density functional theory calculations further r...