The synergistic effect of carbon edges and dopants towards efficient oxygen reduction reaction.
The synergistic effect of carbon edges and dopants towards efficient oxygen reduction reaction.
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碳边缘和掺杂剂对有效氧还原反应的协同效应。
DOI：
10.1016/j.jcis.2021.11.069
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发表时间：
2021-11
影响因子：
9.9
通讯作者：
Tingting Xiang;Zirui Wu;Zhongti Sun;Chao Cheng;Wenlong Wang;Zhenzhong Liu;Juan-Yu Yang;Bing Li-Bin
中科院分区：
文献类型：
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作者：
Tingting Xiang;Zirui Wu;Zhongti Sun;Chao Cheng;Wenlong Wang;Zhenzhong Liu;Juan-Yu Yang;Bing Li-Bin
引入外来原子和增加边缘含量是激活纳米碳氧还原反应（ORR）的两种有效途径。为了进一步提高其固有活性并探索潜在的ORR机制，选择石墨烯纳米带（GNRs）作为理想的催化剂模型。理论模拟表明，通过杂原子掺杂和边缘位置的协同作用，可以显著提高ORR活性。受此启发，通过碳纳米管的氧化解链，然后用尿素掺入氮来合成N-GNRs。通过高分辨透射电子显微镜和X射线光电子能谱分别检测到了充分的边缘和氮掺杂位点。结果，N-GNRs在起始和半波电位、塔菲尔斜率、电子转移数和甲醇耐受性方面表现出比GNRs（没有掺杂的对照样品）或N-CNT（没有丰富边缘的对照样品）显著更高的ORR性质，简单地阐明了掺杂剂和边缘之间的协同作用的意义。因此，这项工作提供了一个简单而有效的策略来制造高性能的氧还原催化剂。
Decoration with alien atoms and increasing the edge content are two valid ways to activate the oxygen reduction reaction (ORR) property of nanocarbons. To further enhance their intrinsic activity and explore the underlying ORR mechanism, graphene nanoribbons (GNRs) were selected as an ideal catalyst model. Theoretical simulations have predicted that with the synergistic effect between heteroatom-doping and edge sites, the ORR activity can be significantly improved. Inspired by this,N-GNRs were synthesized via the oxidative unzipping of CNTs followed by nitrogen incorporation with urea. Ample edges and nitrogen doping sites were detected by high-resolution transmission electron microscopy and X-ray photoelectron spectroscopy, respectively. As a result,N-GNRs exhibited remarkably higher ORR properties in terms of onset and half-wave potentials, Tafel slopes, electron transfer number and methanol tolerance than either GNRs, the control sample without doping, orN-CNTs, the control sample without abundant edges, simply clarifying the significance of synergy between dopants and edges. Thus, this work provides a simple but efficient strategy to fabricate high-performance oxygen reduction catalysts.