Defective N/S-Codoped 3D Cheese-Like Porous Carbon Nanomaterial toward Efficient Oxygen Reduction and Zn-Air Batteries.
Defective N/S-Codoped 3D Cheese-Like Porous Carbon Nanomaterial toward Efficient Oxygen Reduction and Zn-Air Batteries.
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DOI：
10.1002/smll.201800563
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发表时间：
2018-05
期刊：
影响因子：
13.3
通讯作者：
Jiawei Zhu;Wenqiang Li;Shuaihui Li;Jian Zhang;Huang Zhou;Chengtian Zhang;Jianan Zhang;Shichun Mu-Shich
中科院分区：
文献类型：
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作者：
Jiawei Zhu;Wenqiang Li;Shuaihui Li;Jian Zhang;Huang Zhou;Chengtian Zhang;Jianan Zhang;Shichun Mu-Shich
开发一种简便、经济的方法来合成具有优异结构和功能特性的碳基纳米材料已成为能源转换和储存领域最具吸引力的课题之一。在这项研究中，密度泛函理论计算结果揭示了高氧还原反应（ORR）活性的起源，其主要来源于固有缺陷和杂原子掺杂剂（例如，N，S），其调节碳基质的带隙和电荷密度分布。在第一性原理预测的指导下，以超轻生物质废弃物为碳、氮、硫元素的前驱体，成功设计并构建了一种富含缺陷且N/S双掺杂的干酪状多孔碳纳米材料。在此，本征缺陷是根据碱和氨活化而巧妙地产生的。电化学测试表明，该材料具有与商业Pt/C催化剂相当的ORR活性（E1/2 = 0.835 V），沿着具有优异的耐久性和在碱性介质中的甲醇耐受性。此外，作为阴极催化剂，它显示出高的锌-空气电池性能。该催化剂优异的ORR活性可归因于其独特的3D多孔结构、丰富的固有缺陷和碳基质中高含量的活性杂原子掺杂剂。
Developing a facile and cost-efficient method to synthesize carbon-based nanomaterials possessing excellent structural and functional properties has become one of the most attractive topics in energy conversion and storage fields. In this study, density functional theory calculation results reveal the origin of high oxygen reduction reaction (ORR) activity predominantly derived from the synergistic effect of intrinsic defects and heteroatom dopants (e.g., N, S) that modulate the bandgap and charge density distribution of carbon matrix. Under the guidance of the first-principle prediction, by using ultralight biomass waste as precursor of C, N, and S elements, a defect-rich and N/S dual-doped cheese-like porous carbon nanomaterial is successfully designed and constructed. Herein, the intrinsic defects are artfully generated in terms of alkaline and ammonia activation. The electrochemical measurements display that such a material owns a comparable ORR activity (E1/2 = 0.835 V) to the commercial Pt/C catalyst, along with splendid durability and methanol tolerance in alkali media. Furthermore, as cathode catalyst, it displays a high Zn-air battery performance. The excellent ORR activity of the catalyst can be attributed to its unique 3D porous architecture, abundant intrinsic defects, and high-content active heteroatom dopants in the carbon matrix.