Nitrogen-doped carbon shell structure derived from natural leaves as a potential catalyst for oxygen reduction reaction
Nitrogen-doped carbon shell structure derived from natural leaves as a potential catalyst for oxygen reduction reaction
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金属有机骨架 N 掺杂碳包覆 Fe3O4 作为 ORR 高效电催化剂
DOI：
10.1016/j.nanoen.2015.02.031
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发表时间：
2015-04-01
期刊：
影响因子：
17.6
通讯作者：
Wang, Jianji
中科院分区：
文献类型：
--
作者：
Gao, Shuyan;Wei, Xianjun;Wang, Jianji
非贵金属电催化剂对氧还原反应（ORR）的应用福尔斯成为实现成本可承受且高性能的燃料电池和金属/空气电池的中心焦点。最近的第一性原理自旋极化OFT计算模拟了N掺杂C-60富勒烯（N-C-60）上的电催化ORR反应过程，发现O-2可以在N-C-60上化学吸附和还原，表明N-C-60是一种潜在的氢燃料电池阴极催化剂。在这项工作中，一种新的废物资源化的策略，将下降的银杏叶转化为这种新型的ORR电催化剂，氮掺杂富勒烯类碳壳（NDCS），提出。N来源于落下的银杏叶，其中存在10.9-15.5重量%的蛋白质。所得NDCS对四电子途径具有100%的催化选择性，其ORR活性优于大多数现有的碳基催化剂。与商业负载铂的碳催化剂相比，它还显示出对甲醇的耐受性显著改善，并且长期稳定性增强。因此，实验证明，NDCS是一个有前途的未来的ORR催化剂，这是符合量子力学计算。此外，NDCS在锂离子电池中呈现高可逆容量（在0.02 A/g下为750 mA h g（-1））。由于落下的银杏叶很容易获得，我们的研究代表了可持续和低成本能量转换和储存材料的一个令人兴奋的方向。(C)2015爱思唯尔有限公司版权所有。
Implementation of non-precious electrocatalysts towards oxygen reduction reaction (ORR) falls in the central focus on fulfilling cost-affordable and high-performance fuel cells and metal/air batteries. Recent first-principles spin-polarized OFT calculations simulated the electrocatalytic ORR reaction process on N-doped C-60 fullerene (N-C-60) and found that O-2 can be chemisorbed and reduced on N-C-60, indicating that N-C-60 is a potential cathode catalyst for hydrogen fuel cells. In this work, a novel waste-to-resource strategy to convert fallen ginkgo leaves into this new kind of ORR electrocatalyst, nitrogen-doped fullerene-like carbon shell (NDCS), is presented. N is derived from fallen ginkgo leaves, where 10.9-15.5 wt% proteins are present. The obtained NDCS possesses 100% catalysis selectivity towards four-electron pathway, and its ORR activities outperform most of the other existing carbon-based catalysts. It also shows significantly improved tolerance against methanol and enhanced long-term stability, compared with the commercial platinum-loaded carbon catalyst. Thus it is experimentally demonstrated that the NDCS is a promising future ORR catalyst, which is well consistent with the quantum mechanics calculations. Additionally, the NDCS presents a high reversible capacity (750 mA h g(-1) at 0.02 A/g) in Li-ion batteries. Since fallen ginkgo leaves are readily available, our study represents an exciting direction for sustainable and low-cost energy conversion and storage materials. (C) 2015 Elsevier Ltd. All rights reserved.