Li Chunxiao, Xu Wanli, Ye Liangwen, Liu Jingjun, Wang Feng
State Key Laboratory of Chemical Resource Engineering, Beijing Key Laboratory of Electrochemical Process and Technology for, Materials, Beijing University of Chemical Technology, Beijing, 100029, P. R. China.
Chemistry. 2021 Apr 7;27(20):6247-6253. doi: 10.1002/chem.202005112. Epub 2021 Mar 5.
Metal-free carbons have been regarded as one of the promising materials alternatives to precious-metal catalysts for oxygen reduction reaction (ORR) due to their high activity and stability. In this paper, well-defined N-doped hollow carbons (NHCs) are firstly synthesized by using an ammonia-based hydrothermal synthesis that is environmentally friendly and suitable for mass production in industry and a commercial black carbon as raw material. Moreover, the shell thickness of the NHCs can be easily tuned by this hydrothermal strategy. Zn-air battery test results reveal shell thickness-dependent activity and durability for ORR over the NHCs, which exceeds that obtained by commercial Pt/C (20 wt %). The enhanced battery performance can be attributed to the curvature-activated N-C moieties on the hollow carbon surface, which served as the main active sites for ORR as evidenced by DFT calculations. The proposed approach may open a way for designing curved hollow carbons with high graphitization degree and dopant nitrogen level for metal-air batteries or fuel cells.
由于无金属碳具有高活性和稳定性,它们被视为氧还原反应(ORR)中贵金属催化剂的一种有前景的材料替代品。在本文中,首先以环境友好且适合工业大规模生产的氨基水热合成法和商业黑碳为原料,合成了明确的氮掺杂空心碳(NHCs)。此外,通过这种水热策略可以轻松调节NHCs的壳厚度。锌空气电池测试结果表明,NHCs上ORR的活性和耐久性与壳厚度有关,超过了商业Pt/C(20 wt %)的性能。电池性能的提高可归因于空心碳表面的曲率激活N-C部分,DFT计算证明其作为ORR的主要活性位点。所提出的方法可能为设计用于金属空气电池或燃料电池的具有高石墨化程度和掺杂氮水平的弯曲空心碳开辟一条道路。