Dong-Li Meng, Tao-Tao Liu, Ming-Hui Wu, Jing-Wen He, Shao-Wu Du and Yuan-Biao Huang
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引用次数: 0
摘要
掺杂均匀的杂原子双掺杂多孔碳框架具有可调的化学和电子结构,因此要实现高效的氧还原反应(ORR)活性,开发这种框架是非常理想的。在此,研究人员选择 1,3-双(4-氰基苯基)氯化咪唑作为构筑基块,通过自下而上的策略,以简便、可控的方式制备了包含氮/氯碱双掺杂多孔碳网络的多孔共价三嗪基框架(CTFs)。与基准商用 20 wt% Pt/C 催化剂相比,氮/络氨酸双掺杂催化剂 CCTF-700 表现出优异的 ORR 性能,起始电位和半波电位(0.85 V vs. RHE)更正,扩散限制电流密度更高,稳定性显著提高。值得一提的是,CCTF-700 是所有已报道的碱性条件下无金属电催化剂中 ORR 性能最好的催化剂之一。这项工作为采用可控、可靠的策略制备用于能源转换的高效杂原子双掺杂碳催化剂铺平了道路。
Boosting the oxygen reduction activity of non-metallic catalysts via geometric and electronic engineering through nitrogen and chlorine dual-doping†
The development of heteroatom dual-doped porous carbon frameworks with uniform doping is highly desirable for achieving highly efficient oxygen reduction reaction (ORR) activity, due to their tunable chemical and electronic structures. Herein, porous covalent triazine-based frameworks (CTFs) incorporating nitrogen/chorine dual-doped porous carbon networks were fabricated by selecting 1,3-bis(4-cyanophenyl) imidazolium chloride as a building block, in a facile and controllable way via a bottom-up strategy. The resulting nitrogen/chorine dual-doped catalyst CCTF-700 exhibits excellent ORR performance with a more positive onset and half-wave potential (0.85 V vs. RHE), higher diffusion-limited current density and significantly improved stability in comparison with the benchmark commercial 20 wt% Pt/C catalyst. It is worth mentioning that CCTF-700 shows one of the best ORR performances among all the reported metal-free electrocatalysts under alkaline conditions. This work paves the way for a controllable and reliable strategy to craft highly efficient heteroatom dual-doped carbon catalysts for energy conversion.
期刊介绍:
Dalton Transactions is a journal for all areas of inorganic chemistry, which encompasses the organometallic, bioinorganic and materials chemistry of the elements, with applications including synthesis, catalysis, energy conversion/storage, electrical devices and medicine. Dalton Transactions welcomes high-quality, original submissions in all of these areas and more, where the advancement of knowledge in inorganic chemistry is significant.