Deng Wenhui, Luo Yuhao, Wu Kewei, Wang Yanqiu, Liu Hongtao, Qiu Xiaoqing, Liu Kang, Fu Junwei, Li Wenzhang, Liu Min
College of Chemistry and Chemical Engineering, Central South University, Changsha 410083, China.
Hunan Joint International Research Center for Carbon Dioxide Resource Utilization, School of Physics, Central South University, Changsha 410083, China.
J Phys Chem Lett. 2025 Jun 19;16(24):6202-6211. doi: 10.1021/acs.jpclett.5c01105. Epub 2025 Jun 12.
Carbon nanotubes (CNTs) have garnered significant attention due to their large specific surface area and efficient mass transfer properties. However, the construction of well-ordered CNT catalysts with high-efficiency bifunctional oxygen electrocatalytic activity remains a significant challenge. Herein, the uniform size of CNTs with high-density dual-active-site Co/CoN motifs (A-Co/Co-NC) is rationally designed and fabricated through an in situ metal-ligand anchoring method (N → Co) followed by a pyrolysis process. The selected 2,6-diaminopurine (DAP) can anchor and disperse Co ions in N sites, which will form uniform CNTs with Co NPs and CoN active sites during the pyrolysis process. Theoretical calculation and in situ characteristics clearly proved that Co NP works as an OER active unit and that CoN acts as an ORR active site. Benefiting from the high-density dual-active-site Co/CoN motifs, the A-Co/Co-NC catalyst displays superior bifunctional performance ( = 0.76 V). Therefore, the A-Co/Co-NC-based zinc-air battery (ZAB) exhibits distinguished reversibility. Remarkably, the A-Co/Co-NC-based Al-air battery (AAB) has a high power density (129.12 mW cm). This work provides a feasible design concept to obtain well-organized CNTs with highly dispersed active sites.
碳纳米管（CNTs）因其大的比表面积和高效的传质性能而备受关注。然而，构建具有高效双功能氧电催化活性的有序碳纳米管催化剂仍然是一个重大挑战。在此，通过原位金属-配体锚定法（N→Co），然后进行热解过程，合理设计并制备了具有高密度双活性位点Co/CoN基序（A-Co/Co-NC）的尺寸均匀的碳纳米管。所选用的2,6-二氨基嘌呤（DAP）可将Co离子锚定并分散在N位点上，在热解过程中会形成具有Co纳米颗粒和CoN活性位点的均匀碳纳米管。理论计算和原位表征清楚地证明，Co纳米颗粒作为析氧反应（OER）活性单元，而CoN作为氧还原反应（ORR）活性位点。受益于高密度双活性位点Co/CoN基序，A-Co/Co-NC催化剂表现出优异的双功能性能（=0.76V）。因此，基于A-Co/Co-NC的锌空气电池（ZAB）表现出卓越的可逆性。值得注意的是，基于A-Co/Co-NC的铝空气电池（AAB）具有高功率密度（129.12mW/cm²）。这项工作为获得具有高度分散活性位点的有序碳纳米管提供了一种可行的设计概念。
