He Jiawei, Zhao Yuying, Li Yang, Yuan Qixin, Wu Yuhan, Wang Kui, Sun Kang, Wu Jingjie, Jiang Jianchun, Zhang Baohua, Wang Liang, Fan Mengmeng
Jiangsu Co-Innovation Center of Efficient Processing and Utilization of Forest Resources, International Innovation Center for Forest Chemicals and Materials, College of Chemical Engineering, Nanjing Forestry University, Nanjing, 210037, People's Republic of China.
Key Lab of Biomass Energy and Material, Jiangsu Province; Jiangsu Co-Innovation Center of Efficient Processing and Utilization of Forest Resources, Institute of Chemical Industry of Forest Products, Chinese Academy of Forestry, Nanjing, 210042, People's Republic of China.
Nanomicro Lett. 2025 Apr 18;17(1):221. doi: 10.1007/s40820-025-01725-0.
Natural biomass-derived carbon material is one promising alternative to traditional graphene-based catalyst for oxygen electrocatalysis. However, their electrocatalytic performance were constrained by the limited modulating strategy. Herein, using N-doped commercial coconut shell-derived activated carbon (AC) as catalyst model, the controllably enhanced sp-C domains, through an flash Joule heating process, effectively improve the edge defect density and overall graphitization degree of AC catalyst, which tunes the electronic structure of N configurations and accelerates electron transfer, leading to excellent oxygen reduction reaction performance (half-wave potential of 0.884 V, equivalent to commercial 20% Pt/C, with a higher kinetic current density of 5.88 mA cm) and oxygen evolution reaction activity (overpotential of 295 mV at 10 mA cm). In a Zn-air battery, the catalyst shows outstanding cycle stability (over 1200 h) and a peak power density of 121 mW cm, surpassing commercial Pt/C and RuO catalysts. Density functional theory simulation reveals that the enhanced catalytic activity arises from the axial regulation of local sp-C domains. This work establishes a robust strategy for sp-C domain modulation, offering broad applicability in natural biomass-based carbon catalysts for electrocatalysis.
天然生物质衍生的碳材料是用于氧电催化的传统石墨烯基催化剂的一种有前途的替代品。然而，它们的电催化性能受到有限的调控策略的限制。在此，以氮掺杂的商业椰壳衍生活性炭（AC）作为催化剂模型，通过快速焦耳加热过程可控地增强sp-C域，有效提高了AC催化剂的边缘缺陷密度和整体石墨化程度，从而调节了N构型的电子结构并加速了电子转移，导致优异的氧还原反应性能（半波电位为0.884 V，相当于商业20% Pt/C，具有更高的动力学电流密度5.88 mA cm）和析氧反应活性（在10 mA cm下过电位为295 mV）。在锌空气电池中，该催化剂表现出出色的循环稳定性（超过1200小时）和121 mW cm的峰值功率密度，超过了商业Pt/C和RuO催化剂。密度泛函理论模拟表明，增强的催化活性源于局部sp-C域的轴向调控。这项工作建立了一种强大的sp-C域调控策略，在基于天然生物质的碳催化剂用于电催化方面具有广泛的适用性。
