College of Material and Chemical Engineering, Institute of New Energy Science and Technology, School of Future Hydrogen Energy Technology, Zhengzhou University of Light Industry, Zhengzhou, 450001, P. R. China.
Adv Sci (Weinh). 2023 Mar;10(8):e2205786. doi: 10.1002/advs.202205786. Epub 2023 Jan 22.
A defect-rich 2D p-n heterojunction, Co Ni (HITP) /BNSs-P (HITP: 2,3,6,7,10,11-hexaiminotriphenylene), is constructed using a semiconductive metal-organic framework (MOF) and boron nanosheets (BNSs) by in situ solution plasma modification. The heterojunction is an effective catalyst for the electrocatalytic nitrogen reduction reaction (eNRR) under ambient conditions. Interface engineering and plasma-assisted defects on the p-n Co Ni (HITP) /BNSs-P heterojunction led to the formation of both Co-N and B…O dual-active sites. As a result, Co Ni (HITP) /BNSs-P has a high NH yield of 128.26 ± 2.27 µg h mg and a Faradaic efficiency of 52.92 ± 1.83% in 0.1 m HCl solution. The catalytic mechanism for the eNRR is also studied by in situ FTIR spectra and DFT calculations. A Co Ni (HITP) /BNSs-P-based Zn-N battery achieved an unprecedented power output with a peak power density of 5.40 mW cm and an energy density of 240 mA h g in 0.1 m HCl. This study establishes an efficient strategy for the rational design, using defect and interfacial engineering, of advanced eNRR catalysts for ammonia synthesis under ambient conditions.
采用半导体金属有机骨架（MOF）和硼纳米片（BNSs）原位溶液等离子体改性，构建了富含缺陷的二维 p-n 异质结 Co Ni （HITP）/BNSs-P（HITP：2,3,6,7,10,11-六氨基三苯）。该异质结在环境条件下是电催化氮气还原反应（eNRR）的有效催化剂。p-n Co Ni （HITP）/BNSs-P 上的界面工程和等离子体辅助缺陷导致了 Co-N 和 B…O 双活性位的形成。因此，Co Ni （HITP）/BNSs-P 在 0.1 m HCl 溶液中具有 128.26±2.27 µg h mg 的高 NH 3 产率和 52.92±1.83%的法拉第效率。还通过原位傅里叶变换红外光谱和 DFT 计算研究了 eNRR 的催化机制。基于 Co Ni （HITP）/BNSs-P 的 Zn-N 电池在 0.1 m HCl 中实现了前所未有的功率输出，峰值功率密度为 5.40 mW cm，能量密度为 240 mA h g。该研究为在环境条件下合成氨的先进 eNRR 催化剂的合理设计建立了一种有效的策略，利用缺陷和界面工程。
