Lai Jinhua, Li Tan, Ding Liang-Xin, Chen Gao-Feng, Wang Haihui
Guangdong Provincial Key Lab of Green Chemical Product Technology, School of Chemistry and Chemical Engineering, South China University of Technology, Guangzhou, 510640, China.
Faculty of Chemical Engineering, Kunming University of Science and Technology, Kunming, 650500, China.
ChemSusChem. 2025 Mar 15;18(6):e202401912. doi: 10.1002/cssc.202401912. Epub 2024 Nov 12.
The carbon-free electrocatalytic nitrogen reduction reaction (NRR) is an alternative technology to the current Haber-Bosch method, that can be conducted under ambient conditions, and directly converting water and nitrogen (N₂) into ammonia (NH₃). However, the limited activity and selectivity of NH₃ electrosynthesis hinder the practical applications of NRR. In this study, we present a novel type of electrocatalyst called boridene nanosheets enriched with metal vacancies that are specifically designed for efficient electrocatalytic NRR under ambient conditions. Electrochemical testing in a 0.1 M phosphate-buffered saline (PBS) electrolyte demonstrates that boridene exhibits a high Faradaic efficiency of 66.7 % for NH₃ production at -0.2 V vs. RHE, with a maximum NH₃ yield rate of 23.6 μg h mg at -0.4 V vs. RHE. Durability tests show that boridene maintains significant stability throughout multiple cycles of NRR. Mechanistic insights are obtained through in situ Fourier transform infrared spectroscopy, revealing that boridene exhibits a preference for the distal pathway during the process of NRR. These findings highlight the potential of boridene as an efficient and stable catalyst for sustainable NH₃ synthesis.
无碳电催化氮还原反应（NRR）是当前哈伯-博施法的一种替代技术，该反应可在环境条件下进行，能直接将水和氮气（N₂）转化为氨（NH₃）。然而，氨电合成的活性和选择性有限，阻碍了NRR的实际应用。在本研究中，我们提出了一种新型电催化剂，即富含金属空位的硼烯纳米片，其专为在环境条件下高效电催化NRR而设计。在0.1 M磷酸盐缓冲盐水（PBS）电解质中进行的电化学测试表明，相对于可逆氢电极（RHE），硼烯在-0.2 V时对氨生成表现出66.7%的高法拉第效率，在相对于RHE为-0.4 V时，最大氨产率为23.6 μg h mg。耐久性测试表明，硼烯在多个NRR循环中保持显著的稳定性。通过原位傅里叶变换红外光谱获得了机理见解，揭示了硼烯在NRR过程中对远端路径表现出偏好。这些发现突出了硼烯作为可持续氨合成的高效稳定催化剂的潜力。
