Wang Yunhao, Sun Mingzi, Zhou Jingwen, Xiong Yuecheng, Zhang Qinghua, Ye Chenliang, Wang Xixi, Lu Pengyi, Feng Tianyi, Hao Fengkun, Liu Fu, Wang Juan, Ma Yangbo, Yin Jinwen, Chu Shengqi, Gu Lin, Huang Bolong, Fan Zhanxi
Department of Chemistry, City University of Hong Kong, Hong Kong 999077, China.
Department of Applied Biology and Chemical Technology, The Hong Kong Polytechnic University, Hung Hom, Kowloon, Hong Kong 999077, China.
Proc Natl Acad Sci U S A. 2023 Aug 8;120(32):e2306461120. doi: 10.1073/pnas.2306461120. Epub 2023 Jul 31.
Electrochemical nitrate reduction reaction (NORR) to ammonia has been regarded as a promising strategy to balance the global nitrogen cycle. However, it still suffers from poor Faradaic efficiency (FE) and limited yield rate for ammonia production on heterogeneous electrocatalysts, especially in neutral solutions. Herein, we report one-pot synthesis of ultrathin nanosheet-assembled RuFe nanoflowers with low-coordinated Ru sites to enhance NORR performances in neutral electrolyte. Significantly, RuFe nanoflowers exhibit outstanding ammonia FE of 92.9% and yield rate of 38.68 mg h mg (64.47 mg h mg) at -0.30 and -0.65 V (vs. reversible hydrogen electrode), respectively. Experimental studies and theoretical calculations reveal that RuFe nanoflowers with low-coordinated Ru sites are highly electroactive with an increased d-band center to guarantee efficient electron transfer, leading to low energy barriers of nitrate reduction. The demonstration of rechargeable zinc-nitrate batteries with large-specific capacity using RuFe nanoflowers indicates their great potential in next-generation electrochemical energy systems.
电化学硝酸盐还原反应（NORR）制氨被视为平衡全球氮循环的一种有前景的策略。然而，在非均相电催化剂上，尤其是在中性溶液中，它仍然存在法拉第效率（FE）低和氨生成产率有限的问题。在此，我们报道了一种一锅法合成具有低配位Ru位点的超薄纳米片组装RuFe纳米花，以提高其在中性电解质中的NORR性能。值得注意的是，RuFe纳米花在-0.30和-0.65 V（相对于可逆氢电极）时分别表现出92.9%的出色氨法拉第效率和38.68 mg h mg（64.47 mg h mg）的产率。实验研究和理论计算表明，具有低配位Ru位点的RuFe纳米花具有高电活性，其d带中心增加，保证了有效的电子转移，导致硝酸盐还原的能垒较低。使用RuFe纳米花的具有大比容量的可充电硝酸锌电池的展示表明了它们在下一代电化学能源系统中的巨大潜力。
