Wei Yingying, Huang Jingjing, Chen Hong, Zheng Su-Jun, Huang Ren-Wu, Dong Xi-Yan, Li Lin-Ke, Cao Ang, Cai Jinmeng, Zang Shuang-Quan
Green Catalysis Center, and College of Chemistry, Zhengzhou University, Zhengzhou, 450001, China.
College of Chemistry and Chemical Engineering, Henan Polytechnic University, Jiaozuo, 454003, China.
Adv Mater. 2024 Jul;36(30):e2404774. doi: 10.1002/adma.202404774. Epub 2024 May 16.
Green ammonia synthesis through electrocatalytic nitrate reduction reaction (eNORR) can serve as an effective alternative to the traditional energy-intensive Haber-Bosch process. However, achieving high Faradaic efficiency (FE) at industrially relevant current density in neutral medium poses significant challenges in eNORR. Herein, with the guidance of theoretical calculation, a metallic CoNi-terminated catalyst is successfully designed and constructed on copper foam, which achieves an ammonia FE of up to 100% under industrial-level current density and very low overpotential (-0.15 V versus reversible hydrogen electrode) in a neutral medium. Multiple characterization results have confirmed that the maintained metal atom-terminated surface through interaction with copper atoms plays a crucial role in reducing overpotential and achieving high current density. By constructing a homemade gas stripping and absorption device, the complete conversion process for high-purity ammonium nitrate products is demonstrated, displaying the potential for practical application. This work suggests a sustainable and promising process toward directly converting nitrate-containing pollutant solutions into practical nitrogen fertilizers.
通过电催化硝酸盐还原反应(eNORR)合成绿色氨可以作为传统能源密集型哈伯-博施法的有效替代方案。然而,在中性介质中,在工业相关电流密度下实现高法拉第效率(FE)对eNORR来说是重大挑战。在此,在理论计算的指导下,成功地在泡沫铜上设计并构建了一种金属钴镍端基催化剂,该催化剂在中性介质中,在工业级电流密度下实现了高达100%的氨FE,且过电位极低(相对于可逆氢电极-0.15 V)。多项表征结果证实,通过与铜原子相互作用保持的金属原子端基表面在降低过电位和实现高电流密度方面起着关键作用。通过构建自制的气体汽提和吸收装置,展示了高纯度硝酸铵产品的完整转化过程,显示了实际应用潜力。这项工作提出了一种可持续且有前景的方法,可将含硝酸盐的污染溶液直接转化为实用氮肥。