氨的环境电合成：电极孔隙率与成分工程
Ambient Electrosynthesis of Ammonia: Electrode Porosity and Composition Engineering.
作者信息
Wang Hong, Wang Lu, Wang Qiang, Ye Shuyang, Sun Wei, Shao Yue, Jiang Zhiping, Qiao Qiao, Zhu Yimei, Song Pengfei, Li Debao, He Le, Zhang Xiaohong, Yuan Jiayin, Wu Tom, Ozin Geoffrey A
机构信息
Key Laboratory of Functional Polymer Materials of the Ministry of Education, Institute of Polymer Chemistry, College of Chemistry, Nankai University, Tianjin, 300071, P. R. China.
Materials Chemistry and Nanochemistry Research Group, Solar Fuels Cluster, Centre for Inorganic and Polymeric Nanomaterials, Departments of Chemistry, Chemical Engineering and Applied Chemistry, and Electrical and Computing Engineering, University of Toronto, 80 St. George Street, Toronto, Ontario, M5S3H6, Canada.
出版信息
Angew Chem Int Ed Engl. 2018 Sep 17;57(38):12360-12364. doi: 10.1002/anie.201805514. Epub 2018 Jul 9.
Ammonia, a key precursor for fertilizer production, convenient hydrogen carrier, and emerging clean fuel, plays a pivotal role in sustaining life on Earth. Currently, the main route for NH synthesis is by the heterogeneous catalytic Haber-Bosch process (N +3 H →2 NH ), which proceeds under extreme conditions of temperature and pressure with a very large carbon footprint. Herein we report that a pristine nitrogen-doped nanoporous graphitic carbon membrane (NCM) can electrochemically convert N into NH in an acidic aqueous solution under ambient conditions. The Faradaic efficiency and rate of production of NH on the NCM electrode reach 5.2 % and 0.08 g m h , respectively. Functionalization of the NCM with Au nanoparticles dramatically enhances these performance metrics to 22 % and 0.36 g m h , respectively. As this system offers the potential to be scaled to industrial levels it is highly likely that it might displace the century-old Haber-Bosch process.
氨是肥料生产的关键前体、便捷的氢载体以及新兴的清洁燃料，在维持地球生命方面发挥着关键作用。目前，合成氨的主要途径是通过多相催化哈伯-博施法（N₂ + 3H₂ → 2NH₃），该过程在极端的温度和压力条件下进行，碳足迹非常大。在此，我们报告一种原始的氮掺杂纳米多孔石墨碳膜（NCM）能够在环境条件下于酸性水溶液中将氮气电化学转化为氨。在NCM电极上氨的法拉第效率和产率分别达到5.2%和0.08 g m⁻² h⁻¹。用金纳米颗粒对NCM进行功能化处理可将这些性能指标分别显著提高到22%和0.36 g m⁻² h⁻¹。由于该系统具有扩大到工业规模的潜力，极有可能取代有百年历史的哈伯-博施法。
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