Tang Cheng, Qiao Shi-Zhang
School of Chemical Engineering, The University of Adelaide, Adelaide, SA 5005, Australia.
Chem Soc Rev. 2019 Jun 17;48(12):3166-3180. doi: 10.1039/c9cs00280d.
The efficient activation of dinitrogen for the production of ammonia plays a crucial role in our modern society, considering the significant impact of ammonia on food, chemicals, and energy. As an attractive alternative to the century-old Haber-Bosch process which is responsible for 1-2% of global energy consumption, utilization of half the hydrogen produced globally, and ∼1% of global energy-related CO2 emissions, the ambient electrocatalytic nitrogen reduction reaction has attracted tremendous interest during the past few years. Some achievements have revealed the possibility of this process, but have also identified great challenges. The activity and selectivity of the nitrogen reduction reaction are fundamentally limited by competing hydrogen evolution and nitrogen scaling relations, while low production rates and ubiquitous contaminants plague experimental practices. Aiming toward higher accuracy and reproducibility of claimed results, and more meaningful, impactful, and insightful research, this tutorial review summarizes the present status and challenges in the study of ambient electrocatalytic nitrogen reduction, followed by a thorough discussion of various experimental parameters. We then recommend a series of protocols and best practices for experiments, and also highlight some potential directions for future research in this exciting and important field.
考虑到氨对食品、化学品和能源的重大影响,二氮的高效活化以生产氨在我们现代社会中起着至关重要的作用。作为有百年历史的哈伯-博施法(该方法消耗全球1%-2%的能源,消耗全球一半的氢气产量,产生全球约1%的与能源相关的二氧化碳排放)的一种有吸引力的替代方法,常压电催化氮还原反应在过去几年中引起了极大的关注。一些成果揭示了这一过程的可能性,但也发现了巨大的挑战。氮还原反应的活性和选择性从根本上受到竞争性析氢和氮标度关系的限制,而低产率和普遍存在的污染物困扰着实验实践。为了提高所宣称结果的准确性和可重复性,以及开展更有意义、更具影响力和更有洞察力的研究,本综述总结了常压电催化氮还原研究的现状和挑战,随后对各种实验参数进行了深入讨论。我们还推荐了一系列实验方案和最佳实践,并强调了这个令人兴奋且重要的领域未来研究的一些潜在方向。