Ambient ammonia synthesis via palladium-catalyzed electrohydrogenation of dinitrogen at low overpotential
By Jun Wang, Liang Yu, Lin Hu, Gang Chen, H. Xin, Xiaofeng Feng. Nature Communications, 2018
642 citations recorded by the source corpus.
Electrochemical reduction of N2 to NH3 provides an alternative to the Haber−Bosch process for sustainable, distributed production of NH3 when powered by renewable electricity. However, the development of such process has been impeded by the lack of efficient electrocatalysts for N2 reduction. Here we report efficient electroreduction of N2 to NH3 on palladium nanoparticles in phosphate buffer solution under ambient conditions, which exhibits high activity and selectivity with an NH3 yield rate of ~4.5 μg mg−1Pd h−1 and a Faradaic efficiency of 8.2% at 0.1 V vs. the reversible hydrogen electrode (corresponding to a low overpotential of 56 mV), outperforming other catalysts including gold and platinum. Density functional theory calculations suggest that the unique activity of palladium originates from its balanced hydrogen evolution activity and the Grotthuss-like hydride transfer mechanism on α-palladium hydride that lowers the free energy barrier of N2 hydrogenation to *N2H, the rate-limiting step for NH3 electrosynthesis. The Haber-Bosch process, producing NH3 from N2, is a crucial yet energetically demanding reaction, inspiring interest in the exploration of ambient-condition alternatives. Here, authors develop a palladium electrocatalyst that shows a high selectivity and activity for N2 reduction to NH3.
Subfields: Catalysis, Computer Networks and Communications, Renewable Energy, Sustainability and the Environment
View Paper: https://www.semanticscholar.org/paper/11542d48979bb13366da65ff80ef1a1a8974b696
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- Wenjun Zhang
- Xiaolan Xue
- Yi Hu
- Peiyang Zhao
- Changzeng Yan
- Renpeng Chen
- Songyuan Yang
- Zhong Jin
Citations in the corpus
- Review on photocatalytic and electrocatalytic artificial nitrogen fixation for ammonia synthesis at mild conditions: Advances, challenges and perspectives (2019, background): “2) to suppress the competing HER process [121], possibly because the high energy barriers for mass and charge transfer in phosphate buffer solution is not conducive to the kinetics of HER.”