Characterisation and testing of novel electrodes and electrolytes for efficient N2 reduction

目前的氨生产方法，Haber-Bosch工艺，消耗了100亿美元的化石燃料，并排放了大量的温室气体。以可再生能源为动力的电化学氨合成可以提供一种绿色解决方案。然而，存在许多重要的污染源，使合成的定量证明复杂化。此外，任何对氮还原有活性的催化剂都会优先生成氢[1]。该项目将建立在最近首次使用锂介导路线和有机电解质[2]进行氨合成的定量证明的基础上。目的是利用从电池科学转化而来的尖端表征技术来理解电极和电解质的作用。磁控溅射沉积室直接连接到手套箱将用于生长高反应性薄膜电极。这些可以迅速转移到电化学电池，最大限度地减少有害氧化。手套箱将包含一个超灵敏质谱仪，用于测量现场气体演化，以前从未用于非水电化学，以及一个红外光谱仪，用于探测中间体。这些operando技术将辅以各种非原位表征方法，包括二次离子质谱，核磁共振光谱，拉曼光谱和电化学原子力显微镜。新兴的分子尺度图像将阐明高效电化学合成氨的途径尼尔森，A.和斯蒂芬斯，i.e.l。“可持续N2还原”的研究需要对可持续生产燃料和化学品(eds J.K. Norskov, A·拉蒂默& C·F·狄更斯)49 (Energy-X,布鲁塞尔,比利时,2019)[2]安徒生,S . Z。绞痛,V,杨,年代,Schwalbe牌,J . A。Nielander, A·C。McEnaney, J . M。Enemark-Rasmussen, K,贝克,J·G。辛格,A·R。罗尔,b。,文化建设,M . J。布莱尔,S . J。Mezzavilla,年代,Kibsgaard, J。,Vesborg, p C K。Cargnello, M,弯曲,F。,Jaramillo, t·F。斯蒂芬斯,即L, Norskov,J. K. & J. K. Chorkendorff， I.自然，57,504,（2019）

The current method for ammonia production, the Haber-Bosch process, consumes >1% of fossil fuels and emits vast quantities of greenhouse gas. Electrochemical ammonia synthesis, powered by renewable energy, could provide a green solution. However, there exist many significant contamination sources, complicating quantitative proof of synthesis. Additionally, any catalyst active for nitrogen reduction will preferentially evolve hydrogen [1].This project will build on the recent first quantitative proof of ammonia synthesis using a lithium mediated route and an organic electrolyte [2]. The aim is to understand the role of the electrode and electrolyte using cutting-edge characterisation techniques translated from battery science. A magnetron sputter deposition chamber directly attached to a glove box will be used to grow highly reactive thin film electrodes. These can be quickly transferred to an electrochemical cell, minimising deleterious oxidisation. The glove box will contain a hypersensitive mass spectrometer to measure gas evolution in-situ, never used before for non-aqueous electrochemistry, and an infrared spectrometer to probe intermediates. These operando techniques will be complemented by various ex-situ characterisation methods, including secondary ion mass spectrometry, nuclear magnetic resonance spectroscopy, Raman spectroscopy and electrochemical atomic force microscopy. The emergent molecular-scale picture will elucidate pathways towards efficient electrochemical ammonia synthesis.[1] Nilsson, A. & Stephens, I. E. L. "Sustainable N2 reduction" in Research needs towards sustainable production of fuels and chemicals (eds J.K. Norskov, A. Latimer, & C. F. Dickens) 49 (Energy-X, Brussels, Belgium, 2019)[2] Andersen, S. Z., Colic, V., Yang, S., Schwalbe, J. A., Nielander, A. C., McEnaney, J. M., Enemark-Rasmussen, K., Baker, J. G., Singh, A. R., Rohr, B. A., Statt, M. J., Blair, S. J., Mezzavilla, S., Kibsgaard, J., Vesborg, P. C. K., Cargnello, M., Bent, S. F., Jaramillo, T. F., Stephens, I. E. L., Norskov, J. K. & Chorkendorff, I. Nature 570, 504, (2019)