Are There Any Overlooked Catalysts for Electrochemical NH3 Synthesis-New Insights from Analysis of Thermochemical Data.

IScience
Emil Dražević, Egill Skúlason

Abstract

We report relations between nitrogen-binding-energy descriptors obtained from experimental thermochemical data and limiting potentials from density functional theory data. We use the relations to build the largest volcano plot for nitrogen reduction reaction (NRR). We found that (1) Mn, Ga, and In are overlooked catalysts and (2) there are unidentified materials on the top of the volcano. Using experimental exchange current densities of hydrogen evolution reaction (HER) and Pourbaix diagrams we have identified conditions at which Mn, Ga, and In remain stable in water and selectively catalyze NRR over HER. We found that Fe, Au, Cu, Bi, and Pd, on contrary to what was reported earlier, need smaller applied potentials to start the onset of HER than NRR in water. We make a critical discussion about them and other candidates and we believe our results can be used to identify false positive measurements in the research field.

References

Dec 8, 2011·Physical Chemistry Chemical Physics : PCCP·Egill SkúlasonJens K Nørskov
Sep 27, 2014·Journal of the American Chemical Society·Kendra P KuhlThomas F Jaramillo
Dec 3, 2014·Physical Chemistry Chemical Physics : PCCP·Younes AbghouiEgill Skúlason
Aug 4, 2015·Chemical Communications : Chem Comm·Faegheh HoshyargarAnthony P O'Mullane
May 21, 2019·Chemical Society Reviews·Cheng Tang, Shi-Zhang Qiao
Sep 29, 2019·Nature Communications·Yun-Xiao LinJie-Sheng Chen
Oct 8, 2019·Nanoscale·Pétur Már Gíslason, Egill Skúlason
Aug 15, 2020·Science·Stuart LichtShuzhi Liu

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