Designing mixed-metal electrocatalyst systems for photoelectrochemical nitrogen activation Manpreet Kaur 1 , Marc Walker 1 , Steven Hindmarsh 1 , Martin Lees 1 , Charlotte Bolt 1 , Yisong Han 1 , Stephen York 1 , Katharina Brinkert 1,2 1 University of Warwick, UK, 2 University of Bremen, Germany Efficient artificial photosynthesis systems are currently used for photoelectrochemical (PEC) water oxidation while simultaneously recycling CO 2 and generating hydrogen as a solar fuel for storable renewable energy. 1 These systems comprise e.g., integrated semiconductor-electrocatalyst devices which offer several benefits such as high system tunability with respect to the electrocatalyst integration and a directly controllable electron flux for the electrocatalytic process through the adjustability of incoming irradiation. These characteristics could also represent a significant advantage for electrocatalytic dinitrogen reduction, although PEC devices remain little explored for this reaction. 2 We present photoelectrodeposition procedures to fabricate nitrogen-free p-InP photocathodes with integrated bimetallic and alloyed CoMo electrocatalysts as well as first dinitrogen activation studies on these electrodes. Higher photocurrent densities were observed with these electrodes in the presence of dinitrogen than in the presence of argon, indicating the successful activation of dinitrogen. XPS analyses confirm these observations as the electrode surface reveals metal-nitrogen interactions after initial photoelectrochemical tests. We also report on photoelectrodeposition procedures yielding CoMoRu electrocatalyst nanoparticles on p-InP and report on their initial investigation for dinitrogen activation. 3
References 1. W.-H. Cheng, M. H. Richter, M. M. May, J. Ohlmann, D. Lackner, F. Dimroth, T. Hannappel, H. A. Atwater and H.-J. Lewerenz, ACS Energy Lett. , 2018, 3 , 1795–1800. 2. A. R. Singh, B. A. Rohr, J. A. Schwalbe, M. Cargnello, K. Chan, T. F. Jaramillo, I. Chorkendorff and J. K. Nørskov, ACS Catal. , 2017, 7 , 706–709. 3. C. J. H. Jacobsen, S. Dahl, B. S. Clausen, S. Bahn, A. Logadottir and J. K. Nørskov, J. Am. Chem. Soc. , 2001, 123 , 8404–8405.
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