Activity origin and design principles for atomic vanadium anchoring on phosphorene monolayer for nitrogen reduction reac
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Activity origin and design principles for atomic vanadium anchoring on phosphorene monolayer for nitrogen reduction reaction Xiongyi Liang, Xiangxuan Deng, Chen Guo, and Chi-Man Lawrence Wu () Department of Materials Science and Engineering, City University of Hong Kong, Hong Kong, China © Tsinghua University Press and Springer-Verlag GmbH Germany, part of Springer Nature 2020 Received: 8 March 2020 / Revised: 19 June 2020 / Accepted: 23 June 2020
ABSTRACT Conversion of inert N2 molecules into NH3 via electrochemical methods is an environmentally friendly alternative to replace the traditional Haber-Bosch process. However, the development of highly efficient catalyst is still challenging. Herein, we report a density functional theory (DFT) based high-throughput screening to investigate the potential of 23 atomic transition metals (Sc, Ti, V, Cr, Mn, Fe, Co, Ni, Cu, Zn, Y, Zr, Nb, Mo, Tc, Ru, Rh, Pd, Ag, Cd, W, Pt and Au) supported on phosphorene monolayer as electrocatalyst for nitrogen reduction reaction (NRR). Our theoretical results demonstrate that V single atom anchoring on phosphorene monolayer exhibits good thermal stability, selectivity and excellent catalytic activity with a low overpotential of 0.18 V. Importantly, rational design principles and electronic descriptor between the intrinsic electronic properties and activation barrier have been developed. Our work offers a new promising noble metal-free catalyst for NRR and reveals profound insights into the activity origin to guide further design.
KEYWORDS high-throughput screening, density functional theory, phosphorene, electronic descriptor, single atomic catalyst, transition metal
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Introduction
Ammonia (NH3) is an indispensable chemical feedstock in modern industry, widely used in agricultural industries, synthetic fibers, dyes and water treatment [1, 2]. It is reported that the annual production of ammonia has already reached 200 million tons in 2018 and is predicted to explode to over 350 million in 2050 [3]. Currently, industrial ammonia production is still dominated by the traditional Haber-Bosch process, in which N2 is converted into NH3 by a reaction with H2 using a heterogeneous iron-based catalyst. Although this is an exothermic reaction, it requires extreme temperature and pressure to break the strong N≡N triple bond and thus activate N2 molecules. As a result, it consumes more than 2% of the energy generated in the world each year and leads to enormous CO2 emission [4, 5]. In this regard, electrocatalytic nitrogen reduction reaction (NRR) is a highly promising alternative for ammonia production, which is also effective and eco-friendly [6, 7]. Totally different from the Haber-Bosch method, instead of breaking the N≡N triple bond, six protons and electrons are gradually added (N2 + 6H+(aq) + 6e− = 2NH3(g)). Thus, it can react under ambient condition but highly relies on the use of a catalyst. Over the past few decades, a great amount of theoretical and experimental efforts have been devoted into searching and developing efficient electr
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