Electrocatalytic N 2 reduction to NH 3 with high Faradaic efficiency enabled by vanadium phosphide nanoparticle on V foi
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itute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu 610054, China Green Catalysis Center and College of Chemistry, Zhengzhou University, Zhengzhou 450001, China 3 The Key Laboratory of Life-Organic Analysis and Key Laboratory of Pharmaceutical Intermediates and Analysis of Natural Medicine, School of Chemistry and Chemical Engineering, Qufu Normal University, Qufu 273165, China 4 School of Materials Science and Engineering, Henan Normal University, Xinxiang 453007, China § Peipei Wei and Qin Geng contributed equally to this work. 2
© Tsinghua University Press and Springer-Verlag GmbH Germany, part of Springer Nature 2020 Received: 23 April 2020 / Revised: 12 June 2020 / Accepted: 25 June 2020
ABSTRACT To develop highly efficient electrochemical catalysts for N2 fixation is important to sustainable ambient NH3 production through the N2 reduction reaction (NRR). Herein, we demonstrate the development of vanadium phosphide nanoparticle on V foil as a highefficiency and stable catalyst for ambient NH3 production with excellent selectivity. The high Faradaic efficiency of 22% with a large NH3 yield of 8.35 × 10−11 mol·s−1·cm−2 was obtained at 0 V vs. the reversible hydrogen electrode in acid solution, superior to all previously studied V-based NRR catalysts. Density functional theory calculations are also utilized to have an insight into the catalytic mechanism.
KEYWORDS vanadium phosphide nanoparticle, N2 reduction reaction, electrocatalysis, density functional theory
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Introduction
NH3 is widely used in agriculture and industries [1, 2]. Moreover, it provides us with a carbon-free chemical energy carrier that has high hydrogen density [3]. Up to now, industrial NH3 is produced predominantly via the Haber-Bosch process utilizing N2 and H2 as the feeding gases [4]. But this process causes serious energy consumption and heavy CO2 emission. Thus, the development of green and sustainable alternatives is highly required for efficient NH3 production. Electroreduction of N2 to NH3 is a nature-friendly process, which is driven by electric energy utilizing water as proton source (H+) under mild conditions; efficient electrocatalysts however are required to enable the N2 reduction reaction (NRR) [5–8]. The catalysts based on noble metal (Au [9, 10], Ag [11], Pd [12], and Ru [13, 14]) perform well in the process of NRR, however, their shortage and expensiveness severely hinder the widespread application. In this regard, some efforts are made to search and identify cost-effective noble-metal-free NRR catalysts [15–35]. Vanadium (V) has biological implications in natural nitrogenases for ambient N2 fixation [36]. Moreover, V-based complexes [37], oxide [38, 39], carbide [40], and nitride [41] are also active to electrocatalyze the NRR, and the highest current efficiency for these catalysts, however, is only 12.20% [40]. Therefore, it is of significance to study novel V-based NRR electrocatalysts with superior activity. The metalloid properties and great electroconductivi
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