Mass production of high-performance single atomic FeNC electrocatalysts via sequenced ultrasonic atomization and pyrolys
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Published online 30 September 2020 | https://doi.org/10.1007/s40843-020-1464-6
Mass production of high-performance single atomic FeNC electrocatalysts via sequenced ultrasonic atomization and pyrolysis process 1
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Jugang Ma , Liguang Wang , Yida Deng , Weiwei Zhang , Tianpin Wu and Yujun Song ABSTRACT Mass production of highly efficient, durable, and inexpensive single atomic catalysts is currently the major challenge associated with the oxygen reduction reaction (ORR) for fuel cells. In this study, we develop a general strategy that uses a simple ultrasonic atomization coupling with pyrolysis and calcination process to synthesize single atomic FeNC catalysts (FeNC SACs) at large scale. The microstructure characterizations confirm that the active centers root in the single atomic Fe sites chelating to the four-fold pyridinic N atoms. The identified specific Fe active sites with the variable valence states facilitate the transfer of electrons, endowing the FeNC SACs with excellent electrochemical ORR activity. The FeNC SACs were used as cathode catalysts in a homemade Zn-air battery, giving an open-circuit voltage (OCV) of 1.43 V, which is substantially higher than that of commercial Pt/C catalysts. This study provides a simple approach to the synthesis of single atomic catalysts at large scale. Keywords: single atomic catalysts, ultrasonic atomization, oxygen reduction reaction, Zn-air battery
INTRODUCTION Energy conversion via electrochemical reactions for fuel cells has attracted increasing attention because of its advantages over traditional fossil energy sources, such as renewability, eco-friendliness, and high efficiency [1,2]. The oxygen reduction reaction (ORR) is a critical factor associated with electrochemical energy conversion in fuel cells. It is an important cathode reaction in many electrochemical energy conversion devices, including hydrogen fuel cells, direct methanol fuel cells, and metal-air batteries [3,4]. The main difficulty associated with the ORR is the sluggish multi-electron transfer process, 1 2 3
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which is typically catalyzed by precious metals such as Pt, Pd, or one of their alloys [5–7]. However, fuel cells still suffer from limited activity, poor stability, and poor durability, as well as the high cost and low natural abundance of the raw materials from which their components are made, impeding their sustainable commercial application [8–10]. Transition-metal complexes have been widely used in the physical and biological science, where they are essential in the catalysis, chemical synthesis, materials science, photo-physics and bioinorganic chemistry [11–13]. Since 1964, N4-macrocycles of non-noble metals (e.g., cobalt) based on the organometallic complexes and bionics have been developed as fuel cell cathode catalysts [14]. Various nonprecious earth-abundant metal catalysts, especially those based on transition metal-nitrogencarbon (MNC) compounds, have been continuously developed to address the issues related to the cost and earthabundant resources, and their cat
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