Comparative Study on the Catalytic Activity of the TM--N
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概要
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We investigate the interaction of transition metal--nitrogen (TM--N<inf>2</inf>; TM = Mn, Fe, Co, and Ni) active sites with oxygen reduction reaction (ORR) related molecules using the density functional theory (DFT) calculations. Generally, the trend of molecular adsorption energy in TM--N<inf>2</inf>systems is Mn--N<inf>2</inf>> Fe--N<inf>2</inf>> Co--N<inf>2</inf>> NiN<inf>2</inf>. In the case of O<inf>2</inf>adsorption, the O<inf>2</inf>molecule is adsorbed with a symmetric side-on configuration on the TM--N<inf>2</inf>systems, regardless the type of TM atom. We also find that when the reaction of the adsorbed HO<inf>2</inf>molecule and an H atom takes place, instead of forming H<inf>2</inf>O<inf>2</inf>molecule the reaction produces two OH radicals. From the evaluation of the potential energy surface profiles of the oxygen reduction reaction (ORR), we find that a direct four-electron reduction pathway could be facilitated on the TM--N<inf>2</inf>active sites. However, all of the TM--N<inf>2</inf>systems share the same main rate-limiting reaction, which is the OH reduction step. Generally, the edge-like TM--N<inf>2</inf>active site has stronger molecular adsorption energy as compared to the TM--pyrrole-like active site. However, the strong molecular adsorption energy in the edge-like TM--N<inf>2</inf>active site results in uphill energy profiles for some of ORR steps, even at a low electrode potential. This suggests that edge-like TM--N<inf>2</inf>active site will have a relatively slower ORR rate as compared to the TM--pyrrole-like active site.
- 2013-11-15
著者
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Kasai Hideaki
Department Of Applied Physics Faculty Of Engineering Osaka University
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Saputro Adhitya
Department of Applied Physics, Graduate School of Engineering, Osaka University, Suita, Osaka 565-0871, Japan
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Kasai Hideaki
Department of Applied Physics, Graduate School of Engineering, Osaka University, Suita, Osaka 565-0871, Japan
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Kishi Hirofumi
Frontier Technology R&D Division, Daihatsu Motor Co., Ltd., Ryuo, Shiga 520-2593, Japan
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Asazawa Koichiro
Frontier Technology R&D Division, Daihatsu Motor Co., Ltd., Ryuo, Shiga 520-2593, Japan
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Tanaka Hirohisa
Frontier Technology R&D Division, Daihatsu Motor Co., Ltd., Ryuo, Shiga 520-2593, Japan
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Tanaka Hirohisa
Frontier Technology R&D Division, Daihatsu Motor Co., Ltd., Ryuo, Shiga 520-2593, Japan
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Asazawa Koichiro
Frontier Technology R&D Division, Daihatsu Motor Co., Ltd., Ryuo, Shiga 520-2593, Japan
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