화학공학소재연구정보센터
학회 한국재료학회
학술대회 2021년 봄 (05/12 ~ 05/14, 광주 김대중컨벤션센터)
권호 27권 1호
발표분야 특별심포지엄 1. 에너지용 기능성 재료 특별심포지엄-오거나이저: 신병하(KAIST)
제목 Ultrasonic-Plasma Engineering toward Facile Synthesis of Atomic Metal-doped Carbon as Bi-functional Oxygen Electrocatalyst for Rechargeable Metal-air battery
초록 The growing demand for green and renewable energy has inspired the vigorous development of power conversion and storage devices that reveal high power densities and eco-friendly [1]. Among the numerous energy conversion devices, rechargeable metal-air batteries feature much higher theoretical densities compared to metal-ion devices [2]. Yet, their widespread commercialization of these batteries is hindered by the high cost and poor stability of noble-based electrocatalysts during repeated charge-discharge, which involves the oxygen reduction reaction (ORR) and the oxygen evolution reaction (OER) [3]. Atomic transition metal-doped nitrogen-carbon (NC) matrices are promising successors of the corresponding noble-metal-based catalysts, offering the advantages of ultra-high atom utilization efficiency atomic and surface energy [4]. In particular, The superior catalytic activity of Metal-N4 mainly originates from the specific coordination between transition metal atoms and nitrogen, which provides a highly efficient means of modifying local electronic states [5].

Despite these achievements, the fabrication of well-dispersed M-N4/NCs remains challenging. Notably, control of the interfacial contact between the metal atoms and the charcoal support as well as that of metal atom dispersion are crucial for ORR/OER activity enhancement [6].  The synthesis of molecular M-N4/NCs nanomaterials often requires numerous steps and tedious processes [7]. Herein, ultrasonic-plasma engineering allows direct carbonization in a precursor solution containing metal-phthalocyanine and aniline. When combining with the dispersion effect of ultrasonic waves, we successfully fabricated uniform atomic M-N4 (M = Fe, Co) carbon catalysts with a production rate as high as 10 mg/min. The Co-N4/NC presented a potential bifunctional drop of ΔE = 0.79 V, outperforming the benchmark Pt/C-Ru/C catalyst (ΔE = 0.88 V) at the same catalyst loading. Theoretical calculations revealed that Co-N4 was the primary active site with superior O2 adsorption-desorption mechanisms. In a practical Zn-air battery test, the air electrode coated with Co-N4/NC exhibited a specific capacity (762.8 mAh/g) and power density (101.62 mW/cm2), exceeding those of Pt/C-Ru/C (700.8 mAh/g and 89.16 mW/cm2, respectively) at the same catalyst loading. Moreover, for Co-N4/NC, the potential difference increased from 1.16 to 1.47 V after 100 charge-discharge cycles. The proposed innovative and scalable strategy was concluded to be well suited for the fabrication of single-atom-doped carbons as promising bifunctional oxygen evolution/reduction electrocatalysts for metal-air batteries.

References:

[1] N. N. Xu, J. A. Wilson, Y. D. Wang, T. S. Su, Y. N. Wei, J. L. Qiao, X. D. Zhou, Y. X. Zhang, and S. H. Sun.  Appl. Catal. B: Environ. 272 (5), 118953 (2020).  
[2] C. Guan, A. Sumboja, H. J. Wu, W. N. Ren, X. M. Liu, H. Zhang, Z. L. Liu, C. W. Cheng, S. J. Pennycook, and J. Wang.  Adv. Mater. 29, 1704117 (2017).  
[3] Y. F. Yuan, K. Amine, J. Lu, and R. Shahbazian-Yassar. Nat. Commun. 8, 1–14 (2017).
[4] J. X. Han, X. Y. Meng, L. Lu, J. J. Bian, Z. P. Li, and C. W. Sun. Single–atom Fe–Nx–C as an efficient electrocatalyst for zinc–air batteries. Adv. Funct. Mater. 29, 1808872 (2019).  
[5] Z. H. Wang, H. H. Jin, T. Meng, K. Liao, W. Q. Meng, J. L. Yang, D. P. He, Y. L. Xiong, and S. C. Mu. Adv. Funct. Mater. 28 (39), 1802596 (2018).
[6] S. S. Zheng, X. R. Li, B. Y. Yan, Q. Hu, Y. X. Xu, X. Xiao, H. G. Xue, and H. Pang. Adv. Energy Mater. 7 (18), 1602733 (2017).
[7] E. Lam, and J. H. T. Luong. ACS Catal. 4 (10), 3393–3410 (2014).



 
저자 Oi Lun (Helena) LI
소속 부산대
키워드 Plasma Engineering; single-atom metal catalyst; oxygen reduction reaction; oxygen evolution reaction; zinc-air battery; water splitting
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