Apically Dominant Mechanism for Improving Catalytic Activities of N‐Doped Carbon Nanotube Arrays in Rechargeable Zinc–Air Battery,Advanced Energy Materials

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Apically Dominant Mechanism for Improving Catalytic Activities of N‐Doped Carbon Nanotube Arrays in Rechargeable Zinc–Air Battery
Advanced Energy Materials ( IF 24.4 ) Pub Date : 2018-04-14 , DOI: 10.1002/aenm.201800480
Wenhan Niu ₁ , Srimanta Pakhira _{2,

3,

4,

5} , Kyle Marcus ₆ , Zhao Li ₆ , Jose L. Mendoza-Cortes _{2,

3,

4,

5,

7} , Yang Yang _{1,

6}

Affiliation

The oxygen reduction reaction (ORR) and the oxygen evolution reaction (OER) in zinc–air batteries (ZABs) require highly efficient, cost‐effective, and stable electrocatalysts as alternatives to high cost and low poison resistant platinum group metals (PGM) catalysts. Although nitrogen‐doped carbon nanotube (NCNT) arrays are now capable of catalyzing ORR efficiently, their hydrophobic surface and base‐growth mode are found to limit the catalytic performance in the practical ZABs. Here, the concept of an apically dominant mechanism in improving the catalytic performance of NCNT by precisely encapsulating CoNi nanoparticles (NPs) within the apical domain of NCNT on the Ni foam (denoted as CoNi@NCNT/NF) is demonstrated. The CoNi@NCNT/NF exhibits a more excellent catalytic performance toward both ORR and OER than that of traditional NCNT derived from the base‐growth method. The ZAB coin cell using CoNi@NCNT/NF as an air electrode shows a peak power density of 127 mW cm⁻² with an energy density of 845 Wh kg_Zn⁻¹ and rechargeability over 90 h, which outperforms the performance of PGM catalysts. Density functional theory calculations reveal that the ORR catalytic performance of the CoNi@NCNT/NF is mainly attributed to the synergetic contributions from NCNT and the apical active sites on NCNT near to CoNi NPs.

中文翻译：

改善可充电锌空气电池中N掺杂碳纳米管阵列催化活性的明显主导机制

锌空气电池（ZAB）中的氧还原反应（ORR）和氧释放反应（OER）需要高效，经济高效且稳定的电催化剂，以替代成本高且抗毒性低的铂族金属（PGM）催化剂。尽管现在掺氮碳纳米管（NCNT）阵列能够有效催化ORR，但发现它们的疏水表面和碱增长模式限制了实际ZAB中的催化性能。在此，展示了通过将CoNi纳米颗粒（NPs）精确地封装在Ni泡沫（表示为CoNi @ NCNT / NF）上的NCNT的根域内来改善NCNT催化性能的最主要机制的概念。CoNi @ NCNT / NF相对于从碱增长法衍生的传统NCNT表现出对ORR和OER的更优异的催化性能。使用CoNi @ NCNT / NF作为空气电极的ZAB纽扣电池的峰值功率密度为127 mW cm^-2的能量密度为845 Wh kg _Zn^-1，可充电时间超过90小时，优于PGM催化剂的性能。密度泛函理论计算表明，CoNi @ NCNT / NF的ORR催化性能主要归因于NCNT的协同作用和NCNT上靠近CoNi NPs的顶端活性位。

更新日期：2018-04-14

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