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A Co-N/C hollow-sphere electrocatalyst derived from a metanilic CoAl layered double hydroxide for the oxygen reduction reaction, and its active sites in various pH media
  • 时间:0
  • 分类:TQ351.471[化学工程] TQ314[化学工程—高聚物工业]
  • 作者机构:State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, Beijing 100029, China
  • 相关基金:This research was supported by the National Basic Research Program of China (No. 2014CB932103), National Natural Science Foundation of China (Nos. 51272020, 21236003, and U1407118), Beijing Engineering Center for Hierarchical catalysts and Fundamental Research Funds for the Central Universities (No. YS1406).
中文摘要:

Transition-metal-coordinating 做氮的碳催化剂(M-N/C, M = 公司, Fe, Mn, Ni,等等) 为氧减小反应(ORR ) 被认为最有希望的 nonprecious 金属 electrocatalysts 之一。然而,他们受不了低 ORR 催化活动,和他们的活跃地点充分没被识别。此处,我们由在煤分层的双氢氧化物的层之间的 metanilic 阴离子的碳化报导多孔的 Co-N/C 空范围的 electrocatalyst 的合成。同样准备的 Co-N/C 催化剂展出了优秀 ORR 有在碱、中立的溶液的一个高一半波浪潜力和大散开有限水流的催化活动。催化剂的表演比得上商业 Pt/C electrocatalysts 的那些。通过调查面具离子的效果(在 Co-N/C 催化剂的 ORR 活动的 SCN 和 F ),并且在不同 pH 媒介在反对 x 地点的破坏前后比较 ORR 活动,我们断定反对 x 地点在酸、中立的答案直接充当 ORR 活跃地点,但是处于碱的条件在 ORR 活动有可以忽略的效果。

英文摘要:

Transition-metal-coordinating nitrogen-doped carbon catalysts (M-N/C, M = Co, Fe, Mn, Ni, etc.) are considered one of the most promising nonprecious-metal electrocatalysts for the oxygen reduction reaction (ORR). However, they suffer from low ORR catalytic activity, and their active sites have not been fully identified. Herein, we report the synthesis of a porous Co-N/C hollow-sphere electrocatalyst by carbonization of metanilic anions between the layers of a Co-A1 layered double hydroxide. The as-prepared Co-N/C catalyst exhibited excellent ORR catalytic activity with a high half-wave potential and a large diffusion-limited current in alkaline and neutral solutions. The performance of the catalyst was comparable to those of commercial Pt/C electrocatalysts. Through investigating the effects of mask ions (SCN- and F-) on the ORR activity of the Co-N/C catalyst, and comparing the ORR activity before and after the destruction of Co-Nx sites in different pH media, we concluded that the Co-Nx sites act directly as the ORR active sites in acidic and neutral solutions, but have a negligible effect on the ORR activity in alkaline conditions.

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