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原位钴-氧化钴/氮掺杂碳杂化材料作为优异的双功能析氢和析氧电催化剂。

In situ cobalt-cobalt oxide/N-doped carbon hybrids as superior bifunctional electrocatalysts for hydrogen and oxygen evolution.

机构信息

Advanced Materials and Catalysis Group, ZJU-NHU United R&D Center, Center for Chemistry of High-Performance and Novel Materials, Key Lab of Applied Chemistry of Zhejiang Province, Department of Chemistry, Zhejiang University , Hangzhou 310028, P. R. China.

出版信息

J Am Chem Soc. 2015 Feb 25;137(7):2688-94. doi: 10.1021/ja5127165. Epub 2015 Feb 17.

Abstract

Remarkable hydrogen evolution reaction (HER) or superior oxygen evolution reaction (OER) catalyst has been applied in water splitting, however, utilizing a bifunctional catalyst for simultaneously generating H2 and O2 is still a challenging issue, which is crucial for improving the overall efficiency of water electrolysis. Herein, inspired by the superiority of carbon conductivity, the propitious H atom binding energy of metallic cobalt, and better OER activity of cobalt oxide, we synthesized cobalt-cobalt oxide/N-doped carbon hybrids (CoOx@CN) composed of Co(0), CoO, Co3O4 applied to HER and OER by simple one-pot thermal treatment method. CoOx@CN exhibited a small onset potential of 85 mV, low charge-transfer resistance (41 Ω), and considerable stability for HER. Electrocatalytic experiments further indicated the better performance of CoOx@CN for HER can be attributed to the high conductivity of carbon, the synergistic effect of metallic cobalt and cobalt oxide, the stability of carbon-encapsulated Co nanoparticles, and the introduction of electron-rich nitrogen. In addition, when used as catalysts of OER, the CoOx@CN hybrids required 0.26 V overpotential for a current density of 10 mA cm(-2), which is comparable even superior to many other non-noble metal catalysts. More importantly, an alkaline electrolyzer that approached ∼20 mA cm(-2) at a voltage of 1.55 V was fabricated by applying CoOx@CN as cathode and anode electrocatalyst, which opened new possibilities for exploring overall water splitting catalysts.

摘要

在水分解中,已经应用了具有出色的析氢反应 (HER) 或优越的析氧反应 (OER) 催化性能的催化剂,然而,利用双功能催化剂同时产生 H2 和 O2 仍然是一个具有挑战性的问题,这对于提高水分解的整体效率至关重要。在此,受碳导电性的优越性、金属钴有利的 H 原子结合能以及钴氧化物更好的 OER 活性的启发,我们通过简单的一步热处理方法合成了由 Co(0)、CoO 和 Co3O4 组成的钴-钴氧化物/N-掺杂碳杂化物 (CoOx@CN),用于 HER 和 OER。CoOx@CN 表现出 85 mV 的小起始电位、低电荷转移电阻 (41 Ω) 和对 HER 的良好稳定性。电催化实验进一步表明,CoOx@CN 对 HER 的更好性能可归因于碳的高导电性、金属钴和钴氧化物的协同效应、碳封装 Co 纳米粒子的稳定性以及富电子氮的引入。此外,当用作 OER 的催化剂时,CoOx@CN 杂化物需要 0.26 V 的过电位才能达到 10 mA cm(-2) 的电流密度,这与许多其他非贵金属催化剂相当甚至更优。更重要的是,通过应用 CoOx@CN 作为阴极和阳极电催化剂,制造了一个碱性电解槽,在 1.55 V 的电压下接近 20 mA cm(-2) 的电流密度,为探索整体水分解催化剂开辟了新的可能性。

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