Origin of the electrocatalytic oxygen reduction activity of graphene-based catalysts: a roadmap to achieve the best performance.
Origin of the electrocatalytic oxygen reduction activity of graphene-based catalysts: a roadmap to achieve the best performance.
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基于石墨烯的催化剂的电催化还原活性的起源：实现最佳性能的路线图。
DOI：
10.1021/ja500432h
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发表时间：
2014-03-19
影响因子：
15
通讯作者：
Qiao, Shi Zhang
中科院分区：
文献类型：
--
作者：
Jiao, Yan;Zheng, Yao;Jaroniec, Mietek;Qiao, Shi Zhang
采用电化学测量和密度泛函理论（DFT）计算相结合的方法，揭示了石墨烯基电催化剂对氧还原反应（ORR）电催化活性的起源.设计并合成了一系列非金属元素掺杂的石墨烯，并以交换电流密度、起始电位、反应路径选择性和动力学电流密度4个电化学参数评价了它们的ORR性能。结果表明，这些描述符是在良好的协议与DFT计算，允许导出的火山图之间的ORR活性和吸附自由能的中间体上的无金属材料，类似于在金属催化剂的情况下。使用分子轨道概念来证明该火山图，并从理论上预测理想的石墨烯基催化剂的ORR性能，其ORR活性与现有技术的Pt催化剂相当。此外，这项研究可能会刺激其他关键的能量转换过程，包括析氢和析氧反应的无金属电催化剂的发展，并在很大程度上扩展了与能量相关的电催化反应的催化剂谱。
The mutually corroborated electrochemical measurements and density functional theory (DFT) calculations were used to uncover the origin of electrocatalytic activity of graphene-based electrocatalysts for oxygen reduction reaction (ORR). A series of graphenes doped with nonmetal elements was designed and synthesized, and their ORR performance was evaluated in terms of four electrochemical descriptors: exchange current density, on-set potential, reaction pathway selectivity and kinetic current density. It is shown that these descriptors are in good agreement with DFT calculations, allowing derivation of a volcano plot between the ORR activity and the adsorption free energy of intermediates on metal-free materials, similarly as in the case of metallic catalysts. The molecular orbital concept was used to justify this volcano plot, and to theoretically predict the ORR performance of an ideal graphene-based catalyst, the ORR activity of which is comparable to the state-of-the-art Pt catalyst. Moreover, this study may stimulate the development of metal-free electrocatalysts for other key energy conversion processes including hydrogen evolution and oxygen evolution reactions and largely expand the spectrum of catalysts for energy-related electrocatalysis reactions.
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影响因子：
3.3
作者：
Norskov, JK;Rossmeisl, J;Jónsson, H
通讯作者：
Jónsson, H
石墨烯对氧电催化活化的尺寸效应
影响因子：
4.9
作者：
Deng, Dehui;Yu, Liang;Bao, Xinhe
通讯作者：
Bao, Xinhe
影响因子：
21.8
作者：
Greeley, J.;Stephens, I. E. L.;Norskov, J. K.
通讯作者：
Norskov, J. K.
影响因子：
17.1
作者：
Choi, Chang Hyuck;Park, Sung Hyeon;Woo, Seong Ihl
通讯作者：
Woo, Seong Ihl
影响因子：
41.2
作者：
Greeley, Jeff;Jaramillo, Thomas F.;Norskov, Jens K.
通讯作者：
Norskov, Jens K.