Identification of binuclear Co2N5 active sites for oxygen reduction reaction with more than one magnitude higher activity than single atom CoN4 site

Xiao, Meiling; Zhang, Hao; Chen, Yongting; Zhu, Jianbing; Gao, Liqin; Zhao, Jianmin; Ge, Junjie; Jiang, Zheng; Chen, Shengli; Liu, Changpeng; Wang, Xing

doi:10.1016/j.nanoen.2018.02.025

Cited by 349 publications

(275 citation statements)

References 35 publications

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“…Different from other reports in this section, who all report active sites comprising a single metal atom coordinated to nitrogen, Xiao et al reported high activity for a catalyst containing at least in part an active site comprising Co 2 –N 5 , that is, two Co atoms coordinated to nitrogen atoms. Similar to the work by Wang et al, the bi‐metallic catalyst motif performs well in acidic conditions (0.1 m HClO 4 ) with a half wave potential of 0.79 V versus RHE.…”

Section: Cobalt‐based Electrocatalystscontrasting

confidence: 66%

Oxygen Reduction Reactions on Single‐ or Few‐Atom Discrete Active Sites for Heterogeneous Catalysis

Sharifi

Gracia‐Espino

Chen

et al. 2019

Advanced Energy Materials

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The oxygen reduction reaction (ORR) is of great importance in energy‐converting processes such as fuel cells and in metal–air batteries and is vital to facilitate the transition toward a nonfossil dependent society. The ORR has been associated with expensive noble metal catalysts that facilitate the O2 adsorption, dissociation, and subsequent electron transfer. Single‐ or few‐atom motifs based on earth‐abundant transition metals, such as Fe, Co, and Mo, combined with nonmetallic elements, such as P, S, and N, embedded in a carbon‐based matrix represent one of the most promising alternatives. Often these are referred to as single atom catalysts; however, the coordination number of the metal atom as well as the type and nearest neighbor configuration has a strong influence on the function of the active sites, and a more adequate term to describe them is metal‐coordinated motifs. Despite intense research, their function and catalytic mechanism still puzzle researchers. They are not molecular systems with discrete energy states; neither can they fully be described by theories that are adapted for heterogeneous bulk catalysts. Here, recent results on single‐ and few‐atom electrocatalyst motifs are reviewed with an emphasis on reports discussing the function and the mechanism of the active sites.

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Section: Cobalt‐based Electrocatalystscontrasting

confidence: 66%

Oxygen Reduction Reactions on Single‐ or Few‐Atom Discrete Active Sites for Heterogeneous Catalysis

Sharifi

Gracia‐Espino

Chen

et al. 2019

Advanced Energy Materials

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“…For CoN x , the synthetic conditions, such as the Co/Zn ratio or pyrolytic temperature, were found to affect the N‐coordination of the final products. Coordinately unsaturated CoN 2 sites, edge‐hosted CoN 2+2 sites, and binuclear Co 2 N 5 sites have been identified to exhibit superior ORR activity to that of the intact CoN 4 configuration, attributed to the change in the local electronic environment of the Co atom that results in optimized adsorption/desorption strengths of the ORR intermediates. In particular, atomically dispersed Co sites with high atomic density (Co–N–C@F127) have been synthesized by direct pyrolysis of Co and F127 surfactant modified ZIF‐8 MOFs at 900 °C .…”

Section: Atomically Dispersed Single Metal Site Electrocatalysis For mentioning

confidence: 99%

Engineering Local Coordination Environments of Atomically Dispersed and Heteroatom‐Coordinated Single Metal Site Electrocatalysts for Clean Energy‐Conversion

Zhu

Sokolowski

Song

et al. 2019

Advanced Energy Materials

293

240

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Carbon‐based heteroatom‐coordinated single‐atom catalysts (SACs) are promising candidates for energy‐related electrocatalysts because of their low‐cost, tunable catalytic activity/selectivity, and relatively homogeneous morphologies. Unique interactions between single metal sites and their surrounding coordination environments play a significant role in modulating the electronic structure of the metal centers, leading to unusual scaling relationships, new reaction mechanisms, and improved catalytic performance. This review summarizes recent advancements in engineering of the local coordination environment of SACs for improved electrocatalytic performance for several crucial energy‐convention electrochemical reactions: oxygen reduction reaction, hydrogen evolution reaction, oxygen evolution reaction, CO2 reduction reaction, and nitrogen reduction reaction. Various engineering strategies including heteroatom‐doping, changing the location of SACs on their support, introducing external ligands, and constructing dual metal sites are comprehensively discussed. The controllable synthetic methods and the activity enhancement mechanism of state‐of‐the‐art SACs are also highlighted. Recent achievements in the electronic modification of SACs will provide an understanding of the structure–activity relationship for the rational design of advanced electrocatalysts.

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“…What's more, materials with dual sites are also studied and demonstrate a “1 + 1 > 2” phenomena. Xiao and co‐workers elaborated a novel binuclear site structure, as well as controlled the active site structure from single‐atom CoN 4 to Co particles encapsulated in carbon shell via a bimetal‐organic‐framework‐self‐adjusted strategy . The intentionally designed binuclear active site structure Co 2 N x C y determined by EXAFS analysis and DFT study can efficiently catalyze the ORR.…”

Section: Applications Of Mof‐derived Carbon‐supported Sacsmentioning

confidence: 99%

“…b,c) Schematic energy profiles for the ORR pathway on different Co x N y active sites in acidic media. Reproduced with permission . Copyright 2018, Elsevier Ltd. d) Scheme showing the atomic dispersion of Fe and Co active sites.…”

Section: Applications Of Mof‐derived Carbon‐supported Sacsmentioning

confidence: 99%

Recent Advances for MOF‐Derived Carbon‐Supported Single‐Atom Catalysts

et al. 2019

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Single‐atom catalysts have drawn considerable attention because of their unique catalytic properties. However, the high surface energy of single atoms restricts their fabrication and creates significant challenges for further developments. In order to overcome this problem, metal organic framework (MOF)‐derived carbon materials can be served as ideal supports to anchor atomically dispersed metal atoms, due to their tunable particle size and shape features, by providing high surface area, porosity, thermal, and chemical stability. This review highlights the recent advances in i) different types of construction strategies for MOF‐derived carbon‐supported single‐atom catalysts, and ii) the catalytic applications of these MOF‐derived carbon‐supported single‐atom catalysts. Further, this review offers a valuable insight into the current challenges and future opportunities for MOF‐derived carbon‐supported single‐atom catalysts.

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Identification of binuclear Co2N5 active sites for oxygen reduction reaction with more than one magnitude higher activity than single atom CoN4 site

Cited by 349 publications

References 35 publications

Oxygen Reduction Reactions on Single‐ or Few‐Atom Discrete Active Sites for Heterogeneous Catalysis

Oxygen Reduction Reactions on Single‐ or Few‐Atom Discrete Active Sites for Heterogeneous Catalysis

Engineering Local Coordination Environments of Atomically Dispersed and Heteroatom‐Coordinated Single Metal Site Electrocatalysts for Clean Energy‐Conversion

Recent Advances for MOF‐Derived Carbon‐Supported Single‐Atom Catalysts

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