Single Cobalt Atom and N Codoped Carbon Nanofibers as Highly Durable Electrocatalyst for Oxygen Reduction Reaction

Cheng, Qian; Yang, Lijun; Zou, Liangliang; Zou, Zhiqing; Chen, Chi; Hu, Zheng; Yang, Hui

doi:10.1021/acscatal.7b02326

Cited by 261 publications

(173 citation statements)

References 43 publications

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“…Single atom catalysts (SACs) are a class of catalysts newly emerged, which present both high activity and selectivity compared to traditional catalysts . SACs supported on nitrogen‐doped graphene (N–G) have been widely studied both experimentally and theoretically .…”

Section: Introductionmentioning

confidence: 99%

A General Two‐Step Strategy–Based High‐Throughput Screening of Single Atom Catalysts for Nitrogen Fixation

et al. 2018

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Electrocatalytic or photocatalytic N2 reduction holds great promise for green and sustainable NH3 production under ambient conditions, where an efficient catalyst plays a crucial role but remains a long‐standing challenge. Here, a high‐throughput screening of catalysts for N2 reduction among (nitrogen‐doped) graphene‐supported single atom catalysts is performed based on a general two‐step strategy. 10 promising candidates with excellent performance are extracted from 540 systems. Most strikingly, a single W atom embedded in graphene with three C atom coordination (W1C3) exhibits the best performance with an extremely low onset potential of 0.25 V. This study not only provides a series of promising catalysts for N2 fixation, but also paves a new way for the rational design of catalysts for N2 fixation under ambient conditions.

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Section: Introductionmentioning

confidence: 99%

A General Two‐Step Strategy–Based High‐Throughput Screening of Single Atom Catalysts for Nitrogen Fixation

et al. 2018

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“…Based on the above results, we can conclude that A‐Co@CMK‐3‐D catalyst presents the extraordinary catalytic activity due to a certain amount of single Co atoms and a larger specific surface area on hierarchically porous CMK‐3 carbon. Compared to the Co–N coordination of atomic Co species, Co–C coordination also exhibited excellent electrocatalytic activities for ORR, which may attributed to the charge redistribution between Co and carbon atoms . Owing to the electronic structure of Co is changed by the adjoining carbon atoms, these new electronic states of atomic Co centers show an enhanced catalytic performance for ORR.…”

Section: Resultsmentioning

confidence: 99%

Atomic Cobalt on Defective Bimodal Mesoporous Carbon toward Efficient Oxygen Reduction for Zinc–Air Batteries

Lyu

Chen

et al. 2019

Small Methods

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Single‐atom catalysts (SACs) with maximum atom‐utilization efficiency and distinctive properties are emerging as a new frontier in the field of catalysis. Herein, a new strategy for synthesizing stable Co single atoms with content of about 1.52 wt% on defective bimodal mesoporous carbon materials (A‐Co@CMK‐3‐D) is reported. The dispersion and coordination structures of atomic Co species at carbon defect sites are confirmed by both aberration‐corrected high‐resolution transmission electron microscopy (AC‐HRTEM) and X‐ray absorption spectrometry, respectively. The obtained catalyst exhibits efficient electrochemical performance on oxygen reduction reaction (ORR) in an alkaline electrolyte with a half‐wave potential (0.835 V vs RHE), which is comparable to that of Pt/C (0.839 V vs RHE). Furthermore, the Zn–air batteries (ZABs) fabricated by this electrocatalyst display a superior discharging and charging performance with long‐term durability. This work provides a new approach on optimizing SAC‐based carbon materials from multiscale principles (simultaneous regulation of electronic structure and hierarchical morphology) to boost ORR reactivity.

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“…ORR as half‐reaction at the cathode of fuel cells or metal–air battery could directly convert the chemical energy to the electrical energy . In general, there are two types of reaction mechanisms in ORR process, which includes two‐electron (2e − ) and four‐electron (4e − ) pathways in acidic solution . In two‐electron reaction mechanism, the intermediate of hydrogen peroxide was first formed in reduction process of 2e − pathway and then was further reduced to water (reactions and )

{normalO}_{2} + 2 {normalH}^{+} + 2 {normale}^{-} \to {normalH}_{2} {normalO}_{2} (E^{0} = 0.68 normalV, normalvs normalNHE)

{normalH}_{2} {normalO}_{2} + 2 {normalH}^{+} + 2 {normale}^{-} \to 2 {normalH}_{2} O (E^{0} = 1.77 normalV, normalvs normalNHE)

…”

Section: Electrochemical Applications Of Sagmentioning

confidence: 99%

“…It will decrease the amounts of active sites and results in poor catalytic activity. As a result, the substrates with large surface area have to be utilized to disperse these isolated single atoms . Carbon materials are the common substrates to support the single metal atoms due to their large surface, high conductivity, and stable chemical properties.…”

Section: Introductionmentioning

confidence: 99%

Single Atoms on Graphene for Energy Storage and Conversion

et al. 2019

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Single atoms are attracting much attention in the field of energy conversion and storage due to their maximal atomic utilization, high efficiency, and good selectivity. Moreover, their unique electronic structure could improve the intrinsic activity of the active sites. However, the high surface free energy of single atoms inevitably results in their serious aggregation, leading to degraded catalytic activity and poor cycling life. To solve these issues, supports with high surface areas have to be developed to reduce loading density of single atoms and further decrease the surface free energy. Furthermore, engineering the active sites of these substrates can also regulate chemical coordination of single atoms, enhancing their catalytic performance. Owing to high surface area, excellent conductivity and adjustable surface properties, graphene is widely utilized to load atomic metal catalysts. In this review, the fabrication strategies and characterization methods of single atoms on graphene (SAG) are summarized first. Subsequently, the electrochemical applications of SAG on the oxygen reduction reaction, oxygen evolution reaction, hydrogen evolution reaction, carbon dioxide reduction, and methane oxidation are discussed in detail. Finally, the future developments and prospects in fabrication and application of SAG are also discussed.

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Single Cobalt Atom and N Codoped Carbon Nanofibers as Highly Durable Electrocatalyst for Oxygen Reduction Reaction

Cited by 261 publications

References 43 publications

A General Two‐Step Strategy–Based High‐Throughput Screening of Single Atom Catalysts for Nitrogen Fixation

A General Two‐Step Strategy–Based High‐Throughput Screening of Single Atom Catalysts for Nitrogen Fixation

Atomic Cobalt on Defective Bimodal Mesoporous Carbon toward Efficient Oxygen Reduction for Zinc–Air Batteries

Single Atoms on Graphene for Energy Storage and Conversion

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