Easy enrichment of graphitic nitrogen to prepare highly catalytic carbons for oxygen reduction reaction

Quílez‐Bermejo, Javier; Pérez-Rodríguez, S.; Canevesi, Rafael Luan Sehn; Torres, Daniel; Morallón, Emilia; Cazorla‐Amorós, D.; Celzard, Alain; Fierro, Vanessa

doi:10.1016/j.carbon.2022.05.032

Cited by 12 publications

(7 citation statements)

References 78 publications

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“…Although there is some controversy, many reports have demonstrated graphitic-N to be the most promising species toward ORR and OER. 16,18,34 Taken together, in addition to Scheme 1. Formation of Pyrrolic-N from Polybenzoxazine Species acting as an emulsion stabilizer, EDTA may also serve as a new source to functionalize carbon nanospheres for electrocatalysis.…”

Section: ■ Results and Discussionmentioning

confidence: 99%

“…Interestingly, the nitrogen in CNS-E-600 primarily existed as graphitic-N at a high level of 42.66%, whereas the control sample, CNS-600, only contained 25.24% (Table S2). Although there is some controversy, many reports have demonstrated graphitic-N to be the most promising species toward ORR and OER. ,, Taken together, in addition to acting as an emulsion stabilizer, EDTA may also serve as a new source to functionalize carbon nanospheres for electrocatalysis.…”

Section: Resultsmentioning

confidence: 99%

“… 10 In both cases, the carbon nanospheres were not adequately functionalized with nitrogen (N) heteroatoms, the crucial active sites needed to achieve superior electrocatalysis and enhanced wettability. 16 − 19 As a result, these carbon nanospheres would have limited use as metal-free electrocatalysts. To our knowledge, there is no report on the use of a nitrogen-containing phenolic derivative such as 3-aminophenol to produce uniform, N-doped carbon nanospheres with tunable diameters below 200 nm.…”

Section: Introductionmentioning

confidence: 99%

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EDTA-Assisted Synthesis of Nitrogen-Doped Carbon Nanospheres with Uniform Sizes for Photonic and Electrocatalytic Applications

et al. 2023

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We report a robust method for the facile synthesis of N-doped carbon nanospheres with uniform and tunable sizes. Instead of involving a surfactant or other templates, this synthesis relies on the incorporation of ethylenediaminetetraacetic acid (EDTA) into the emulsion droplets of phenolic resin oligomers. The EDTA provides a high density of surface charges to effectively increase the electrostatic repulsion between the droplets and thereby prevent them from coalescing into irregular structures during polymerization-induced hardening. The EDTA-loaded polymer nanospheres are highly uniform in terms of both size and shape for easy crystallization into opaline structures. While maintaining good uniformity, the diameters of the resultant N-doped carbon nanospheres can be readily tuned from 100 to 375 nm, allowing for the fabrication of opaline lattices with brilliant structural colors. The EDTA also serves as an additional nitrogen source to promote the formation of graphitic-N, making the N-doped carbon nanospheres highly active, metal-free bifunctional electrocatalysts toward oxygen reduction and oxygen evolution reactions.

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Section: ■ Results and Discussionmentioning

confidence: 99%

Section: Resultsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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EDTA-Assisted Synthesis of Nitrogen-Doped Carbon Nanospheres with Uniform Sizes for Photonic and Electrocatalytic Applications

et al. 2023

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“…To verify further the role of TM in ORR catalytic activity, the pristine C 1 N 1 was evaluated as electrocatalysts since quaternary nitrogen species were also found to be active for the ORR. [31,32] Figure S12 (Supporting Information) shows the poor catalytic activity of C 1 N 1 compared to Fe@CN x and Mn@CN x , revealing the crucial role of metal nanoclusters and single atoms embedded in the C 1 N 1derived carbon structure. Furthermore, the heat treatment temperature for the most catalytic TM@CN x material was optimized.…”

Section: Oxygen Reduction Reaction (Orr)mentioning

confidence: 99%

Advanced Design of Metal Nanoclusters and Single Atoms Embedded in C₁N₁‐Derived Carbon Materials for ORR, HER, and OER

Quílez‐Bermejo

García‐Dalí

Daouli

et al. 2023

Adv Funct Materials

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Single atoms and nanoclusters of Fe, Ni, Co, Cu, and Mn are systematically designed and embedded in a well‐defined C1N1‐type material that has internal cavities of ≈0.6 nm based on four N atoms. These N atoms serve as perfect anchoring points for the nucleation of small nanoclusters of different metal natures through the creation of metal‐nitrogen (TM‐N4) bonds. After pyrolysis at 800 °C, TM@CNx‐type structures are obtained, where TM is the transition metal and x < 1. Fe@CNx and Co@CNx are the most promising for oxygen reduction reaction and hydrogen evolution reaction, respectively, with a Pt‐like performance, and Ni@CNx is the most active for oxygen evolution reaction (OER) with an EOER of 1.59 V versus RHE, far outperforming the commercial IrO2 (EOER = 1.72 V). This systematic and benchmarking study can serve as a basis for the future design of advanced multi‐functional electrocatalysts by modulating and combining the metallic nature of nanoclusters and single atoms.

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“…[28][29][30][31] Therefore, enhance the loading-density of desired single-atom sites is the main challenge in the efficient fabrication of MÀ N x À C catalysts. [9,[32][33][34] Zhou reports a multilayer stabilization strategy for preparing high-loading M-SACs catalysts via the confinement of organometallic precursors inside other two type of organic molecule and polymer. [35] Zhao et al also publishes a clicking confinement strategy to transition metal single-atom sites by pre-anchoring Co-coordinated porphyrin units in the surface of CNT.…”

Section: Introductionmentioning

confidence: 99%

Construction of Cu Single‐Atom Catalysts by Taking Spatial‐Confinement and Chemical‐Anchoring Effect of Hyperbranched Phthalocyanine Copper for Efficient Oxygen Reduction Reaction

Chen,

Li,

et al. 2024

ChemistrySelect

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Atomically dispersed nonprecious metal‐based catalysts have been considered as the most promising alternatives to Pt‐based catalysts since their excellent catalytic activities and almost 100 % atom utilization in oxygen reduction reaction. However, the agglomeration of metal atoms is unavoidable during pyrolysis process, thus leads to the decrease of electrocatalytic performance. Herein, hyperbranched phthalocyanine copper (HCuPc) wrapping nano‐silica is synthesized via in situ polymerization and served as precursor for preparing atomically dispersed Cu−N−C electrocatalysts. Owing to the confinement effect of chemical‐anchoring and spatial‐hindrance, the migration and agglomeration of Cu atoms are restricted in carbonization process. The aberration‐corrected high‐angle annular dark‐field scanning transmission electron microscopy and X‐ray photoelectron spectroscopy (XPS) are performed to confirm the atomically dispersed of as‐synthesized catalyst, which is labelled as HCu−N−C/SiO2. In addition, the HCu−N−C/SiO2 possess superior ORR electrocatalytic activities with a half‐wave potential of 0.874 V vs RHE and a limiting current density of 5.7 mA cm−2. The zinc‐air batteries assembled with HCu−N−C/SiO2 catalyst exhibit a high specific capacity of 789 mAh g−1 as well as a maximum discharge power density of 176 mW cm−2. This work proves that hyperbranched phthalocyanine structure could be a useful confined framework to the fabrication of singles‐atom catalysts.

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Easy enrichment of graphitic nitrogen to prepare highly catalytic carbons for oxygen reduction reaction

Cited by 12 publications

References 78 publications

EDTA-Assisted Synthesis of Nitrogen-Doped Carbon Nanospheres with Uniform Sizes for Photonic and Electrocatalytic Applications

EDTA-Assisted Synthesis of Nitrogen-Doped Carbon Nanospheres with Uniform Sizes for Photonic and Electrocatalytic Applications

Advanced Design of Metal Nanoclusters and Single Atoms Embedded in C₁N₁‐Derived Carbon Materials for ORR, HER, and OER

Construction of Cu Single‐Atom Catalysts by Taking Spatial‐Confinement and Chemical‐Anchoring Effect of Hyperbranched Phthalocyanine Copper for Efficient Oxygen Reduction Reaction

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Easy enrichment of graphitic nitrogen to prepare highly catalytic carbons for oxygen reduction reaction

Cited by 12 publications

References 78 publications

EDTA-Assisted Synthesis of Nitrogen-Doped Carbon Nanospheres with Uniform Sizes for Photonic and Electrocatalytic Applications

EDTA-Assisted Synthesis of Nitrogen-Doped Carbon Nanospheres with Uniform Sizes for Photonic and Electrocatalytic Applications

Advanced Design of Metal Nanoclusters and Single Atoms Embedded in C1N1‐Derived Carbon Materials for ORR, HER, and OER

Construction of Cu Single‐Atom Catalysts by Taking Spatial‐Confinement and Chemical‐Anchoring Effect of Hyperbranched Phthalocyanine Copper for Efficient Oxygen Reduction Reaction

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Advanced Design of Metal Nanoclusters and Single Atoms Embedded in C₁N₁‐Derived Carbon Materials for ORR, HER, and OER