Clarifying the critical roles of iron in boosting oxygen reduction: Single Fe atoms anchored on carbon vacancies as efficient active sites

Tan, Feng; Li, Wei; Wang, Jingsong; Min, Chungang; Li, Zhanping; Zhang, Bingsen; Zheng, Xusheng; Li, Lina; Zhang, Longzhou; Zhou, Liexing; Shi, Qi; Yang, Xianfeng

doi:10.1016/j.apcatb.2021.121035

Cited by 29 publications

(13 citation statements)

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“…Based on the exploration of new sustainable energy systems, electrochemical energy conversion technology has been developed rapidly. Electrocatalysts play a key role in energy conversion technology because they improve the rate and efficiency of the chemical conversion involved. − However, commercial electrocatalysts are largely dependent on precious metals, such as Pt, Pd, Ru, Rh, and so forth. − For example, platinum (Pt)- and iridium (Ir)/ruthenium (Ru)-based catalysts are deemed to be the best catalysts for oxygen reduction reaction (ORR), but their high cost and scarcity limit the development and application of electrochemical energy conversion technology. − With the development of technology and the demand for high performance of electrocatalysts, the low-cost transition metal-based materials with efficient electrocatalystic activities are widely considerable. , …”

Section: Introductionmentioning

confidence: 99%

Electrostatic Interaction in Amino Protonated Chitosan–Metal Complex Anion Hydrogels: A Simple Approach to Porous Metal Carbides/N-Doped Carbon Aerogels for Energy Conversion

Liu

Wang

Kong

et al. 2022

ACS Appl. Mater. Interfaces

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In the face of the increasingly serious rapid depletion of fossil fuels, exploring alternative energy conversion technologies may be a promising choice to alleviate this crisis. Transition metal carbides (TMCs)/carbon composites are considered as prospective electrocatalysts due to their high catalytic activities and structural stability. In this work, we report the simple synthesis of TMCs/N-doping carbon aerogels (TMCs/NCAs, including Fe3C/NCA, Mo3C2/NCA, and Fe3C-Mo2C/NCA) for the oxygen reduction reaction (ORR) using protonated chitosan/metal complex anion-chelated aerogels. Among them, the Fe3C/NCA composite possesses efficient ORR activity (similar to Pt/C), and the Fe3C/NCA-assembled Zn–air battery exhibits high power densities of about 250 mW cm–2. The density functional theory calculation reveals that the presence of graphite-N, pyridine-N, and carbon defects in the carbon framework effectively reduces the free energy of ORR occurring in Fe3C. This work provides a simple and extensible strategy for the preparation of TMCs from chitosan, which is expected to be extended to other metal carbides.

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Section: Introductionmentioning

confidence: 99%

Electrostatic Interaction in Amino Protonated Chitosan–Metal Complex Anion Hydrogels: A Simple Approach to Porous Metal Carbides/N-Doped Carbon Aerogels for Energy Conversion

Liu

Wang

Kong

et al. 2022

ACS Appl. Mater. Interfaces

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“…This is the possible reason why V C -N–C materials performed some catalytic activity on the luminol–dissolved oxygen CL reaction (Figure B). Moreover, the adjacent carbon vacancies can directly trap Fe atom to form single Fe atom, creating active sites for oxygen reduction reaction . Under the same experimental conditions, we got the O 2 –• EPR spectra of V C -Fe–N–C SACs solution and Fe–N–C SACs solution, and the O 2 –• EPR signal of V C -Fe–N–C SACs solution was much stronger than that of Fe–N–C SAC solution (Figure S5).…”

Section: Resultsmentioning

confidence: 99%

Carbon Vacancy-Enhanced Activity of Fe–N–C Single Atom Catalysts toward Luminol Chemiluminescence in the Absence of H₂O₂

Li,

Hou,

Liu

et al. 2023

Anal. Chem.

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The classic luminol−H 2 O 2 chemiluminescence (CL) systems suffer from easy self-decomposition of H 2 O 2 at room temperature, hindering the practical applications of the luminol−H 2 O 2 CL system. In this work, unexpectedly, we found that the carbon vacancy-modified Fe−N−C single atom catalysts (V C -Fe−N-C SACs) can directly trigger a luminol solution to generate strong CL emission in the absence of H 2 O 2 . The Fe-based SACs were prepared through the conventional pyrolysis of zeolitic imidazolate frameworks. The massive carbon vacancies were readily introduced into Fe−N−C SACs through a tannic acid-etching process. Carbon vacancy significantly enhanced the catalytic activity of Fe−N−C SACs on the CL reaction of luminol− dissolved oxygen. The V C -Fe−N−C SACs performed a 13.4-fold CL enhancement compared with the classic luminol−Fe 2+ system. It was found that the introduction of a carbon vacancy could efficiently promote dissolved oxygen to convert to reactive oxygen species. As a proof of concept, the developed CL system was applied to detect alkaline phosphatase with a linear range of 0.005−1 U/L as well as a detection limit of 0.003 U/L. This work demonstrated that V C −Fe−N-C SAC is a highly efficient CL catalyst that can promote the analytic application of the luminol CL system.

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“…Recently, due to facile syntheses and stability in high potentials, increasing attention has been paid to metal-based materials, such as metal oxide, metal nitride, metal sulfide, and metal phosphide. Meanwhile, highly dispersed SACs have been well anchored on metal-based supports by various defects, such as cation vacancies and anion vacancies ( Tan et al, 2022 ; Xiao et al, 2022 ). In this part, we turn our focus to metal-based defective materials stabilizing single metal atoms.…”

Section: Defect Engineering On Metal-based Materialsmentioning

confidence: 99%

Recent advances in the design of single-atom electrocatalysts by defect engineering

Chen

Jiang

et al. 2022

Front. Chem.

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Single-atom catalysts (SACs) with isolated metal atoms dispersed on supports have attracted increasing attention due to their maximum atomic utilization and excellent catalytic performance in various electrochemical reactions. However, SACs with a high surface-to-volume ratio are fundamentally less stable and easily agglomerate, which weakens their activity. In addition, another issue that restricts the application of SACs is the low metal loading. Defect engineering is the most effective strategy for the precise synthesis of nanomaterials to catch and immobilize single atoms through the modulation of the electronic structure and coordination environment. Herein, in this mini-review, the latest advances in designing SACs by defect engineering have been first highlighted. Then, the heteroatom doping or intrinsic defects of carbon-based support and anion vacancies or cation vacancies of metal-based supports are systematically evaluated. Subsequently, the structure-activity relationships between a single-atom coupled defect structure and electrocatalytic performance are illustrated by combining experimental results and theoretical calculations. Finally, a perspective to reveal the current challenges and opportunities for controllable preparation, in situ characterization, and commercial applications is further proposed.

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Clarifying the critical roles of iron in boosting oxygen reduction: Single Fe atoms anchored on carbon vacancies as efficient active sites

Cited by 29 publications

References 50 publications

Electrostatic Interaction in Amino Protonated Chitosan–Metal Complex Anion Hydrogels: A Simple Approach to Porous Metal Carbides/N-Doped Carbon Aerogels for Energy Conversion

Electrostatic Interaction in Amino Protonated Chitosan–Metal Complex Anion Hydrogels: A Simple Approach to Porous Metal Carbides/N-Doped Carbon Aerogels for Energy Conversion

Carbon Vacancy-Enhanced Activity of Fe–N–C Single Atom Catalysts toward Luminol Chemiluminescence in the Absence of H₂O₂

Recent advances in the design of single-atom electrocatalysts by defect engineering

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Clarifying the critical roles of iron in boosting oxygen reduction: Single Fe atoms anchored on carbon vacancies as efficient active sites

Cited by 29 publications

References 50 publications

Electrostatic Interaction in Amino Protonated Chitosan–Metal Complex Anion Hydrogels: A Simple Approach to Porous Metal Carbides/N-Doped Carbon Aerogels for Energy Conversion

Electrostatic Interaction in Amino Protonated Chitosan–Metal Complex Anion Hydrogels: A Simple Approach to Porous Metal Carbides/N-Doped Carbon Aerogels for Energy Conversion

Carbon Vacancy-Enhanced Activity of Fe–N–C Single Atom Catalysts toward Luminol Chemiluminescence in the Absence of H2O2

Recent advances in the design of single-atom electrocatalysts by defect engineering

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Carbon Vacancy-Enhanced Activity of Fe–N–C Single Atom Catalysts toward Luminol Chemiluminescence in the Absence of H₂O₂