Local structure tuning in Fe-N-C catalysts through support effect for boosting CO2 electroreduction

Tuo, Jinqin; Lin, Yunxiang; Zhu, Yihua; Jiang, Hongliang; Li, Yuhang; Cheng, Ling; Pang, Ruichao; Shen, Jianhua; Li, Song; Li, Chunzhong

doi:10.1016/j.apcatb.2020.118960

Cited by 62 publications

(33 citation statements)

References 35 publications

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“…The D 3 band is also observed, arising from interstitial defects of amorphous sp 2 carbon [45,46]. The ratio between the intensity of D and G bands (I D /I G ) was 1.04, in good agreement with others metal/nitrogen-doped carbon catalysts reported in literature [47][48][49][50]. Such value is related to the density of functional groups in the carbon framework [51,52], confirming the role of nitrogen-containing precursor and ammonia atmosphere in the carbon matrix functionalization with iron and nitrogen functionalities.…”

Section: Resultssupporting

confidence: 86%

Nanostructured Fe-N-C as Bifunctional Catalysts for Oxygen Reduction and Hydrogen Evolution

et al. 2021

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The development of electrocatalysts for energy conversion and storage devices is of paramount importance to promote sustainable development. Among the different families of materials, catalysts based on transition metals supported on a nitrogen-containing carbon matrix have been found to be effective catalysts toward oxygen reduction reaction (ORR) and hydrogen evolution reaction (HER) with high potential to replace conventional precious metal-based catalysts. In this work, we developed a facile synthesis strategy to obtain a Fe-N-C bifunctional ORR/HER catalysts, involving wet impregnation and pyrolysis steps. Iron (II) acetate and imidazole were used as iron and nitrogen sources, respectively, and functionalized carbon black pearls were used as conductive support. The bifunctional performance of the Fe-N-C catalyst toward ORR and HER was investigated by cyclic voltammetry, rotating ring disk electrode experiments, and electrochemical impedance spectroscopy in alkaline environment. ORR onset potential and half-wave potential were 0.95 V and 0.86 V, respectively, indicating a competitive performance in comparison with the commercial platinum-based catalyst. In addition, Fe-N-C had also a good HER activity, with an overpotential of 478 mV @10 mAcm−2 and Tafel slope of 133 mVdec−1, demonstrating its activity as bifunctional catalyst in energy conversion and storage devices, such as alkaline microbial fuel cell and microbial electrolysis cells.

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Section: Resultssupporting

confidence: 86%

Nanostructured Fe-N-C as Bifunctional Catalysts for Oxygen Reduction and Hydrogen Evolution

et al. 2021

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“…Reproduced with permission. [ 19 ] Copyright 2020, Elsevier. e) The molecular catalyst with a well‐defined structure immobilized on carbon support by noncovalent intercalation and computed CO binding energies.…”

Section: Classification Of Carbon‐supported Sacs For the Co2rrmentioning

confidence: 99%

“…The molecular catalysts could be covalently [ 28 ] /noncovalently [ 13a,29 ] absorbed on the substrates (Figure 1e), or anchored by axial coordination intercalation between the metal centers and the heteroatoms on substrates (Figure 1d). [ 19 ] Most immobilization conditions only involve simple liquid mixing of the precursors with a gentle heating treatment, which guarantees high structure correlation between the metal complexes and the derived heterogeneous catalysts. Unlike MN x C y catalysts that often comprise complex coordination environments, the heterogeneous molecular catalysts have apparent advantages due to their uniform and well‐defined structures, facilitating the understanding of the CO 2 RR mechanism at the molecular level.…”

Section: Classification Of Carbon‐supported Sacs For the Co2rrmentioning

confidence: 99%

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Carbon‐Supported Single Metal Site Catalysts for Electrochemical CO₂ Reduction to CO and Beyond

Zhu

Yang

Peng

et al. 2021

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The electrochemical CO 2 reduction reaction (CO 2 RR) is a promising strategy to achieve electrical-to-chemical energy storage while closing the global carbon cycle. The carbon-supported single-atom catalysts (SACs) have great potential for electrochemical CO 2 RR due to their high efficiency and low cost. The metal centers' performance is related to the local coordination environment and the long-range electronic intercalation from the carbon substrates. This review summarizes the recent progress on the synthesis of carbon-supported SACs and their application toward electrocatalytic CO 2 reduction to CO and other C 1 and C 2 products. Several SACs are involved, including MN x catalysts, heterogeneous molecular catalysts, and the covalent organic framework (COF) based SACs. The controllable synthesis methods for anchoring single-atom sites on different carbon supports are introduced, focusing on the influence that precursors and synthetic conditions have on the final structure of SACs. For the CO 2 RR performance, the intrinsic activity difference of various metal centers and the corresponding activity enhancement strategies via the modulation of the metal centers' electronic structure are systematically summarized, which may help promote the rational design of active and selective SACs for CO 2 reduction to CO and beyond.

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“…In electrocatalytic reduction, two-compartment electrochemical cells are usually used to evaluate the performance of SACs in the electrocatalytic reduction of CO 2 to CO. Electronic structure and electrical conductivity are the main factors affecting its catalytic activity. Tuo et al [61] loaded single-atom metal Fe on aminated carbon nanotubes for electrocatalytic reduction of CO 2 to CO. Electrochemical tests showed that the catalyst containing aminated carbon nanotubes had low potential (0.39 V) and CO selectivity of up to 95.47 %. Density functional theory calculations show that, compared with planar FeÀ N coordination, additional axial FeÀ N coordination can reduce the free energy required for CO desorption from the adsorption site and inhibit the hydrogen evolution reaction, thus reducing the adsorption rate of CO and improving the selectivity of CO (Figure 11a-11 c).…”

Section: Electrocatalytic Co 2 Reductionmentioning

confidence: 99%

Single‐Atom Catalysts‐Enabled Reductive Upgrading of CO₂

Tan

Yang

2021

ChemCatChem

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Single-atom catalysts (SACs) have attracted extensive attention since their emergence. During the single-atomic catalytic process, the "active center" exists in the form of atomical monodispersion, with nearly 100 % utilization of metal atoms. Uniform and atomically dispersed catalytic centers give SACs pronounced reaction activity and chemical selectivity. Here, we review the development processes, synthetic strategies, charac-terization methods, and applications of SACs in CO 2 reductive upgrading. Also, a comparison of SACs with conventional heterogeneous catalysts in catalytic CO 2 reduction is made and discussed. SACs have built a bridge between homogeneous and heterogeneous catalysis and have the advantages of both, showing a broad prospect in the field of catalysis.

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Local structure tuning in Fe-N-C catalysts through support effect for boosting CO2 electroreduction

Cited by 62 publications

References 35 publications

Nanostructured Fe-N-C as Bifunctional Catalysts for Oxygen Reduction and Hydrogen Evolution

Nanostructured Fe-N-C as Bifunctional Catalysts for Oxygen Reduction and Hydrogen Evolution

Carbon‐Supported Single Metal Site Catalysts for Electrochemical CO₂ Reduction to CO and Beyond

Single‐Atom Catalysts‐Enabled Reductive Upgrading of CO₂

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Local structure tuning in Fe-N-C catalysts through support effect for boosting CO2 electroreduction

Cited by 62 publications

References 35 publications

Nanostructured Fe-N-C as Bifunctional Catalysts for Oxygen Reduction and Hydrogen Evolution

Nanostructured Fe-N-C as Bifunctional Catalysts for Oxygen Reduction and Hydrogen Evolution

Carbon‐Supported Single Metal Site Catalysts for Electrochemical CO2 Reduction to CO and Beyond

Single‐Atom Catalysts‐Enabled Reductive Upgrading of CO2

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Product

Resources

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Carbon‐Supported Single Metal Site Catalysts for Electrochemical CO₂ Reduction to CO and Beyond

Single‐Atom Catalysts‐Enabled Reductive Upgrading of CO₂