Graphitizing N-doped mesoporous carbon nanospheres via facile single atom iron growth for highly efficient oxygen reduction reaction

Xu, Yunshi; Zhu, Liping; Cui, Xuexue; Zhao, Mingyu; Li, Yaling; Chen, Leilei; Jiang, Weicun; Jiang, Ting; Yang, Shuguang; Wang, Yi

doi:10.1007/s12274-020-2689-9

Cited by 55 publications

(25 citation statements)

References 36 publications

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“…For Fe‐SAC/NPC and Fe‐SAC/NC, an extra peak at ≈399.1 eV was present, assigned to the Fe‐N coordination [14] . Moreover, both Fe‐SAC/NPC and Fe‐SAC/NC exhibited a higher percentage of quaternary‐N than the Fe‐free samples, attributed to the in situ graphitization of carbon matrix catalyzed by single Fe atoms during high‐temperature pyrolysis [14c] . The Fe 2p signals of Fe‐SAC/NPC and Fe‐SAC/NC showed a weak peak at ≈709.8 eV (Figure S7e).…”

Section: Figurementioning

confidence: 99%

Phosphorus Induced Electron Localization of Single Iron Sites for Boosted CO₂ Electroreduction Reaction

et al. 2021

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Electrochemical reduction of carbon dioxide (CO2) into chemicals and fuels has recently attracted much interest, but normally suffers from a high overpotential and low selectivity. In this work, single P atoms were introduced into a N‐doped carbon supported single Fe atom catalyst (Fe‐SAC/NPC) mainly in the form of P−C bonds for CO2 electroreduction to CO in an aqueous solution. This catalyst exhibited a CO Faradaic efficiency of ≈97 % at a low overpotential of 320 mV, and a Tafel slope of only 59 mV dec−1, comparable to state‐of‐the‐art gold catalysts. Experimental analysis combined with DFT calculations suggested that single P atom in high coordination shells (n≥3), in particular the third coordination shell of Fe center enhanced the electronic localization of Fe, which improved the stabilization of the key *COOH intermediate on Fe, leading to superior CO2 electrochemical reduction performance at low overpotentials.

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Section: Figurementioning

confidence: 99%

Phosphorus Induced Electron Localization of Single Iron Sites for Boosted CO₂ Electroreduction Reaction

et al. 2021

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“…To activate pristine carbon materials, heteroatoms such as N, S, O, and P have to be doped into carbon matrix to induce charge polarization of carbon atoms, alter the electronic structure and local density of states, or introduce structural defects, which may possibly bring about distinct catalytic properties. [199][200][201][202] Heteroatom doped carbon materials have been widely used for efficiently catalyzing hydrogen evolution reaction, oxygen reduction reaction, electrochemical CO 2 reduction, oxygen evolution reaction, etc. [22,81,116,200,201] Regarding OER in acidic electrolytes, carbon based electrocatalysts including heteroatom doped carbon and hybrid carbon materials have been developed to boost the reaction kinetics.…”

Section: Carbon-based Nanomaterialsmentioning

confidence: 99%

Recent Progress in Advanced Electrocatalyst Design for Acidic Oxygen Evolution Reaction

et al. 2021

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more promising approach to generating H 2 with high purity. Electrochemical water splitting, driven by renewable electricity, proceeds through hydrogen evolution reaction (HER) at the cathode side and oxygen evolution reaction (OER) at the anode side of an electrochemical cell. [7,10] The HER, a two-electron transfer process, is the simplest electrochemical reaction and relatively easy to occur. On the contrary, OER involving four-electron transfer is a much more complicated multistep reaction. A considerably large overpotential is thus added to the actual water splitting process because of the complexity of OER, leading to sluggish reaction kinetics and distinctly reducing the energy efficiency. [11] Therefore, efficient electrocatalysts with high activity and durable stability are needed to overcome the high energy barrier.OER is an electrochemical process of producing molecular O 2 through a series of proton-electron coupled steps. [12][13][14] Depending on the pH of the electrolytes, the reaction pathways of producing O 2 are totally different. In alkaline electrolytes, hydroxyl groups (OH − ) are oxidized and converted to H 2 O and O 2 . In acidic media, two water molecules (H 2 O) are oxidized generating four protons (H + ) and O 2 . Compared to acidic OER, alkaline OER possesses more favorable reaction kinetics because of the abundant hydroxyl groups in the electrolyte. For acidic OER, however, the break of the strong covalent OH bond of H 2 O requires high energy thus leading to more sluggish kinetics. Another advantage for alkaline OER lies in the wide range of catalysts such as transition metal (e.g., Ni, Co, and Fe) based oxides and hydroxides as well as carbon materials. [15][16][17][18][19][20][21][22] The electrocatalysts for acidic OER are mostly related to iridium (Ir) and ruthenium (Ru) based materials currently. [19,[23][24][25][26][27][28][29][30][31] In spite of the more favorable kinetics and wide range of catalysts for alkaline OER, however, acidic OER is more preferable than alkaline OER because of the diversified advantages of proton exchange membrane water electrolyzers over alkaline water electrolyzers. [19,23] Proton exchange membrane (PEM) is an acidic solid polymer electrolyte membrane with much smaller gas crossover than that of the alkaline solid polymer, which can ensure a larger load range and much safer operation of an acidic electrolyzer by largely avoiding forming H 2 /O 2 mixture. [32] Furthermore, the fully developed PEMs can provide high proton conductivity, resulting in low Ohmic loss and high current density. [32] Proton exchange membrane (PEM) water electrolyzers hold great significance for renewable energy storage and conversion. The acidic oxygen evolution reaction (OER) is one of the main roadblocks that hinder the practical application of PEM water electrolyzers. Highly active, cost-effective, and durable electrocatalysts are indispensable for lowering the high kinetic barrier of OER to achieve boosted reaction kinetics. To date, a wide spectrum of advanced electroca...

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“…On the other hand, from the insight of theoretical understanding, rational designing ORR catalysts must meet the standards that the adsorption of O 2 molecule on the specific sites should neither too strong nor too weak, because the later reaction steps are greatly affected by the binding energy of O and active sites. [197,198] The whole electrochemical ORR proceeds through either a direct four-electron (4e − ) pathway or two-electron (2e − ) transfer by reducing O 2 to H 2 O or OH − as final products in acidic or basic solution, respectively. The former pathway is preferred in fuel cell device, and the latter pathway proposes a green synthesis method for versatile clean oxidant H 2 O 2 .…”

Section: Orrmentioning

confidence: 99%

Rational Design of Single‐Atom Site Electrocatalysts: From Theoretical Understandings to Practical Applications

2021

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inflicting the foreign potential. Up to now, the state-of-the-art electrocatalysts mainly depend on the noble-metal-based catalysts, such as platinum (Pt), Palladium (Pd), ruthenium (Ru), Iridium (Ir), rhodium (Rh), and gold (Au). [1,2] While the high cost and low storage of noble-metals compel the sluggish pullulation of electrocatalytic applications. [3] The avenues to overcome this bottleneck issue mainly include two aspects. One strategy is to seek a promising substituendum with superior catalytic activity to replace the traditional noble-metal catalysts. Based on this strategy, enormous breakthroughs have been reported via modulating the macroscopic physical and chemical properties, such as shape, structure, size, crystal face, and composition. [4][5][6][7][8][9][10][11][12][13] Another strategy is to minimize the usage of noble-metals without weakening electrocatalytic performance. In comparison with the conventional bulk catalysts, reducing the usage of noble metal via downsizing the particles to clusters or even the single atoms can trigger the immeasurably electrocatalytic performance based on the site isolation effect and size effect, as illustrated in Figure 1. [14][15][16] The catalytic reactions, involving the heterogeneous and homogeneous, usually occur on the surface of catalysts, of which the serviceable active sites are restricted to small fraction of surface atoms. Thus, isolating the active sites individually to prepare the single-atom site electrocatalysts (SACs) can greatly elevate the atomic utilization. From the microscopic view, although the atomically dispersed metal atoms could present their maximized utilization, the high surface free energy of single atoms suffer from the migration and aggregation. [17,18] Anchoring the single atom on the suitable supports is the key prerequisite for realizing the efficient catalysis. Some compounds, such as metals, metal oxides, metal chlorides/carbides/ nitrides/sulfides, layered double hydroxides (LDHs), and other modified carbon materials, are used as the supports to stabilize the single atoms. [19][20][21] In addition, enormous preparation strategies of stable and high-efficiency electrocatalysts are also presented, such as the impregnation and coprecipitation strategy, spatial confinement strategy, coordination site construction strategy, defect/vacant design strategy, electrochemical method, atomic layer deposition (ALD) method, synthesizing SACs from bulk metals or metal oxide powers, ball-milling method, and so on.Atomically dispersed metal-based electrocatalysts have attracted increasing attention due to their nearly 100% atomic utilization and excellent catalytic performance. However, current fundamental comprehension and summaries to reveal the underlying relationship between single-atom site electrocatalysts (SACs) and corresponding catalytic application are rarely reported. Herein, the fundamental understandings and intrinsic mechanisms underlying SACs and corresponding electrocatalytic applications are systemically summarized. Different ...

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Graphitizing N-doped mesoporous carbon nanospheres via facile single atom iron growth for highly efficient oxygen reduction reaction

Cited by 55 publications

References 36 publications

Phosphorus Induced Electron Localization of Single Iron Sites for Boosted CO₂ Electroreduction Reaction

Phosphorus Induced Electron Localization of Single Iron Sites for Boosted CO₂ Electroreduction Reaction

Recent Progress in Advanced Electrocatalyst Design for Acidic Oxygen Evolution Reaction

Rational Design of Single‐Atom Site Electrocatalysts: From Theoretical Understandings to Practical Applications

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Graphitizing N-doped mesoporous carbon nanospheres via facile single atom iron growth for highly efficient oxygen reduction reaction

Cited by 55 publications

References 36 publications

Phosphorus Induced Electron Localization of Single Iron Sites for Boosted CO2 Electroreduction Reaction

Phosphorus Induced Electron Localization of Single Iron Sites for Boosted CO2 Electroreduction Reaction

Recent Progress in Advanced Electrocatalyst Design for Acidic Oxygen Evolution Reaction

Rational Design of Single‐Atom Site Electrocatalysts: From Theoretical Understandings to Practical Applications

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Phosphorus Induced Electron Localization of Single Iron Sites for Boosted CO₂ Electroreduction Reaction

Phosphorus Induced Electron Localization of Single Iron Sites for Boosted CO₂ Electroreduction Reaction