First-row transition metals and nitrogen co-doped carbon nanotubes: The exact origin of the enhanced activity for oxygen reduction reaction

Li, Tuanfeng; Deng, Haijing; Liu, Jingjun; Jin, Chun; Song, Ye; Wang, Rui

doi:10.1016/j.carbon.2018.12.007

Cited by 48 publications

(19 citation statements)

References 53 publications

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“…Meanwhile, CoFe nanoparticles modified N‐doped carbon nanotubes entangled with graphene oxide was also synthesized through chemical vapor deposition and possessed better ORR activities . Particularly, the N‐doped carbon nanotubes were also extensively researched and exhibited excellent ORR activities but inferior OER activities . Based on these pioneering works, doping nitrogen into the carbon matrix structure is a method that can be used to regulate the distribution of electrons on the adjacent carbon atoms, which creates more effective active sites that improve the ORR activity.…”

Section: Introductionmentioning

confidence: 99%

Self‐Catalyzed Growth of Co, N‐Codoped CNTs on Carbon‐Encased CoS_x Surface: A Noble‐Metal‐Free Bifunctional Oxygen Electrocatalyst for Flexible Solid Zn–Air Batteries

Lü

Zou

et al. 2019

Adv Funct Materials

236

126

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The self‐catalyzed growth of nanostructures on material surfaces is one of the most time‐ and cost‐effective ways to design multifunctional catalysts for a wide range of applications. Herein, the use of this technique to develop a multicomponent composite catalyst with CoSx core encapsulated in an ultrathin porous carbon shell entangled with Co, N‐codoped carbon nanotubes is reported. The as‐prepared catalyst has a superior catalytic activity for oxygen evolution and oxygen reduction reactions, an ultralow potential gap of 0.74 V, and outstanding durability, surpassing most previous reports. Such superiority is ascribed, in part, to the unique 3D electrode architecture of the composite, which is favorable for transporting oxygen species and electrons and creates a synergy between the components with different functionalities. Moreover, the flexible solid Zn–air battery assembled with such an air electrode shows a steady discharge voltage plateau of 1.25 V and a round‐trip efficiency of 70% at 1 mA cm−2. This work presents a simple strategy to design highly efficient bifunctional oxygen electrocatalysts and may pave the way for the practical application of these materials in many energy conversion/storage devices.

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Section: Introductionmentioning

confidence: 99%

Self‐Catalyzed Growth of Co, N‐Codoped CNTs on Carbon‐Encased CoS_x Surface: A Noble‐Metal‐Free Bifunctional Oxygen Electrocatalyst for Flexible Solid Zn–Air Batteries

Lü

Zou

et al. 2019

Adv Funct Materials

236

126

View full text Add to dashboard Cite

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“…Since the first report of the single-atom catalyst Pt 1 /FeO x with high catalytic activity and selectivity in 2011, single-atom catalysts − have attracted worldwide attention. The studies on the single transition-metal and nitrogen codoped carbon materials (TMN x -C) indicated that they exhibit excellent catalytic efficiency and high stability for ORR. − In experimental study, a series of the first-row transition-metal and nitrogen codoped carbon nanotubes (TM–N-CNTs) have been synthesized, and among them, Fe–N-CNT has high catalytic activity with a positive half-wave potential of 0.87 V . FeN 4 -doped graphene shows high stability and is poisoning resistant compared with Pt/C catalyst, and ORR activity is comparable to the commercial 40 wt % Pt/C .…”

Section: Introductionmentioning

confidence: 99%

Improved Oxygen Reduction Activity in Heteronuclear FeCo-Codoped Graphene: A Theoretical Study

Meng

Yin

et al. 2019

ACS Sustainable Chem. Eng.

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Recently, binuclear transition-metal-doped carbon materials have attracted particular interest because of the enhanced catalytic activity. Herein, a series of homonuclear (M2, M = Mn–Cu) and heteronuclear (FeM, M = Mn–Cu) binuclear transition-metal and nitrogen codoped graphene (M2N6/FeMN6-Gra) has been investigated based on the density functional method. The calculated formation energies and molecular dynamics simulations indicate that these catalysts are stable thermodynamically. Scaling relationships, that is, ΔG *O versus ΔG *OH, ΔG *O versus ΔG *OOH, and ΔG *OH versus ΔG *OOH, are obtained. Interestingly, there is a strong linear relationship for overpotential and the electronegativity difference (between Fe and another metal). Volcano plots, that is, ΔG *O versus equilibrium potential, ΔG *OH versus overpotential, and d band center versus overpotential, are established. The results show that FeMN6-Gra (M = Co, Fe and Ni) has high catalytic activity. This means that ΔG *O, ΔG *OH, and the d band center are good descriptors to evaluate the oxygen reduction reaction (ORR) activity. For FeCoN6-Gra, the working potential is 0.97 V and energy barrier is 0.34 eV in the rate-determining step, which are better than those of Pt (0.78 V and 0.80 eV). These results suggest that binuclear transition-metal and nitrogen codoped graphene are good ORR catalysts and further study toward this direction would provide a novel method for the development of high efficient electrocatalysts.

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“… 10 Based on experimental studies performed on TM-N co-doped carbon nanotubes (TM-N-CNTs), the Fe-N-CNT half-wave potential is 0.87 V, which has high catalytic activity. 11 Specifically, the experimental activity of FeN 4 -doped graphene catalysts is very close to that of commercial 40% Pt/C catalysts. 12 Multistage porous Co–N functionalized graphene aerogels are also effective catalysts for ORR in acidic electrolytes.…”

Section: Introductionmentioning

confidence: 65%

Dual-Metal Active Sites Mediated by p-Block Elements: Knowledge-Driven Design of Oxygen Reduction Reaction Catalysts

et al. 2022

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In this study, the oxygen reduction reaction (ORR) process of dual-metal active site catalysts (FeMN 6 -Gra, M = Mn, Ni, Co, or Cu) mediated by p-block elements was investigated using density functional theory calculations. The obtained results demonstrate that, in most cases, the B-doped FeMN 6 -Gra (M = Mn, Ni, Co, or Cu) catalysts exhibit higher catalytic performance than their undoped counterparts. Among the investigated catalysts, FeNiN 6 -Gra doping by B modulates the adsorption strength of the metal center on the oxygen-containing intermediates, showing the largest increase in the onset potential (from 0.66 to 0.94 V). Importantly, we found a new law that B-doping affects the total charge of the metal adsorption site and the four surrounding N atoms and that there is a linear relationship between the total charge and the Gibbs free energy. Transition state analysis shows that the energy barrier of the thermodynamic rate-determining step (*OH hydrogenation to H 2 O) in the FeNiN 6 B1-Gra-catalyzed ORR process is 0.17 eV, which is smaller than that of the FeNiN 6 -Gra-catalyzed process (0.28 eV). Overall, the results demonstrate that B-doping can improve the activity of FeMN 6 -Gra catalysts and provide a new method for the future development of efficient electrocatalysts.

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First-row transition metals and nitrogen co-doped carbon nanotubes: The exact origin of the enhanced activity for oxygen reduction reaction

Cited by 48 publications

References 53 publications

Self‐Catalyzed Growth of Co, N‐Codoped CNTs on Carbon‐Encased CoS_x Surface: A Noble‐Metal‐Free Bifunctional Oxygen Electrocatalyst for Flexible Solid Zn–Air Batteries

Self‐Catalyzed Growth of Co, N‐Codoped CNTs on Carbon‐Encased CoS_x Surface: A Noble‐Metal‐Free Bifunctional Oxygen Electrocatalyst for Flexible Solid Zn–Air Batteries

Improved Oxygen Reduction Activity in Heteronuclear FeCo-Codoped Graphene: A Theoretical Study

Dual-Metal Active Sites Mediated by p-Block Elements: Knowledge-Driven Design of Oxygen Reduction Reaction Catalysts

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First-row transition metals and nitrogen co-doped carbon nanotubes: The exact origin of the enhanced activity for oxygen reduction reaction

Cited by 48 publications

References 53 publications

Self‐Catalyzed Growth of Co, N‐Codoped CNTs on Carbon‐Encased CoSx Surface: A Noble‐Metal‐Free Bifunctional Oxygen Electrocatalyst for Flexible Solid Zn–Air Batteries

Self‐Catalyzed Growth of Co, N‐Codoped CNTs on Carbon‐Encased CoSx Surface: A Noble‐Metal‐Free Bifunctional Oxygen Electrocatalyst for Flexible Solid Zn–Air Batteries

Improved Oxygen Reduction Activity in Heteronuclear FeCo-Codoped Graphene: A Theoretical Study

Dual-Metal Active Sites Mediated by p-Block Elements: Knowledge-Driven Design of Oxygen Reduction Reaction Catalysts

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Self‐Catalyzed Growth of Co, N‐Codoped CNTs on Carbon‐Encased CoS_x Surface: A Noble‐Metal‐Free Bifunctional Oxygen Electrocatalyst for Flexible Solid Zn–Air Batteries

Self‐Catalyzed Growth of Co, N‐Codoped CNTs on Carbon‐Encased CoS_x Surface: A Noble‐Metal‐Free Bifunctional Oxygen Electrocatalyst for Flexible Solid Zn–Air Batteries