Covalent Grafting of Carbon Nanotubes with a Biomimetic Heme Model Compound To Enhance Oxygen Reduction Reactions

Wei, Ping‐Jie; Yu, Guanlong; Naruta, Yoshinori; Liu, Jingang

doi:10.1002/anie.201403133

Cited by 226 publications

(150 citation statements)

References 48 publications

Supporting

Mentioning

138

Contrasting

Order By: Relevance

“…[28][29][30] Moreover, for tuning the coordination of Fe atoms, the traditional methods mainly focus on introducing the reacting gas atmosphere (e.g., NH 3 ) during the pyrolysis treatment, or adding extra ligand species (e.g., pyridine and imidazole) for Fe atoms. [21,24,31] Nevertheless, it still remains a large challenge to prepare single-atomic Fe catalysts by a facial and effective method for their commercial and technological feasibility.…”

Section: Introductionmentioning

confidence: 99%

Biomass Derived N-Doped Porous Carbon Supported Single Fe Atoms as Superior Electrocatalysts for Oxygen Reduction

Zhang

Gao

Dou

et al. 2017

Small

147

105

View full text Add to dashboard Cite

Exploring sustainable and high-performance electrocatalysts for the oxygen reduction reaction (ORR) is the crucial issue for the large-scale application of fuel cell technology. A new strategy is demonstrated to utilize the biomass resource for the synthesis of N-doped hierarchically porous carbon supported single-atomic Fe (SA-Fe/NHPC) electrocatalyst toward the ORR. Based on the confinement effect of porous carbon and high-coordination natural iron source, SA-Fe/NHPC, derived from the hemin-adsorbed bio-porphyra-carbon by rapid heat-treatment up to 800 °C, presents the atomic dispersion of Fe atoms in the N-doped porous carbon. Compared with the molecular hemin and nanoparticle Fe samples, the as-prepared SA-Fe/NHPC exhibits a superior catalytic activity (E = 0.87 V and J = 4.1 mA cm , at 0.88 V), remarkable catalytic stability (≈1 mV negative shift of E , after 3000 potential cycles), and outstanding methanol-tolerance, even much better than the state-of-the-art Pt/C catalyst. The sustainable and effective strategy for utilizing biomass to achieve high-performance single-atom catalysts can also provide an opportunity for other catalytic applications in the atomic scale.

show abstract

Section: Introductionmentioning

confidence: 99%

Biomass Derived N-Doped Porous Carbon Supported Single Fe Atoms as Superior Electrocatalysts for Oxygen Reduction

Zhang

Gao

Dou

et al. 2017

Small

147

105

View full text Add to dashboard Cite

show abstract

“…[1][2][3] In addition to the scarcity, Pt-based materials as ORR electrocatalysts also suffer from activity decline due to the relatively low instability under the harsh oxidizing conditions of the ORR and the poor tolerance to the poisoning molecules such as methanol. [7][8][9][10][11][12][13][14][15][16][17][18][19][20][21][22][23] As compared with Pt-based materials, however, most of these electrocatalysts are much less efficient in electrochemical environments. 4,5 Porphyry type of metal-nitrogen (Me-N) macrocyclic complexes such as Fe/Co porphyrins and phthalocyanines have long been known as excellent molecular catalysts for O 2 reduction.…”

Section: Introductionmentioning

confidence: 99%

“…[14][15][16][17][18][19][20][21][22][23][24] Especially, it has been shown that the composites of Me-N macrocyclic complexes supported on various novel nanocarbons such as graphene and carbon nanotubes (CNTs) can efficiently catalyze the ORR. [14][15][16][17][18][19][20][21][22][23][24] Especially, it has been shown that the composites of Me-N macrocyclic complexes supported on various novel nanocarbons such as graphene and carbon nanotubes (CNTs) can efficiently catalyze the ORR.…”

Section: Introductionmentioning

confidence: 99%

Tailoring molecular architectures of Fe phthalocyanine on nanocarbon supports for high oxygen reduction performance

Zhang

Hua

et al. 2015

J. Mater. Chem. A

View full text Add to dashboard Cite

Cost-effective non-precious metal electrocatalysts for the oxygen reduction reaction (ORR) is the key for fuel cells to become a viable electricity generation technology. Metal macrocyclic compounds such as Fe/ Co porphyrins and phthalocyanines are excellent molecular catalysts for O 2 reduction; but they are still considerably less competitive than Pt-based materials when catalyzing the ORR in electrochemical environments. Using Fe phthalocyanine (FePc) as a model compound, we show that the electrocatalytic activity of metal macrocyclic compounds for the ORR can be greatly enhanced through tailoring assembling architectures on high-surface-area nanocarbons. By simply ball-milling FePc with nanocarbons, such as graphene nanosheets and carbon-black nanoparticles, molecular architectures of FePc from nanorods to uniform thin shells are obtained. The resulting carbon-supported FePc composites exhibit ORR performance much superior to the state-of-the-art carbon-supported Pt in alkaline solution, with up to a 60 mV positive shift in the half-wave potential and more than 5 times increase in the mass activity. As well as showing that the molecule-support interaction provides a degree of control on the molecular architectures of metal macrocyclic compounds, the present work reveals that the FePc molecule is intrinsically much more efficient than Pt in catalyzing the ORR in alkaline media, and therefore has great prospects as a cathode electrocatalyst in alkaline fuel cells.

show abstract

“…[11,12] To date,t he pyrolysis of precursors containing Fe,N ,a nd Ct og enerate unsaturated Fe atoms with Nand Ccoordination (Fe-N/C) serves as one of the most important routes to Fe-N/C complex ORR catalysts. [14,15] However,i tr emains ac hallenge to develop desirable coordination environments for the Fe atoms in the carbon-supported Fe-containing precursors so as to avoid aggregation during pyrolysis. [12a,14] Therefore,d irect pyrolysis of N-rich Fe precursors presupported on carbon substrates has recently attracted considerable attention to allow adequate control of the activeside structure.…”

mentioning

confidence: 99%

Efficient Oxygen Reduction Reaction (ORR) Catalysts Based on Single Iron Atoms Dispersed on a Hierarchically Structured Porous Carbon Framework

et al. 2018

View full text Add to dashboard Cite

Single Fe atoms dispersed on hierarchically structured porous carbon (SA-Fe-HPC) frameworks are prepared by pyrolysis of unsubstituted phthalocyanine/iron phthalocyanine complexes confined within micropores of the porous carbon support. The single-atom Fe catalysts have aw elldefined atomic dispersion of Fe atoms coordinated by Nligands on the 3D hierarchically porous carbon support. These SA-Fe-HPC catalysts are comparable to the commercial Pt/C electrode even in acidic electrolytes for oxygen reduction reaction (ORR) in terms of the ORR activity (E 1/2 = 0.81 V), but have better long-term electrochemical stability (7 mV negative shift after 3000 potential cycles) and fuel selectivity. In alkaline media, the SA-Fe-HPC catalysts outperform the commercial Pt/C electrode in ORR activity (E 1/2 = 0.89 V), fuel selectivity,a nd long-term stability (1 mV negative shift after 3000 potential cycles). Thus,t hese nSA-Fe-HPCs are promising non-platinum-group metal ORR catalysts for fuel-cell technologies.Supportinginformation and the ORCID identification number(s) for the author(s) of this article can be found under: https://doi.

show abstract

Covalent Grafting of Carbon Nanotubes with a Biomimetic Heme Model Compound To Enhance Oxygen Reduction Reactions

Cited by 226 publications

References 48 publications

Biomass Derived N-Doped Porous Carbon Supported Single Fe Atoms as Superior Electrocatalysts for Oxygen Reduction

Biomass Derived N-Doped Porous Carbon Supported Single Fe Atoms as Superior Electrocatalysts for Oxygen Reduction

Tailoring molecular architectures of Fe phthalocyanine on nanocarbon supports for high oxygen reduction performance

Efficient Oxygen Reduction Reaction (ORR) Catalysts Based on Single Iron Atoms Dispersed on a Hierarchically Structured Porous Carbon Framework

Contact Info

Product

Resources

About