Scalable and Cost‐Effective Synthesis of Highly Efficient Fe<sub>2</sub>N‐Based Oxygen Reduction Catalyst Derived from Seaweed Biomass

Liu, Long; Yang, Xianfeng; Ma, Na; Liu, Haitao; Xia, Yanzhi; Chen, Cheng-Meng; Yang, Dongjiang; Yao, Xiangdong

doi:10.1002/smll.201503305

Cited by 148 publications

(109 citation statements)

References 34 publications

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“…[29,30] Such 3D metal-organic polymer supramolecular structure could efficiently disperse and stabilize Fe ions via chelating metal-oxygen bonds, and make the resulting Fe-N x sites atomically distributed in highly porous (surface area up to 1200 m 2 g −1 ) and sheet-like structures after pyrolyzing with nitrogen precursor. SA consists of α-l-guluronic (G-block) and β-d-mannuronic (M-block) acid units that are rich with hydrophilic groups (e.g.,-COOH,-OH).…”

mentioning

confidence: 99%

Atomically Dispersed Fe‐N_x/C Electrocatalyst Boosts Oxygen Catalysis via a New Metal‐Organic Polymer Supramolecule Strategy

Miao

Wang

Tsai

et al. 2018

Advanced Energy Materials

224

114

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the-state-of-the-art ORR catalysts but their uses are largely restricted by the prohibitive cost and limited activity/stability. [3][4][5][6][7] In this regard, the development of non-Pt group metal (non-PGM) catalysts derived from earth-abundant elements for ORR is the fundamental solution for the widespread applications of PEMFCs. [8][9][10] Among various non-PGM ORR catalysts developed in last decade, transition metalnitrogen-carbon (M-N-C) catalysts with M-N x coordination active sites embedded in the basal planes of carbon matrixes were the most promising ones due to their decent activity in both acidic and alkaline media and ease of scale-up production. [11][12][13][14][15] The ORR performance of M-N-C electrocatalysts in alkaline electrolyte has been well demonstrated notwithstanding, [9,[16][17][18][19][20] their performance in acidic environment is still deficient and often degrades rapidly due to the etching of metal species and/or decomposition of active sites. [21,22] Generally, the M-N-C catalysts are prepared via high-temperature (T > 800 °C) pyrolysis process of transition metal (e.g., Fe, Co, Ni), nitrogen, and carbon precursors, during which the metal atoms are very easy to agglomerate into large particles. The aggregated metal and metal oxide/carbide particles will hinder the accessibility of M-N x /C active sites and lower the utilization of M atoms seriously, thus compromising their ORR activity. Furthermore, metal aggregates will be easily etched away in acid, leading to The development of high-performance oxygen reduction reaction (ORR) catalysts derived from non-Pt group metals (non-PGMs) is urgent for the wide applications of proton exchange membrane fuel cells (PEMFCs). In this work, a facile and cost-efficient supramolecular route is developed for making non-PGM ORR catalyst with atomically dispersed Fe-N x /C sites through pyrolyzing the metal-organic polymer coordinative hydrogel formed between Fe 3+ and α-L-guluronate blocks of sodium alginate (SA). High-angle annular dark field scanning transmission electron microscopy (HAADF-STEM) and X-ray absorption spectroscopy (XAS) verify that Fe atoms achieve atomic-level dispersion on the obtained SA-Fe-N nanosheets and a possible fourfold coordination with N atoms. The best-performing SA-Fe-N catalyst exhibits excellentORR activity with half-wave potential (E 1/2 ) of 0.812 and 0.910 V versus the reversible hydrogen electrode (RHE) in 0.5 m H 2 SO 4 and 0.1 m KOH, respectively, along with respectable durability. Such performance surpasses that of most reported non-PGM ORR catalysts. Density functional theory calculations suggest that the relieved passivation effect of OH* on Fe-N 4 /C structure leads to its superior ORR activity to Pt/C in alkaline solution. The work demonstrates a novel strategy for developing high-performance non-PGM ORR electrocatalysts with atomically dispersed and stable M-N x coordination sites in both acidic and alkaline media.

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confidence: 99%

Atomically Dispersed Fe‐N_x/C Electrocatalyst Boosts Oxygen Catalysis via a New Metal‐Organic Polymer Supramolecule Strategy

Miao

Wang

Tsai

et al. 2018

Advanced Energy Materials

224

114

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“…In Fig. 4d, two peaks in the Si2p XPS spectrum situated at 101.7 and 102.9 were attributed to the Si-O in the PDMS [33] and SiO 2 in the wood, respectively. In the Fe region (Fig.…”

Section: Resultsmentioning

confidence: 96%

Biomimetic taro leaf-like films decorated on wood surfaces using soft lithography for superparamagnetic and superhydrophobic performance

et al. 2017

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The surfaces of plants represent multifunctional interfaces between the organisms and the environment. In this paper, biomimetic taro leaf-like structures with superparamagnetic and superhydrophobic performances were exactly copied on the wood surface through the soft lithography to improve the wood properties. Fe 3 O 4 nanoparticles were mixed into poly(dimethylsiloxane) PDMS suspensions to obtain Fe 3 O 4 /PDMS suspensions that commonly endow coats magnetic and microwave absorption properties, which were then cast onto the wood surface and packaged by PDMS stamps replicated from fresh taro leaves. Fe 3 O 4 /PDMS films, which coexisted superhydrophobic surface and superparamagnetic property, were created on the wood surface after the being dried and stamps were peeled off. The as-prepared wood surface exhibited unique taro leaf-like micro-and nanostructures, microwave absorption, superparamagnetism performances with maximum saturation magnetization (M s ) of 22.9 emu g -1 and superior static superhydrophobicity with a water contact angle of 152°± 2°. This research may provide a feasible pathway for constructing naturally biomorphic structures on the wood surface with tailored functions.

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“…Figure 3a shows the XPS survey spectrum of Fe/CuÀN-rGO/CNT that suggests the presence and content of C, N (7.03 at %), Fe (0.34 at %), Cu (0.76 at %) and O. High-resolution XPS spectra can provide further information about the chemical bonding structure of composites. [39,40] 1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 The Cu2p core level XP spectrum showed peaks around 931.4 and 951.3 eV, which were attributed to the Cu2p3/2 and Cu2p1/2 BE values, respectively ( Figure 3d). [37] The higher ratios of pyrrolic nitrogen and pyridinic nitrogen were revealed for the Fe/CuÀN-rGO/CNT composites.…”

Section: Resultsmentioning

confidence: 99%

Doping Copper Ions into an Fe/N/C Composite Promotes Catalyst Performance for the Oxygen Reduction Reaction

Wei

Wang

et al. 2017

ChemElectroChem

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Developing new non-precious-metal catalysts for the cathodic oxygen reduction reaction (ORR) in low-temperature fuel cells is highly desirable for replacing Pt-based noble-metal electrocatalysts. Herein, we report a two-step method to prepare Fe, Cu, and N-doped reduced graphene oxide/carbon nanotube (rGO/CNT) composites through the low-temperature hydrothermal treatment of iron-porphyrin-modified graphene and copper-chloride-loaded CNTs followed by high-temperature calcination, for use as efficient and stable electrocatalysts for the ORR. The optimized Fe/CuÀN-rGO/CNT catalyst exhibited higher ORR activity and superior stability, as compared to a commercial Pt/C catalyst in 0.1 mol · L À1 KOH solutions, and also demonstrates good stability in acidic electrolytes. These results suggest that additional doping of Cu ions into the Fe/N/C catalyst significantly promotes the catalyst ORR performance.

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Scalable and Cost‐Effective Synthesis of Highly Efficient Fe₂N‐Based Oxygen Reduction Catalyst Derived from Seaweed Biomass

Cited by 148 publications

References 34 publications

Atomically Dispersed Fe‐N_x/C Electrocatalyst Boosts Oxygen Catalysis via a New Metal‐Organic Polymer Supramolecule Strategy

Atomically Dispersed Fe‐N_x/C Electrocatalyst Boosts Oxygen Catalysis via a New Metal‐Organic Polymer Supramolecule Strategy

Biomimetic taro leaf-like films decorated on wood surfaces using soft lithography for superparamagnetic and superhydrophobic performance

Doping Copper Ions into an Fe/N/C Composite Promotes Catalyst Performance for the Oxygen Reduction Reaction

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Scalable and Cost‐Effective Synthesis of Highly Efficient Fe2N‐Based Oxygen Reduction Catalyst Derived from Seaweed Biomass

Cited by 148 publications

References 34 publications

Atomically Dispersed Fe‐Nx/C Electrocatalyst Boosts Oxygen Catalysis via a New Metal‐Organic Polymer Supramolecule Strategy

Atomically Dispersed Fe‐Nx/C Electrocatalyst Boosts Oxygen Catalysis via a New Metal‐Organic Polymer Supramolecule Strategy

Biomimetic taro leaf-like films decorated on wood surfaces using soft lithography for superparamagnetic and superhydrophobic performance

Doping Copper Ions into an Fe/N/C Composite Promotes Catalyst Performance for the Oxygen Reduction Reaction

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Scalable and Cost‐Effective Synthesis of Highly Efficient Fe₂N‐Based Oxygen Reduction Catalyst Derived from Seaweed Biomass

Atomically Dispersed Fe‐N_x/C Electrocatalyst Boosts Oxygen Catalysis via a New Metal‐Organic Polymer Supramolecule Strategy

Atomically Dispersed Fe‐N_x/C Electrocatalyst Boosts Oxygen Catalysis via a New Metal‐Organic Polymer Supramolecule Strategy