scholarly journals Superior FexN electrocatalyst derived from 1,1′-diacetylferrocene for oxygen reduction reaction in alkaline and acidic media

2020 ◽  
Vol 9 (1) ◽  
pp. 843-852
Author(s):  
Hunan Jiang ◽  
Jinyang Li ◽  
Mengni Liang ◽  
Hanpeng Deng ◽  
Zuowan Zhou

AbstractAlthough Fe–N/C catalysts have received increasing attention in recent years for oxygen reduction reaction (ORR), it is still challenging to precisely control the active sites during the preparation. Herein, we report FexN@RGO catalysts with the size of 2–6 nm derived from the pyrolysis of graphene oxide and 1,1′-diacetylferrocene as C and Fe precursors under the NH3/Ar atmosphere as N source. The 1,1′-diacetylferrocene transforms to Fe3O4 at 600°C and transforms to Fe3N and Fe2N at 700°C and 800°C, respectively. The as-prepared FexN@RGO catalysts exhibited superior electrocatalytic activities in acidic and alkaline media compared with the commercial 10% Pt/C, in terms of electrochemical surface area, onset potential, half-wave potential, number of electrons transferred, kinetic current density, and exchange current density. In addition, the stability of FGN-8 also outperformed commercial 10% Pt/C after 10000 cycles, which demonstrates the as-prepared FexN@RGO as durable and active ORR catalysts in acidic media.

Author(s):  
M. Daarain Haider ◽  
Naseem Iqbal ◽  
Syed Aun M. Rizvi ◽  
Tayyaba Noor ◽  
Saadia Hanif ◽  
...  

Abstract In the present study, the catalytic activity of copper-loaded cobalt-based metal–organic framework (ZIF-67) composites was studied for their electrochemical oxygen reduction reaction (ORR). The Cu-ZIF-67 composite was prepared by the solvothermal method. After pyrolysis under argon atmosphere at 700 °C, the composite was characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), energy dispersive spectroscopy (EDS), and Fourier transform infrared spectroscopy (FTIR). The electrochemical activity of the composites was tested for ORR in 0.1 M alkaline media using the three-electrode system by cyclic voltammetry (CV), Tafel plots, and electrochemical impedance spectroscopy (EIS). The composites showed variable activity with a current density of 1.32 mA cm−2 at 0.71 V (versus reversible hydrogen electrode (RHE)) onset potential for 70 wt% Cu-ZIF-67, 7.5 mA cm−2 at 0.82 V (versus RHE) onset potential for 50 wt% Cu-ZIF-67, and 11.85 mA cm−2 at 0.85 V (versus RHE) for 30% Cu-ZIF-67. The increasing ratio of the ZIF-67 effect can be attributed to the increased activity of ZIF-67 with the synergistic effect of Cu toward increased current density.


2017 ◽  
Vol 5 (32) ◽  
pp. 16605-16610 ◽  
Author(s):  
Wenhua Zhong ◽  
Jiaxiang Chen ◽  
Peixin Zhang ◽  
Libo Deng ◽  
Lei Yao ◽  
...  

Plasma etching removed less stable carbons and exposed the active sites in Fe–N/C catalysts which resulted in excellent performances towards the oxygen reduction reaction in both acidic and alkaline media.


Catalysts ◽  
2020 ◽  
Vol 10 (11) ◽  
pp. 1326
Author(s):  
Xiuxiang Liao ◽  
Xiaobo Wang ◽  
Cuiyu Huang ◽  
Lihua Zhu

Copper- and nitrogen-codoped reduced graphene oxide material (Cu/N-rGO) was prepared with a hydrothermal method. Its versatile catalytic performances were demonstrated toward the oxidative degradation of rhodamine B (RhB) and oxygen reduction reaction (ORR). The Cu and N codoping of graphene enhanced not only its activation ability toward H2O2, but also its electrocatalytic ability for ORR. It was observed that the use of 3%Cu/N-rGO together with 40 mmol·L−1 H2O2 and 4 mmol·L−1 Na2CO3 could remove more than 94% of the added RhB (30 mg·L−1) in 20 min through a catalytic Fenton-like degradation. Quenching experiments and electron paramagnetic resonance (EPR) measurements indicated that the main reactive species generated in the catalytic oxidation process were surface-bound •OH. The modified graphene also showed good electrocatalytic activity for ORR reaction in alkaline media through a four-electron mechanism. On the electrode of Cu/N-rGO, the ORR reaction exhibited an onset potential of −0.1 V and a half-wave potential of −0.248 V, which were correspondingly close to those on a Pt/C electrode. In comparison with a Pt/C electrode, the 3%Cu/N-rGO electrode showed much greater tolerance to methanol. Such outstanding catalytic properties are attributed to the abundant active sites and the synergism between Cu and N in Cu/N-rGO.


NANO ◽  
2018 ◽  
Vol 13 (01) ◽  
pp. 1850006 ◽  
Author(s):  
Zhongliang Deng ◽  
Qingfeng Yi ◽  
Yuanyuan Zhang ◽  
Huidong Nie ◽  
Guang Li ◽  
...  

In this study, we report the findings that the C–N composites containing Ni and Co (Ni1Co1/C–N, Ni3Co1/C–N, Ni6Co1/C–N, Ni9Co1/C–N, Ni[Formula: see text]Co0/C–N and Ni0Co[Formula: see text]/C–N) can be produced by direct pyrolysis of the NiCo-doped polyaniline (PANI) precursors in N2 atmosphere at 800[Formula: see text]C and show efficient electroactivity for oxygen reduction reaction (ORR) in alkaline media. Distribution and compositions of the catalysts were characterized by SEM, TEM, EDS and XRD techniques. The catalysts were loaded on carbon paper to prepare gas diffusion electrodes, in which electrocatalytic activity for ORR in alkaline media was investigated by voltammetric techniques. The ORR current density on these carbon paper-supported NiCo/C–N catalysts exhibits a linear increase with the negative shift of ORR potential. The ORR onset potential is around [Formula: see text]0.2[Formula: see text]V (versus Ag/AgCl) in alkaline media. Among the prepared catalysts, the catalyst Ni6Co1/C–N presents the largest ORR current density, which is 68.5[Formula: see text]mA[Formula: see text]cm[Formula: see text]@[Formula: see text]0.8[Formula: see text]V (versus Ag/AgCl) in alkaline media. Moreover, Ni6Co1/C–N catalyst also presents good electrocatalytic activity stability for ORR.


2019 ◽  
Vol 9 (3) ◽  
pp. 611-619 ◽  
Author(s):  
Mitsuharu Chisaka ◽  
Hiroyuki Morioka

Phosphor and nitrogen atoms were co-doped into rutile TiO2 phase on TiN to produce new active sites for oxygen reduction reaction.


ACS Catalysis ◽  
2016 ◽  
Vol 6 (10) ◽  
pp. 7249-7259 ◽  
Author(s):  
Kuldeep Mamtani ◽  
Deeksha Jain ◽  
Dmitry Zemlyanov ◽  
Gokhan Celik ◽  
Jennifer Luthman ◽  
...  

Energies ◽  
2019 ◽  
Vol 12 (20) ◽  
pp. 3846 ◽  
Author(s):  
Xiao Luo ◽  
Wuli Han ◽  
Han Ren ◽  
Qingzuo Zhuang

Oxygen reduction reaction (ORR) provides a vital role for microbial fuel cells (MFCs) due to its slow reaction kinetics compared with the anodic oxidation reaction. How to develop new materials with low cost, high efficacy, and eco-friendliness which could replace platinum-based electrocatalysis is a challenge that we have to resolve. In this work, we accomplished this successfully by means of a facile strategy to synthesize a metallic organic framework-derived Fe, N, S co-doped carbon with FeS as the main phase. The Fe/S@N/C-0.5 catalyst demonstrated outstandingly enhanced ORR activity in neutral PBS and alkaline media, compared to that of commercial 20% Pt-C catalyst. Here, we started-up and operated two parallel single-chamber microbial fuel cells of an air cathode, and those cathode catalysts were Fe/S@N/C-0.5 and commercial Pt-C (20% Pt), respectively. Scanning electron microscopy (SEM) elaborated that the Fe/S@N/C-0.5 composite did not change the polyhedron morphology of ZIF-8. According to X-ray diffractometry(XRD) curves, the main crystal phase of the resulted Fe/S@N/C-0.5 was FeS. The chemical environment of N, S, and Fe which are anticipated to be the high-efficiency active sites of ORR for MFCs were investigated by X-ray photoelectron spectroscopic(XPS). Nitrogen adsorption/desorption techniques were used to calculate the pore diameter distribution. In brief, the obtained Fe/S@N/C-0.5 material exhibited a pronounced reduction potential at 0.861 V (versus Reversible Hydrogen Electrode(RHE)) in 0.1M KOH solution and –0.03 V (vs. SCE) in the PBS solution, which both outperform the benchmark platinum-based catalysts. Fe/S@N/C-0.5-MFC had a higher Open Circuit Voltage(OCV) (0.71 V), stronger maximum power density (1196 mW/m2), and larger output voltage (0.47 V) than the Pt/C-MFC under the same conditions.


ACS Catalysis ◽  
2014 ◽  
Vol 4 (10) ◽  
pp. 3454-3462 ◽  
Author(s):  
Deepika Singh ◽  
Kuldeep Mamtani ◽  
Christopher R. Bruening ◽  
Jeffrey T. Miller ◽  
Umit S. Ozkan

2014 ◽  
Vol 2 (8) ◽  
pp. 2663-2670 ◽  
Author(s):  
Ulrike I. Kramm ◽  
Iris Herrmann-Geppert ◽  
Sebastian Fiechter ◽  
Gerald Zehl ◽  
Ivo Zizak ◽  
...  

This work presents two strategies on how the disintegration of FeN4 sites by iron carbide formation can be avoided.


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