Double activation of oxygen intermediates of oxygen reduction reaction by dual inorganic/organic hybrid electrocatalysts

Nano Energy ◽  
2021 ◽  
pp. 106048
Author(s):  
Dong-Gyu Lee ◽  
Su Hwan Kim ◽  
Jiyun Lee ◽  
Seokmin Shin ◽  
Se Hun Joo ◽  
...  
2021 ◽  
Vol 6 (34) ◽  
pp. 9101-9111
Author(s):  
Yashwant P. Kharwar ◽  
Tamilselvi Gurusamy ◽  
Sudip Mandal ◽  
Kothandaraman Ramanujam

2017 ◽  
Vol 53 (96) ◽  
pp. 12942-12945 ◽  
Author(s):  
Naomi Levy ◽  
Jennifer S. Shpilman ◽  
Hilah C. Honig ◽  
Dan T. Major ◽  
Lior Elbaz

An unexpected trend in oxygen reduction reaction activity with four different beta-substituted cobalt-corroles.


2019 ◽  
Vol 7 (36) ◽  
pp. 20952-20957 ◽  
Author(s):  
He Sun ◽  
Mengfan Wang ◽  
Xinchuan Du ◽  
Yu Jiao ◽  
Sisi Liu ◽  
...  

A boron dopant is experimentally and theoretically confirmed to effectively modulate the d-band center of a single-atom catalyst, enabling favorable adsorption kinetics of oxygen intermediates and thus greatly improving the ORR performance.


2021 ◽  
Author(s):  
Xueli Li ◽  
Zhonghua Xiang

Abstract Atomically dispersed Fe and N co-doped carbon (Fe–N–C) catalysts exhibited superior acid oxygen reduction reaction (ORR) activities and recently been considered as the most promising alternatives to the benchmark Pt-based catalysts for proton exchange membrane fuel cells. The atomic configuration between Fe, N and C is one of the key factors to affect ORR activity. However, the traditional synthetic methods that rely on pyrolysis of the mixtures of Fe, N and C precursors often result in the plurality of local environment for the FeNx site. Unveiling the effect of covalent-bonded carbon matrix to FeNx sites towards ORR activity is important but still a great challenge due to inevitable connection of diverse N as well as random defects during the pyrolysis process. Here, we report a proof-of-concept study on the evaluation of covalent-bonded carbon environment connected to FeN4 sites on their catalytic activity via pyrolysis-free approach. Basing on the closed π conjugated phthalocyanine-based intrinsic covalent organic polymers (COPs) with well-designed structures, we directly synthesized a series of atomically dispersed Fe-N-C catalysts with various pure carbon environment without any N doping directly connected to the same FeN4 sites. Experiments coupled with density functional theory demonstrate that the catalytic activities appear a volcano plot with the increase of degree of delocalized π electrons from the carbon matrix. The delocalized π electrons changed anti-bonding d-state energy level of the single FeN4 moieties, hence tailored the adsorption between active centers and oxygen intermediates and altered the rate-determining step of oxygen reduction reaction.


2018 ◽  
Vol 20 (17) ◽  
pp. 11776-11786 ◽  
Author(s):  
Jun Huang ◽  
Jianbo Zhang ◽  
Michael Eikerling

A theoretical framework relates formation of oxygen intermediates to basic electronic and electrostatic properties of the catalytic surface.


2020 ◽  
Vol 16 (4) ◽  
pp. 625-638
Author(s):  
Leila Samiee ◽  
Sedigheh Sadegh Hassani

Background: Porous carbon materials are promising candidate supports for various applications. In a number of these applications, doping of the carbon framework with heteroatoms provides a facile route to readily tune the carbon properties. The oxygen reduction reaction (ORR), where the reaction can be catalyzed without precious metals is one of the common applications for the heteroatom-doped carbons. Therefore, heteroatom doped catalysts might have a promising potential as a cathode in Microbial fuel cells (MFCs). MFCs have a good potential to produce electricity from biological oxidization of wastes at the anode and chemical reduction at the cathode. To the best of our knowledge, no studies have been yet reported on utilizing Sulfur trioxide pyridine (STP) and CMK-3 for the preparation of (N and S) doped ordered porous carbon materials. The presence of highly ordered mesostructured and the synergistic effect of N and S atoms with specific structures enhance the oxygen adsorption due to improving the electrocatalytic activity. So the optimal catalyst, with significant stability and excellent tolerance of methanol crossover can be a promising candidate for even other storage and conversion devices. Methods: The physico-chemical properties of the prepared samples were determined by Small Angle X-ray Diffraction (SAXRD), N2 sorption-desorption, Transmission Electron Microscopy (TEM), Field Emission Scanning Electron Microscopy (FESEM) and X-ray Photoelectron Spectroscopy (XPS). The prepared samples were further applied for oxygen reduction reaction (ORR) and the optimal cathode was tested with the Microbial Fuel Cell (MFC) system. Furthermore, according to structural analysis, The HRTEM, and SAXRD results confirmed the formation of well-ordered hexagonal (p6mm) arrays of mesopores in the direction of (100). The EDS and XPS approved that N and S were successfully doped into the CMK-3 carbon framework. Results: Among all the studied CMK-3 based catalysts, the catalyst prepared by STP precursor and pyrolysis at 900°C exhibited the highest ORR activity with the onset potential of 1.02 V vs. RHE and 4 electron transfer number per oxygen molecule in 0.1 M KOH. The high catalyst durability and fuel-crossover tolerance led to stable performance of the optimal cathode after 5000 s operation, while the Pt/C cathode-based was considerably degraded. Finally, the MFC system with the optimal cathode displayed 43.9 mW·m-2 peak power density showing even reasonable performance in comparison to a Pt/C 20 wt.%.cathode. Conclusions: The results revealed that the synergistic effect of nitrogen and sulfur co-doped on the carbon substrate structure leads to improvement in catalytic activity. Also, it was clearly observed that the porous structure and order level of the carbon substrate could considerably change the ORR performance.


2021 ◽  
Vol 154 (3) ◽  
pp. 034705
Author(s):  
Minchan Li ◽  
Ning Qin ◽  
Zongwei Ji ◽  
Qingmeng Gan ◽  
Zhenyu Wang ◽  
...  

Author(s):  
Dingding Li ◽  
Zheng Han ◽  
Kunyue Leng ◽  
Shenghua Ma ◽  
Yi Wang ◽  
...  

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