scholarly journals Two-Dimensional MoS2: Structural Properties, Synthesis Methods, and Regulation Strategies toward Oxygen Reduction

Micromachines ◽  
2021 ◽  
Vol 12 (3) ◽  
pp. 240
Author(s):  
Hanwen Xu ◽  
Jiawei Zhu ◽  
Qianli Ma ◽  
Jingjing Ma ◽  
Huawei Bai ◽  
...  

Compared with three-dimensional (3D) and other materials, two-dimensional (2D) materials with unique properties such as high specific surface area, structurally adjustable band structure, and electromagnetic properties have attracted wide attention. In recent years, great progress has been made for 2D MoS2 in the field of electrocatalysis, and its exposed unsaturated edges are considered to be active sites of electrocatalytic reactions. In this review, we focus on the latest progress of 2D MoS2 in the oxygen reduction reaction (ORR) that has not received much attention. First, the basic properties of 2D MoS2 and its advantages in the ORR are introduced. Then, the synthesis methods of 2D MoS2 are summarized, and specific strategies for optimizing the performance of 2D MoS2 in ORRs, and the challenges and opportunities faced are discussed. Finally, the future of the 2D MoS2-based ORR catalysts is explored.

2019 ◽  
Vol 9 (1) ◽  
Author(s):  
Jae-Hyung Wee ◽  
Chang Hyo Kim ◽  
Hun-Su Lee ◽  
Go Bong Choi ◽  
Doo-Won Kim ◽  
...  

AbstractNitrogen (N)-doped nanostructured carbons have been actively examined as promising alternatives for precious-metal catalysts in various electrochemical energy generation systems. Herein, an effective approach for synthesizing N-doped single-walled carbon nanohorns (SWNHs) with highly electrocatalytic active sites via controlled oxidation followed by N2 plasma is presented. Nanosized holes were created on the conical tips and sidewalls of SWNHs under mild oxidation, and subsequently, the edges of the holes were easily decorated with N atoms. The N atoms were present preferentially in a pyridinic configuration along the edges of the nanosized holes without significant structural change of the SWNHs. The enriched edges decorated with the pyridinic-N atoms at the atomic scale increased the number of active sites for the oxygen reduction reaction, and the inherent spherical three-dimensional feature of the SWNHs provided good electrical conductivity and excellent mass transport. We demonstrated an effective method for promoting the electrocatalytic active sites within N-doped SWNHs by combining defect engineering with the preferential formation of N atoms having a specific configuration.


Author(s):  
Yuepeng Liu ◽  
Zhongfang Li ◽  
Chongyun Sun ◽  
Shuaifeng Wang ◽  
Likai Wang ◽  
...  

The development of oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) catalysts with high performance and excellent stability is meaningful for fuel cells. Herein, two-dimensional closely packed amide polyphthalocyanine...


Catalysts ◽  
2018 ◽  
Vol 8 (8) ◽  
pp. 301 ◽  
Author(s):  
Dongbin Xiong ◽  
Xifei Li ◽  
Linlin Fan ◽  
Zhimin Bai

The oxygen reduction reaction (ORR) at the cathode is a fundamental process and functions a pivotal role in fuel cells and metal–air batteries. However, the electrochemical performance of these technologies has been still challenged by the high cost, scarcity, and insufficient durability of the traditional Pt-based ORR electrocatalysts. Heteroatom-doped nanocarbon electrocatalysts with competitive activity, enhanced durability, and acceptable cost, have recently attracted increasing interest and hold great promise as substitute for precious-metal catalysts (e.g., Pt and Pt-based materials). More importantly, three-dimensional (3D) porous architecture appears to be necessary for achieving high catalytic ORR activity by providing high specific surface areas with more exposed active sites and large pore volumes for efficient mass transport of reactants to the electrocatalysts. In this review, recent progress on the design, fabrication, and performance of 3D heteroatom-doped nanocarbon catalysts is summarized, aiming to elucidate the effects of heteroatom doping and 3D structure on the ORR performance of nanocarbon catalysts, thus promoting the design of highly active nanocarbon-based ORR electrocatalysts.


2020 ◽  
Author(s):  
Travis Marshall-Roth ◽  
Nicole J. Libretto ◽  
Alexandra T. Wrobel ◽  
Kevin Anderton ◽  
Nathan D. Ricke ◽  
...  

Iron- and nitrogen-doped carbon (Fe-N-C) materials are leading candidates to replace platinum in fuel cells, but their active site structures are poorly understood. A leading postulate is that iron active sites in this class of materials exist in an Fe-N<sub>4</sub> pyridinic ligation environment. Yet, molecular Fe-based catalysts for the oxygen reduction reaction (ORR) generally feature pyrrolic coordination and pyridinic Fe-N<sub>4</sub> catalysts are, to the best of our knowledge, non-existent. We report the synthesis and characterization of a molecular pyridinic hexaazacyclophane macrocycle, (phen<sub>2</sub>N<sub>2</sub>)Fe, and compare its spectroscopic, electrochemical, and catalytic properties for oxygen reduction to a prototypical Fe-N-C material, as well as iron phthalocyanine, (Pc)Fe, and iron octaethylporphyrin, (OEP)Fe, prototypical pyrrolic iron macrocycles. N 1s XPS signatures for coordinated N atoms in (phen<sub>2</sub>N<sub>2</sub>)Fe are positively shifted relative to (Pc)Fe and (OEP)Fe, and overlay with those of Fe-N-C. Likewise, spectroscopic XAS signatures of (phen<sub>2</sub>N<sub>2</sub>)Fe are distinct from those of both (Pc)Fe and (OEP)Fe, and are remarkably similar to those of Fe-N-C with compressed Fe–N bond lengths of 1.97 Å in (phen<sub>2</sub>N<sub>2</sub>)Fe that are close to the average 1.94 Å length in Fe-N-C. Electrochemical studies establish that both (Pc)Fe and (phen<sub>2</sub>N<sub>2</sub>)Fe have relatively high Fe(III/II) potentials at ~0.6 V, ~300 mV positive of (OEP)Fe. The ORR onset potential is found to directly correlate with the Fe(III/II) potential leading to a ~300 mV positive shift in the onset of ORR for (Pc)Fe and (phen<sub>2</sub>N<sub>2</sub>)Fe relative to (OEP)Fe. Consequently, the ORR onset for (phen<sub>2</sub>N<sub>2</sub>)Fe and (Pc)Fe is within 150 mV of Fe-N-C. Unlike (OEP)Fe and (Pc)Fe, (phen<sub>2</sub>N<sub>2</sub>)Fe displays excellent selectivity for 4-electron ORR with <4% maximum H<sub>2</sub>O<sub>2</sub> production, comparable to Fe-N-C materials. The aggregate spectroscopic and electrochemical data establish (phen<sub>2</sub>N<sub>2</sub>)Fe as a pyridinic iron macrocycle that effectively models Fe-N-C active sites, thereby providing a rich molecular platform for understanding this important class of catalytic materials.<p><b></b></p>


2021 ◽  
Author(s):  
Dongsheng Xia ◽  
Chenchen Yu ◽  
Yinghao Zhao ◽  
Yinping Wei ◽  
Haiyan Wu ◽  
...  

The severe degradation of Fe-N-C electrocatalysts during long-term oxygen reduction reaction (ORR) has become a major obstacle for application in proton-exchange membrane fuel cells. Understanding the degradation mechanism and regeneration...


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.


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