Improving the oxygen evolution reaction using electronic structure modulation of sulfur-retaining nickel-based electrocatalysts

Author(s):  
Man Ho Han ◽  
Min-wook Pin ◽  
Jai Hyun Koh ◽  
Jong Hyeok Park ◽  
Jihyun Kim ◽  
...  

The sulfurization of transition metals is a promising method for improving their catalytic activities in the oxygen evolution reaction (OER). However, experimental studies regarding the effects of undissolved, remaining S...

2D Materials ◽  
2021 ◽  
Author(s):  
Zhiqiang Zheng ◽  
Yurui Xue ◽  
Yaqi Gao ◽  
Zhongqiang Wang ◽  
Shuya Zhao ◽  
...  

Abstract Developing high-performance metal-free electrocatalysts for acidic oxygen evolution reaction (AOER) is highly desirable but remains great challenge. Here we report a rationally substituting sp-C strategy for the synthesis of methyl- and hydrogen-substituted graphdiyne (MGDY, HGDY) nanowires arrays as 3D porous flexible metal-free electrodes for AOER. Methyl group in MGDY with stronger electron-pushing effect makes electrons around the acetylenic carbon atoms more delocalized, resulting in more uneven distributed surface charge, and higher intrinsic catalytic activities for AOER than HGDY, with the smaller overpotential of 406 mV at 10 mA cm−2 than HGDY and previously reported metal-free electrocatalysts. Our results reveal that the modulation of the electronic structure of GDY by selectively substituting sp-C allows for facilitating charge transfer kinetics, improving adsorption of reaction intermediate, and thereby accelerating the sluggish kinetics of AOER. This work provides us an ideal opportunity for studying the exact HER/OER mechanisms of metal-free carbon materials.


Nano Research ◽  
2021 ◽  
Author(s):  
Yao Kang ◽  
Shuo Wang ◽  
Kwan San Hui ◽  
Shuxing Wu ◽  
Duc Anh Dinh ◽  
...  

AbstractStructural reconstruction of nanomaterials offers a fantastic way to regulate the electronic structure of active sites and promote their catalytic activities. However, how to properly facilitate surface reconstruction to overcome large overpotential that stimulate the surface reconstruction has remained elusive. Herein, we adopt a facile approach to activate surface reconstruction on Ni(OH)2 by incorporating F anions to achieve electro-derived structural oxidation process and further boost its oxygen evolution reaction (OER) activity. Ex situ Raman and X-ray photoemission spectroscopy studies indicate that F ions incorporation facilitated surface reconstruction and promotes the original Ni(OH)2 transformed into a mesoporous and amorphous F-NiOOH layer during the electrochemical process. Density functional theory (DFT) calculation reveals that this self-reconstructed NiOOH induces a space-charge effect on the p-n junction interface, which not only promotes the absorption of intermediates species (*OH, *O, and *OOH) and charge-transfer process during catalysis, but also leads to a strong interaction of the p-n junction interface to stabilize the materials. This work opens up a new possibility to regulate the electronic structure of active sites and promote their catalytic activities.


Author(s):  
Cheng Wang ◽  
Hongyuan Shang ◽  
Yuan Wang ◽  
Hui Xu ◽  
Jie Li ◽  
...  

Interface and electronic structure modulation are widely recognized as promising avenue for optimizing the physiochemical and electrochemical properties of nanomaterials, which are crucial to improving the electrocatalytic oxygen evolution reaction...


Author(s):  
wei yang ◽  
Wenbin Gong ◽  
Yanhong Shi ◽  
Xiaona Wang ◽  
Yulian Wang ◽  
...  

Platinum nanocatalysts mediated by 3d transition metals show improved activity for oxygen reduction reaction (ORR) but poor activity for oxygen evolution reaction (OER). Herein, we report the preparation of a...


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