scholarly journals N-Doped Graphene as an Efficient Metal-Free Electrocatalyst for Indirect Nitrate Reduction Reaction

Nanomaterials ◽  
2021 ◽  
Vol 11 (9) ◽  
pp. 2418
Author(s):  
Jujiao Zhao ◽  
Bo Shang ◽  
Jun Zhai

N-doped graphene samples with different N species contents were prepared by a two-step synthesis method and evaluated as electrocatalysts for the nitrate reduction reaction (NORR) for the first time. In an acidic solution with a saturated calomel electrode as reference, the pyridinic-N dominant sample (NGR2) had an onset of 0.932 V and a half-wave potential of 0.833 V, showing the superior activity towards the NORR compared to the pyrrolic-N dominant N-doped graphene (onset potential: 0.850 V, half-wave potential: 0.732 V) and the pure graphene (onset potential: 0.698 V, half-wave potential: 0.506 V). N doping could significantly boost the NORR performance of N-doped graphene, especially the contribution of pyridinic-N. Density functional theory calculation revealed the pyridinic-N facilitated the desorption of NO, which was kinetically involved in the process of the NORR. The findings of this work would be valuable for the development of metal-free NORR electrocatalysts.

2021 ◽  
Vol 56 (14) ◽  
pp. 8600-8612
Author(s):  
Qing Zhao ◽  
Cheng Wang ◽  
Haifeng Wang ◽  
Jianlong Wang

AbstractDevelopment of the more stable nonprecious oxygen reduction reaction (ORR) catalyst is of great significance nowadays. Herein, a high-performance iron-doped integral uniform macrocyclic organic framework (MOF–FeZn) catalyst is synthesized through a combined hydrothermal and pyrolysis process, showing favorable ORR activity and stability in acid. This as-synthesized MOF–FeZn catalyst displays high porous and graphitic structures with sufficient catalytic active dopants of pyridinic N, Fe–N, pyrrolic N, graphitic N, making it a promising ORR candidate catalyst with high electrochemical stability. The onset potential, half-wave potential and limited diffusion current density of MOF–FeZn are 0.93 V @ 0.1 mA cm−2, 0.768 V@ 2.757 mA cm−2 and 5.5 mA cm−2, respectively, which are comparable to the state-of-the-art nonprecious catalyst and commercial Pt/C. ORR catalysis on MOF–FeZn follows the nearly four-electron path. What is more, MOF–FeZn can sustain the 10,000 cycles electrochemical potential cycling process in acid with the half-wave potential changed only 21 mV, superior to the reduction of 149 mV for Pt/C. The well-developed integral uniform structures, homogeneously dispersed carbides and nitrides protected by the highly graphitic carbon layers and the better agglomeration suppression of nanoparticles by the confined graphitic carbon layers on catalyst can significantly enhance the catalytic activity and stability of MOF–FeZn.


Catalysts ◽  
2021 ◽  
Vol 11 (11) ◽  
pp. 1354
Author(s):  
Vera Bogdanovskaya ◽  
Inna Vernigor ◽  
Marina Radina ◽  
Vladimir Sobolev ◽  
Vladimir Andreev ◽  
...  

In order to develop highly efficient and stable catalysts for oxygen reduction reaction (ORR) that do not contain precious metals, it is necessary to modify carbon nanotubes (CNT) and define the effect of the modification on their activity in the ORR. In this work, the modification of CNTs included functionalization by treatment in NaOH or HNO3 (soft and hard conditions, respectively) and subsequent doping with nitrogen (melamine was used as a precursor). The main parameters that determine the efficiency of modified CNT in ORR are composition and surface area (XPS, BET), hydrophilic–hydrophobic surface properties (method of standard contact porosimetry (MSP)) and zeta potential (dynamic light scattering method). The activity of CNT in ORR was assessed following half-wave potential, current density within kinetic potential range and the electrochemically active surface area (SEAS). The obtained results show that the modification of CNT with oxygen-containing groups leads to an increase in hydrophilicity and, consequently, SEAS, as well as the total (overall) current. Subsequent doping with nitrogen ensures further increase in SEAS, higher zeta potential and specific activity in ORR, reflected in the shift of the half-wave potential by 150 mV for CNTNaOH-N and 110 mV for CNTHNO3-N relative to CNTNaOH and CNTHNO3, respectively. Moreover, the introduction of N into the structure of CNTHNO3 increases their corrosion stability.


2020 ◽  
Vol 56 (32) ◽  
pp. 4488-4491 ◽  
Author(s):  
Haobin Zhong ◽  
Changwei Shi ◽  
Jiantao Li ◽  
Ruohan Yu ◽  
Qiang Yu ◽  
...  

Cobalt decorated nitrogen-doped carbon bowls (Co@NCB) demonstrate better ORR performance than Pt/C in terms of half-wave potential and stability.


1973 ◽  
Vol 26 (5) ◽  
pp. 971 ◽  
Author(s):  
SC Khurana ◽  
CM Gupta

The electrode reduction reaction of lead malate, involving deprotonated malate ion and a proton, between pK1 and pK2 values of the acid has been investigated. At pH < pK1 protonated ion participates and a proton is involved. The effect of ligand concentration on the half-wave potential of Pb2+ has been investigated and the stability constants of species so formed computed.


2020 ◽  
Vol 7 (4) ◽  
pp. 946-952 ◽  
Author(s):  
Kaili Li ◽  
Daohao Li ◽  
Liangkui Zhu ◽  
Zhuangzhuang Gao ◽  
Qianrong Fang ◽  
...  

A high-performance electrocatalytic material was derived from a new bimetallic ZIF precursor, exhibiting excellent oxygen reduction reaction performance with a half-wave potential (E1/2) of 0.849 V, superior to that of commercial Pt/C.


2014 ◽  
Vol 50 (37) ◽  
pp. 4839-4842 ◽  
Author(s):  
Xin Wang ◽  
Jie Wang ◽  
Deli Wang ◽  
Shuo Dou ◽  
Zhaoling Ma ◽  
...  

Novel N and S co-doped graphene (NSG) was prepared by annealing GO with thiourea. The NSG electrodes show a direct four-electron reaction pathway, higher onset potential, current density and stability than undoped graphene.


RSC Advances ◽  
2016 ◽  
Vol 6 (27) ◽  
pp. 22781-22790 ◽  
Author(s):  
Mei Wu ◽  
Zhiyu Dou ◽  
Jingjing Chang ◽  
Lili Cui

N–S-GAs 900 exhibit an interconnected porous 3D network with random orientation, crumpled sheets in SEM. The onset potential and limiting current density of N–S-GAs 900 are more positive and larger than other catalysts.


1969 ◽  
Vol 2 (3) ◽  
pp. 123-132 ◽  
Author(s):  
J. Badoz-lambling ◽  
G. Demange-guerin

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