.png){kind=icon}
Return
Buffer Effects on Nitrite Reduction Electrocatalysis
.png){kind=icon}
OA
AI
DOI：10.1021/acscatal.4c07765.png)
.png){kind=icon}
Original request for help.png){kind=icon}
Share.png){kind=icon}
Save
Abstract
En 中文
The Haber-Bosch process has provided an energy-intensive way to produce ammonia for over 100 years. However, alternative methods are required to lower pollution and enhance energy efficiency. Unfortunately, key mechanistic insights into the heterogeneous reduction of nitrogen and its intermediates are lacking. The nitrite reduction reaction (NO2RR) is an important electrochemical reaction in the nitrogen cycle, playing a significant role in ammonia-based energy storage and wastewater remediation. Although the NO2RR involves the transfer of multiple protons competing with the hydrogen evolution reaction (HER), the effect of the proton donor has not been investigated in heterogeneous electrocatalysis. We now present an electrochemical study of nitrite reduction in four buffer systems acting as proton donors: citrate, phosphate, 2-(N-morpholino)ethanesulfonic acid, and borate buffers. The chosen catalyst was a typical iron- and nitrogen-codoped carbon (FeNC) with atomically dispersed FeN4 sites. All buffers except borate enhanced the NO2RR considerably, while the reduction mechanism was independent of buffer identity. The kinetics of the reaction depended more strongly on buffer concentration than on the NO 2 - concentration. Furthermore, we propose a double role for the protonated buffer species: a crucial proton donor during the rate-determining reduction of an NO x intermediate and an efficient pH regulator near the electrode. These key mechanistic insights into heterogeneous nitrite reduction help to understand proton-coupled electrocatalysis and contribute to the development of alternative nitrogen-based fuels.
Keywords:
nitrogen cycle
nitrite reduction
buffer effect
proton donor
single atom catalyst
FeNC catalyst
Journal
IF:
13.1
Papers:
1.6W
Citations:
15.0W
Organization
Cited Papers
Electrochemical reduction of nitrate and nitrite in alkaline media at CuNi alloy electrodes.png)
ELECTROCHIMICA ACTA
ELECTROCHIMICA ACTAIF5.6
PREAI
ShareSaveBuffer Assists Electrocatalytic Nitrite Reduction by a Cobalt Macrocycle ComplexINORGANIC CHEMISTRY
INORGANIC CHEMISTRYIF4.7
PREAI
ShareSaveElucidation of the Electrocatalytic Nitrite Reduction Mechanism by Bio-Inspired Copper ComplexesACS CATALYSIS
OAAI
ACS CATALYSISIF13.1
OAAIShareSaveStructure Sensitivity of Pd Facets for Enhanced Electrochemical Nitrate Reduction to AmmoniaACS CATALYSIS
ACS CATALYSISIF13.1
PREAI
ShareSaveShareSaveElectrocatalytic Multielectron Nitrite Reduction in Water by an Iron ComplexACS CATALYSIS
ACS CATALYSISIF13.1
PREAI
ShareSave
View more