scholarly journals Electrochemical Reduction of CO2 on Au Electrocatalysts in a Zero-Gap, Half-Cell Gas Diffusion Electrode Setup: a Systematic Performance Evaluation and Comparison to a H-cell Setup

Author(s):  
Shima Alinejad ◽  
Jonathan Quinson ◽  
Gustav K.H. Wiberg ◽  
Nicolas Schlegel ◽  
Damin Zhang ◽  
...  

Based on H-cell measurements, gold (Au) is one of the most selective catalysts for the CO2 reduction reaction (CO2RR) to CO. To ensure a high dispersion, typically Au small nanoparticles (NPs) are used as catalyst. However, the preparation of small Au NPs based on conventional synthesis methods often requires the use of surfactants such as polyvinylpyrrolidone (PVP). Here, we present a systematic evaluation of the performance of laser-generated, surfactant-free Au NPs for the CO2RR in a gas diffusion electrode (GDE) setup and compare the results to investigations in an H-cell configuration. The GDE setup supplies a continuous CO2 stream at the electrode−electrolyte interface to circumvent CO2 mass transport limitations encountered in conventional H-cells. We investigate the influence of the catalyst loading and the effect of PVP. Comparing the two screening methods, i.e. GDE and H-cell measurements, it is shown that the performance of the same catalyst can be substantially different in the two environments. In the GDE setup without liquid electrolyte-catalyst interface a higher reaction rate, but lower faradaic efficiendy is determined. Independent of the setup, the presence of PVP favours the hydrogen evolution reaction (HER), however, in the GDE setup PVP is more detrimental for the performance than in the H-cell.

Catalysts ◽  
2021 ◽  
Vol 11 (4) ◽  
pp. 482
Author(s):  
Hilmar Guzmán ◽  
Federica Zammillo ◽  
Daniela Roldán ◽  
Camilla Galletti ◽  
Nunzio Russo ◽  
...  

Electrochemical CO2 reduction is a promising carbon capture and utilisation technology. Herein, a continuous flow gas diffusion electrode (GDE)-cell configuration has been studied to convert CO2 via electrochemical reduction under atmospheric conditions. To this purpose, Cu-based electrocatalysts immobilised on a porous and conductive GDE have been tested. Many system variables have been evaluated to find the most promising conditions able to lead to increased production of CO2 reduction liquid products, specifically: applied potentials, catalyst loading, Nafion content, KHCO3 electrolyte concentration, and the presence of metal oxides, like ZnO or/and Al2O3. In particular, the CO productivity increased at the lowest Nafion content of 15%, leading to syngas with an H2/CO ratio of ~1. Meanwhile, at the highest Nafion content (45%), C2+ products formation has been increased, and the CO selectivity has been decreased by 80%. The reported results revealed that the liquid crossover through the GDE highly impacts CO2 diffusion to the catalyst active sites, thus reducing the CO2 conversion efficiency. Through mathematical modelling, it has been confirmed that the increase of the local pH, coupled to the electrode-wetting, promotes the formation of bicarbonate species that deactivate the catalysts surface, hindering the mechanisms for the C2+ liquid products generation. These results want to shine the spotlight on kinetics and transport limitations, shifting the focus from catalytic activity of materials to other involved factors.


2021 ◽  
Author(s):  
Shima Alinejad ◽  
Jonathan Quinson ◽  
Yao Li ◽  
Ying Kong ◽  
Sven Reichenberger ◽  
...  

The lack of a robust and standardized experimental test bed to investigate the performance of catalyst materials for the electrochemical CO2 reduction reaction (ECO2RR) is one of the major challenges in this field of research. To best reproduce and mimic commercially relevant conditions for catalyst screening and testing, gas diffusion electrode (GDE) setups attract a rising attention as an alternative to conventional aqueous-based setups such as the H-cell configuration. In particular a zero-gap design shows promising features for upscaling to the commercial scale. In this study, we develop further our recently introduced zero-gap GDE setup for the CO2RR using an Au electrocatalyst as model system and identify/report the key experimental parameters to control in the catalyst layer preparation in order to optimize the activity and selectivity of the catalyst.


2019 ◽  
Vol 73 (11) ◽  
pp. 922-927 ◽  
Author(s):  
María de Jesús Gálvez-Vázquez ◽  
Shima Alinejad ◽  
Huifang Hu ◽  
Yuhui Hou ◽  
Pavel Moreno-García ◽  
...  

In this work, we discuss the application of a gas diffusion electrode (GDE) setup for benchmarking electrocatalysts for the reductive conversion of CO2 (CO2 RR: CO2 reduction reaction). Applying a silver nanowire (Ag-NW) based catalyst, it is demonstrated that in the GDE setup conditions can be reached, which are relevant for the industrial conversion of CO2 to CO. This reaction is part of the so-called 'Rheticus' process that uses the CO for the subsequent production of butanol and hexanol based on a fermentation approach. In contrast to conventional half-cell measurements using a liquid electrolyte, in the GDE setup CO2 RR current densities comparable to technical cells (>100 mA cm–2) are reached without suffering from mass transport limitations of the CO2 reactant gas. The results are of particular importance for designing CO2 RR catalysts exhibiting high faradaic efficiencies towards CO at technological reaction rates.


2020 ◽  
Vol 8 (18) ◽  
pp. 9032-9038 ◽  
Author(s):  
Jinkyu Lim ◽  
Phil Woong Kang ◽  
Sun Seo Jeon ◽  
Hyunjoo Lee

Productivity of formates from electrochemical CO2 reduction was enhanced by using a Sn catalyst with dense tips electrodeposited on a gas diffusion electrode.


2020 ◽  
Vol 142 (36) ◽  
pp. 15438-15444 ◽  
Author(s):  
Xu Lu ◽  
Chongqin Zhu ◽  
Zishan Wu ◽  
Jin Xuan ◽  
Joseph S. Francisco ◽  
...  

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