Empirical Insights into the CO2 Reduction Reaction Mechanism: A Study of the Reduction of CO2, CO and Formaldehyde on Cu Electrodes By Differential Electrochemical Mass Spectrometry

2019 ◽  
Author(s):  
Sahithi Ananthaneni ◽  
Rees Rankin

<div>Electrochemical reduction of CO2 to useful chemical and fuels in an energy efficient way is currently an expensive and inefficient process. Recently, low-cost transition metal-carbides (TMCs) are proven to exhibit similar electronic structure similarities to Platinum-Group-Metal (PGM) catalysts and hence can be good substitutes for some important reduction reactions. In this work, we test graphenesupported WC (Tungsten Carbide) nanocluster as an electrocatalyst for the CO2 reduction reaction. Specifically, we perform DFT studies to understand various possible reaction mechanisms and determine the lowest thermodynamic energy landscape of CO2 reduction to various products such as CO, HCOOH, CH3OH, and CH4. This in-depth study of reaction energetics could lead to improvements and develop more efficient electrocatalysts for CO2 reduction.<br></div>


Author(s):  
Yingchun Zhang ◽  
Changsheng Cao ◽  
Xintao Wu ◽  
Qi-Long Zhu

Bismuth (Bi)-based nanomaterials are considered as the promising electrocatalysts for electrocatalytic CO2 reduction reaction (CO2RR), but it is challenging to achieve high current density and selectivity in a wide potential...


Catalysts ◽  
2019 ◽  
Vol 9 (7) ◽  
pp. 604
Author(s):  
Sahithi Ananthaneni ◽  
Zachery Smith ◽  
Rees B. Rankin

Electrochemical reduction of CO2 to useful chemical and fuels in an energy efficient way is currently an expensive and inefficient process. Recently, low-cost transition metal-carbides (TMCs) have been proven to exhibit similar electronic structure similarities to Platinum-Group-Metal (PGM) catalysts and hence, can be good substitutes for some important reduction reactions. In this work, we test graphene-supported WC (Tungsten Carbide) nanoclusters as an electrocatalyst for the CO2 reduction reaction. Specifically, we perform density functional theory (DFT) studies to understand various possible reaction mechanisms and determine the lowest thermodynamic energy landscape of CO2 reduction to various products, such as CO, HCOOH, CH3OH, and CH4. This in-depth study of reaction energetics could lead to improvements and development of more efficient electrocatalysts for CO2 reduction.


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.


2020 ◽  
Vol 10 (10) ◽  
pp. 3487 ◽  
Author(s):  
Changyeon Kim ◽  
Seokhoon Choi ◽  
Min-Ju Choi ◽  
Sol A Lee ◽  
Sang Hyun Ahn ◽  
...  

The photoelectrochemical reduction of CO2 to syngas that is used for many practical applications has been emerging as a promising technique to relieve the increase of CO2 in the atmosphere. Si has been considered to be one of the most promising materials for photoelectrodes, but the integration of electrocatalysts is essential for the photoelectrochemical reduction of CO2 using Si. We report an enhancement of catalytic activity for CO2 reduction reaction by Ag catalysts of tuned morphology, active sites, and electronic structure through reducing anodic treatment. Our proposed photocathode structure, a SiO2 patterned p-Si photocathode with these reduced Ag catalysts, that was fabricated using electron-beam deposition and electrodeposition methods, provides a low onset-potential of −0.16 V vs. the reversible hydrogen electrode (RHE), a large saturated photocurrent density of −9 mA/cm2 at −1.23 V vs. RHE, and faradaic efficiency for CO of 47% at −0.6 V vs. RHE. This photocathode can produce syngas in the ratio from 1:1 to 1:3, which is an appropriate proportion for practical application. This work presents a new approach for designing photocathodes with a balanced catalytic activity and light absorption to improve the photoelectrochemical application for not only CO2 reduction reaction, but also water splitting or N2 reduction reaction.


Energies ◽  
2019 ◽  
Vol 12 (16) ◽  
pp. 3132 ◽  
Author(s):  
Robert Sacci ◽  
Stephanie Velardo ◽  
Lu Xiong ◽  
Daniel Lutterman ◽  
Joel Rosenthal

The ability to synthesize value-added chemicals directly from CO2 will be an important technological advancement for future generations. Using solar energy to drive thermodynamically uphill electrochemical reactions allows for near carbon-neutral processes that can convert CO2 into energy-rich carbon-based fuels. Here, we report on the use of inexpensive CuSn alloys to convert CO2 into CO in an acetonitrile/imidazolium-based electrolyte. Synergistic interactions between the CuSn catalyst and the imidazolium cation enables the electrocatalytic conversion of CO2 into CO at −1.65 V versus the standard calomel electrode (SCE). This catalyst system is characterized by overpotentials for CO2 reduction that are similar to more expensive Au- and Ag-based catalysts, and also shows that the efficacy of the CO2 reduction reaction can be tuned by varying the CuSn ratio.


Author(s):  
Nael Yasri ◽  
Tareq Al-Attas ◽  
Jinguang Hu ◽  
Md Golam Kibria

Developing catalysts that exhibit high efficiencies for the electrochemical CO2 reduction reaction (CO2RR) in aqueous media is vital in both aspects of the healthier environment and for the practical implementation...


2021 ◽  
Author(s):  
Weibin Xie ◽  
Jiasheng Xu ◽  
Ubaidah Md Idros ◽  
Jouji Katsuhira ◽  
Masaaki Fuki ◽  
...  

The increasing CO2 concentration in the atmosphere is an urgent social problem that has to be resolved. Reducing CO2 into compounds useful as energy sources and carbon materials is desirable. For the CO2 reduction reaction (CO2RR) to be operational on a global scale, the catalyst system must: (1) use only renewable energy, (2) be built from abundantly available elements, and (3) not require high-energy reactants. Although light is an alluring energy source, most existing methods utilize electricity. Furthermore, catalyst systems are based on rare heavy metals. Herein, we present a transition-metal-free catalyst system for CO2RR using visible light and containing a carbazole photocatalyst and an organohydride co-catalyst based on benzimidazoline. It produced formate with a turnover number exceeding 8000. No other reduced products such as H2 and CO were generated, confirming the high selectivity of the system. This finding is essential for operating artificial photosynthesis on a useful scale.


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