Electrochemical reduction of carbon dioxide with nearly 100% carbon monoxide faradaic efficiency from vacancy-stabilized single-atom active sites

Author(s):  
Chenbao Lu ◽  
Kaiyue Jiang ◽  
Diana Tranca ◽  
Ning Wang ◽  
Hui Zhu ◽  
...  

Single-atom catalysts (SACs) have been rapidly rising as emerging materials in the field of energy conversion, especially for CO2 reduction reaction. However, the selectivity and running current are still beyond...

Author(s):  
Danni Zhou ◽  
Xinyuan Li ◽  
Huishan Shang ◽  
Fengjuan Qin ◽  
Wenxing Chen

Metal-organic framework (MOF) derived single-atom catalysts (SACs), featured unique active sites and adjustable topological structures, exhibit high electrocatalytic performance on carbon dioxide reduction reactions (CO2RR). By modulating elements and atomic...


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.


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):  
Xu Hu ◽  
Sai Yao ◽  
Letian Chen ◽  
Xu Zhang ◽  
Menggai Jiao ◽  
...  

Electrochemical CO2 reduction reaction (CO2RR) is a very important approach to realize sustainable development. Single-atom catalysts show advantages in both homogeneous and heterogeneous catalysis, and considerable progress has been made...


Author(s):  
Rajasekaran Elakkiya ◽  
Govindhan Maduraiveeran

Design of high-performance and Earth-abundant electrocatalysts for electrochemical carbon dioxide (CO2) reduction reaction (CO2RR) into fuels and value-added chemicals offers an emergent pathway for environment and energy sustainable concerns. Herein,...


2019 ◽  
Vol 23 (04n05) ◽  
pp. 453-461
Author(s):  
Sumana Tawil ◽  
Hathaichanok Seelajaroen ◽  
Amorn Petsom ◽  
Niyazi Serdar Sariciftci ◽  
Patchanita Thamyongkit

A clam-shaped molecule comprising a Zn(II)-porphyrin and a Zn(II)-cyclam is synthesized and characterized. Its electrochemical behavior and catalytic activity for homogeneous electrochemical reduction of carbon dioxide (CO[Formula: see text] are investigated by cyclic voltammetry and compared with those of Zn(II)-meso-tetraphenylporphyrin and Zn(II)-cyclam. Under N2-saturated conditions, cyclic voltammetry of the featured complex has characteristics of its two constituents, but under CO2-saturated conditions, the target compound exhibits significant current enhancement. Iterative reduction under electrochemical conditions indicated the target compound has improved stability relative to Zn(II)-cyclam. Controlled potential electrolysis demonstrates that, without addition of water, methane (CH[Formula: see text] is the only detectable product with 1% Faradaic efficiency (FE). The formation of CH4 is not observed under the catalysis of the Zn(II)-porphyrin benchmark compound, indicating that the CO2-capturing function of the Zn(II)-cyclam unit contributes to the catalysis. Upon addition of 3% v/v water, the electrochemical reduction of CO2 in the presence of the target compound gives carbon monoxide (CO) with 28% FE. Dominance of CO formation under these conditions suggests enhancement of proton-coupled reduction. Integrated action of these Zn(II)-porphyrin and Zn(II)-cyclam units offers a notable example of a molecular catalytic system where the cyclam ring captures and brings CO2 into the proximity of the porphyrin catalysis center.


2018 ◽  
Vol 28 (21) ◽  
pp. 1800499 ◽  
Author(s):  
Song Liu ◽  
Hongbin Yang ◽  
Xiang Huang ◽  
Linghui Liu ◽  
Weizheng Cai ◽  
...  

ACS Catalysis ◽  
2019 ◽  
Vol 9 (9) ◽  
pp. 7668-7678 ◽  
Author(s):  
Tristan Asset ◽  
Samuel T. Garcia ◽  
Sergio Herrera ◽  
Nalin Andersen ◽  
Yechuan Chen ◽  
...  

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.


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