scholarly journals Alkali Cation Effect on CO2 Electroreduction to CO: A Local Colligative Property

2021 ◽  
Author(s):  
Seung-Jae Shin ◽  
Hansol Choi ◽  
Stefan Ringe ◽  
Da Hye Won ◽  
Chang Hyuck Choi ◽  
...  
Keyword(s):  
Interface Design ◽  
High Performance ◽  
Effective Means ◽  
Co2 Reduction ◽  
Multiscale Simulation ◽  
Reduction Reaction ◽  
Cation Effect ◽  
Cation Concentration ◽  
Electrochemical Co2 Reduction ◽  
Co2 Electroreduction

Converting carbon dioxide (CO2) into valuable products is one of the most important processes for a sustainable society. Especially, the electrochemical CO2 reduction reaction (CO2RR) offers an effective means, but its reaction mechanism is not yet fully understood. Here, we demonstrate that cation-coupled electron transfer (CCET) is a rate-determining step in the CO2RR to carbon monoxide. The first-principles-based multiscale simulation identifies a single cation that coordinates a CO2− intermediate adsorbed on Ag electrode. The CCET is experimentally verified by a collapse of the CO2RR polarization curves upon correcting Nernstianly for a bulk cation concentration. As further confirmation, a kinetic study shows that the CO2RR obeys first-order kinetics on a local cation concentration. Finally, this work unveils that the cation effect on CO2RR originates from the local colligative property, and further highlights the importance of ion-pairing tendency for electrochemical interface design to achieve high-performance CO2 electrolysis.

scholarly journals Alkali Cation Effect on CO2 Electroreduction to CO: A Local Colligative Property

2021 ◽  
Author(s):  
Seung-Jae Shin ◽  
Hansol Choi ◽  
Stefan Ringe ◽  
Da Hye Won ◽  
Chang Hyuck Choi ◽  
...  
Keyword(s):  
Interface Design ◽  
High Performance ◽  
Effective Means ◽  
Multiscale Simulation ◽  
Reduction Reaction ◽  
Cation Effect ◽  
Cation Concentration ◽  
Rate Determining Step ◽  
First Order Kinetics ◽  
Co2 Electroreduction

Abstract Converting carbon dioxide (CO2) into valuable products is one of the most important processes for a sustainable society. Especially, the electrochemical CO2 reduction reaction (CO2RR) offers an effective means, but its reaction mechanism is not yet fully understood. Here, we demonstrate that cation-coupled electron transfer (CCET) is a rate-determining step in the CO2RR to carbon monoxide. The first-principles-based multiscale simulation identifies a single cation that coordinates a CO2− intermediate adsorbed on Ag electrode. The CCET is experimentally verified by a collapse of the CO2RR polarization curves upon correcting Nernstianly for a bulk cation concentration. As further confirmation, a kinetic study shows that the CO2RR obeys first-order kinetics on a local cation concentration. Finally, this work unveils that the cation effect on CO2RR originates from the local colligative property, and further highlights the importance of ion-pairing tendency for electrochemical interface design to achieve high-performance CO2 electrolysis.

scholarly journals Concerted Cation–Electron Transfer Mechanism for CO2 Electroreduction

2021 ◽  
Author(s):  
Seung-Jae Shin ◽  
Hansol Choi ◽  
Stefan Ringe ◽  
Da Hye Won ◽  
Chang Hyuck Choi ◽  
...  
Keyword(s):  
Electron Transfer ◽  
Interface Design ◽  
High Performance ◽  
Alkali Metal Cation ◽  
Effective Means ◽  
Co2 Reduction ◽  
Multiscale Simulation ◽  
Electron Transfer Mechanism ◽  
Electrochemical Co2 Reduction ◽  
Co2 Electroreduction

Converting carbon dioxide (CO2) into valuable products is one of the most important processes for a sustainable society. Especially, the electrochemical CO2 reduction reaction (CO2RR) offers an effective means, but its reaction mechanism is not yet fully understood. Here, we demonstrate that concerted cation–electron transfer (CCET) is a key catalytic step in the CO2RR to carbon monoxide. The first-principles-based multiscale simulation identifies a single cation that coordinates a CO2− intermediate adsorbed on Ag electrode. The CCET is experimentally verified by a collapse of the CO2RR polarization curves upon correcting for the thermodynamic activity of the cation. As further confirmation, a kinetic study shows that the CO2RR obeys first-order kinetics on the local cation concentration at the electric double layer (estimated by measuring the electrode surface charge). Finally, this work unveils the fundamental origin of different CO2RR activity depending on the species of alkali metal cation, and further highlights the importance of ion-pairing tendency of the cations for electrochemical interface design to achieve high-performance CO2 electrolysis.

Understanding the role of axial O in CO2 electroreduction on NiN4 single-atom catalysts via simulations in realistic electrochemical environment

2021 ◽  
Author(s):  
Xu Hu ◽  
Sai Yao ◽  
Letian Chen ◽  
Xu Zhang ◽  
Menggai Jiao ◽  
...  
Keyword(s):  
Sustainable Development ◽  
Heterogeneous Catalysis ◽  
Co2 Reduction ◽  
Reduction Reaction ◽  
Single Atom ◽  
Electrochemical Co2 Reduction ◽  
Co2 Electroreduction ◽  
Important Approach ◽  
Co2 Reduction Reaction

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...

scholarly journals Water-Dispersible CsPbBr3 Perovskite Nanocrystals with Ultra-Stability and its Application in Electrochemical CO2 Reduction

2021 ◽  
Vol 13 (1) ◽  
Author(s):  
Keqiang Chen ◽  
Kun Qi ◽  
Tong Zhou ◽  
Tingqiang Yang ◽  
Yupeng Zhang ◽  
...  
Keyword(s):  
High Performance ◽  
Co2 Reduction ◽  
Reduction Reaction ◽  
Aqueous Environment ◽  
Light Emitting ◽  
Water Dispersible ◽  
Electrochemical Co2 Reduction ◽  
Operation Stability ◽  
Halide Perovskites ◽  
First Time

AbstractThanks to the excellent optoelectronic properties, lead halide perovskites (LHPs) have been widely employed in high-performance optoelectronic devices such as solar cells and light-emitting diodes. However, overcoming their poor stability against water has been one of the biggest challenges for most applications. Herein, we report a novel hot-injection method in a Pb-poor environment combined with a well-designed purification process to synthesize water-dispersible CsPbBr3 nanocrystals (NCs). The as-prepared NCs sustain their superior photoluminescence (91% quantum yield in water) for more than 200 days in an aqueous environment, which is attributed to a passivation effect induced by excess CsBr salts. Thanks to the ultra-stability of these LHP NCs, for the first time, we report a new application of LHP NCs, in which they are applied to electrocatalysis of CO2 reduction reaction. Noticeably, they show significant electrocatalytic activity (faradaic yield: 32% for CH4, 40% for CO) and operation stability (> 350 h).

Tandem catalysis in electrochemical CO2 reduction reaction

Nano Research ◽  
2021 ◽  
Author(s):  
Yating Zhu ◽  
Xiaoya Cui ◽  
Huiling Liu ◽  
Zhenguo Guo ◽  
Yanfeng Dang ◽  
...  
Keyword(s):  
Co2 Reduction ◽  
Reduction Reaction ◽  
Tandem Catalysis ◽  
Electrochemical Co2 Reduction ◽  
Co2 Reduction Reaction

Surface overgrowth on gold nanoparticles modulating high-energy facets for efficient electrochemical CO2 reduction

Nanoscale ◽  
2021 ◽  
Author(s):  
Woong Choi ◽  
Joon Woo Park ◽  
Woonghyeon Park ◽  
Yousung Jung ◽  
Hyunjoon Song
Keyword(s):  
Gold Nanoparticles ◽  
Renewable Energy ◽  
Renewable Energy Sources ◽  
Co2 Reduction ◽  
High Energy ◽  
Reduction Reaction ◽  
Chemical Energy ◽  
Energy Sources ◽  
Electrochemical Co2 Reduction

Electrochemical CO2 reduction reaction (eCO2RR) has been considered one of the potential technologies to store electricity from renewable energy sources into chemical energy. For this aim, designing catalysts with high...

Atomic regulation of metal-organic framework derived carbon-based single-atom catalysts for electrochemical CO2 reduction reaction

2021 ◽  
Author(s):  
Danni Zhou ◽  
Xinyuan Li ◽  
Huishan Shang ◽  
Fengjuan Qin ◽  
Wenxing Chen
Keyword(s):  
Active Sites ◽  
Metal Organic Framework ◽  
Co2 Reduction ◽  
Carbon Dioxide Reduction ◽  
Reduction Reaction ◽  
Single Atom ◽  
Electrochemical Co2 Reduction ◽  
Metal Organic ◽  
Co2 Reduction Reaction ◽  
Organic Framework

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...

Hierarchical three-dimensional copper selenide nanocubes microelectrodes for improved carbon dioxide reduction reaction

2021 ◽  
Author(s):  
Rajasekaran Elakkiya ◽  
Govindhan Maduraiveeran
Keyword(s):  
Carbon Dioxide ◽  
High Performance ◽  
Three Dimensional ◽  
Co2 Reduction ◽  
Value Added ◽  
Carbon Dioxide Reduction ◽  
Reduction Reaction ◽  
Earth Abundant ◽  
Carbon Dioxide Co2 ◽  
Co2 Reduction Reaction

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,...

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