Atomic-level active sites of efficient imidazolate framework-derived nickel catalysts for CO2 reduction

2019 ◽  
Vol 7 (46) ◽  
pp. 26231-26237 ◽  
Author(s):  
Fuping Pan ◽  
Hanguang Zhang ◽  
Zhenyu Liu ◽  
David Cullen ◽  
Kexi Liu ◽  
...  
Keyword(s):  
Active Sites ◽  
Co2 Reduction ◽  
Nickel Catalysts ◽  
Atomic Level ◽  
Single Atom ◽  
Dangling Bond

Active sites of single-atom nickel catalysts for CO2 reduction were revealed to be edge-located Ni–N2+2 sites with dangling bond-containing carbon atoms, which facilitate the dissociation of the C–O bond of *COOH intermediate.

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...

Synthesis of a Nickel Single-Atom Catalyst Based on Ni–N4–xCx Active Sites for Highly Efficient CO2 Reduction Utilizing a Gas Diffusion Electrode

2020 ◽  
Vol 3 (9) ◽  
pp. 8739-8745
Author(s):  
Syed Asad Abbas ◽  
Jun Tae Song ◽  
Ying Chuan Tan ◽  
Ki Min Nam ◽  
Jihun Oh ◽  
...  
Keyword(s):  
Active Sites ◽  
Co2 Reduction ◽  
Gas Diffusion ◽  
Gas Diffusion Electrode ◽  
Single Atom ◽  
Highly Efficient

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

2021 ◽  
Author(s):  
Chenbao Lu ◽  
Kaiyue Jiang ◽  
Diana Tranca ◽  
Ning Wang ◽  
Hui Zhu ◽  
...  
Keyword(s):  
Carbon Dioxide ◽  
Carbon Monoxide ◽  
Energy Conversion ◽  
Electrochemical Reduction ◽  
Active Sites ◽  
Co2 Reduction ◽  
Reduction Reaction ◽  
Single Atom ◽  
Faradaic Efficiency ◽  
Co2 Reduction Reaction

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...

scholarly journals Atomic-level regulation of single-atom sites catalysts for electrochemical CO2 reduction reaction

2021 ◽  
Author(s):  
Qingyun Qu ◽  
Shufang Ji ◽  
Yuanjun Chen ◽  
Dingsheng Wang ◽  
Yadong Li
Keyword(s):  
Greenhouse Gas ◽  
Co2 Reduction ◽  
Reduction Reaction ◽  
Atomic Level ◽  
Single Atom ◽  
Industrial Products ◽  
Electrochemical Co2 Reduction ◽  
Co2 Reduction Reaction

Electrochemical CO2 reduction reaction (CO2RR) is viewed as a promising way to remove the greenhouse gas CO2 from atmosphere and convert them to useful industrial products like methane, methanol, formate,...

scholarly journals Investigation of Gas Diffusion Electrode Systems for the Electrochemical CO2 Conversion

Catalysts ◽  
2021 ◽  
Vol 11 (4) ◽  
pp. 482
Author(s):  
Hilmar Guzmán ◽  
Federica Zammillo ◽  
Daniela Roldán ◽  
Camilla Galletti ◽  
Nunzio Russo ◽  
...  
Keyword(s):  
Carbon Capture ◽  
Active Sites ◽  
Co2 Reduction ◽  
Gas Diffusion ◽  
Gas Diffusion Electrode ◽  
Catalyst Loading ◽  
Co2 Conversion ◽  
Atmospheric Conditions ◽  
Electrochemical Co2 Reduction ◽  
Liquid Products

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.

Rational Fabrication of Low‐Coordinate Single‐Atom Ni Electrocatalysts by MOFs for Highly Selective CO2 Reduction

2021 ◽  
Author(s):  
Hai-Long Jiang ◽  
Yan Zhang ◽  
Long Jiao ◽  
Weijie Yang ◽  
Chenfan Xie
Keyword(s):  
Co2 Reduction ◽  
Single Atom

scholarly journals Insights on forming N,O-coordinated Cu single-atom catalysts for electrochemical reduction CO2 to methane

2021 ◽  
Vol 12 (1) ◽  
Author(s):  
Yanming Cai ◽  
Jiaju Fu ◽  
Yang Zhou ◽  
Yu-Chung Chang ◽  
Qianhao Min ◽  
...  
Keyword(s):  
Energy Barrier ◽  
Active Sites ◽  
Theoretical Calculations ◽  
High Energy ◽  
Single Atom ◽  
Faradaic Efficiency ◽  
High Energy Barrier ◽  
Catalytic Sites ◽  
Electron Reduction ◽  
First Time

AbstractSingle-atom catalysts (SACs) are promising candidates to catalyze electrochemical CO2 reduction (ECR) due to maximized atomic utilization. However, products are usually limited to CO instead of hydrocarbons or oxygenates due to unfavorable high energy barrier for further electron transfer on synthesized single atom catalytic sites. Here we report a novel partial-carbonization strategy to modify the electronic structures of center atoms on SACs for lowering the overall endothermic energy of key intermediates. A carbon-dots-based SAC margined with unique CuN2O2 sites was synthesized for the first time. The introduction of oxygen ligands brings remarkably high Faradaic efficiency (78%) and selectivity (99% of ECR products) for electrochemical converting CO2 to CH4 with current density of 40 mA·cm-2 in aqueous electrolytes, surpassing most reported SACs which stop at two-electron reduction. Theoretical calculations further revealed that the high selectivity and activity on CuN2O2 active sites are due to the proper elevated CH4 and H2 energy barrier and fine-tuned electronic structure of Cu active sites.

scholarly journals Electronic metal–support interaction modulates single-atom platinum catalysis for hydrogen evolution reaction

2021 ◽  
Vol 12 (1) ◽  
Author(s):  
Yi Shi ◽  
Zhi-Rui Ma ◽  
Yi-Ying Xiao ◽  
Yun-Chao Yin ◽  
Wen-Mao Huang ◽  
...  
Keyword(s):  
Hydrogen Evolution ◽  
Hydrogen Evolution Reaction ◽  
Structure Activity Relationship ◽  
Atomic Level ◽  
Single Atom ◽  
Activity Relationship ◽  
Support Interaction ◽  
Structure Activity ◽  
Metal Support Interaction ◽  
Metal Support

AbstractTuning metal–support interaction has been considered as an effective approach to modulate the electronic structure and catalytic activity of supported metal catalysts. At the atomic level, the understanding of the structure–activity relationship still remains obscure in heterogeneous catalysis, such as the conversion of water (alkaline) or hydronium ions (acid) to hydrogen (hydrogen evolution reaction, HER). Here, we reveal that the fine control over the oxidation states of single-atom Pt catalysts through electronic metal–support interaction significantly modulates the catalytic activities in either acidic or alkaline HER. Combined with detailed spectroscopic and electrochemical characterizations, the structure–activity relationship is established by correlating the acidic/alkaline HER activity with the average oxidation state of single-atom Pt and the Pt–H/Pt–OH interaction. This study sheds light on the atomic-level mechanistic understanding of acidic and alkaline HER, and further provides guidelines for the rational design of high-performance single-atom catalysts.

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