Molecular electrocatalysts can mediate fast, selective CO2 reduction in a flow cell

Science ◽  
2019 ◽  
Vol 365 (6451) ◽  
pp. 367-369 ◽  
Author(s):  
Shaoxuan Ren ◽  
Dorian Joulié ◽  
Danielle Salvatore ◽  
Kristian Torbensen ◽  
Min Wang ◽  
...  
Keyword(s):  
Flow Reactor ◽  
Co2 Reduction ◽  
Reduction Reaction ◽  
Operating Conditions ◽  
High Current ◽  
Membrane Flow ◽  
Molecular Catalyst ◽  
Current Densities ◽  
Molecular Catalysts ◽  
Distinct Approach

Practical electrochemical carbon dioxide (CO2) conversion requires a catalyst capable of mediating the efficient formation of a single product with high selectivity at high current densities. Solid-state electrocatalysts achieve the CO2 reduction reaction (CO2RR) at current densities ≥ 150 milliamperes per square centimeter (mA/cm2), but maintaining high selectivities at high current densities and efficiencies remains a challenge. Molecular CO2RR catalysts can be designed to achieve high selectivities and low overpotentials but only at current densities irrelevant to commercial operation. We show here that cobalt phthalocyanine, a widely available molecular catalyst, can mediate CO2 to CO formation in a zero-gap membrane flow reactor with selectivities > 95% at 150 mA/cm2. The revelation that molecular catalysts can work efficiently under these operating conditions illuminates a distinct approach for optimizing CO2RR catalysts and electrolyzers.

scholarly journals A Water-Soluble Sodium Pectate Complex with Copper as an Electrochemical Catalyst for Carbon Dioxide Reduction

Molecules ◽  
2021 ◽  
Vol 26 (18) ◽  
pp. 5524
Author(s):  
Kirill V. Kholin ◽  
Mikhail N. Khrizanforov ◽  
Vasily M. Babaev ◽  
Guliya R. Nizameeva ◽  
Salima T. Minzanova ◽  
...  
Keyword(s):  
Co2 Reduction ◽  
Reduction Reaction ◽  
Water Soluble ◽  
Molecular Catalyst ◽  
Electrochemical Catalyst ◽  
Highly Active ◽  
Electrochemical Co2 Reduction ◽  
The Stability ◽  
Molecular Catalysts ◽  
Co2 Reduction Reaction

A selective noble-metal-free molecular catalyst has emerged as a fruitful approach in the quest for designing efficient and stable catalytic materials for CO2 reduction. In this work, we report that a sodium pectate complex of copper (PG-NaCu) proved to be highly active in the electrocatalytic conversion of CO2 to CH4 in water. Stability and selectivity of conversion of CO2 to CH4 as a product at a glassy carbon electrode were discovered. The copper complex PG-NaCu was synthesized and characterized by physicochemical methods. The electrochemical CO2 reduction reaction (CO2RR) proceeds at −1.5 V vs. Ag/AgCl at ~10 mA/cm2 current densities in the presence of the catalyst. The current density decreases by less than 20% within 12 h of electrolysis (the main decrease occurs in the first 3 h of electrolysis in the presence of CO2). This copper pectate complex (PG-NaCu) combines the advantages of heterogeneous and homogeneous catalysts, the stability of heterogeneous solid materials and the performance (high activity and selectivity) of molecular catalysts.

Three-dimensional porous copper-decorated bismuth-based nanofoam for boosting electrochemical reduction of CO2 to formate

2021 ◽  
Author(s):  
Yingchun Zhang ◽  
Changsheng Cao ◽  
Xintao Wu ◽  
Qi-Long Zhu
Keyword(s):  
Current Density ◽  
High Current Density ◽  
Three Dimensional ◽  
Co2 Reduction ◽  
Reduction Reaction ◽  
High Current ◽  
Porous Copper ◽  
Reduction Of Co2 ◽  
Co2 Reduction Reaction ◽  
Wide Potential

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...

scholarly journals Molecular electrocatalysts transform CO into C2+ products effectively in a flow cell

2020 ◽  
Author(s):  
Shaoxuan Ren ◽  
Arthur Fink ◽  
Eric Lees ◽  
Zishuai Zhang ◽  
Wen Yu Wu ◽  
...  
Keyword(s):  
Copper Phthalocyanine ◽  
Co2 Reduction ◽  
Product Formation ◽  
Flow Cell ◽  
Reduction Reaction ◽  
Flow Cells ◽  
New Class ◽  
Current Densities ◽  
Co2 Reduction Reaction ◽  
Co2 Electrolysis

Abstract The highest performance flow cells capable of electrolytically converting CO2 into higher value chemicals and fuels pass a concentrated hydroxide electrolyte across the cathode. A major problem for CO2 electrolysis is that this strongly alkaline medium converts the majority of CO2 into unreactive HCO3– and CO32– rather than CO2 reduction reaction (CO2RR) products. The electrolysis of CO (instead of CO2) does not suffer from this same problem because CO does not react with hydroxide. Moreover, CO can be more readily converted into products containing two or more carbon atoms (i.e., C2+ products). While several solid-state electrocatalysts have proven competent at converting CO into C2+ products, we demonstrate here that molecular electrocatalysts are also effective at mediating this transformation in a flow cell. Using a molecular copper phthalocyanine (CuPc) electrocatalyst, CO was electrolyzed into C2+ products at high rates of product formation (i.e., current densities J ≥200 mA/cm2), and at high Faradaic efficiencies for C2+ production (FEC2+; 72% at 200 mA/cm2). These findings present a new class of electrocatalysts for making carbon-neutral chemicals and fuels.

scholarly journals Analysis of Mass Flows and Membrane Cross-over in CO2 Reduction at High Current Densities in an MEA-Type Electrolyzer

2019 ◽  
Vol 11 (44) ◽  
pp. 41281-41288 ◽  
Author(s):  
Gastón O. Larrazábal ◽  
Patrick Strøm-Hansen ◽  
Jens P. Heli ◽  
Kevin Zeiter ◽  
Kasper T. Therkildsen ◽  
...  
Keyword(s):  
Co2 Reduction ◽  
High Current ◽  
Current Densities ◽  
Mass Flows

scholarly journals CO2 reduction on gas-diffusion electrodes and why catalytic performance must be assessed at commercially-relevant conditions

2019 ◽  
Vol 12 (5) ◽  
pp. 1442-1453 ◽  
Author(s):  
Thomas Burdyny ◽  
Wilson A. Smith
Keyword(s):  
Local Reaction ◽  
Co2 Reduction ◽  
Catalytic Performance ◽  
Gas Diffusion ◽  
High Current ◽  
Gas Diffusion Electrodes ◽  
Current Densities ◽  
Current Practices

The substantial implications of high current densities on the local reaction environment and design of catalysts for electrochemical CO2 reduction are addressed. The presented perspectives also reflect on current practices within the field and offer new opportunities for both future catalyst and system-focused research efforts.

Engineering conductive network of atomically thin bismuthene with rich defects enables CO2 reduction to formate with industry-compatible current densities and stability

2021 ◽  
Author(s):  
Min Zhang ◽  
Wenbo Wei ◽  
Shenghua Zhou ◽  
Dong-Dong Ma ◽  
Aihui Cao ◽  
...  
Keyword(s):  
Co2 Reduction ◽  
Value Added ◽  
Reduction Reaction ◽  
Conductive Network ◽  
Electrochemical Co2 Reduction ◽  
Liquid Products ◽  
Current Densities ◽  
Co2 Reduction Reaction

Electrochemical CO2 reduction reaction (CO2RR) to value-added and readily collectable liquid products is promising but remains a great challenge due to the lack of efficient and robust electrocatalysts. Herein, a...

Long-term-stability continuous flow CO2 reduction electrolysers with high current efficiency

2021 ◽  
Author(s):  
Yueyuan Gu ◽  
Jucai Wei ◽  
Jindong Li ◽  
Luyang Wang ◽  
Xu Wu
Keyword(s):  
Continuous Flow ◽  
Co2 Reduction ◽  
Carbon Dioxide Reduction ◽  
Reduction Reaction ◽  
Liquid Electrolyte ◽  
High Current ◽  
High Current Efficiency ◽  
Long Term Stability ◽  
Water Based

One of the intrinsic problems relating to electrolysers for the electrochemical carbon dioxide reduction reaction is that the water-based liquid electrolyte induces the hydrogen evolution reaction.

scholarly journals Substituent-induced electronic localization of nickel phthalocyanine with enhanced electrocatalytic CO2 reduction

2021 ◽  
Author(s):  
Kejun Chen ◽  
Maoqi Cao ◽  
Yiyang Lin ◽  
Junwei Fu ◽  
Hanxiao Liao ◽  
...  
Keyword(s):  
Co2 Reduction ◽  
Catalytic Performance ◽  
Flow Cell ◽  
Reduction Reaction ◽  
Nickel Phthalocyanine ◽  
Localization Strategy ◽  
Current Densities ◽  
Electronic Localization ◽  
Novel Strategy ◽  
Electron Deficiency

Abstract Designing efficient catalysts with high activity and selectivity is desirable and challenging for CO2 reduction reaction (CO2RR). Nickel phthalocyanine (NiPc) is a promising molecule catalyst for CO2RR. However, the pristine NiPc suffers from poor CO2 adsorption and activation due to its electron deficiency of Ni–N4 site, which leads to inferior activity and stability during CO2RR. Here, we develop a substituent-induced electronic localization strategy to improve CO2 adsorption and activation, and thus catalytic performance. Theoretic calculations and experimental results indicate that the electronic localization on the Ni site induced by electron-donating substituents (hydroxyl or amino) of NiPc greatly enhances the CO2 adsorption and activation, which is positively associated with the electron-donating abilities of substituents. Employing the optimal catalyst of amino-substituted NiPc to catalyze CO2 into CO in flow cell can achieve an ultrahigh activity and selectivity of 99.8% at the current densities up to 400 mA cm-2. This work offers a novel strategy to regulate the electronic structure of the active site by introducing substituents for highly efficient CO2RR.

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