Advances and Challenges for the Electrochemical Reduction of CO₂ to CO: From Fundamentals to Industrialization

Angewandte Chemie International Edition, Journal Year: 2021, Volume and Issue: 60(38), P. 20627 - 20648

Published: April 17, 2021

Abstract The electrochemical carbon dioxide reduction reaction (CO 2 RR) provides an attractive approach to convert renewable electricity into fuels and feedstocks in the form of chemical bonds. Among different CO RR pathways, conversion is considered one most promising candidate reactions because its high technological economic feasibility. Integrating catalyst electrolyte design with understanding catalytic mechanism will yield scientific insights promote this technology towards industrial implementation. Herein, we give overview recent advances challenges for selective CO. Multidimensional engineering are also summarized. Furthermore, studies on large‐scale production highlighted facilitate industrialization . To conclude, remaining future directions application generate highlighted.

Language: Английский

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Bismuth Single Atoms Resulting from Transformation of Metal–Organic Frameworks and Their Use as Electrocatalysts for CO₂ Reduction

Journal of the American Chemical Society, Journal Year: 2019, Volume and Issue: 141(42), P. 16569 - 16573

Published: Oct. 5, 2019

The electrocatalytic reduction reaction of CO2 (CO2RR) is a promising strategy to promote the global carbon balance and combat climate change. Herein, exclusive Bi-N4 sites on porous networks can be achieved through thermal decomposition bismuth-based metal-organic framework (Bi-MOF) dicyandiamide (DCD) for CO2RR. Interestingly, in situ environmental transmission electron microscopy (ETEM) analysis not only directly shows from Bi-MOF into Bi nanoparticles (NPs) but also exhibits subsequent atomization NPs assisted by NH3 released DCD. Our catalyst high intrinsic activity CO conversion, with Faradaic efficiency (FECO up 97%) turnover frequency 5535 h-1 at low overpotential 0.39 V versus reversible hydrogen electrode. Further experiments density functional theory results demonstrate that single-atom site dominating active center simultaneously activation rapid formation key intermediate COOH* free energy barrier.

Language: Английский

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Molecular engineering of dispersed nickel phthalocyanines on carbon nanotubes for selective CO2 reduction

Nature Energy, Journal Year: 2020, Volume and Issue: 5(9), P. 684 - 692

Published: Aug. 10, 2020

Language: Английский

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Regulating Photocatalysis by Spin-State Manipulation of Cobalt in Covalent Organic Frameworks

Journal of the American Chemical Society, Journal Year: 2020, Volume and Issue: 142(39), P. 16723 - 16731

Published: Sept. 7, 2020

While catalysis is highly dependent on the electronic structure of catalyst, understanding catalytic performance affected by electron spin regulation remains challenging and rare. Herein, we have developed a facile strategy to manipulation cobalt state over covalent organic frameworks (COFs), COF-367-Co, simply changing oxidation Co centered in porphyrin. Density functional theory (DFT) calculations together with experimental results confirm that CoII CoIII are embedded COF-367 S = 1/2 0 ground states, respectively. Remarkably, photocatalytic CO2 reduction indicate COF-367-CoIII exhibits favorable activity significantly enhanced selectivity HCOOH, accordingly much reduced CO CH4, sharp contrast COF-367-CoII. The highlight spin-state transition greatly regulates performance. Theoretical further disclose presence COF-367-Co preferable formation HCOOH but detrimental its conversion, which clearly accounts for distinctly different photocatalysis To best our knowledge, this first report regulating COFs.

Language: Английский

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An industrial perspective on catalysts for low-temperature CO2 electrolysis

Nature Nanotechnology, Journal Year: 2021, Volume and Issue: 16(2), P. 118 - 128

Published: Jan. 11, 2021

Language: Английский

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Transition metal-based catalysts for the electrochemical CO₂reduction: from atoms and molecules to nanostructured materials

Chemical Society Reviews, Journal Year: 2020, Volume and Issue: 49(19), P. 6884 - 6946

Published: Jan. 1, 2020

An overview of the main strategies for rational design transition metal-based catalysts electrochemical conversion CO₂, ranging from molecular systems to single-atom and nanostructured catalysts.

Language: Английский

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Electrocatalytic reduction of carbon dioxide: opportunities with heterogeneous molecular catalysts

Energy & Environmental Science, Journal Year: 2019, Volume and Issue: 13(2), P. 374 - 403

Published: Dec. 24, 2019

Electrocatalytic CO₂ reduction by heterogeneous molecular catalysts is emerging as an important area for utilization.

Language: Английский

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Porphyrin-based frameworks for oxygen electrocatalysis and catalytic reduction of carbon dioxide

Chemical Society Reviews, Journal Year: 2021, Volume and Issue: 50(4), P. 2540 - 2581

Published: Jan. 1, 2021

The recent progress made on porphyrin-based frameworks and their applications in energy-related conversion technologies (e.g., ORR, OER CO₂RR) storage Zn–air batteries).

Language: Английский

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A Mn-N3 single-atom catalyst embedded in graphitic carbon nitride for efficient CO2 electroreduction

Nature Communications, Journal Year: 2020, Volume and Issue: 11(1)

Published: Aug. 28, 2020

Abstract Developing effective catalysts based on earth abundant elements is critical for CO 2 electroreduction. However, simultaneously achieving a high Faradaic efficiency (FE) and current density of ( j ) remains challenge. Herein, we prepare Mn single-atom catalyst (SAC) with Mn-N 3 site embedded in graphitic carbon nitride. The prepared exhibits 98.8% FE 14.0 mA cm −2 at low overpotential 0.44 V aqueous electrolyte, outperforming all reported SACs. Moreover, higher 29.7 obtained an ionic liquid electrolyte 0.62 overpotential. In situ X-ray absorption spectra functional theory calculations demonstrate that the remarkable performance attributed to site, which facilitates formation key intermediate COOH * through lowered free energy barrier.

Language: Английский

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Molecular catalysis of CO₂ reduction: recent advances and perspectives in electrochemical and light-driven processes with selected Fe, Ni and Co aza macrocyclic and polypyridine complexes

Chemical Society Reviews, Journal Year: 2020, Volume and Issue: 49(16), P. 5772 - 5809

Published: Jan. 1, 2020

Recent developments in (photo)electrochemical CO₂ reduction combining Fe, Ni, and Co molecular complexes (semi)conductive materials have led to high catalytic performances.

Language: Английский

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