Electrocatalysis for CO₂conversion: from fundamentals to value-added products

Chemical Society Reviews, Journal Year: 2021, Volume and Issue: 50(8), P. 4993 - 5061

Published: Jan. 1, 2021

This timely and comprehensive review mainly summarizes advances in heterogeneous electroreduction of CO₂: from fundamentals to value-added products.

Language: Английский

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Single-atom catalysis in advanced oxidation processes for environmental remediation

Chemical Society Reviews, Journal Year: 2021, Volume and Issue: 50(8), P. 5281 - 5322

Published: Jan. 1, 2021

This review presents the recent advances in synthetic strategies, characterisation, and computations of carbon-based single-atom catalysts, as well their innovative applications mechanisms advanced oxidation technologies.

Language: Английский

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Architectural Design for Enhanced C₂ Product Selectivity in Electrochemical CO₂ Reduction Using Cu-Based Catalysts: A Review

ACS Nano, Journal Year: 2021, Volume and Issue: 15(5), P. 7975 - 8000

Published: May 6, 2021

Electrochemical CO2 reduction to value-added chemicals and fuels is a promising approach mitigate the greenhouse effect arising from anthropogenic emission energy shortage caused by depletion of nonrenewable fossil fuels. The generation multicarbon (C2+) products, especially hydrocarbons oxygenates, great interest for industrial applications. To date, Cu only metal known catalyze C–C coupling in electrochemical reaction (eCO2RR) with appreciable efficiency kinetic viability produce wide range C2 products aqueous solutions. Nonetheless, poor product selectivity associated main technical problem application eCO2RR technology on global scale. Based extensive research efforts, delicate rational design electrocatalyst architecture using principles nanotechnology likely significantly affect adsorption energetics some key intermediates hence inherent pathways. In this review, we summarize recent progress that has been achieved tailoring efficient conversion target products. By considering experimental computational results, further analyze underlying correlations between catalyst its toward Finally, major challenges are outlined, directions future development suggested.

Language: Английский

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Sub‐Second Time‐Resolved Surface‐Enhanced Raman Spectroscopy Reveals Dynamic CO Intermediates during Electrochemical CO₂ Reduction on Copper

Angewandte Chemie International Edition, Journal Year: 2021, Volume and Issue: 60(30), P. 16576 - 16584

Published: April 15, 2021

Abstract The electrocatalytic carbon dioxide (CO 2 ) reduction reaction RR) into hydrocarbons is a promising approach for greenhouse gas mitigation, but many details of this dynamic remain elusive. Here, time‐resolved surface‐enhanced Raman spectroscopy (TR‐SERS) employed to successfully monitor the dynamics CO RR intermediates and Cu surfaces with sub‐second time resolution. Anodic treatment at 1.55 V vs. RHE subsequent surface oxide (below −0.4 RHE) induced roughening electrode surface, which resulted in hotspots TR‐SERS, enhanced resolution (down ≈0.7 s) fourfold improved efficiency toward ethylene. With initial restructuring was followed (<7 s), after stable surrounded by increased local alkalinity formed. Our measurements revealed that highly intermediate, characteristic vibration below 2060 cm −1 , related C−C coupling ethylene production (−0.9 RHE), whereas lower cathodic bias (−0.7 gaseous from isolated static species distinct 2092 .

Language: Английский

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Transition Metal Complexes as Catalysts for the Electroconversion of CO₂: An Organometallic Perspective

Angewandte Chemie International Edition, Journal Year: 2021, Volume and Issue: 60(21), P. 11628 - 11686

Published: Jan. 19, 2021

The electrocatalytic transformation of carbon dioxide has been a topic interest in the field CO2 utilization for long time. Recently, area seen increasing dynamics as an alternative strategy to catalytic hydrogenation reduction. While many studies focus on direct electron transfer molecule at electrode material, molecular transition metal complexes solution offer possibility act catalysts transfer. C1 compounds such monoxide, formate, and methanol are often targeted main products, but more elaborate transformations also possible within coordination sphere center. This perspective article will cover selected examples illustrate categorize currently favored mechanisms electrochemically induced promoted by homogeneous complexes. insights be corroborated with concepts elementary steps organometallic catalysis derive potential strategies broaden diversity products.

Language: Английский

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Porphyrins and phthalocyanines as biomimetic tools for photocatalytic H₂production and CO₂reduction

Chemical Society Reviews, Journal Year: 2022, Volume and Issue: 51(16), P. 6965 - 7045

Published: Jan. 1, 2022

This review summarizes the recent advances in light driven catalytic H 2 evolution and CO reduction systems towards production of solar fuels, utilizing porphyrin or phthalocyanine derivatives.

Language: Английский

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Recent Progresses in Electrochemical Carbon Dioxide Reduction on Copper‐Based Catalysts toward Multicarbon Products

Advanced Functional Materials, Journal Year: 2021, Volume and Issue: 31(37)

Published: June 26, 2021

Abstract Electrochemical carbon dioxide reduction reaction (CO 2 RR) offers a promising way of effectively converting CO to value‐added chemicals and fuels by utilizing renewable electricity. To date, the electrochemical single‐carbon products, especially monoxide formate, has been well achieved. However, efficient conversion more valuable multicarbon products (e.g., ethylene, ethanol, n ‐propanol, ‐butanol) is difficult still under intense investigation. Here, recent progresses in using copper‐based catalysts are reviewed. First, mechanism RR briefly described. Then, representative approaches catalyst engineering introduced toward formation RR, such as composition, morphology, crystal phase, facet, defect, strain, surface interface. Subsequently, key aspects cell for including electrode, electrolyte, design, also discussed. Finally, advances summarized some personal perspectives this research direction provided.

Language: Английский

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NiSn Atomic Pair on an Integrated Electrode for Synergistic Electrocatalytic CO₂ Reduction

Angewandte Chemie International Edition, Journal Year: 2020, Volume and Issue: 60(13), P. 7382 - 7388

Published: Dec. 15, 2020

Abstract The development of efficient electrocatalysts for the CO 2 reduction reaction (CO RR) remains a challenge. Demonstrated here is NiSn atomic‐pair electrocatalyst (NiSn‐APC) on hierarchical integrated electrode, which exhibits synergistic effect in simultaneously promoting activity and selectivity RR to formate. atomic pair consists adjacent Ni Sn, each coordinated with four nitrogen atoms (N 4 ‐Ni‐Sn‐N ). as‐prepared NiSn‐APC displays exceptional formate turnover frequency 4752 h −1 , productivity 36.7 mol g Sn an utilization degree active sites (57.9 %), are superior previously reported single‐atomic catalysts. Both experimental data density‐functional theory calculations verify electron redistribution imposed by Ni, reduces energy barrier *OCHO intermediate makes this potential‐determining step thermodynamically spontaneous. This catalysis provides successful paradigm rational design preparation enhanced performance.

Language: Английский

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Radical Chain Reduction via Carbon Dioxide Radical Anion (CO₂^•–)

Journal of the American Chemical Society, Journal Year: 2021, Volume and Issue: 143(24), P. 8987 - 8992

Published: June 9, 2021

We developed an effective method for reductive radical formation that utilizes the anion of carbon dioxide (CO2•–) as a powerful single electron reductant. Through polarity matched hydrogen atom transfer (HAT) between electrophilic and formate salt, CO2•– occurs key element in new chain reaction. Here, initiation can be performed through photochemical or thermal means, we illustrate ability this approach to accomplish activation range substrate classes. Specifically, employed strategy intermolecular hydroarylation unactivated alkenes with (hetero)aryl chlorides/bromides, deamination arylammonium salts, aliphatic ketyl formation, sulfonamide cleavage. show reactivity electron-poor olefins results either reduction alkene hydrocarboxylation, where potentials utilized predict reaction outcome.

Language: Английский

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Porous organic polymers for CO₂capture, separation and conversion

Chemical Society Reviews, Journal Year: 2022, Volume and Issue: 51(23), P. 9831 - 9852

Published: Jan. 1, 2022

Porous organic polymers (POPs) have long been considered as prime candidates for carbon dioxide (CO2) capture, separation, and conversion. Especially their permanent porosity, structural tunability, stability relatively low cost are key factors in such considerations. Whereas heteratom-rich microporous networks well amine impregnation/functionalization actively exploited to boost the CO2 affinity of POPs, recently, focus has shifted engineering pore environment, resulting a new generation highly POPs rich heteroatoms featuring abundant catalytic sites capture conversion into value-added products. In this review, we aim provide insights structure-property relationships governing using highlight recent advances field.

Language: Английский

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