Electrocatalytic CO2 conversion to C2 products: Catalysts design, market perspectives and techno-economic aspects

Renewable and Sustainable Energy Reviews, Год журнала: 2022, Номер 161, С. 112329 - 112329

Опубликована: Март 9, 2022

The energy crisis caused by the incessant growth in global demand joint to its associated greenhouse emissions motivates urgent need control and mitigate atmospheric CO2 levels. Leveraging as carbon pool produce value-added products represents a cornerstone of circular economy. Among utilization strategies, electrochemical reduction conversion fuels chemicals is booming due versatility end-product flexibility. Herein most studies focused on C1 although C2 C2+ compounds are chemically economically more appealing targets requiring advanced catalytic materials. Still, despite complex pathways for formation, their multiple assorted applications have motivated search suitable electrocatalysts. In this review, we gather analyse comprehensive manner progress made regarding considering not only catalyst design electrochemistry features but also techno-economic aspects order envisage profitable scenarios. This state-of-the-art analysis showcases that will play key role decarbonisation chemical industry paving way towards low-carbon future.

Язык: Английский

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Efficient Electrocatalytic Reduction of CO₂to Ethane over Nitrogen-Doped Fe₂O₃

Journal of the American Chemical Society, Год журнала: 2022, Номер 144(32), С. 14769 - 14777

Опубликована: Авг. 4, 2022

Non-copper electrocatalysts are seldom reported to generate C2+ products, and the efficiency over these catalysts is low. In this work, we report a nitrogen-doped γ-Fe2O3 (xFe2O3-N@CN) electrocatalyst, which yield C2H6 as major product in an H-cell. At −2.0 V vs Ag/Ag+, Faradaic (FE) for ethane reaches 42% with current density of 32 mA cm–2. This first about selective CO2 reduction (C2H6) iron-based catalyst. The results showed that catalyst possessing FeO1.5–nNn sites enriched oxygen vacancies was beneficial stabilization *COOH intermediates. exposure two adjacent surfaces Fe atoms conducive lowering energy barrier C–C coupling sites, facilitating generation C2H6. work provides strategy design novel tunable local coordination electronic structures converting into C2 products CO2RR.

Язык: Английский

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Challenges and Perspectives of Single-Atom-Based Catalysts for Electrochemical Reactions

JACS Au, Год журнала: 2023, Номер 3(3), С. 736 - 755

Опубликована: Фев. 16, 2023

Single-atom catalysts (SACs) are emerging as the most promising for various electrochemical reactions. The isolated dispersion of metal atoms enables high density active sites, and simplified structure makes them ideal model systems to study structure–performance relationships. However, activity SACs is still insufficient, stability usually inferior but has received little attention, hindering their practical applications in real devices. Moreover, catalytic mechanism on a single site unclear, leading development rely trial-and-error experiments. How can one break current bottleneck sites density? further increase activity/stability sites? In this Perspective, we discuss underlying reasons challenges identify precisely controlled synthesis involving designed precursors innovative heat-treatment techniques key high-performance SACs. addition, advanced operando characterizations theoretical simulations essential uncovering true electrocatalytic an site. Finally, future directions that may arise breakthroughs discussed.

Язык: Английский

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Interlayer Spacing Regulation by Single‐Atom Indium^δ+–N₄ on Carbon Nitride for Boosting CO₂/CO Photo‐Conversion

Advanced Functional Materials, Год журнала: 2023, Номер 33(35)

Опубликована: Май 17, 2023

Abstract Simultaneous optimization on bulk photogenerated‐carrier separation and surface atomic arrangement of catalyst is crucial for reactivity CO 2 photo‐reduction. Rare studies capture the detail that, better than in‐plane regulation, interlayer‐spacing regulation may significantly influence carrier transport bulk‐catalyst thereby affecting its photo‐reduction in g ‐C 3 N 4 . Herein, through a single atom‐assisted thermal‐polymerization process, single‐atom In‐bonded N‐atom (In δ + –N ) (002) crystal planes originally constructed. This In reduces interplanar spacing by electrostatic adsorption, which enhances carriers greatly promotes photoreduction. The photo‐conversion performance this resulted modified superior to other atom loaded carbon nitride catalysts. Moreover, adsorption , *COOH formation energy, optimizes reaction path. It achieves remarkable 398.87 µmol −1 h yield rate, 0.21% apparent quantum efficiency, nearly 100% selectivity without any cocatalyst or sacrificial agent. Through d modulation atom, study provides ground‐breaking insight enhancement from double‐gain view structural control ‐reduction photocatalysts.

Язык: Английский

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Atomically Precise Copper Nanoclusters for Highly Efficient Electroreduction of CO₂ towards Hydrocarbons via Breaking the Coordination Symmetry of Cu Site

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(36)

Опубликована: Июль 20, 2023

Abstract We propose an effective highest occupied d‐orbital modulation strategy engendered by breaking the coordination symmetry of sites in atomically precise Cu nanocluster (NC) to switch product CO 2 electroreduction from HCOOH/CO higher‐valued hydrocarbons. An well‐defined 6 NC with symmetry‐broken Cu−S N 1 active (named (MBD) , MBD=2‐mercaptobenzimidazole) was designed and synthesized a judicious choice ligand containing both S atoms. Different previously reported high HCOOH selectivity NCs 3 sites, structure shows Faradaic efficiency toward hydrocarbons 65.5 % at −1.4 V versus reversible hydrogen electrode (including 42.5 CH 4 23 C H ), partial current density −183.4 mA cm −2 . Theoretical calculations reveal that can rearrange 3d orbitals as d‐orbital, thus favoring generation key intermediate *COOH instead *OCHO favor *CO formation, followed hydrogenation and/or C−C coupling produce This is first attempt regulate mode atom for generation, provides new inspiration designing efficient RR towards highly‐valued products.

Язык: Английский

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