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

Angewandte Chemie International Edition, Год журнала: 2021, Номер 60(38), С. 20627 - 20648

Опубликована: Апрель 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.

Язык: Английский

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Highly Selective CO₂ Electroreduction to C₂H₄ Using a Metal–Organic Framework with Dual Active Sites

Journal of the American Chemical Society, Год журнала: 2021, Номер 143(19), С. 7242 - 7246

Опубликована: Май 6, 2021

Conversion from CO2 to C2H4 is important for the development of energy and environment, but high barrier hydrogenation *CO intermediate C–C coupling step tend result in C1 compounds as main product thus restrict generation C2H4. Here, we report a metal–organic framework (denoted PcCu-Cu-O), composed 2,3,9,10,16,17,23,24-octahydroxyphthalo-cyaninato)copper(II) (PcCu-(OH)8) ligands square-planar CuO4 nodes, electrocatalyst Compared with discrete molecular copper-phthalocyanine (Faradaic efficiency (FE) = 25%), PcCu-Cu-O exhibits much higher performance electrocatalytic reduction FE 50(1)% current density 7.3 mA cm–2 at potential −1.2 V vs RHE 0.1 M KHCO3 solution, representing best reported date. In-situ infrared spectroscopy control experiments suggested that enhanced electrochemical may be ascribed synergistic effect between CuPc unit unit, namely CO on CO-producing site (CuO4 site) can efficiently migrate dimerize adsorbed C2H4-producing (CuPc), giving lower dimerization barrier.

Язык: Английский

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Phosphorus Induced Electron Localization of Single Iron Sites for Boosted CO₂ Electroreduction Reaction

Angewandte Chemie International Edition, Год журнала: 2021, Номер 60(44), С. 23614 - 23618

Опубликована: Авг. 31, 2021

Electrochemical reduction of carbon dioxide (CO2 ) into chemicals and fuels has recently attracted much interest, but normally suffers from a high overpotential low selectivity. In this work, single P atoms were introduced N-doped supported Fe atom catalyst (Fe-SAC/NPC) mainly in the form P-C bonds for CO2 electroreduction to CO an aqueous solution. This exhibited Faradaic efficiency ≈97 % at 320 mV, Tafel slope only 59 mV dec-1 , comparable state-of-the-art gold catalysts. Experimental analysis combined with DFT calculations suggested that coordination shells (n≥3), particular third shell center enhanced electronic localization Fe, which improved stabilization key *COOH intermediate on leading superior electrochemical performance overpotentials.

Язык: Английский

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Single-Atom (Iron-Based) Catalysts: Synthesis and Applications

Chemical Reviews, Год журнала: 2021, Номер 121(21), С. 13620 - 13697

Опубликована: Окт. 13, 2021

Supported single-metal atom catalysts (SACs) are constituted of isolated active metal centers, which heterogenized on inert supports such as graphene, porous carbon, and oxides. Their thermal stability, electronic properties, catalytic activities can be controlled via interactions between the center neighboring heteroatoms nitrogen, oxygen, sulfur. Due to atomic dispersion amount required for catalysis decreased, thus offering new possibilities control selectivity a given transformation well improve catalyst turnover frequencies numbers. This review aims comprehensively summarize synthesis Fe-SACs with focus anchoring single atoms (SA) carbon/graphene supports. The characterization these advanced materials using various spectroscopic techniques their applications in diverse research areas described. When applicable, mechanistic investigations conducted understand specific behavior Fe-SACs-based highlighted, including use theoretical models.

Язык: Английский

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

Angewandte Chemie, Год журнала: 2021, Номер 133(38), С. 20795 - 20816

Опубликована: Апрель 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.

Язык: Английский

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Recent Advances in Electrocatalysts for Efficient Nitrate Reduction to Ammonia

Advanced Functional Materials, Год журнала: 2023, Номер 33(43)

Опубликована: Июнь 25, 2023

Abstract Ammonia as an irreplaceable chemical has been widely demanded to keep the sustainable development of modern society. However, its industrial production consumes huge energy and releases extraordinary green‐house gases, leading various environmental issues. To achieve green ammonia is a great challenge that extensively pursued recently. In review, most promising strategy, electrochemical nitrate reduction reaction (e‐NO 3 RR) for purpose comprehensively investigated give full understanding mechanism provide guidance future directions. Particularly, electrocatalysts focused realize high yield rate Faraday efficiency applications. The recent‐developed catalysts, including noble metallic materials, alloys, metal compounds, single‐metal‐atom metal‐free are systematically discussed review effects factors on catalytic performance in e‐NO RR. Accordingly, strategies, defects engineering, coordination environment modulating, surface controlling, hybridization, carefully improve performance, such intrinsic activity selectivity. Finally, perspectives challenges given out. This shall insightful advanced systems efficiently industry.

Язык: Английский

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Atomically Dispersed Ni–Cu Catalysts for pH‐Universal CO₂ Electroreduction

Advanced Materials, Год журнала: 2023, Номер 35(13)

Опубликована: Янв. 10, 2023

CO2 electroreduction is of great significance to reduce emissions and complete the carbon cycle. However, unavoidable carbonate formation low utilization efficiency in neutral or alkaline electrolytes hinder its application at commercial scale. The development reduction under acidic conditions provides a promising strategy, but inhibition hydrogen evolution reaction difficult. Herein, first work design Ni-Cu dual atom catalyst supported on hollow nitrogen-doped reported for pH-universal CO. shows high CO Faradaic ≈99% acidic, neutral, electrolytes, partial current densities reach 190 ± 11, 225 10, 489 14 mA cm-2 , respectively. In particular, reaches 64.3%, which twice as that conditions. Detailed study indicates existence electronic interaction between Ni Cu atoms. atoms push d-band center further toward Fermi level, thereby accelerating *COOH. addition, operando characterizations density functional theory calculation are used elucidate possible mechanism electrolytes.

Язык: Английский

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Integrating Single Atoms with Different Microenvironments into One Porous Organic Polymer for Efficient Photocatalytic CO₂ Reduction

Advanced Materials, Год журнала: 2021, Номер 33(33)

Опубликована: Июль 8, 2021

Abstract The precise identification of single‐atom catalysts (SACs) activity and boosting their efficiency toward CO 2 conversion is imperative yet quite challenging. Herein, for the first time a series porous organic polymers designed prepared simultaneously, containing well‐defined M–N 4 O sites. Such strategy not only offers multiactive sites to promote catalytic but also provides more direct chance identify metal center activity. photoreduction results indicate that introduction salphen unit with Ni–N centers into pristine phthalocyanine‐based framework achieves remarkable generation ability (7.77 mmol g –1 ) high selectivity 96% over H . In combination control experiments, as well theoretical studies, moiety evidenced active site RR compared traditional moiety, which can be ascribed effectively reducing energy barrier, facilitating adsorption reaction radicals *COOH, improving charge transportation. This work might shed some light on designing efficient SACs reduction through modification coordination environments.

Язык: Английский

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A rational design of functional porous frameworks for electrocatalytic CO₂reduction reaction

Chemical Society Reviews, Год журнала: 2023, Номер 52(4), С. 1382 - 1427

Опубликована: Янв. 1, 2023

Rational design of functional porous frameworks for electrocatalytic CO 2 reduction reaction.

Язык: Английский

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Recent advances of single-atom catalysts in CO₂conversion

Energy & Environmental Science, Год журнала: 2023, Номер 16(7), С. 2759 - 2803

Опубликована: Янв. 1, 2023

The catalytic transformation of CO 2 into valuable fuels/chemicals is a promising and economically profitable process because it offers an alternative toward fossil feedstocks the benefit transforming cycling on scale-up.

Язык: Английский

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