A rational design of functional porous frameworks for electrocatalytic CO₂reduction reaction

Chemical Society Reviews, Journal Year: 2023, Volume and Issue: 52(4), P. 1382 - 1427

Published: Jan. 1, 2023

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

Language: Английский

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Advances on Axial Coordination Design of Single-Atom Catalysts for Energy Electrocatalysis: A Review

Nano-Micro Letters, Journal Year: 2023, Volume and Issue: 15(1)

Published: Oct. 13, 2023

Abstract Single-atom catalysts (SACs) have garnered increasingly growing attention in renewable energy scenarios, especially electrocatalysis due to their unique high efficiency of atom utilization and flexible electronic structure adjustability. The intensive efforts towards the rational design synthesis SACs with versatile local configurations significantly accelerated development efficient sustainable electrocatalysts for a wide range electrochemical applications. As an emergent coordination avenue, intentionally breaking planar symmetry by adding ligands axial direction metal single atoms offers novel approach tuning both geometric structures, thereby enhancing electrocatalytic performance at active sites. In this review, we briefly outline burgeoning research topic axially coordinated provide comprehensive summary recent advances synthetic strategies Besides, challenges outlooks field also been emphasized. present review provides in-depth understanding SACs, which could bring new perspectives solutions fine regulation structures catering high-performing electrocatalysis.

Language: Английский

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Microwave‐Assisted Rapid Synthesis of MOF‐Based Single‐Atom Ni Catalyst for CO₂ Electroreduction at Ampere‐Level Current

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(10)

Published: Jan. 17, 2024

Carbon-based single-atom catalysts (SACs) have attracted tremendous interest in heterogeneous catalysis. However, the common electric heating techniques to produce carbon-based SACs usually suffer from prolonged time and tedious operations. Herein, a general facile microwave-assisted rapid pyrolysis method is developed afford within 3 min without inert gas protection. The obtained present high porosity comparable carbonization degree those by techniques. Specifically, Ni implanted N-doped carbon (Ni

Language: Английский

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Enhancing CO₂ Electroreduction to Ethylene via Copper−Silver Tandem Catalyst in Boron‐Imidazolate Framework Nanosheet

Advanced Energy Materials, Journal Year: 2023, Volume and Issue: 13(19)

Published: March 31, 2023

Abstract Copper‐based tandem catalysts with a well‐defined Cu coordination environment for the electrochemical CO 2 reduction reaction (CO RR) are highly desirable, due to their unique geometric‐electronic properties and helpfulness revealing structure–property correlations. Here, this work synthesizes catalyst at atomic configuration scale, Ag@BIF‐104NSs(Cu), by using ultrathin boron imidazolate framework (BIF) nanosheets as support load Ag nanoparticles (NPs). Due ordered benzoate ligands decorated on sites of BIF‐104NSs(Cu), NPs located in proximity via effect. Electrochemical RR measurements show improves selectivity activity ethylene. The faradaic efficiency (FE C2H4 ) 21.43% is significantly higher than that BIF‐104NSs(Cu) (3.82%). Further, density functional theory calculations reveal composite can efficiently reduce *CO, subsequently migrate sites. Thereafter, Cu–Ag atom pair responsible C–C coupling local enriched *CO further formation C H 4 .

Language: Английский

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Axial Dual Atomic Sites Confined by Layer Stacking for Electroreduction of CO₂ to Tunable Syngas

Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: 145(24), P. 13462 - 13468

Published: June 9, 2023

Arranging atoms in an orderly manner at the atomic scale to create stable polyatomic structures is a very challenging task. In this study, we have developed three-dimensional confinement areas on two-dimensional surface by creating regional defects. These are composed of vertically stacked graphene layers, where Ni and Fe anchored concentrically form axial dual sites high yield. can be used produce tunable syngas through electroreduction CO2. Theoretical calculations indicate that regulate charge distribution adjacent layer below, resulting lower d-band center. This, turn, weakens adsorption *CO intermediate inhibits production H2 site. Our research presents novel approach for concentrated creation building confinement-selective surface.

Language: Английский

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Electrocatalytic synthesis of C–N coupling compounds from CO₂ and nitrogenous species

SusMat, Journal Year: 2024, Volume and Issue: 4(2)

Published: March 12, 2024

Abstract The electrocatalytic synthesis of C–N coupling compounds from CO 2 and nitrogenous species not only offers an effective avenue to achieve carbon neutrality reduce environmental pollution, but also establishes a route synthesize valuable chemicals, such as urea, amide, amine. This innovative approach expands the application range product categories beyond simple carbonaceous in reduction, which is becoming rapidly advancing field. review summarizes research progress urea synthesis, using N , NO − 3 species, explores emerging trends electrosynthesis amide amine nitrogen species. Additionally, future opportunities this field are highlighted, including amino acids other containing bonds, anodic reactions water oxidation, catalytic mechanism corresponding reactions. critical captures insights aimed at accelerating development electrochemical reactions, confirming superiority method over traditional techniques.

Language: Английский

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Continuously Producing Highly Concentrated and Pure Acetic Acid Aqueous Solution via Direct Electroreduction of CO₂

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(1), P. 1144 - 1152

Published: Jan. 2, 2024

It is crucial to achieve continuous production of highly concentrated and pure C2 chemicals through the electrochemical CO2 reduction reaction (eCO2RR) for artificial carbon cycling, yet it has remained unattainable until now. Despite one-pot tandem catalysis (dividing eCO2RR into two catalytical reactions CO C2) offering potential significantly enhancing efficiency, its mechanism remains unclear performance unsatisfactory. Herein, we selected different CO2-to-CO catalysts CO-to-acetate construct several catalytic systems acetic acid. Among them, a system comprising covalent organic framework (PcNi-DMTP) metal–organic (MAF-2) as catalysts, respectively, exhibited faradaic efficiency 51.2% with current density 410 mA cm–2 an ultrahigh acetate yield rate 2.72 mmol m–2 s–1 under neutral conditions. After electrolysis 200 h, 1 working electrode can continuously produce 20 mM acid aqueous solution relative purity 95+%. Comprehensive studies revealed that influenced not only by supply–demand relationship electron competition between processes in but also CO-to-C2 catalyst diluted

Language: Английский

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Dual-axial engineering on atomically dispersed catalysts for ultrastable oxygen reduction in acidic and alkaline solutions

Proceedings of the National Academy of Sciences, Journal Year: 2024, Volume and Issue: 121(6)

Published: Jan. 30, 2024

Atomically dispersed catalysts are a promising alternative to platinum group metal for catalyzing the oxygen reduction reaction (ORR), while limited durability during electrocatalytic process severely restricts their practical application. Here, we report an atomically Co-doped carbon−nitrogen bilayer catalyst with unique dual-axial Co–C bonds (denoted as Co/DACN) by smart phenyl-carbon-induced strategy, realizing highly efficient ORR in both alkaline and acidic media. The corresponding half-wave potential is up 0.85 0.77 V (vs. reversible hydrogen electrode (RHE)) 0.5 M H 2 SO 4 0.1 KOH, respectively, representing best activity among all non-noble reported date. Impressively, Zn–air battery (ZAB) equipped Co/DACN cathode achieves outstanding after 1,688 h operation at 10 mA cm −2 high current density (154.2 ) peak power (210.1 mW ). Density functional theory calculations reveal that cross-linking Co−C of significantly enhance stability also facilitate 4e − pathway forming joint electron pool due improved interlayer mobility. We believe axial engineering opens broad avenue develop high-performance heterogeneous electrocatalysts advanced energy conversion storage.

Language: Английский

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Synergy of Ni Nanoclusters and Single Atom Site: Size Effect on the Performance of Electrochemical CO₂ Reduction Reaction and Rechargeable Zn−CO₂ Batteries

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(33)

Published: April 18, 2024

Abstract The design of bifunctional electrocatalysts toward reduction reaction carbon dioxide (ECO 2 RR) and oxygen evolution (OER) in aqueous rechargeable Zn─CO batteries (ZABs) still poses a significant challenge. Herein, Ni clusters (Ni x ) 0.5 0.8 nm diameter coupled with single site (Ni−N 4 −C), denoted as Ni−N /Ni 5 8 , respectively, are synthesized the size effect nanoclusters studied. exhibits an ≈100% Faradaic efficiency ( FE CO ECO RR for from −0.4 to −0.8 V versus reversible hydrogen electrode, superior that −C = 55.0%) 80.0%). OER performance or comparable commercial RuO but outperform −C. Theoretical calculation indicates * COOH intermediates bond synergistically atom site, promoting activation reducing energy barrier potential determining step RR. Such is strongly size‐dependent larger result too strong binding intermediates, impede formation CO. As cathode electrocatalyst alkaline ZABs, peak power density 11.7 mW cm −2 cycling durability over 1200 cycles 420 h.

Language: Английский

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Regulating the Electronic Configuration of Ni Sites by Breaking Symmetry of Ni‐Porphyrin to Facilitate CO₂ Photocatalytic Reduction

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(25)

Published: Feb. 10, 2024

Abstract Adapting the coordination environment to influence electronic configuration of active sites represents an efficient approach for improving photocatalytic performance CO 2 reduction reaction (CO RR) but how execute it precisely remains challenging. Herein, heteroatom‐substitution in Ni‐porphyrin break symmetry Ni center is proposed be effective solution. Based on this, two symmetry‐breaking Ni‐porphyrins, namely Ni(Cl)ON 3 Por and Ni(Cl)SN , are designed successfully prepared. By theoretical calculation, found that efficiently regulates d orbital energy levels center. Furthermore, experimental findings jointly revealed Ni‐porphyrins facilitates generation highly reactive I species during catalytic process, effectively stabilizing reducing barrier formation key * COOH intermediate. As a result, gave production rates 24.7 38.8 mmol g −1 h as well selectivity toward 94.0% 96.4%, respectively, outperforming symmetric NiN 4 rate 6.6 82.8%). These offer microscopic insights into modulate activity by tuning rational design competent catalyst RR photocatalysis.

Language: Английский

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