Electrochemical reduction of carbon dioxide to multicarbon (C₂₊) products: challenges and perspectives

Energy & Environmental Science, Год журнала: 2023, Номер 16(11), С. 4714 - 4758

Опубликована: Янв. 1, 2023

This review analyzes advanced catalysts and C 2+ synthesis mechanisms based on theoretical explorations in situ / operando characterizations. Triphasic interface optimization is discussed for the potential of industry-compatible stability.

Язык: Английский

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A Tandem Strategy for Enhancing Electrochemical CO₂ Reduction Activity of Single‐Atom Cu‐S₁N₃ Catalysts via Integration with Cu Nanoclusters

Angewandte Chemie International Edition, Год журнала: 2021, Номер 60(45), С. 24022 - 24027

Опубликована: Сен. 9, 2021

We developed a tandem electrocatalyst for CO2 -to-CO conversion comprising the single Cu site co-coordinated with N and S anchored carbon matrix (Cu-S1 N3 ) atomically dispersed clusters (Cux ), denoted as Cu-S1 /Cux . The as-prepared composite presents 100 % Faradaic efficiency towards CO generation (FECO at -0.65 V vs. RHE high FECO over 90 from -0.55 to -0.75 V, outperforming analogues Cu-N4 only 54 -0.7 V) 70 configurations. unsymmetrical atomic interface in basal plane possesses an optimized binding energy key intermediate *COOH compared site. At same time, adjacent Cux effectively promotes protonation of *CO2- by accelerating water dissociation offering *H active sites. This work provides strategy facilitating proton-coupled electron transfer atomic-level catalytic

Язык: Английский

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Halide-guided active site exposure in bismuth electrocatalysts for selective CO2 conversion into formic acid

Nature Catalysis, Год журнала: 2023, Номер 6(9), С. 796 - 806

Опубликована: Авг. 17, 2023

Abstract It remains a challenge to identify the active sites of bismuth catalysts in electrochemical CO 2 reduction reaction. Here we show through situ characterization that activation oxyhalide electrocatalysts metallic is guided by halides. In X-ray diffraction results bromide promotes selective exposure planar surfaces, whereas chloride and iodide result more disordered sites. Furthermore, find bromide-activated outperform counterparts, achieving high current density (>100 mA cm –2 ) formic acid selectivity (>90%), suggesting surfaces are for addition, absorption spectroscopy measurements reveal reconstruction proceeds rapidly chloride-activated gradually when present, facilitating formation ordered surfaces. These findings pivotal role halogens on facet activated bismuth-based during

Язык: Английский

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Electron‐Rich Bi Nanosheets Promote CO₂⋅⁻ Formation for High‐Performance and pH‐Universal Electrocatalytic CO₂ Reduction

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(11)

Опубликована: Янв. 20, 2023

Electrochemical CO2 reduction reaction (CO2 RR) to chemical fuels such as formate offers a promising pathway carbon-neutral future, but its practical application is largely inhibited by the lack of effective activation molecules and pH-universal feasibility. Here, we report an electronic structure manipulation strategy electron-rich Bi nanosheets, where electrons transfer from Cu donor acceptor in bimetallic Cu-Bi, enabling RR towards with concurrent high activity, selectivity stability (acidic, neutral alkaline) electrolytes. Combined situ Raman spectra computational calculations unravel that promotes ⋅- formation activate molecules, enhance adsorption strength *OCHO intermediate up-shifted p-band center, thus leading superior activity formate. Further integration robust nanosheets into III-V-based photovoltaic solar cell results unassisted artificial leaf solar-to-formate (STF) efficiency 13.7 %.

Язык: Английский

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Local reaction environment in electrocatalysis

Chemical Society Reviews, Год журнала: 2024, Номер 53(4), С. 2022 - 2055

Опубликована: Янв. 1, 2024

Beyond conventional electrocatalyst engineering, recent studies have unveiled the effectiveness of manipulating local reaction environment in enhancing performance electrocatalytic reactions. The general principles and strategies environmental engineering for different processes been extensively investigated. This review provides a critical appraisal advancements aiming to comprehensively assess this emerging field. It presents interactions among surface structure, ions distribution electric field relation environment. Useful protocols such as interfacial reactant concentration, mass transport rate, adsorption/desorption behaviors, binding energy are in-depth discussed toward modifying Meanwhile, electrode physical structures cell configurations viable optimization methods environments. In combination with

Язык: Английский

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Oxygen‐Bridged Indium‐Nickel Atomic Pair as Dual‐Metal Active Sites Enabling Synergistic Electrocatalytic CO₂ Reduction

Angewandte Chemie International Edition, Год журнала: 2022, Номер 62(7)

Опубликована: Дек. 15, 2022

Abstract Single‐atom catalysts offer a promising pathway for electrochemical CO 2 conversion. However, it is still challenge to optimize the performance of dual‐atom catalysts. Here, an atomic indium‐nickel dual‐sites catalyst bridged by axial oxygen atom (O‐In‐N 6 ‐Ni moiety) was anchored on nitrogenated carbon (InNi DS/NC). InNi DS/NC exhibits superior selectivity with Faradaic efficiency higher than 90 % over wide potential range from −0.5 −0.8 V versus reversible hydrogen electrode (vs. RHE). Moreover, industrial partial current density up 317.2 mA cm −2 achieved at −1.0 vs. RHE in flow cell. In situ ATR‐SEIRAS combined theory calculations reveal that synergistic effect In‐Ni and O bridge not only reduces reaction barrier formation *COOH, but also retards undesired evolution reaction. This work provides feasible strategy construct dual‐site towards energy

Язык: Английский

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Single‐Product Faradaic Efficiency for Electrocatalytic of CO₂ to CO at Current Density Larger than 1.2 A cm⁻² in Neutral Aqueous Solution by a Single‐Atom Nanozyme

Angewandte Chemie International Edition, Год журнала: 2022, Номер 61(44)

Опубликована: Сен. 7, 2022

Electroreduction of CO2 to CO is a promising approach for the cycling use , while it still suffers from impractical current density and durability. Here we report single-atom nanozyme (Ni-N5 -C) that achieves industrial-scale performance -to-CO conversion with Faradaic efficiency (FE) exceeded 97 % over -0.8--2.4 V vs. RHE. The at -2.4 RHE reached maximum 1.23 A cm-2 (turnover frequency 69.7 s-1 ) an FE 99.6 %. No obvious degradation was observed 100 hours continuous operation. Compared planar Ni-N4 site, square-pyramidal Ni-N5 site has increase decrease in dz2${{{\rm d}}_{{z}^{2}}}$ dxz/yz orbital energy levels, respectively, as revealed by functional theory calculations. Thus, catalytic more superior activate molecule reduce barriers well promote desorption, thus boosting kinetic activation process activity.

Язык: Английский

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A comprehensive review on recent trends in carbon capture, utilization, and storage techniques

Journal of environmental chemical engineering, Год журнала: 2023, Номер 11(6), С. 111393 - 111393

Опубликована: Ноя. 3, 2023

Язык: Английский

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Heteroatoms Induce Localization of the Electric Field and Promote a Wide Potential‐Window Selectivity Towards CO in the CO₂ Electroreduction

Angewandte Chemie International Edition, Год журнала: 2022, Номер 61(44)

Опубликована: Сен. 8, 2022

Carbon dioxide electroreduction (CO2 RR) is a sustainable way of producing carbon-neutral fuels. Product selectivity in CO2 RR regulated by the adsorption energy reaction-intermediates. Here, we employ differential phase contrast-scanning transmission electron microscopy (DPC-STEM) to demonstrate that Sn heteroatoms on Ag catalyst generate very strong and atomically localized electric fields. In situ attenuated total reflection infrared spectroscopy (ATR-IR) results verified field enhances *COOH, thus favoring production CO during RR. The Ag/Sn exhibits an approximately 100 % at wide range potentials (from -0.5 -1.1 V, versus reversible hydrogen electrode), with remarkably high efficiency (EE) 76.1 %.

Язык: Английский

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Ferroelectric Materials and Their Applications in Activation of Small Molecules

ACS Omega, Год журнала: 2023, Номер 8(7), С. 6164 - 6174

Опубликована: Фев. 9, 2023

The demand for renewable and environmentally friendly energy sources has attracted extensive research on high-performance catalysts. Ferroelectrics, a class of materials with switchable polarization, are unique promising catalyst candidates due to the significant effects polarization surface chemistry physics. band bending at ferroelectric/semiconductor interface induced by flip promotes charge separation transfer, thereby enhancing photocatalytic performance. More importantly, reactants can be selectively adsorbed ferroelectric depending direction, which effectively lift basic limitations as imposed Sabatier's principle catalytic activity. This Review summarizes latest developments introduces ferroelectric-related applications. possible directions 2D in chemical catalysis discussed end. is expected inspire interests from physical, chemical, science communities.

Язык: Английский

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