InBi Bimetallic Sites for Efficient Electrochemical Reduction of CO₂ to HCOOH

Small, Journal Year: 2023, Volume and Issue: 19(41)

Published: June 13, 2023

Formic acid is receiving intensive attention as being one of the most progressive chemical fuels for electrochemical reduction carbon dioxide. However, majority catalysts suffer from low current density and Faraday efficiency. To this end, an efficient catalyst In/Bi-750 with InOx nanodots load prepared on a two-dimensional nanoflake Bi2 O2 CO3 substrate, which increases adsorption * CO2 due to synergistic interaction between bimetals exposure sufficient active sites. In H-type electrolytic cell, formate efficiency (FE) reaches 97.17% at -1.0 V (vs reversible hydrogen electrode (RHE)) no significant decay over 48 h. A 90.83% also obtained in flow cell higher 200 mA cm-2 . Both in-situ Fourier transform infrared spectroscopy (FT-IR) theoretical calculations show that BiIn bimetallic site can deliver superior binding energy OCHO intermediate, thereby fundamentally accelerating conversion HCOOH. Furthermore, assembled Zn-CO2 exhibits maximum power 6.97 mW cm-1 stability 60

Language: Английский

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Dynamic reconstructuring of CuS/SnO2-S for promoting CO2 electroreduction to formate

Journal of Energy Chemistry, Journal Year: 2023, Volume and Issue: 82, P. 497 - 506

Published: March 24, 2023

Language: Английский

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Reconstructed Bismuth Oxide through in situ Carbonation by Carbonate‐containing Electrolyte for Highly Active Electrocatalytic CO₂ Reduction to Formate

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 63(9)

Published: Dec. 26, 2023

The catalyst-reconstruction makes it challenging to clarify the practical active sites and unveil actual reaction mechanism during CO

Language: Английский

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Recent Advances in Electrochemical CO₂‐to‐Multicarbon Conversion: From Fundamentals to Industrialization

Advanced Energy Materials, Journal Year: 2023, Volume and Issue: 13(47)

Published: Nov. 2, 2023

Abstract The electrochemical CO 2 (eCO )‐to‐multicarbon conversion with higher value is regarded as a potential way to promote the transformation of industrial production and green balance carbon cycle. Recently, series advances have been achieved in progress eCO ‐to‐multicarbon conversion, including in‐depth exploration coupling mechanisms, up‐to‐date development characterization techniques, novel interdisciplinary design strategies catalysts electrolytic systems. Therefore, it essential systematically overview from fundamentals industrialization, compensating for limited insufficient reviews that reported. To fill aforementioned research gap, this focused on industrialization. First, possible catalytic mechanisms are accordingly summarized order reduction, small molecule‐coupled tandem conversion. Second, situ technologies assisting rationalization presented. Third, optimizing systems briefly classified advance industrialization process. Finally, challenges perspectives further reasonably proposed, aiming offer insights following work field.

Language: Английский

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Hydrothermal Synthesis of CuS Catalysts for Electrochemical CO₂ Reduction: Unraveling the Effect of the Sulfur Precursor

ACS Applied Energy Materials, Journal Year: 2023, Volume and Issue: 6(3), P. 1340 - 1354

Published: Jan. 24, 2023

Copper-based catalysts have been recognized as promising candidates for electrochemical conversion of CO2 to value-added chemicals and synthetic fuels. Yet, the challenges high overpotential low product selectivity motivated rational electrode engineering. In present work, we prepared CuS using different sulfur precursors, aimed elucidate precursor-dependent effect on their structure–property–activity relationships reduction. The precursors exhibited varied S release rates in hydrothermal synthesis, which had induced distinct surface morphological features diverse vacancy concentrations, intrinsic catalytic activity would be affected. desired CuS-TU catalyst synthesized thiourea precursor featured a flower-like morphology highest concentration. nanoflower offered expanded space considerable undercoordinated sites facilitated interfacial mass transfer Density functional theory calculations confirmed that abundant played an important role strengthening adsorption *COOH intermediates surface, promoted CO production via pathway. therefore relatively higher 72.67% at −0.51 V vs RHE. These findings will provide more insights into improving reduction performance copper-based by structure

Language: Английский

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Recent advances in p-block metal chalcogenide electrocatalysts for high-efficiency CO2 reduction

eScience, Journal Year: 2023, Volume and Issue: 4(2), P. 100172 - 100172

Published: Aug. 5, 2023

Electrocatalytic CO2 reduction (ECR) to high-value fuels and chemicals offers a promising conversion technology for achieving sustainable carbon cycles. In recent years, although great efforts have been made develop high-efficiency ECR catalysts, challenges remain in high activity long durability simultaneously. Taking advantage of the adjustable structure, tunable component, M–Ch (M = Sn, In, Bi, etc., Ch S, Se, Te) covalent bonds stabilized metal centers, p-block chalcogenides (PMC) based electrocatalysts shown potential converting into CO or formates. addition, unique electron structure can suppress competitive hydrogen evolution reaction enhance adsorption intermediates. Seeking systematically understand structure–activity relationship PMC-based this review summarizes advances designing PMC on fundamental aspects heterogeneous process, including advanced strategies optimizing intrinsic improving loading density catalytic sites, constructing highly stable tuning product selectivities. Subsequently, we outline perspectives developing high-performance catalysts practical applications.

Language: Английский

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Strongly coupled design of zinc oxide-nanorods/copper tin sulfide-nanoflowers nanostructures: An electrochemical study in 4-nitrochlorobenzene detection

Chemical Engineering Journal, Journal Year: 2023, Volume and Issue: 479, P. 147747 - 147747

Published: Nov. 29, 2023

Language: Английский

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Cu–Sn Bimetallic Activated Carbon–Carbon Coupling for Efficient Furfural Electroreduction

ACS Catalysis, Journal Year: 2024, Volume and Issue: 14(8), P. 5817 - 5826

Published: April 2, 2024

Electrochemically driven carbon–carbon coupling utilizing renewable electricity under ambient conditions has emerged as an innovative approach for synthesizing high-value chemicals, which still faces inherent challenges such low conversion rates and poor selectivity. While electroreducing furfural to hydrofuroin can produce high-quality biofuel, its efficiency need be promoted. Herein, Cu–Sn bimetallic catalyst been developed with a rate of >97% selectivity >67% through equilibrium the interfacial intermediate *H *fur-CHOH, exhibits greatest state-of-the-art overall performance. Characterization theoretical calculation reveal that Cu serves active site generating whose electron density decreased by introducing Sn, results in higher *fur-CHOH coverage lower energy barrier dimerization. Moreover, adding Sn also enables sluggish formation balance *H, leading reduced hydrogenation byproducts. The as-developed provides valuable insights optimizing other C–C electrocoupling reactions synthesis chemicals.

Language: Английский

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Interfacial Electronic Interaction in Amorphous–Crystalline CeO_x‐Sn Heterostructures for Optimizing CO₂ to Formate Conversion

Small, Journal Year: 2024, Volume and Issue: 20(32)

Published: March 18, 2024

Abstract Formate, a crucial chemical raw material, holds significant promise for industrial applications in the context of CO 2 electroreduction reaction (CO RR). Despite its potential, challenges, such as poor selectivity and low formation rate at high current densities persist, primarily due to competing hydrogen evolution (HER) energy barriers associated with *OCHO intermediate generation. Herein, one‐step co‐reduction strategy is employed construct an amorphous–crystalline CeO x ‐Sn heterostructure, demonstrating remarkable catalytic performance converting formate. The optimized heterostructures reach density 265.1 mA cm −2 formate Faraday efficiency 95% −1.07 V versus RHE. Especially, achieves 444.4 production 9211.8 µmol h −1 −1.67 RHE, surpassing most previously reported materials. Experimental results, coupled （density functional theory）DFT calculations confirm that robust interface interaction between Sn active center induces electron transfer from crystalline site amorphous , some Ce 4+ get electrons convert unsaturated 3+ optimizing electronic structure Sn. This heterostructure promotes during RR, reducing barrier formed by intermediates, thus achieving efficient reduction

Language: Английский

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Visualizing Catalytic Dynamics of Single-Cu-Atom-Modified SnS₂ in CO₂ Electroreduction via Rapid Freeze-Quench Mössbauer Spectroscopy

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(35), P. 24368 - 24376

Published: Aug. 21, 2024

Effective design and engineering of catalysts for an optimal performance depend extensively on a profound understanding the intricate catalytic dynamics under reaction conditions. In this work, we showcase rapid freeze-quench (RFQ) Mössbauer spectroscopy as powerful technique quantitatively monitoring single-Cu-atom-modified SnS2 (Cu1/SnS2) in electrochemical CO2 reduction (CO2RR). Utilizing newly established RFQ 119Sn methodology, clearly identified dynamic transformation Cu1/SnS2 to Cu1/SnS Cu1/Sn during CO2RR, resulting outstanding Faradaic efficiency formate production (∼90.9%) with partial current density 158 mA cm–2. Results from operando Raman spectroscopy, attenuated total reflection surface-enhanced infrared absorption (ATR-SEIRAS), quasi situ electron microscopy, X-ray photoelectron (XPS) measurements indicate that anchored single Cu atom can accelerate SnS formation CO2RR conditions, which effectively promote generation *CO2–/*OCHO intermediates. Theoretical calculations further support formed works active sites catalyzing reduces energy barrier activation *OCHO intermediate, thereby facilitating conversion formate. The results work provide thorough evolution Sn-based shed light atoms optimized performance. We anticipate will emerge advanced spectroscopic enabling genuine visualization across various systems.

Language: Английский

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