Steering the Reconstruction of Oxide-Derived Cu by Secondary Metal for Electrosynthesis of n-Propanol from CO

Journal of the American Chemical Society, Год журнала: 2024, Номер 146(7), С. 4632 - 4641

Опубликована: Фев. 10, 2024

As fuel and an important chemical feedstock, n-propanol is highly desired in electrochemical CO2/CO reduction on Cu catalysts. However, the precise regulation of localized structure still challenging poorly understood, thus hindering selective electrosynthesis. Herein, by decorating Au nanoparticles (NPs) CuO nanosheets (NSs), we present a counterintuitive transformation into undercoordinated sites locally around NPs during CO reduction. In situ spectroscopic techniques reveal Au-steered formation abundant removal oxygen CuO. First-principles accuracy molecular dynamic simulation demonstrates that atoms tend to rearrange disordered layer rather than (111) close-packed plane observed bare NSs. These facilitate binding, enabling electroreduction with high Faradaic efficiency 48% flow cell. This work provides new insight oxide-derived catalysts reconstruction secondary metal component.

Язык: Английский

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Steering the Site Distance of Atomic Cu‐Cu Pairs by First‐Shell Halogen Coordination Boosts CO2‐to‐C2 Selectivity

Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(46)

Опубликована: Авг. 6, 2024

Electrocatalytic reduction of CO

Язык: Английский

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In-depth understanding and precise modulation of surface reconstruction during heterogeneous electrocatalysis: From model to practical catalyst

Chem, Год журнала: 2025, Номер 11(1), С. 102345 - 102345

Опубликована: Янв. 1, 2025

Язык: Английский

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Fluorine Doping‐Assisted Reconstruction of Isolated Cu Sites for CO₂ Electroreduction Toward Multicarbon Products

Advanced Materials, Год журнала: 2025, Номер unknown

Опубликована: Янв. 19, 2025

Abstract The electrocatalytic synthesis of multicarbon compounds from CO 2 is a promising method for storing renewable electricity and addressing global issues. Single‐atom catalysts are candidates reduction, but producing high‐value (C 2+ ) products using single‐atom structure remains significant challenge. In this study, fluorine doping strategy proposed to facilitate the reconstruction isolated Cu atoms, promoting generation. in situ formed nanocrystals contain substantial amount stable + species, demonstrating remarkable activity −to‐multicarbon conversion. Notably, they achieve highest utilization, with C partial current density −2.01 A mg per −1 formation rate 7.03 mmol h at ≈−1 V versus RHE. Raman spectroscopy functional theory calculations confirm crucial role atoms structural evolution electrolysis.

Язык: Английский

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Direct Electrochemical Reduction of CO₂ to C₂₊ Chemicals: Catalysts, Microenvironments, and Mechanistic Understanding

ACS Energy Letters, Год журнала: 2025, Номер 10(1), С. 600 - 619

Опубликована: Янв. 2, 2025

The electrochemical reduction reaction of CO2 (eCO2RR) to chemicals presents a viable solution for addressing climate change and sustainable manufacturing. In this Review, we describe the recent advancements in eCO2RR multicarbon (C2+) production from aspects catalyst structure, microenvironments, mechanistic understanding. We draw experimental theoretical comparisons between systems containing bulk highly dispersed metals, alloys, metal compounds recount new results microenvironmental impacts as well catalytic mechanism. From our own studies, offer some viewpoints on electrocatalytic mechanism during complex multistep proton-coupled electron transfers propose several research directions unlocking full potential scalable industrial CO2-to-C2+ conversion.

Язык: Английский

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Ultralow Coordination Copper Sites Compartmentalized within Ordered Pores for Highly Efficient Electrosynthesis of n-Propanol from CO₂

Journal of the American Chemical Society, Год журнала: 2025, Номер unknown

Опубликована: Янв. 25, 2025

Coordinatively unsaturated copper (Cu) has been demonstrated to be effective for electrifying CO2 reduction into C3 products by adjusting the coupling of C1-C2 intermediates. Nevertheless, intuitive impacts ultralow coordination Cu sites on are scarcely elucidated due lack synthetic recipes with low numbers and its vulnerability aggregation under reductive potentials. Herein, computational predictions revealed that higher levels coordinative unsaturation favored adsorption C1 C2 Building upon correlations, we constructed an catalyst from in situ oxide nanoparticles (CuO NPs) compartmentalized within ordered porous matrix, achieving a remarkable Faradaic efficiency (FE) n-propanol (n-PrOH) electroreduction, reaching up 27.4% H-cell at -0.8 VRHE 11.8% 300 mA cm-2 flow cell. The presence maintenance during rigorous electrolysis process contributed outstanding performances, as verified combination spectroscopy techniques, disclosing formed featured strong *C1 *C2 intermediates lead n-PrOH.

Язык: Английский

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Best practices for in-situ and operando techniques within electrocatalytic systems

Nature Communications, Год журнала: 2025, Номер 16(1)

Опубликована: Март 16, 2025

In-situ and operando techniques in heterogeneous electrocatalysis are a powerful tool used to elucidate reaction mechanisms. Ultimately, they key determining concrete links between catalyst's physical/electronic structure its activity en route designing next-generation systems. To this end, the exact execution interpretation of these lines experiments is critical as determines strength conclusions that can be drawn what uncertainties remain. Instead focusing on how were understand systems, case with most reviews topic, work instead initiates nuanced discussion 1) best carry out each technique 2) initiate analysis which level insights from set in-situ or experiments/controls carried out. We focus several commonly techniques, including vibrational (IR, Raman) spectroscopy, X-ray absorption spectroscopy electrochemical mass spectrometry. In addition this, we include sections reactor design link theoretical modelling applicable across all techniques. While electrocatalysis, make when appropriate areas photo- thermo-catalytic highlight common pitfalls field, avoid them, sets complementary may strengthen analysis. end an overview gaps remain innovations must made overcome them. situ useful towards mechanistic investigations electrocatalytic systems but interpreted properly. Here, authors provide guidelines for practices use methods.

Язык: Английский

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Synthesis and Electrocatalytic Applications of Layer‐Structured Metal Chalcogenides Composites

Small, Год журнала: 2024, Номер 20(26)

Опубликована: Янв. 14, 2024

Abstract Featured with the attractive properties such as large surface area, unique atomic layer thickness, excellent electronic conductivity, and superior catalytic activity, layered metal chalcogenides (LMCs) have received considerable research attention in electrocatalytic applications. In this review, approaches developed to synthesize LMCs‐based electrocatalysts are summarized. Recent progress composites for electrochemical energy conversion applications including oxygen reduction reaction, carbon dioxide evolution hydrogen overall water splitting, nitrogen reaction is reviewed, potential opportunities practical obstacles development of high‐performing active substances also discussed. This review may provide an inspiring guidance developing high‐performance LMCs

Язык: Английский

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Promoting Water Activation via Molecular Engineering Enables Efficient Asymmetric C–C Coupling during CO₂ Electroreduction

Journal of the American Chemical Society, Год журнала: 2024, Номер 146(47), С. 32870 - 32879

Опубликована: Ноя. 13, 2024

Water activation plays a crucial role in CO

Язык: Английский

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Electrocatalytic upcycling of plastic waste: Progress, challenges, and future

Electron, Год журнала: 2024, Номер 2(3)

Опубликована: Авг. 1, 2024

Abstract The escalating accumulation of plastic waste has been developed into a formidable global environmental challenge. Traditional disposal methods such as landfilling and incineration not only exacerbate degradation by releasing harmful chemicals greenhouse gases, but also squander finite resources that could otherwise be recycled or repurposed. Upcycling is kind recycling technology converts high‐value helps to avoid resource pollution. Electrocatalytic upcycling emerges novel distinguished its mild operational conditions, high transformation efficiency product selectivity. This review commences with an overview the employed in management respective advantages inherent limitations are delineated. different types upcycled electrocatalytic strategy then discussed process examined together mechanisms underlying upcycling. Furthermore, structure‐activity relationships between electrocatalysts performance elucidated. aims furnish readers comprehensive understanding techniques for provide guidance design towards efficient transformation.

Язык: Английский

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