Multi‐Sites Electrocatalysis in High‐Entropy Alloys

Advanced Functional Materials, Journal Year: 2021, Volume and Issue: 31(47)

Published: Aug. 26, 2021

Abstract High‐entropy alloys (HEAs) have attracted widespread attention in electrocatalysis due to their unique advantages (adjustable composition, complex surface, high tolerance, etc.). They allow for the formation of new and tailorable active sites multiple elements adjacent each other, interaction can be tailored by rational selection element configuration composition. However, it needs further explored catalyst design, elements, determination sites. This review article focuses on important progress multi‐sites HEAs. The classification is done basis catalytic reaction, including hydrogen evolution oxygen reduction alcohol oxidation carbon dioxide nitrogen reaction. Based experiments theories, a more in‐depth exploration activity HEAs will conducted, (the special role catalysis) effect. provide design some reactions, adjust compositions improve intrinsic activity. Furthermore, remaining challenges future directions promising research fields are also provided.

Language: Английский

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Recent advances in innovative strategies for the CO₂ electroreduction reaction

Energy & Environmental Science, Journal Year: 2020, Volume and Issue: 14(2), P. 765 - 780

Published: Dec. 15, 2020

This review underlines innovative design strategies for CO₂RR system, also distinctively presents the current status and new trend.

Language: Английский

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Controllable Cu⁰‐Cu⁺ Sites for Electrocatalytic Reduction of Carbon Dioxide

Angewandte Chemie International Edition, Journal Year: 2021, Volume and Issue: 60(28), P. 15344 - 15347

Published: April 27, 2021

Abstract Cu‐based electrocatalysts facilitate CO 2 electrochemical reduction (CO ER) to produce multi‐carbon products. However, the roles of Cu 0 and + mechanistic understanding remain elusive. This paper describes controllable construction ‐Cu sites derived from well‐dispersed cupric oxide particles supported on copper phyllosilicate lamella enhance ER performance. 20 % Cu/CuSiO 3 shows superior performance with 51.8 C H 4 Faraday efficiency at −1.1 V vs reversible hydrogen electrode during 6 hour test. In situ attenuated total reflection infrared spectra density functional theory (DFT) calculations were employed elucidate reaction mechanism. The enhancement in activity is mainly attributed synergism pairs: activates facilitates following electron transfers; strengthens *CO adsorption further boost C−C coupling. We provide a strategy rationally design catalysts viable valence states ER.

Language: Английский

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Architectural Design for Enhanced C₂ Product Selectivity in Electrochemical CO₂ Reduction Using Cu-Based Catalysts: A Review

ACS Nano, Journal Year: 2021, Volume and Issue: 15(5), P. 7975 - 8000

Published: May 6, 2021

Electrochemical CO2 reduction to value-added chemicals and fuels is a promising approach mitigate the greenhouse effect arising from anthropogenic emission energy shortage caused by depletion of nonrenewable fossil fuels. The generation multicarbon (C2+) products, especially hydrocarbons oxygenates, great interest for industrial applications. To date, Cu only metal known catalyze C–C coupling in electrochemical reaction (eCO2RR) with appreciable efficiency kinetic viability produce wide range C2 products aqueous solutions. Nonetheless, poor product selectivity associated main technical problem application eCO2RR technology on global scale. Based extensive research efforts, delicate rational design electrocatalyst architecture using principles nanotechnology likely significantly affect adsorption energetics some key intermediates hence inherent pathways. In this review, we summarize recent progress that has been achieved tailoring efficient conversion target products. By considering experimental computational results, further analyze underlying correlations between catalyst its toward Finally, major challenges are outlined, directions future development suggested.

Language: Английский

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Linking the Dynamic Chemical State of Catalysts with the Product Profile of Electrocatalytic CO₂ Reduction

Angewandte Chemie International Edition, Journal Year: 2021, Volume and Issue: 60(32), P. 17254 - 17267

Published: March 8, 2021

Abstract The promoted activity and enhanced selectivity of electrocatalysts is commonly ascribed to specific structural features such as surface facets, morphology, atomic defects. However, unraveling the factors that really govern direct electrochemical reduction CO 2 (CO RR) still very challenging since state dynamic difficult predict under working conditions. Moreover, theoretical predictions from viewpoint thermodynamics alone often fail specify actual configuration a catalyst for RR process. Herein, we re‐survey recent studies with emphasis on revealing chemical Cu sites conditions extracted by in situ/operando characterizations, further validate critical link between product profile RR. This point view provides generalizable concept chemical‐state‐driven offers an inspiration both fundamental understanding efficient design.

Language: Английский

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Interfacial Electrolyte Effects on Electrocatalytic CO₂ Reduction

ACS Catalysis, Journal Year: 2021, Volume and Issue: 12(1), P. 331 - 362

Published: Dec. 16, 2021

Electrocatalytic CO2 reduction (CO2RR), powered by renewable energy, has great potential in decreasing the concentration of atmosphere, as well producing high value-added fuels or chemicals. The electrode and electrolyte together determine catalytic performance CO2RR. Despite substantial progress been made design preparation high-performance catalysts, role at electrode–electrolyte interface (EEI) which could largely affect local environment not understood thoroughly. To maximize balance (i.e., activity, selectivity, stability) CO2RR from a standpoint application, fundamental understanding interfacial effects should be emphasized with equal importance to intrinsic properties catalyst. In this Review, we will focus on discussion (effects) electrolytes for We summarize according their compositions chemical environment, include solvents, pH, cations, anions, impurities, additives, modifiers. addition, in-depth investigations detection intermediates during reactions using situ spectroscopy techniques are included. mechanisms, current challenges, future developments, perspectives discussed.

Language: Английский

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“Two Ships in a Bottle” Design for Zn–Ag–O Catalyst Enabling Selective and Long-Lasting CO₂ Electroreduction

Journal of the American Chemical Society, Journal Year: 2021, Volume and Issue: 143(18), P. 6855 - 6864

Published: April 14, 2021

Electrochemical CO2 reduction (CO2RR) using renewable energy sources represents a sustainable means of producing carbon-neutral fuels. Unfortunately, low efficiency, poor product selectivity, and rapid deactivation are among the most intractable challenges CO2RR electrocatalysts. Here, we strategically propose "two ships in bottle" design for ternary Zn–Ag–O catalysts, where ZnO Ag phases twinned to constitute an individual ultrafine nanoparticle impregnated inside nanopores ultrahigh-surface-area carbon matrix. Bimetallic electron configurations modulated by constructing interface, density reconfiguration arising from delocalization enhances stabilization *COOH intermediate favorable CO production, while promoting selectivity suppressing HCOOH generation altering rate-limiting step toward high thermodynamic barrier forming HCOO*. Moreover, pore-constriction mechanism restricts bimetallic particles nanosized dimensions with abundant heterointerfaces exposed active sites, meanwhile prohibiting detachment agglomeration nanoparticles during enhanced stability. The designed catalysts realize 60.9% efficiency 94.1 ± 4.0% Faradaic CO, together remarkable stability over 6 days. Beyond providing high-performance electrocatalyst, this work presents promising catalyst-design strategy efficient conversion.

Language: Английский

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Potential‐Dependent Morphology of Copper Catalysts During CO₂ Electroreduction Revealed by In Situ Atomic Force Microscopy

Angewandte Chemie International Edition, Journal Year: 2020, Volume and Issue: 60(5), P. 2561 - 2568

Published: Oct. 9, 2020

Electrochemical AFM is a powerful tool for the real-space characterization of catalysts under realistic electrochemical CO2 reduction (CO2 RR) conditions. The evolution structural features ranging from micrometer to atomic scale could be resolved during RR. Using Cu(100) as model surface, distinct nanoscale surface morphologies and their potential-dependent transformations granular smoothly curved mound-pit surfaces or structures with rectangular terraces are revealed RR in 0.1 m KHCO3 . density undercoordinated copper sites shown increase decreasing potential. In situ atomic-scale imaging reveals specific adsorption occurring at cathodic potentials impacting observed catalyst structure. These results show complex interrelation morphology, structure, defect density, applied potential, electrolyte catalysts.

Language: Английский

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Carbon-Based Materials for Electrochemical Reduction of CO₂ to C₂₊ Oxygenates: Recent Progress and Remaining Challenges

ACS Catalysis, Journal Year: 2021, Volume and Issue: 11(4), P. 2076 - 2097

Published: Feb. 2, 2021

Electrochemical reduction of CO2 to multicarbon (C2+) products is desirable because the higher energy density and economic value C2+ significant scientific issue for coupling multicarbons. However, efficient conversion into remains challenging difficulty in C–C coupling. Recently, numerous papers have reported carbon-based materials production from electrochemical reduction. Because unique properties production, can be used as a potential alternative electrocatalytic CO2. This Review summarized recent progresses formation oxygenates on materials. In this Review, we highlighted strategies available achieving electrocatalysts revealed relationships between intermediate adsorption selectivity oxygenate Moreover, provided understandings fabricating active sites related mechanisms generation. The remaining challenges opportunities were discussed.

Language: Английский

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Two-Dimensional Conjugated Metal–Organic Frameworks for Electrocatalysis: Opportunities and Challenges

ACS Nano, Journal Year: 2022, Volume and Issue: 16(2), P. 1759 - 1780

Published: Jan. 20, 2022

A highly effective electrocatalyst is the central component of advanced electrochemical energy conversion. Recently, two-dimensional conjugated metal-organic frameworks (2D c-MOFs) have emerged as a class promising electrocatalysts because their advantages including 2D layered structure with high in-plane conjugation, intrinsic electrical conductivity, permanent pores, large surface area, chemical stability, and structural diversity. In this Review, we summarize recent advances c-MOF for First, introduce design principles synthetic strategies reported c-MOFs, well functional electrocatalysis. Subsequently, present representative in various reactions, such hydrogen/oxygen evolution, reduction reactions oxygen, carbon dioxide, nitrogen. We highlight property tuning to boost catalytic performance, offer our perspectives regard challenges be overcome.

Language: Английский

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