High-entropy alloys in electrocatalysis: from fundamentals to applications

Chemical Society Reviews, Journal Year: 2023, Volume and Issue: 52(23), P. 8319 - 8373

Published: Jan. 1, 2023

In this review, we provide a comprehensive summary of recent advances in the synthesis strategies, design principles, and characterization technologies high entropy alloys, their applications various electrocatalytic conversion reactions.

Language: Английский

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Optimizing Intermediate Adsorption via Heteroatom Ensemble Effect over RuFe Bimetallic Alloy for Enhanced Nitrate Electroreduction to Ammonia

Advanced Energy Materials, Journal Year: 2023, Volume and Issue: 13(31)

Published: June 30, 2023

Abstract The electrochemical nitrate reduction reaction (NO 3 RR) is a promising approach for removal and NH synthesis at ambient conditions. As complex eight‐electron/nine‐proton transfer process, its performance relies heavily on the adsorption ability of intermediates catalyst surface, which determined by geometric electronic configurations active sites. In this work, heteroatom ensemble effect deliberately triggered over RuFe bimetallic alloy to optimize intermediate NO RR. A record‐high yield rate 118.8 mg h −1 high Faradaic efficiency 92.2% are achieved −1.4 V vs reversible hydrogen electrode, ranking top state‐of‐the‐art. Experimental computational results reveal that characteristics induced play crucial roles. Both Ru Fe display continuous state throughout Fermi level, suggesting electron density benefits whole result, facilitated − , efficient stabilization key intermediates, as well timely desorption simultaneously achieved, thus significantly promoting direct .

Language: Английский

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Reduction of CO2 to chemicals and Fuels: Thermocatalysis versus electrocatalysis

Chemical Engineering Journal, Journal Year: 2023, Volume and Issue: 472, P. 145033 - 145033

Published: July 28, 2023

Language: Английский

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Molecular Imprinting Technology Enables Proactive Capture of Nitrogen for Boosted Ammonia Synthesis under Ambient Conditions

Advanced Materials, Journal Year: 2023, Volume and Issue: 35(51)

Published: Aug. 9, 2023

Electrochemical nitrogen reduction reaction (NRR) is a burgeoning field for green and sustainable ammonia production, in which numerous potential catalysts emerge endlessly. However, satisfactory performances are still not realized under practical applications due to the limited solubility sluggish diffusion of at interface. Herein, molecular imprinting technology adopted construct an adlayer with abundant imprints on electrocatalyst, capable selectively recognizing proactively aggregating high-concentrated interface while hindering access overwhelming water simultaneously. With this favorable microenvironment, can preferentially occupy active surface, NRR equilibrium be positively shifted facilitate kinetics. Approximately threefold improvements both production rate (185.7 µg h-1 mg-1 ) Faradaic efficiency (72.9%) achieved by metal-free catalyst compared bare one. It believed that strategy should general method find further applicability or even other reactions facing similar challenges.

Language: Английский

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Optimizing Intermediate Adsorption over PdM (M=Fe, Co, Ni, Cu) Bimetallene for Boosted Nitrate Electroreduction to Ammonia

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(18)

Published: March 7, 2024

Electrochemical reduction of nitrate to ammonia (NO

Language: Английский

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Stabilizing the oxidation state of catalysts for effective electrochemical carbon dioxide conversion

Chemical Society Reviews, Journal Year: 2024, Volume and Issue: 53(12), P. 6295 - 6321

Published: Jan. 1, 2024

Developing sophisticated strategies to stabilize oxidative metal catalysts based on the correlation between dynamic oxidation state and product profile is favorable for efficient electrochemical CO 2 conversion.

Language: Английский

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Donor‐Site‐Acceptor Covalent Organic Frameworks Enable Spontaneous Nitrogen Dissociation for Boosted Photoelectrochemical Ammonia Synthesis

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(24)

Published: Feb. 5, 2024

Abstract Photoelectrochemical (PEC) technology offers new opportunities for pushing the renewable energy‐driven ammonia synthesis toward a practical level, while still facing unsatisfactory efficiency due to obstacle of dissociating inert nitrogen triple‐bonds. Herein, novel donor‐site‐acceptor system is constructed in covalent organic frameworks tackle this challenge highly efficient PEC synthesis. Highly active boron site elaborately embedded between donor and acceptor units, which can be effectively activated with continuous electron flow upon photoexcitation. With assistance solar irradiation, stubborn dissociation successfully changed from passive endothermic reaction spontaneous exothermic process, completely eliminating energy barrier rate‐determining step facilitating overall kinetics. The proof‐of‐concept achieved an excellent NRR performance remarkable Faradaic 91.6%, reaching target set by U.S. Department Energy (90%).

Language: Английский

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Optimizing Intermediate Adsorption over PdM (M=Fe, Co, Ni, Cu) Bimetallene for Boosted Nitrate Electroreduction to Ammonia

Angewandte Chemie, Journal Year: 2024, Volume and Issue: 136(18)

Published: March 7, 2024

Abstract Electrochemical reduction of nitrate to ammonia (NO 3 RR) is a promising and eco‐friendly strategy for production. However, the sluggish kinetics eight‐electron transfer process poor mechanistic understanding strongly impedes its application. To unveil internal laws, herein, library Pd‐based bimetallene with various transition metal dopants (PdM (M=Fe, Co, Ni, Cu)) are screened learn their structure–activity relationship towards NO RR. The ultra‐thin structure metallene greatly facilitates exposure active sites, metals break electronic balance upshift d‐band center, thus optimizing intermediates adsorption. anisotropic characteristics these make RR activity in order PdCu>PdCo≈PdFe>PdNi>Pd, record‐high NH yield rate 295 mg h −1 cat along Faradaic efficiency 90.9 % achieved neutral electrolyte on PdCu bimetallene. Detailed studies further reveal that moderate N‐species (*NO *NO 2 ) adsorption ability, enhanced activation, reduced HER facilitate We believe our results will give systematic guidance future design catalysts.

Language: Английский

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Deciphering engineering principle of three-phase interface for advanced gas-involved electrochemical reactions

Journal of Energy Chemistry, Journal Year: 2023, Volume and Issue: 80, P. 302 - 323

Published: Feb. 13, 2023

Language: Английский

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Eliminating Concentration Polarization with Cationic Covalent Organic Polymer to Promote Effective Overpotential of Nitrogen Fixation

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(36)

Published: July 14, 2023

Electrocatalytic nitrogen reduction reaction offers a sustainable alternative to the conventional Haber-Bosch process. However, it is currently restricted by low effective overpotential due concentration polarization, which arises from accumulated products, ammonium, at interface. Here, novel covalent organic polymer with ordered periodic cationic sites proposed tackle this challenge. The whole network exhibits strong positive charge and effectively repels positively charged enabling an ultra-low interfacial product concentration, successfully driving equilibrium forward direction. With given potential unchanged, suppressed can be much liberated, ultimately leading continuous high-level rate. As expected, when tailored microenvironment coupled transition metal-based catalyst, 24-fold improvement generated in Faradaic efficiency (73.74 %) as compared bare one. strategy underscores importance of optimizing dynamic processes means improving overall performance electrochemical syntheses.

Language: Английский

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