Asymmetric CO–CHO Coupling over Pr Single-Atom Alloy Enables Industrial-Level Electrosynthesis of Ethylene

Journal of the American Chemical Society, Journal Year: 2025, Volume and Issue: unknown

Published: April 24, 2025

The electrocatalytic conversion of carbon dioxide (CO2) to ethylene (C2H4) holds great promise for sustainable chemical synthesis, yet achieving industrially relevant production rates remains a significant challenge. Through computational screening, we have identified praseodymium (Pr) single-atom alloy embedded in copper (Cu) catalyst (Pr@Cu) that exhibits superior CO2 activation and remarkably low energy barrier asymmetric *CO-*CHO coupling, primarily by facilitating the *CHO intermediate formation. Our optimized catalyst, Pr@Cu-2 (6 wt % Pr), achieves C2H4 Faradaic efficiency (FE) 64.2% at -1.6 V versus reversible hydrogen electrode (RHE) under high current density 1200 mA cm-2 reduction reaction (CO2RR). Furthermore, when integrated into 100 cm2 membrane assembly (MEA) electrolyzer, demonstrates robust performance, maintaining continuous rate 21.3 mL min-1 20 A over 200 h. This work provides fundamental insights role Pr alloys CO2RR highlights their potential scalable electrosynthesis.

Language: Английский

---

Progress of Advanced Electrocatalysts towards Electrochemical Selectivity Reduction CO2 to Formic Acid

Applied Catalysis A General, Journal Year: 2025, Volume and Issue: unknown, P. 120330 - 120330

Published: May 1, 2025

Language: Английский

---

Fabrication of Interface with Capping-bonding Synergy to Boost CO2 Electroreduction to Formate

Applied Catalysis B Environment and Energy, Journal Year: 2024, Volume and Issue: unknown, P. 124760 - 124760

Published: Oct. 1, 2024

Language: Английский

---

Metalloid Phosphorus Induces Tunable Defect Engineering in High Entropy Oxide Toward Advanced Lithium‐Ion Batteries

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: unknown

Published: Nov. 5, 2024

Abstract The inferior electrical conductivity and sluggish lithium storage kinetics of conventional high‐entropy oxide (HEO) are critical issues hindering their commercialization. high electronegativity metalloids can ameliorate this predicament by altering the electronic configuration HEO compared to metals. Herein, metalloid phosphorus doping in spinel‐type (P x A 1‐x )B 2 O 4 (A/B = Cr, Mn, Fe, Co, Ni) (P‐HEO) is achieved through a facile sol–gel process. facilitates transfer electrons from transition metal sites phosphorus‐doped sites, resulting formation electron‐rich electron‐deficient local regions on surface conducive an increase total number active electrochemical reaction Density functional theory calculation reveals Li adsorption energy synthesized P‐HEO only −1.102 eV, demonstrating that enables strong coupling between ions P‐HEO. Furthermore, also leads oxygen vacancies lattice distortion, which significantly enhances charge efficiency diffusion results enhanced performance with impressive rate capability long‐term stability. These findings provide valuable insights for design lattice‐engineered as versatile electrodes future applications.

Language: Английский

---

Tandem modulation strategy for copper-based catalysts: Towards efficient C-C coupling in the electrochemical reduction of carbon dioxide

Journal of Environmental Sciences, Journal Year: 2024, Volume and Issue: unknown

Published: Nov. 1, 2024

Language: Английский

---

Preferentially Stabilizing the Watershed Intermediates by Adsorbate‐adsorbate Interaction to Accelerate CO₂ Electroreduction to Ethanol

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: unknown

Published: Dec. 26, 2024

Abstract Returning CO 2 to liquid ethanol powered by clean energy offers considerable economic benefits and contributes reaching the goal of carbon neutrality, but it remains a formidable challenge achieve high selectivity due inevitable strong competition among various pathways. Herein, an investigation is presented accelerate electroreduction via preferentially stabilizing precarious watershed intermediates ( * CHCOH) creating adsorbate‐adsorbate interaction. The highly ordered CuOx nanoplates (HO‐CuOx NPLs) featuring abundant amorphous‐crystalline interface exhibit exceptional Faradaic efficiency (FE EtOH ) 63.8% ethanol‐to‐ethylene ratio 6.1 at large partial current density j 232.8 mA cm −2 . findings decipher that in‐between nanogaps in enhance adsorption OH, which can strengthen C─O bonds while weakening Cu─C interaction CHCOH through interaction, thereby enabling predilection for conversion. Beyond efficient ethanol‐oriented RR electrocatalyst, investigations provide in‐depth understanding on key steps precise regulation, be extended range conversion technologies.

Language: Английский

---

Bismuth oxide nanoflakes grown on defective microporous carbon endows high-efficient CO2 reduction at ampere level

Journal of Colloid and Interface Science, Journal Year: 2024, Volume and Issue: 678, P. 309 - 316

Published: Sept. 14, 2024

Language: Английский

---

Bi Doped In2O3 Nanofiber for Efficient Electrocatalytic CO2 Reduction

ChemCatChem, Journal Year: 2024, Volume and Issue: unknown

Published: Oct. 9, 2024

Abstract Electrocatalytic carbon dioxide reduction reaction (CO 2 RR) to formic acid (HCOOH) is attracted for superfluous CO removal and HCOOH production under ambient conditions. Indium‐based catalysts has considered as a good candidate material RR due their environmentally friendly features. However, the catalytic efficiency limited by poor Faradaic (FE) high overpotential of electrocatalyst, activity stability indium‐based are unsatisfactory, especially in industrial current density that critical commercialization. Herein, fiber Bi‐doped In O 3 was synthesized through electrospinning method, it demonstrate FE 88.2% at −1.5 V versus RHE (reversible hydrogen electrode) with partial −21.8 mA cm −2 H type cell. Specially, Bi‐In electrocatalyst also reach standard, which can work −400 92.7% (yield 6.9 mmol h −1 ) home‐made Flow Importantly, shows 24 long‐term test −300 . The improvement catalyst ascribed optimized electronic structure site, reduced function value beneficial reducing formation energy key *OCHO intermediates.

Language: Английский

---

In Situ Reconstructed Hydroxyl‐Rich Atomic‐Thin Bi₂O₂CO₃ Enables Ampere‐Scale Synthesis of Formate from CO₂ with Activated Water Dissociation

Advanced Materials, Journal Year: 2024, Volume and Issue: unknown

Published: Dec. 23, 2024

Abstract Renewable electricity‐driven CO 2 electroreduction provides a promising route toward carbon neutrality and sustainable chemical production. Nevertheless, the viability of this faces constraints catalytic efficiency durability in near‐neutral electrolytes at industrial‐scale current densities, mechanistically originating from unfavorable accommodation * H species water dissociation. Herein, new strategy is reported to accelerate dissociation by rich surface hydroxyl on bismuth subcarbonate nanosheets situ electrochemical transformed hydroxide nanotube precursors. This catalyst enables electrosynthesis formate densities up 1000 mA cm −2 with >96% faradaic efficiencies flow cells, 200 h durable membrane electrode assembly dilute environment. Combined kinetic studies, characterizations, theoretical calculations reveal that atomic thickness strengthens adsorption, highly localized electron configuration, hydroxyl‐functionalized more affinitive oxygenated species, thus lowering barrier for crucial hydrogenation step proton‐coupled transfer OCHO HCOOH.

Language: Английский

---

Enhancing CO2 electroreduction to formate on bismuth catalyst via sulfur doping

Chemical Engineering Journal, Journal Year: 2024, Volume and Issue: 501, P. 157404 - 157404

Published: Nov. 5, 2024

Language: Английский

---