Importing Atomic Rare‐Earth Sites to Activate Lattice Oxygen of Spinel Oxides for Electrocatalytic Oxygen Evolution

Angewandte Chemie International Edition, Год журнала: 2024, Номер unknown

Опубликована: Окт. 9, 2024

Abstract Spinel oxides have emerged as highly active catalysts for the oxygen evolution reaction (OER). Owing to covalency competition, OER process on spinel often follows an arduous adsorbate mechanism (AEM) pathway. Herein, we propose a novel rare‐earth sites substitution strategy tune lattice redox of and bypass AEM scaling relationship limitation. Taking NiCo 2 O 4 model, incorporation Ce into octahedral site induces formation Ce−O−M (M=Ni, Co) bridge, which triggers charge redistribution within . The developed Ce−NiCo exhibits remarkable activity with low overpotential, satisfactory electrochemical stability, good practicability in anion‐exchange membrane water electrolyzer. Theoretical analyses reveal that surface more favorable (LOM) pathway non‐concerted proton‐electron transfers compared pure , also verified by pH‐dependent behavior situ Raman analysis. 18 O‐labeled mass spectrometry provides direct evidence released during originates from We discover electron delocalization f states through favoring antibonding state occupation Ni−O bonding [Ce−O−Ni] unit site, thereby activating OER. This work new perspective designing offers significant insights rare‐earth‐enhanced LOM mechanism.

Язык: Английский

---

Non‐Noble‐Metal‐Based Electrocatalysts for Acidic Oxygen Evolution Reaction: Recent Progress, Challenges, and Perspectives

Small, Год журнала: 2024, Номер 20(48)

Опубликована: Авг. 25, 2024

Abstract The oxygen evolution reaction (OER) plays a pivotal role in diverse renewable energy storage and conversion technologies, including water electrolysis, electrochemical CO 2 reduction, nitrogen fixation, metal‐air batteries. Among various electrolysis techniques, proton exchange membrane (PEM)‐based devices offer numerous advantages, high current densities, exceptional chemical stability, excellent conductivity, high‐purity H . Nevertheless, the prohibitive cost associated with Ir/Ru‐based OER electrocatalysts poses significant barrier to broad‐scale application of PEM‐based splitting. Consequently, it is crucial advance development non‐noble metal catalysis substance acid‐activity thereby fostering their widespread integration into PEM electrolyzers (PEMWEs). In this review, comprehensive analysis acidic mechanism, encompassing adsorbate mechanism (AEM), lattice (LOM) oxide path (OPM) offered. Subsequently, systematic summary recently reported noble‐metal‐free catalysts transition metal‐based, carbon‐based other types provided. Additionally, compilation situ/operando characterization techniques provided, serving as invaluable tools for furnishing experimental evidence comprehend catalytic mechanism. Finally, present challenges future research directions concerning precious‐metal‐free are comprehensively summarized discussed review.

Язык: Английский

---

High entropy catalysts in electrolytic water splitting: A review from properties to applications

Chemical Engineering Journal, Год журнала: 2024, Номер 498, С. 155736 - 155736

Опубликована: Сен. 12, 2024

Язык: Английский

---

Spiral‐concave Prussian Blue Crystals with Rich Steps: Growth Mechanism and Coordination Regulation

Angewandte Chemie International Edition, Год журнала: 2024, Номер 64(2)

Опубликована: Авг. 29, 2024

Abstract Investigating the formation and transformation mechanisms of spiral‐concave crystals holds significant potential for advancing innovative material design comprehension. We examined kinetics‐controlled nucleation growth Prussian Blue with spiral concave structures, constructed a detailed crystal phase diagram. The hexacyanoferrate (SC‐HCF) crystals, characterized by high‐density surface steps low stress‐strain architecture, exhibit enhanced activity due to their facile interaction reactants. Notably, coordination environment SC‐HCF can be precisely modulated introduction diverse metals. Utilizing X‐ray absorption fine structure spectroscopy in situ ultraviolet‐visible spectroscopy, we elucidated mechanism Co‐HCF facilitated oriented adsorption‐ion exchange (OA‐IE) process. Both experimental data, density functional theory confirm that possesses an optimized energy band structure, capable adjusting local electronic enhancing performance oxygen evolution reaction. This work not only elucidates regulation rich HCF, but also offers novel perspective constructing nanocrystals intricate structures.

Язык: Английский

---

Recycling Spent Lithium-Ion Battery Cathodes to Multimetallic Phosphides for High-Efficiency Oxygen Evolution Reaction

ACS Sustainable Chemistry & Engineering, Год журнала: 2025, Номер unknown

Опубликована: Фев. 6, 2025

Язык: Английский

---

Advanced Characterization Techniques for Probing Redox Reaction Mechanisms in High‐Performance Li–S Batteries

Carbon Neutralization, Год журнала: 2025, Номер 4(2)

Опубликована: Фев. 19, 2025

ABSTRACT The development of high‐performance energy storage systems requires several key attributes, including high and power density, cost‐effectiveness, safety, environmental sustainability. Among the various potential technologies, lithium–sulfur batteries stand out as a promising contender for future solutions due to their exceptional theoretical specific density (2600 Wh kg⁻¹) relatively capacity (1675 mAh g⁻¹). However, commercialization faces significant challenges, such low sulfur loading, rapid degradation, poor cycling stability. At heart these issues lies limited understanding complex conversion chemistry involved in batteries. In recent years, progress has been made elucidating reaction mechanisms, thanks use both ex situ characterization techniques. Methods optical spectroscopy, time‐of‐flight secondary ion mass spectrometry, synchrotron X‐ray, neural network analysis have demonstrated great uncovering redox processes lithium polysulfides underlying significantly advancing research battery systems. This review focuses on major advancements research, particularly study electrocatalytic mechanisms using emerging We discuss aspects accurately revealing through advanced diagnostic methods, well main challenges techniques face. Finally, we explore prospects commercialization.

Язык: Английский

---

Triggering the water oxidation kinetics and reaction pathway via S-doping in layered hydroxides for enhanced electrocatalytic performance

Applied Catalysis B Environment and Energy, Год журнала: 2025, Номер 371, С. 125227 - 125227

Опубликована: Март 5, 2025

Язык: Английский

---

Spin effects in electrocatalysis: Mechanisms, catalyst engineering, modulation, and applications

Materials Science and Engineering R Reports, Год журнала: 2025, Номер 164, С. 100967 - 100967

Опубликована: Март 5, 2025

Язык: Английский

---

Triggered factors and structure-activity relationship in the dynamic reconstruction processing of MOF for the alkaline oxygen evolution reaction

Coordination Chemistry Reviews, Год журнала: 2024, Номер 522, С. 216235 - 216235

Опубликована: Окт. 1, 2024

Язык: Английский

---

Electrochemical hydrogen production through anion exchange membrane water electrolysis (AEMWE): Recent progress and associated challenges in hydrogen production

International Journal of Hydrogen Energy, Год журнала: 2024, Номер 94, С. 1174 - 1211

Опубликована: Ноя. 16, 2024

Язык: Английский

---