Importing Atomic Rare‐Earth Sites to Activate Lattice Oxygen of Spinel Oxides for Electrocatalytic Oxygen Evolution DOI Creative Commons
Xuan Wang,

Jinrui Hu,

Tingyu Lu

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: unknown

Published: Oct. 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.

Language: Английский

Mesopore and macropore engineering in metal–organic frameworks for energy environment-related applications DOI
Xin Yu, Yue Cao, Jie Yang

et al.

Journal of Materials Chemistry A, Journal Year: 2024, Volume and Issue: 12(9), P. 4931 - 4970

Published: Jan. 1, 2024

The fabrication strategies of mesopores and macropores in metal–organic frameworks (MOFs) their emerging applications are summarized. In addition, the challenges future perspectives pore engineering MOF design also indicated.

Language: Английский

Citations

19

Optimizing Ionomer Distribution in Anode Catalyst Layer for Stable Proton Exchange Membrane Water Electrolysis DOI
Han Liu, Xinhui Wang,

Kejie Lao

et al.

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(28)

Published: April 25, 2024

Abstract The high cost of proton exchange membrane water electrolysis (PEMWE) originates from the usage precious materials, insufficient efficiency, and lifetime. In this work, an important degradation mechanism PEMWE caused by dynamics ionomers over time in anode catalyst layer (ACL), which is a purely mechanical microstructure, identified. Contrary to conventional understanding that microstructure ACL static, micropores are inclined be occupied due localized swelling/creep/migration, especially near ACL/PTL (porous transport layer) interface, where they form channels reactant/product couples. Consequently, with increased at PTL/ACL interface exhibit rapid continuous degradation. addition, close correlation between ink discovered. Specifically, if more migrate top ink, accumulate ACL/PEM leaving fewer interface. Therefore, ionomer distribution successfully optimized, exhibits reduced enriches reducing decay rate factor three when operated 2.0 A cm −2 80 °C. findings provide general way achieve low‐cost hydrogen production.

Language: Английский

Citations

19

Atomically engineered interfaces inducing bridging oxygen-mediated deprotonation for enhanced oxygen evolution in acidic conditions DOI Creative Commons
Han Wu,

Jiangwei Chang,

Jingkun Yu

et al.

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: Nov. 28, 2024

The development of efficient and stable electrocatalysts for water oxidation in acidic media is vital the commercialization proton exchange membrane electrolyzers. In this work, we successfully construct Ru–O–Ir atomic interfaces oxygen evolution reaction (OER). catalysts achieve overpotentials as low 167, 300, 390 mV at 10, 500, 1500 mA cm−2 0.5 M H2SO4, respectively, with electrocatalyst showing robust stability >1000 h operation 10 negligible degradation after 200,000 cyclic voltammetry cycles. Operando spectroelectrochemical measurements together theoretical investigations reveal that OER pathway over active site near-optimal, where bridging Ir–OBRI serves acceptor to accelerate transfer on an adjacent Ru centre, breaking typical adsorption-dissociation linear scaling relationship a single thus enhancing activity. Here, show rational design multiple sites can break activity/stability trade-off commonly encountered catalysts, offering good approaches towards high-performance catalysts. Efficient are essential authors report enable oxygen-mediated deprotonation pathways, overcoming evolution.

Language: Английский

Citations

19

Isolated Octahedral Pt-Induced Electron Transfer to Ultralow-Content Ruthenium-Doped Spinel Co3O4 for Enhanced Acidic Overall Water Splitting DOI
Di Li,

Danyun Xu,

Yuhou Pei

et al.

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: unknown

Published: Sept. 13, 2024

The development of a highly active and stable oxygen evolution reaction (OER) electrocatalyst is desirable for sustainable efficient hydrogen production via proton exchange membrane water electrolysis (PEMWE) powered by renewable electricity yet challenging. Herein, we report robust Pt/Ru-codoped spinel cobalt oxide (PtRu-Co

Language: Английский

Citations

18

Importing Atomic Rare‐Earth Sites to Activate Lattice Oxygen of Spinel Oxides for Electrocatalytic Oxygen Evolution DOI Creative Commons
Xuan Wang,

Jinrui Hu,

Tingyu Lu

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: unknown

Published: Oct. 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.

Language: Английский

Citations

18