Thermal‐Driven Orderly Assembly of Ir‐atomic Chains on α‐MnO2 with Enhanced Performance for Acidic Oxygen Evolution DOI

Junan Gao,

Xiaokuan Wu,

Xinying Teng

et al.

ChemPlusChem, Journal Year: 2024, Volume and Issue: 89(5)

Published: Jan. 24, 2024

Abstract The development of acid‐stable oxygen evolution reaction electrocatalysts is essential for high‐performance acidic water electrolysis. Herein, we report the results one‐dimensional (1D) nanorods (NRs) IrCeMnO@Ir containing ~20 wt . % Iridium (Ir) as an efficient anode electrocatalyst, synthesized via a one‐step cation exchange strategy. Owing to presence 1D channels nanorod architecture and unique electronic structure, exhibited 69 folds more mass activity than that commercial IrO 2 well over 400 h stability with only 20 mV increase in overpotential. DFT calculations control experiments demonstrated CeO serves electron buffer accelerate kinetics rate‐determined step significantly enhanced suppress over‐oxidation Ir species their dissolution impressively promoted under practical conditions. Our work opens up feasible strategy boost OER simultaneously.

Language: Английский

Tensile straining of iridium sites in manganese oxides for proton-exchange membrane water electrolysers DOI Creative Commons
Hui Su, Chenyu Yang, Meihuan Liu

et al.

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

Published: Jan. 2, 2024

Abstract Although the acidic oxygen evolution reaction (OER) plays a crucial role in proton-exchange membrane water electrolysis (PEMWE) devices, challenges remain owing to lack of efficient and acid-stable electrocatalysts. Herein, we present low-iridium electrocatalyst which tensile-strained iridium atoms are localized at manganese-oxide surface cation sites (TS-Ir/MnO 2 ) for high sustainable OER activity. In situ synchrotron characterizations reveal that TS-Ir/MnO can trigger continuous lattice oxygen-mediated (L-LOM) mechanism. particular, L-LOM process could substantially boost adsorption transformation H O molecules over vacancies around Ir prevent further loss inner MnO bulk optimize structural integrity catalyst. Importantly, resultant PEMWE device fabricated using delivers current density 500 mA cm −2 operates stably 200 h.

Language: Английский

Citations

84

Recent advances in Ru/Ir-based electrocatalysts for acidic oxygen evolution reaction DOI Creative Commons

Guoliang Gao,

Zixu Sun, Xueli Chen

et al.

Applied Catalysis B Environment and Energy, Journal Year: 2023, Volume and Issue: 343, P. 123584 - 123584

Published: Dec. 1, 2023

The electrocatalytic process of water splitting offers a promising approach to produce sustainable hydrogen. However, the slow kinetics oxygen evolution reaction (OER) presents notable challenge, especially in acidic environment proton exchange membrane (PEM) systems. Despite extensive progress made catalyst development for hydrogen production through electrolysis last century, significant advancements have been accomplished. quest OER catalysts that possess both high activity and stability, while also being affordable, continues be challenging. Currently, Ru/Ir-based electrocatalysts are only practical anode available. Therefore, it is crucial explore feasible strategies enhance performance longevity catalysts. This review comprehensive assessment obstacles prospective Additionally, underscores areas research concentration, providing valuable perspectives future endeavors development.

Language: Английский

Citations

66

Improving Electrocatalytic Oxygen Evolution through Local Field Distortion in Mg/Fe Dual‐site Catalysts DOI

Jing Zhang,

Yufeng Zhao, Wanting Zhao

et al.

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(52)

Published: Nov. 9, 2023

Transition metal single atom electrocatalysts (SACs) with metal-nitrogen-carbon (M-N-C) configuration show great potential in oxygen evolution reaction (OER), whereby the spin-dependent electrons must be allowed to transfer along reactants (OH- /H2 O, singlet spin state) and products (O2 , triplet state). Therefore, it is imperative modulate M-N-C enhance spin-sensitive OER energetics, which however remains a significant challenge. Herein, we report local field distortion induced intermediate low transition by introducing main-group element (Mg) into Fe-N-C architecture, decode underlying origin of enhanced activity. We unveil that, large ionic radii mismatch between Mg2+ Fe2+ can cause FeN4 in-plane square deformation, triggers favorable from (dxy2 dxz2 dyz1 dz21 2.96 μB ) dyz2 0.95 ), consequently regulate thermodyna-mics elementary step desired Gibbs free energies. The as-obtained Mg/Fe dual-site catalyst demonstrates superior activity an overpotential 224 mV at 10 mA cm-2 electrolysis voltage only 1.542 V overall water splitting, outperforms those state-of-the-art SACs.

Language: Английский

Citations

47

Distance effect of single atoms on stability of cobalt oxide catalysts for acidic oxygen evolution DOI Creative Commons
Zhirong Zhang, Chuanyi Jia, Peiyu Ma

et al.

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

Published: Feb. 26, 2024

Abstract Developing efficient and economical electrocatalysts for acidic oxygen evolution reaction (OER) is essential proton exchange membrane water electrolyzers (PEMWE). Cobalt oxides are considered promising non-precious OER catalysts due to their high activities. However, the severe dissolution of Co atoms in acid media leads collapse crystal structure, which impedes application PEMWE. Here, we report that introducing acid-resistant Ir single into lattice spinel cobalt can significantly suppress keep them highly stable during process. Combining theoretical experimental studies, reveal stabilizing effect induced by heteroatoms exhibits a strong dependence on distance adjacent atoms, where stability continuously improves with decreasing distance. When reduces about 0.6 nm, present no obvious degradation over 60-h test OER, suggesting potential practical applications.

Language: Английский

Citations

38

Spin‐state Conversion by Asymmetrical Orbital Hybridization in Ni‐doped Co3O4 to Boost Singlet Oxygen Generation for Microbial Disinfection DOI

Meilin Duan,

Chao Huang,

Gong Zhang

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(12)

Published: Jan. 25, 2024

Singlet oxygen (1 O2 ) plays a significant role in environmental and biomedical disinfection fields. Electrocatalytic processes hold great potential for 1 generation, but remain challenging. Herein, facile Ni doping converted spin-state transition approach is reported boosting production. Magnetic analysis theoretical calculations reveal that occupied at the octahedral site of Co3 O4 can effectively induce low-to-high transition. The high-spin Ni-Co3 generate appropriate binding strength enhance electron transfer between Co centers with intermediates, thereby improving catalytic activity effective generating . In neutral conditions, 1×106 CFU mL-1 Gram-negative ESBL-producing Escherichia coli (E. coli) could be inactivated by system within 5 min. Further antibacterial mechanisms indicate lead to cell membrane damage DNA degradation so as irreversible death. Additionally, developed inactivate bacteria from wastewater bioaerosols. This work provides an strategy designing electrocatalysis boost generation process.

Language: Английский

Citations

20

Boosting electrocatalytic performance via electronic structure regulation for acidic oxygen evolution DOI Creative Commons
Qian Wu,

Gao Qingping,

Wang Xingpeng

et al.

iScience, Journal Year: 2023, Volume and Issue: 27(1), P. 108738 - 108738

Published: Dec. 19, 2023

High-purity hydrogen produced by water electrolysis has become a sustainable energy carrier. Due to the corrosive environments and strong oxidizing working conditions, main challenge faced acidic oxidation is decrease in activity stability of anodic electrocatalysts. To address this issue, efficient strategies have been developed design electrocatalysts toward OER with excellent intrinsic performance. Electronic structure modification achieved through defect engineering, doping, alloying, atomic arrangement, surface reconstruction, constructing metal-support interactions provides an effective means boost OER. Based on introducing mechanism commonly present environments, review comprehensively summarizes for regulating electronic catalytic materials. Finally, several promising research directions are discussed inspire synthesis high-performance

Language: Английский

Citations

27

Enriched Oxygen Coverage Localized within Ir Atomic Grids for Enhanced Oxygen Evolution Electrocatalysis DOI
Hao Lin,

Qian Qian Yang,

Miao Lin

et al.

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

Published: Aug. 23, 2024

Abstract Inefficient active site utilization of oxygen evolution reaction (OER) catalysts have limited the energy efficiency proton exchange membrane (PEM) water electrolysis. Here, an atomic grid structure is demonstrated composed high‐density Ir sites (≈10 atoms per nm 2 ) on reactive MnO 2–x support which mediates coverage‐enhanced OER process. Experimental characterizations verify low‐valent Mn species with decreased coordination in exert a pivotal impact enriched coverage surface during process, and distributed grids, where highly electrophilic Ir─O (II‐δ)− bonds proceed rapidly, render intense nucleophilic attack radicals. Thereby, this metal‐support cooperation achieves ultra‐low overpotentials 166 mV at 10 mA cm −2 283 500 , together striking mass activity 380 times higher than commercial IrO 1.53 V. Moreover, its high performance also markedly surpasses black catalyst PEM electrolyzers long‐term stability.

Language: Английский

Citations

14

Enhanced Oxygen Evolution Kinetics via Single‐Atom Catalyst Design: A Review DOI Creative Commons

Zhen Yuan,

Yingjie Yu,

Qiao Xie

et al.

Advanced Materials Interfaces, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 25, 2025

Abstract This review highlights recent advancements in enhancing oxygen evolution reaction kinetics through the design of single‐atom catalysts. By leveraging unique properties catalysts (SACs), including high atom utilization and tunable electronic structures, researchers have developed with superior activity stability for (OER). Key strategies SACs design, such as support selection, coordination environment, doping effects are discussed, while also examining role advanced characterization techniques elucidating catalytic mechanisms. Finally, future directions challenges field outlined to guide development next‐generation OER

Language: Английский

Citations

1

Metal‐Free Catalytic Formation of a Donor‐Acceptor‐Donor Molecule and Its Lewis Acid‐Adduct Singlet Diradical with High‐Efficient NIR‐II Photothermal Conversion DOI

Shanshan Kong,

Li‐Ming Yang,

Quanchun Sun

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(19)

Published: March 5, 2024

Abstract We have synthesized a quinone‐incorporated bistriarylamine donor‐acceptor‐donor (D–A–D) semiconductor 1 by B(C 6 F 5 ) 3 (BCF) catalyzed C−H/C−H cross coupling via radical ion pair intermediates. Coordination of Lewis acids BCF and Al(OR (R =C(CF to the afforded diradical zwitterions 2 integer electron transfer. Upon binding acids, LUMO energy is significantly lowered band gap narrowed from 1.93 eV ( 1.01 1.06 ). are rare near‐infrared (NIR) dyes with broad absorption both centered around 1500 nm. By introducing photo generator, can be generated light‐dependent control. Furthermore, transfer process also reversibly regulated addition CH CN. In addition, temperature sharply increased reached as high 110 °C in 10 s upon irradiation near‐infrared‐II (NIR‐II) laser (1064 nm, 0.7 W cm −2 ), exhibiting fast response laser. It displays excellent photothermal stability (PT) conversion efficiency 62.26 % high‐quality PT imaging.

Language: Английский

Citations

8

Generic heterostructure interfaces bound to Co9S8 for efficient overall water splitting supported by photothermal DOI
Lei Yang,

Mengxiang Wang,

Hai Shan

et al.

Journal of Colloid and Interface Science, Journal Year: 2024, Volume and Issue: 662, P. 748 - 759

Published: Feb. 18, 2024

Language: Английский

Citations

6