Atomic Gap-State Engineering of MoS2 for Alkaline Water and Seawater Splitting DOI
Tao Sun, Tong Yang, Wenjie Zang

et al.

ACS Nano, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 11, 2025

Transition-metal dichalcogenides (TMDs), such as molybdenum disulfide (MoS2), have emerged a generation of nonprecious catalysts for the hydrogen evolution reaction (HER), largely due to their theoretical adsorption energy close that platinum. However, efforts activate basal planes TMDs primarily centered around strategies introducing numerous atomic vacancies, creating vacancy–heteroatom complexes, or applying significant strain, especially acidic media. These approaches, while potentially effective, present substantial challenges in practical large-scale deployment. Here, we report gap-state engineering strategy controlled activation S atom MoS2 through metal single-atom doping, effectively tackling both efficiency and stability alkaline water seawater splitting. A versatile synthetic methodology allows fabrication series single-metal atom-doped materials (M1/MoS2), featuring widely tunable densities with each dopant replacing Mo site. Among these (Mn1, Fe1, Co1, Ni1), Co1/MoS2 demonstrates outstanding HER performance media, overpotentials at mere 159 164 mV 100 mA cm–2, Tafel slopes 41 45 dec–1, respectively, which surpasses all reported TMD-based benchmark Pt/C during splitting, can be attributed an optimal modulation associated sulfur atoms. Experimental data correlating doping density identity performance, conjunction calculations, also reveal descriptor linked near-Fermi gap state modulation, corroborated by observed increase unoccupied 3p states.

Language: Английский

Geometric and Electronic Engineering of Atomically Dispersed Copper‐Cobalt Diatomic Sites for Synergistic Promotion of Bifunctional Oxygen Electrocatalysis in Zinc–Air Batteries DOI
Zhijun Li, Siqi Ji, Chun Wang

et al.

Advanced Materials, Journal Year: 2023, Volume and Issue: 35(25)

Published: April 11, 2023

The development of rechargeable zinc-air batteries is heavily dependent on bifunctional oxygen electrocatalysts to offer exceptional reduction/evolution reaction (ORR/OER) activities. However, the design such with high activity and durability challenging. Herein, a strategy proposed create an electrocatalyst comprised copper-cobalt diatomic sites highly porous nitrogen-doped carbon matrix (Cu-Co/NC) abundantly accessible metal optimal geometric electronic structures. Experimental findings theoretical calculations demonstrate that synergistic effect Cu-Co dual-metal metal-N4 coordination induce asymmetric charge distributions moderate adsorption/desorption behavior intermediates. This exhibits extraordinary electrocatalytic activities in alkaline media, half-wave potential 0.92 V for ORR low overpotential 335 mV at 10 mA cm-2 OER. In addition, it demonstrates acidic (0.85 V) neutral (0.74 media. When applied battery, achieves operational performance outstanding (510 h), ranking as one most efficient reported date. work importance engineering isolated boosting electrochemical energy devices.

Language: Английский

Citations

148

Advancements in Microwave Absorption Motivated by Interdisciplinary Research DOI Open Access
Zehao Zhao, Yuchang Qing, Luo Kong

et al.

Advanced Materials, Journal Year: 2023, Volume and Issue: 36(4)

Published: Oct. 23, 2023

Abstract Microwave absorption materials (MAMs) are originally developed for military purposes, but have since evolved into versatile with promising applications in modern technologies, including household use. Despite significant progress bench‐side research over the past decade, MAMs remain limited their scope and yet to be widely adopted. This review explores history of from first‐generation coatings second‐generation functional absorbers, identifies bottlenecks hindering maturation. It also presents potential solutions such as exploring broader spatial scales, advanced characterization, introducing liquid media, utilizing novel toolbox (machine learning, ML), proximity lab end‐user. Additionally, it meticulously compelling medicine, mechanics, energy, optics, sensing, which go beyond efficiency, along current development status prospects. interdisciplinary direction differs previous primarily focused on meeting traditional requirements (i.e., thin, lightweight, wide, strong), can defined next generation smart absorbers. Ultimately, effective utilization ubiquitous electromagnetic (EM) waves, aided by third‐generation MAMs, should better aligned future expectations.

Language: Английский

Citations

136

Atomically precise electrocatalysts for oxygen reduction reaction DOI Creative Commons
Yan Li, Panpan Li,

Qingyi Zhu

et al.

Chem, Journal Year: 2023, Volume and Issue: 9(2), P. 280 - 342

Published: Feb. 1, 2023

Language: Английский

Citations

134

Unlocking the Transition of Electrochemical Water Oxidation Mechanism Induced by Heteroatom Doping DOI Open Access
Xuan Li, Chen Deng, Yan Kong

et al.

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(40)

Published: Aug. 15, 2023

Abstract Heteroatom doping has emerged as a highly effective strategy to enhance the activity of metal‐based electrocatalysts toward oxygen evolution reaction (OER). It is widely accepted that does not switch OER mechanism from adsorbate (AEM) lattice‐oxygen‐mediated (LOM), and enhanced attributed optimized binding energies intermediates. However, this seems inconsistent with fact overpotential doped (<300 mV) considerably smaller than limit AEM (>370 mV). To determine origin inconsistency, we select phosphorus (P)‐doped nickel‐iron mixed oxides model observe enhances covalency metal‐oxygen bonds drive pathway transition LOM, thereby breaking adsorption linear relation between *OH *OOH in AEM. Consequently, obtained P‐doped display small 237 mV at 10 mA cm −2 . Beyond P, similar also observed on sulfur doping. These findings offer new insights into substantially originating heteroatom

Language: Английский

Citations

110

Rechargeable Zinc–Air Batteries with an Ultralarge Discharge Capacity per Cycle and an Ultralong Cycle Life DOI
Xiongwei Zhong, Yangfan Shao, Biao Chen

et al.

Advanced Materials, Journal Year: 2023, Volume and Issue: 35(30)

Published: April 17, 2023

A conventional two-electrode rechargeable zinc-air battery (RZAB) has two major problems: 1) opposing requirements for the oxygen reduction (ORR) and evolution (OER) reactions from catalyst at air cathode; 2) zinc-dendrite formation, hydrogen generation, zinc corrosion anode. To tackle these problems, a three-electrode RZAB (T-RZAB) including hydrophobic discharge cathode, hydrophilic charge zinc-free anode is developed. The decoupled cathodes enable fast ORR OER kinetics, avoid oxidization of catalyst. using tin-coated copper foam that induces growth (002)Zn planes, suppresses evolution, prevents Zn corrosion. As result, T-RZABs have high capacity per cycle 800 mAh cm-2 , low voltage gap between discharge/charge platforms 0.66 V, an ultralong life 5220 h current density 10 mA . large T-RZAB with Ah no obvious degradation after cycling 1000 Finally, pack energy 151.8 Wh kg-1 cost 46.7 US dollars kWh-1 assembled.

Language: Английский

Citations

94

Activating Amorphous Ru Metallenes Through Co Integration for Enhanced Water Electrolysis DOI Open Access

Vishal Jose,

Viet‐Hung Do,

P. Prabhu

et al.

Advanced Energy Materials, Journal Year: 2023, Volume and Issue: 13(28)

Published: June 11, 2023

Abstract Designing efficient bifunctional electrocatalysts with excellent activity and robust stability presents a central challenge for the large‐scale commercialization of water electrolysis. Herein, facile approach is reported construct atomically thin amorphous RuM (MCo, Fe, or Ni) bimetallenes as high‐performance toward both electrochemical hydrogen evolution reaction (HER) oxygen (OER). The RuCo bimetallene manifests characterized by low required overpotentials, superior price activity, durability well cell potential splitting performance, outperforming Pt/C RuO 2 benchmark catalysts. Combined operando X‐ray absorption spectroscopy investigation theoretical simulations reveal synergism taking place between binary constituents, in which Co serves promotive role along HER/OER pathway, contributing via optimal binding to *OH dissociation modulating Ru electronic structure favorably, hence rendering high catalytic centers alkaline HER OER.

Language: Английский

Citations

92

Advances in heterogeneous single-cluster catalysis DOI
Xinzhe Li, Sharon Mitchell, Yiyun Fang

et al.

Nature Reviews Chemistry, Journal Year: 2023, Volume and Issue: 7(11), P. 754 - 767

Published: Oct. 9, 2023

Language: Английский

Citations

91

Atomically dispersed Ni activates adjacent Ce sites for enhanced electrocatalytic oxygen evolution activity DOI Creative Commons
Zhihao Pei, Huabin Zhang, Zhi‐Peng Wu

et al.

Science Advances, Journal Year: 2023, Volume and Issue: 9(26)

Published: June 28, 2023

Manipulating the intrinsic activity of heterogeneous catalysts at atomic level is an effective strategy to improve electrocatalytic performances but remains challenging. Here, atomically dispersed Ni anchored on CeO2 particles entrenched peanut-shaped hollow nitrogen-doped carbon structures (a-Ni/CeO2@NC) rationally designed and synthesized. The as-prepared a-Ni/CeO2@NC catalyst exhibits substantially boosted greatly reduced overpotential for oxygen evolution reaction. Experimental theoretical results demonstrate that decoration isolated species over induces electronic coupling redistribution, thus resulting in activation adjacent Ce sites around atoms accelerated kinetics. This work provides a promising explore regulation improvement level, thereby improving activity.

Language: Английский

Citations

87

Biomass derived diverse carbon nanostructure for electrocatalysis, energy conversion and storage DOI

Feng Ying,

Junjie Jiang, Yaxuan Xu

et al.

Carbon, Journal Year: 2023, Volume and Issue: 211, P. 118105 - 118105

Published: May 11, 2023

Language: Английский

Citations

70

Heterogeneous Fe-Co dual-atom catalyst outdistances the homogeneous counterpart for peroxymonosulfate-assisted water decontamination: New surface collision oxidation path and diatomic synergy DOI
Changqing Zhu,

Fenxian Cun,

Zhongwei Fan

et al.

Water Research, Journal Year: 2023, Volume and Issue: 241, P. 120164 - 120164

Published: June 1, 2023

Language: Английский

Citations

64