Ligand Effect-Induced Electronic Structure Manipulation of Media-Entropy Alloy for Remarkable Stability over 50,000 Cycles in Oxygen Reduction DOI
Sijie Chen,

Dingli Bao,

Luping Zhang

et al.

Inorganic Chemistry, Journal Year: 2024, Volume and Issue: unknown

Published: Nov. 19, 2024

Modulating the "trade-off" between activity and durability of Pd-based alloys while eliminating dissolution nonprecious metal element issue is highly significant for advancement commercializing anion-exchange membrane fuel cells (AEMFCs). Herein, by harmonizing composition ligand effects targeting stability concerns alloys, we propose PdRhNi ternary medium-entropy-alloy (MEA) networks (PdRhNi ANs) as exceptionally efficient oxygen reduction reaction (ORR) electrocatalysts via effect. The results theoretical calculations provide compelling evidence that effect Ni in ANs, which can endow an inductive to reshape electronic configuration induce a reduced energy barrier rate-determining steps, optimizes adsorption O-related intermediates lowers d-band center species, collectively boosting anti-CO capacity ORR efficiency. Consequently, as-made ANs not only demonstrate significantly enhanced electrocatalytic properties with half-wave potential 0.85 V excellent resistance CO toxicity, contrast those commercial Pt/C binary counterparts, but also exhibit negligible decline after 50,000 cycle examination. More excitingly, homemade AEMFC AN air cathode delivers higher power density 109 mW cm–2, surpassing PdRh AN-based battery, highlighting promising prospects implementing MEA materials engineering environments.

Language: Английский

Spin‐Polarized PdCu–Fe3O4 In‐Plane Heterostructures with Tandem Catalytic Mechanism for Oxygen Reduction Catalysis DOI
Menggang Li, Guanghui Han, Fenyang Tian

et al.

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

Published: Oct. 23, 2024

Abstract Alloying has significantly upgraded the oxygen reduction reaction (ORR) of Pd‐based catalysts through regulating thermodynamics oxygenated intermediates. However, unsatisfactory activation ability alloys toward O 2 molecules limits further improvement ORR kinetics. Herein, precise synthesis nanosheet assemblies spin‐polarized PdCu–Fe 3 4 in‐plane heterostructures for drastically activating and boosting kinetics is reported. It demonstrated that deliberate‐engineered not only tailor d ‐band center Pd sites with weakened adsorption intermediates but also endow electrophilic Fe strong to activate molecules, which make exhibit highest specific activity among state‐of‐art so far. In situ electrochemical spectroscopy theoretical investigations reveal a tandem catalytic mechanism on ─Fe initially molecular generate being transferred finish subsequent proton‐coupled electron transfer steps.

Language: Английский

Citations

4
Enhancing Near-Infrared Photothermal Activity through Precise In-Plane Interface Engineering in CuS-Au and CuS@Au Ultrathin Nanoplates for Combating Multidrug-Resistant Bacteria DOI
Yuxin Wu, Qi He, Heng Zhang

et al.

Journal of Materials Chemistry C, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 1, 2025

Ultrathin two-dimensional hybrid nanostructures are crafted with well-designed copper sulfide–gold interfaces, demonstrating exceptional near-infrared photothermal properties to kill multidrug-resistant bacteria.

Language: Английский

Citations

0
The advances in innovative amorphous noble-metal-based electrocatalysts DOI

Xiaoyu Fan,

Kexin Yin,

Huiqing Wang

et al.

Chem Catalysis, Journal Year: 2025, Volume and Issue: unknown, P. 101324 - 101324

Published: March 1, 2025

Language: Английский

Citations

0
Interface-rich porous Fe-doped hcp-PtBi/fcc-Pt heterostructured nanoplates enhanced the C C bond cleavage of C3 alcohols electrooxidation DOI
Xiaotong Yang,

Kaiyu Dong,

Zhe Zheng

et al.

Journal of Colloid and Interface Science, Journal Year: 2024, Volume and Issue: 678, P. 153 - 161

Published: Sept. 3, 2024

Language: Английский

Citations

2
Sub-2 nm Amorphous PdSn/C Nanocatalyst for Enhanced Ethanol Oxidation DOI Creative Commons
Xiaoxuan Yang, Xiang Li,

Zitong Jiang

et al.

ACS electrochemistry., Journal Year: 2024, Volume and Issue: unknown

Published: Nov. 5, 2024

Amorphous palladium-based catalysts exhibit unique advantages in catalytic reactions due to their large number of uncoordinated atoms and dangling bonds. However, the strong interaction between metal atoms, it is easy form crystalline structures thus, synthesis amorphous structure difficult. Here, sub-2 nm PdSn nanoparticles were synthesized one step by liquid phase reduction method. The with different compositions obtained fine-tuning concentration precursor. Compared commercial Pd/C catalyst, those showed significantly enhanced efficiency ethanol electrocatalytic oxidation reaction. Among them, PdSn0.87 nanoparticle best mass activity specific (3026 mA mgPd–1, 10.77 cm–2), which 6.55 4.14 times than that catalyst (462 2.60 respectively. Density functional theory (DFT) calculation shows nanocatalysts can effectively enhance adsorption energy CH3CH2OH* on its surface weaken CO*, thus promoting conversion molecules surface. This research paves way for development highly efficient tailored properties reactions.

Language: Английский

Citations

2
Switchable Acidic Oxygen Evolution Mechanisms on Atomic Skin of Ruthenium Metallene Oxides DOI
Tianyi Gao,

Dongxu Jiao,

Lina Wang

et al.

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

Published: Dec. 25, 2024

RuO2 has been considered as a promising, low-cost, and highly efficient catalyst in the acidic oxygen evolution reaction (OER). However, it suffers from poor stability due to inevitable involvement of lattice mechanism (LOM). Here, we construct unique metallene-based core-skin structure unveil that OER pathway atomic skin can be regulated LOM an adsorbate by altering core species metallene oxides metallenes. This switch is achieved without sacrificing number active sites, enabling Pd@RuO2 metallenes exhibit outstanding activity with low overpotential 189 mV at 10 mA cm–2, which 54 lower than counterpart PdO@RuO2 Additionally, they also robust negligible decay over 100 h 50 outperforming most reported RuO2-based catalysts. Multiple spectroscopic analyses theoretical calculations demonstrate Pd-metallene core, acting electron donor, increases migration energy subsurface atoms optimizes adsorption intermediates on Ru mechanism. Such offers novel way for tuning catalytic behaviors electrocatalysts.

Language: Английский

Citations

2
Microkinetic Model to Rationalize the Lifetime of Electrocatalysis: Trade-off between Activity and Stability DOI
Hideshi Ooka,

Marie E. Wintzer,

Hirokazu Komatsu

et al.

The Journal of Physical Chemistry Letters, Journal Year: 2024, Volume and Issue: unknown, P. 10079 - 10085

Published: Sept. 30, 2024

Electrocatalysts which can operate for several years are required to produce hydrogen and commodity chemicals in an environmentally friendly manner. However, designing materials with long operational lifetimes is challenging, due the lack of a conceptual framework predict catalytic quantitatively. Here, we report microkinetic equation quantifies lifetime electrocatalyst undergoing dissolution. This was obtained by taking advantage fact that catalysis much faster than deactivation, allows ordinary differential equations be solved via quasi steady-state approximation. All chemical reactions were modeled as irreversible, first-order elementary reactions. Under this assumption, rate correlates linearly deactivation rate, leading trade-off relationship between activity stability. Our model supported correlation theoretical experimental (

Language: Английский

Citations

1
Interface engineering of supported palladium electrocatalyst with covalent organic polymer towards oxygen reduction reaction DOI

Huimin Sun,

Jinyan Wang, Hailong Hu

et al.

Journal of Colloid and Interface Science, Journal Year: 2024, Volume and Issue: 682, P. 157 - 164

Published: Nov. 27, 2024

Language: Английский

Citations

1
Defect Engineering of Metal‐Based Atomically Thin Materials for Catalyzing Small‐Molecule Conversion Reactions DOI Open Access

Juanjuan Huo,

Yuhai Dou, Chao Wu

et al.

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

Published: Dec. 20, 2024

Abstract Recently, metal‐based atomically thin materials (M‐ATMs) have experienced rapid development due to their large specific surface areas, abundant electrochemically accessible sites, attractive chemistry, and strong in‐plane chemical bonds. These characteristics make them highly desirable for energy‐related conversion reactions. However, the insufficient active sites slow reaction kinetics leading unsatisfactory electrocatalytic performance limited commercial application. To address these issues, defect engineering of M‐ATMs has emerged increase modify electronic structure, enhance catalytic reactivity stability. This review provides a comprehensive summary strategies M‐ATM nanostructures, including vacancy creation, heteroatom doping, amorphous phase/grain boundary generation, heterointerface construction. Introducing recent advancements in application electrochemical small molecule reactions (e.g., hydrogen, oxygen, carbon dioxide, nitrogen, sulfur), which can contribute circular economy by recycling molecules like H 2 , O CO N S. Furthermore, crucial link between reconstruction atomic‐level structure activity via analyzing dynamic evolution during process is established. The also outlines challenges prospects associated with M‐ATM‐based catalysts inspire further research efforts developing high‐performance M‐ATMs.

Language: Английский

Citations

1
Support‐Free, Connected Core–Shell Nanoparticle Catalysts Synthesized via a Low‐Temperature Process for Advanced Oxygen Reduction Performance DOI Creative Commons

Aparna Chitra Sudheer,

Gopinathan M. Anilkumar, Hidenori Kuroki

et al.

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

Published: Dec. 26, 2024

Nanostructured Pt-based catalysts have attracted considerable attention for fuel-cell applications. This study introduces a novel one-pot and low-temperature polyol approach synthesizing support-free, connected nanoparticles with non-Pt metal cores Pt shells. Unlike conventional heat treatment methods, the developed support-free Fe-free Pd

Language: Английский

Citations

1