Manipulating Oxygen Reduction Mechanisms of Platinum with Nonmetallic Phosphorus and Metallic Copper Synergistic Alloying DOI Open Access
Yizhe Chen, Liangyu Sun,

Yuzhou Jiao

et al.

Small, Journal Year: 2025, Volume and Issue: unknown

Published: March 16, 2025

Abstract Alloying of platinum (Pt) nanostructures with heteroelements, commonly including transition‐metals and nonmetals, is an effective strategy to improve the electrocatalytic performance for oxygen reduction reaction (ORR). However, distinct mechanisms by which metal/nonmetal alloying improves ORR activity remain unclear. Herein, based on successful porous network Pt nanospheres (NSs) metallic copper (Cu) non‐metallic phosphorus (P) systematically integrating electrochemical tests, density functional theory calculations, in situ Raman spectroscopy, this study reveals that internal Cu‐alloying responsible modulating binding strength oxygenated intermediates lower free energy barrier potential‐determining step (PDS) along associative mechanism, while further surface P‐alloying can transform pathway dissociative PDS has a quite low barrier. As result, carbon‐supported P/Cu co‐alloyed (P‐PtCu NSs /C) catalyst synthesized confinement growth post‐phosphorization demonstrates excellent stability compared commercial Pt/C both half‐cells proton exchange membrane fuel cells. In particular, hydrogen (H 2 )‐oxygen (O ) single cell P‐PtCu /C as cathode achieves high mass 0.52 A mg −1 at voltage 0.90 V, surpassing U.S. Department Energy's current target.

Language: Английский

Modulating Electronic Metal‐Support Interactions to Boost Visible‐Light‐Driven Hydrolysis of Ammonia Borane: Nickel‐Platinum Nanoparticles Supported on Phosphorus‐Doped Titania DOI Creative Commons
Chao Wan, Li Gui, Jiapei Wang

et al.

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

Published: June 9, 2023

Abstract Ammonia borane (AB) is a promising material for chemical H 2 storage owing to its high density (up 19.6 wt %). However, the development of an efficient catalyst driving evolution through AB hydrolysis remains challenging. Therefore, visible‐light‐driven strategy generating was implemented in this study using Ni−Pt nanoparticles supported on phosphorus‐doped TiO (Ni‐Pt/P‐TiO ) as photocatalysts. Through surface engineering, P‐TiO prepared by phytic‐acid‐assisted phosphorization and then employed ideal support immobilizing via facile co‐reduction strategy. Under visible‐light irradiation at 283 K, Ni 40 Pt 60 /P‐TiO exhibited improved recyclability turnover frequency 967.8 mol −1 min . Characterization experiments functional theory calculations indicated that enhanced performance originated from combination alloying effect, Mott–Schottky junction metal‐semiconductor interface, strong metal‐support interactions. These findings not only underscore benefits utilizing multipronged effects construct highly active AB‐hydrolyzing catalysts, but also pave path toward designing high‐performance catalysts engineering modulate electronic interactions other visible‐light‐induced reactions.

Language: Английский

Citations

105

Intermetallic Nanocrystals for Fuel-Cells-Based Electrocatalysis DOI

Fangxu Lin,

Menggang Li, Lingyou Zeng

et al.

Chemical Reviews, Journal Year: 2023, Volume and Issue: 123(22), P. 12507 - 12593

Published: Nov. 1, 2023

Electrocatalysis underpins the renewable electrochemical conversions for sustainability, which further replies on metallic nanocrystals as vital electrocatalysts. Intermetallic have been known to show distinct properties compared their disordered counterparts, and long explored functional improvements. Tremendous progresses made in past few years, with notable trend of more precise engineering down an atomic level investigation transferring into practical membrane electrode assembly (MEA), motivates this timely review. After addressing basic thermodynamic kinetic fundamentals, we discuss classic latest synthetic strategies that enable not only formation intermetallic phase but also rational control other catalysis-determinant structural parameters, such size morphology. We demonstrate emerging nanomaterials potentially advancement energy electrocatalysis. Then, state-of-the-art characterizations representative electrocatalysts emphasis oxygen reduction reaction evaluated a MEA setup. summarize review by laying out existing challenges offering perspective future research directions toward practicing conversions.

Language: Английский

Citations

92

Tailoring Local Chemical Ordering via Elemental Tuning in High-Entropy Alloys DOI
Zhennan Huang, Tangyuan Li, Boyang Li

et al.

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(3), P. 2167 - 2173

Published: Jan. 12, 2024

Due to the large multi-elemental space desired for property screening and optimization, high-entropy alloys (HEAs) hold greater potential over conventional a range of applications, such as structural materials, energy conversion, catalysis. However, relationship between HEA composition its local structural/elemental configuration is not well understood, particularly in noble-metal-based nanomaterials, hindering design development nano-HEAs conversion catalysis applications. Herein, we determined precise atomic-level elemental arrangements model HEAs composed RhPtPdFeCo RuPtPdFeCo unveil their characteristics. Notably, by changing just one constituent element (Rh Ru), found dramatic changes arrangement from complete random mixing single ordering feature. Additionally, demonstrate that can be further controlled varying Ru concentration, allowing us toggle clustering distinct heterostructures multicomponent systems. Overall, our study presents practical approach manipulating atomic structures systems, which could provide in-depth knowledge mechanistically understand functionality nanomaterials

Language: Английский

Citations

26

Surface Strain Effect on Electrocatalytic Hydrogen Evolution Reaction of Pt-Based Intermetallics DOI
Ziying Zhong, Yuanhua Tu, Longhai Zhang

et al.

ACS Catalysis, Journal Year: 2024, Volume and Issue: 14(5), P. 2917 - 2923

Published: Feb. 12, 2024

Elucidating the relationship between electrocatalytic activity and surface strain is pivotal for designing highly efficient electrocatalysts acidic hydrogen evolution reaction (HER). However, a general correlation currently absent due to lack of ideal catalytic materials platforms with well-defined structures components. Herein, we select L10 L12 Pt-based intermetallic compounds as model construct series core–shell catalysts strained Pt skins (IMC@Pt) establish HER performance. Density functional theory calculations were performed determine degree, d-band center, key descriptor ΔGH* HER. By combining theoretical experimental data, propose volcano-type trend IMC@Pt an apex at 4% compressive strain. In addition, demonstrate class active durable Among them, Pt3V@Pt catalyst exhibits highest intrinsic specific 4.24 mA cmPt–2 overpotential 20 mV, which 4 times higher than that Pt. This work provides solid understanding essential nature PtM alloy can guide design high-performance water electrolyzers.

Language: Английский

Citations

20

Concentrated solar CO2 reduction in H2O vapour with >1% energy conversion efficiency DOI Creative Commons

Yuqi Ren,

Yiwei Fu, Naixu Li

et al.

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

Published: June 1, 2024

Abstract H 2 O dissociation plays a crucial role in solar-driven catalytic CO methanation, demanding high temperature even for solar-to-chemical conversion efficiencies <1% with modest product selectivity. Herein, we report an oxygen-vacancy (V o ) rich CeO catalyst single-atom Ni anchored around its surface V sites by replacing Ce atoms to promote and achieve effective photothermal reduction under concentrated light irradiation. The photon flux reduces the apparent activation energy CH 4 production prevents from depletion. defects coordinated Ni, significantly capture of charges local phonons at d -impurity orbitals, thereby inducing more activation. presents yield 192.75 µmol/cm /h, efficiency 1.14% selectivity ~100%. mechanistic insights uncovered this study should help further development O-activating catalysts expedite practical utilization technologies.

Language: Английский

Citations

18

Synergistic Effects of PtRhNiFeCu High Entropy Alloy Nanocatalyst for Hydrogen Evolution and Oxygen Reduction Reactions DOI
Zhiwei Hu,

Kuangyin Chen,

Yihua Zhu

et al.

Small, Journal Year: 2024, Volume and Issue: 20(26)

Published: Jan. 17, 2024

The unique properties of high entropy alloy (HEA) catalysts, particularly their severe lattice distortion and the synergistic effect multiple components, endow them with exceptional multifunctional catalytic performance. Herein, it is revealed for first time, that ultrasmall PtRhNiFeCu HEA nanoparticles catalyst shows outstanding activity both hydrogen evolution reaction (HER) oxygen reduction (ORR). exhibits an impressively low overpotential 13 mV at 10 mA cm

Language: Английский

Citations

17

Metal Hydrogel‐Based Integrated Wearable Biofuel Cell for Self‐Powered Epidermal Sweat Biomarker Monitoring DOI
Yao Chen,

Xinhao Wan,

Guanglei Li

et al.

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

Published: May 6, 2024

Abstract Wearable sensors for continuous monitoring of biomarkers in body fluids have gained significant attention their potential disease diagnostics and health management, but lack sustainable power supply advanced sensing strategies. Herein, sweat wearable biofuel cells (w‐BFCs) based on metal hydrogels are demonstrated with high output outstanding stability, which harvest energy directly from human simultaneously enable self‐powered epidermal biomarkers. Experimental computational results elucidate that the highly porous flexible exhibit superior electrocatalytic capabilities oxidizing ascorbic acid (AA), a metabolite at anode, reducing O 2 cathode. Consequently, assembled AA/O BFC delivers stable output, maximum density 35 µW cm −2 an ultralow AA concentration long‐term stability over 30 days, self‐powered, sensitive detection. When applied to skin volunteers, this integrated w‐BFC powers biosensor using as fuel allowing real‐time signal via smartphone. This work not only advances harvesting also paves new avenues real‐time, online

Language: Английский

Citations

17

Strain Effects in Ru‐Au Bimetallic Aerogels Boost Electrocatalytic Hydrogen Evolution DOI Creative Commons
Wei Wei, Fei Guo, Cui Wang

et al.

Small, Journal Year: 2024, Volume and Issue: 20(25)

Published: Jan. 26, 2024

Abstract To improve the sluggish kinetics of hydrogen evolution reaction (HER), a key component in water‐splitting applications, there is an urgent desire to develop efficient, cost‐effective, and stable electrocatalysts. Strain engineering proving efficient strategy for increasing catalytic activity This work presents development Ru‐Au bimetallic aerogels by simple one‐step situ reduction‐gelation approach, which exhibits strain effects electron transfer create remarkable HER stability alkaline environment. The surface induced segregated structure shifts d ‐band center downward, enhancing catalysis balancing processes water dissociation, OH* adsorption, H* adsorption. Specifically, optimized catalyst shows low overpotentials only 24.1 mV at current density 10 mA cm −2 electrolytes, surpassing commercial Pt/C. study can contribute understanding electrocatalysts atomic scale.

Language: Английский

Citations

15

Ultradurable Pt-Based Catalysts for Oxygen Reduction Electrocatalysis DOI Open Access
Ziting Li, Peng Zhou, Yuxin Zhao

et al.

Catalysts, Journal Year: 2024, Volume and Issue: 14(1), P. 57 - 57

Published: Jan. 12, 2024

An oxygen reduction reaction (ORR) is the key half of proton exchange membrane fuel cells (PEMFCs), and highly dependent on Pt-based nanocrystals as core electrocatalysts. Despite exceptional ORR activity from adjusting electronic structures surface or near-surface atoms, several serious issues, including corrosion carbon supports, preferential leaching active metal elements, instability low-coordinated atoms sintering/agglomeration nanocrystals, still exist, challenging durability developed catalysts. From point view catalyst structure design, in this review, we summarized state-of-the-art structural regulation strategies for improving The current limitation binary catalysts electrocatalysis firstly discussed, detailed are further classified into optimization metal-doped alloys, core/shell structures, intermetallics high-entropy etc. structure–performance relationship detailedly explained, especially emphasizing elimination above restrictions. Finally, existing challenges future research direction presented, aiming at practicing PEMFC devices ultradurable

Language: Английский

Citations

11

Designing and modeling fuel cells made of mixed transition metal dichalcogenide and carbon-based nanostructure electrodes for renewable energy storage DOI

Mahdi Soleimani Moghaddam,

Ali Bahari, Hajar Rajaei Litkohi

et al.

Journal of Power Sources, Journal Year: 2024, Volume and Issue: 604, P. 234514 - 234514

Published: April 10, 2024

Language: Английский

Citations

9