Unraveling the electronegativity-dominated intermediate adsorption on high-entropy alloy electrocatalysts

Nature Communications, Journal Year: 2022, Volume and Issue: 13(1)

Published: May 13, 2022

Abstract High-entropy alloys have received considerable attention in the field of catalysis due to their exceptional properties. However, few studies hitherto focus on origin outstanding performance and accurate identification active centers. Herein, we report a conceptual experimental approach overcome limitations single-element catalysts by designing FeCoNiXRu (X: Cu, Cr, Mn) system with various sites that different adsorption capacities for multiple intermediates. The electronegativity differences between mixed elements HEA induce significant charge redistribution create highly Co Ru optimized energy barriers simultaneously stabilizing OH * H intermediates, which greatly enhances efficiency water dissociation alkaline conditions. This work provides an in-depth understanding interactions specific opens up fascinating direction breaking scaling relation issues multistep reactions.

Language: Английский

---

The Critical Impacts of Ligands on Heterogeneous Nanocatalysis: A Review

ACS Catalysis, Journal Year: 2021, Volume and Issue: 11(10), P. 6020 - 6058

Published: May 4, 2021

Ligand utilization is a necessary and powerful technique for the colloidal synthesis of nanoparticles (NPs) with controllable sizes regulated morphologies. For catalysis applications, it commonly believed that surface ligands on metal NPs block active catalytic sites reduce activity. Nevertheless, since 2010, an increasing number research groups have demonstrated unexpected benefits improve activity and/or selectivity. These can be ascribed to construction inorganic–organic interface, through which series factors, such as steric, electronic, solubility effects, utilized produce favorable changes interfacial environment. Considering tremendous developments in this emerging field, compile comprehensive systematic overview recent advances. In Review, we summarize critical impacts heterogeneous nanocatalysis. First, introduce vital roles colloid syntheses shapes. Second, detrimental effects nanocatalysis are described basis traditional views. Third, strategies ligand removal reviewed compared. Fourth, has been conducted past decade, three main beneficial (steric, solubility) classified discussed. each effect, possible corresponding mechanism presented, typical examples provided. Recent advances regarding density functional theory (DFT) calculations regulation coverage dedicated explaining ligand-promotion searching optimal nanocatalysts. Fifth, stabilities cutting-edge ligand-capped nanocatalysts before after reactions Finally, highlight remaining challenges propose future perspectives. Although much progress achieved, activities multifaceted still debatable. We hope Review will deepen readers' understanding actual catalysis.

Language: Английский

---

Water splitting performance of metal and non-metal-doped transition metal oxide electrocatalysts

Coordination Chemistry Reviews, Journal Year: 2022, Volume and Issue: 474, P. 214864 - 214864

Published: Oct. 12, 2022

Language: Английский

---

Thermo-photo catalysis: a whole greater than the sum of its parts

Chemical Society Reviews, Journal Year: 2022, Volume and Issue: 51(9), P. 3609 - 3647

Published: Jan. 1, 2022

This review provides an up-to-date understanding on emerging thermo-photo catalytic processes with emphasis the synergetic effects of thermal and photo energies.

Language: Английский

---

Intermetallic Nanocrystals for Fuel-Cells-Based Electrocatalysis

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

---

Recent Progress on Phase Engineering of Nanomaterials

Chemical Reviews, Journal Year: 2023, Volume and Issue: 123(23), P. 13489 - 13692

Published: Nov. 14, 2023

As a key structural parameter, phase depicts the arrangement of atoms in materials. Normally, nanomaterial exists its thermodynamically stable crystal phase. With development nanotechnology, nanomaterials with unconventional phases, which rarely exist their bulk counterparts, or amorphous have been prepared using carefully controlled reaction conditions. Together these methods are beginning to enable engineering (PEN), i.e., synthesis phases and transformation between different obtain desired properties functions. This Review summarizes research progress field PEN. First, we present representative strategies for direct modulation diverse kinds nanomaterials. We cover ranging from metal nanostructures such as Au, Ag, Cu, Pd, Ru, alloys; oxides, borides, carbides; transition dichalcogenides (TMDs) 2D layered review growth wet-chemical reduction seed-mediated epitaxial chemical vapor deposition (CVD), high pressure transformation, electron ion-beam irradiation. After that, summarize significant influence on various unconventional-phase also discuss potential applications developed areas including catalysis, electrochemical energy storage (batteries supercapacitors), solar cells, optoelectronics, sensing. Finally, existing challenges future directions

Language: Английский

---

Scalable and Controllable Synthesis of Pt‐Ni Bunched‐Nanocages Aerogels as Efficient Electrocatalysts for Oxygen Reduction Reaction

Advanced Energy Materials, Journal Year: 2023, Volume and Issue: 13(20)

Published: March 26, 2023

Abstract Developing efficient and stable Pt‐based oxygen reduction reaction (ORR) electrocatalysts via both economical controllable routes is critical for the practical application of electrochemical energy devices. Herein, a scalable, controllable, general ambient‐O 2 ‐involved aqueous‐solution cultivating strategy to prepare Pt x M y (M = Ni, Fe, Co) bunched‐nanocages aerogels (BNCs AG) demonstrated, based on newly established high‐M‐to‐Pt‐precursor‐ratio‐and‐B‐incorporation‐facilitated M‐rich core Pt‐rich shell hydrogel formation process. The 83 Ni 17 BNCs AG shows prominent ORR performance with mass activity (MA) 1.95 A mg −1 specific 3.55 mA cm −2 , which are 8.9‐times 9.6‐times that supported carbon (Pt/C), respectively. Particularly, displays greatly enhanced durability (MA 82.6% retention) compared Pt/C 31.8% after 20 000‐cycles accelerated test. Systematic studies including density functional theory calculations uncover excellent closely related optimized ligand strain effects content in this aerogel; outstanding endowed by lowered‐down leaching Pt/Ni ratio inhibited sintering due its appropriate porosity. This work provides new perspectives development high low cost.

Language: Английский

---

Construction of Gold/Rhodium Freestanding Superstructures as Antenna-Reactor Photocatalysts for Plasmon-Driven Nitrogen Fixation

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(11), P. 7734 - 7742

Published: March 6, 2024

Precisely controlling the architecture and spatial arrangement of plasmonic heterostructures offers unique opportunities to tailor catalytic property, whereas lack a wet-chemistry synthetic approach fabricating nanostructures with high-index facets limits their practical applications. Herein, we describe universal strategy construct Au/Rh freestanding superstructures (SSs) through selective growth ordered Rh nanoarrays on high-index-faceted Au nanobipyramids (NBPs). This works various metal nanocrystal substrates can yield diverse Pd/Rh SSs. Especially, obtained NBP/Rh SSs exhibit high photocatalytic activity toward N2 fixation as result spatially separated architecture, local electric field enhancement, antenna-reactor mechanism. Both theoretical experimental results reveal that NBPs function nanoantennas for light-harvesting generate hot charge carriers driving fixation, while serve active sites adsorption activation synergistically promote overall in work new avenues rationally designing constructing photocatalysts high-efficiency

Language: Английский

---

A review on sustainable iron oxide nanoparticles: syntheses and applications in organic catalysis and environmental remediation

Green Chemistry, Journal Year: 2024, Volume and Issue: 26(13), P. 7579 - 7655

Published: Jan. 1, 2024

In this review paper, recent developments of iron oxide nanoparticles are highlighted and discussed in the field organic catalysis environmental remediation.

Language: Английский

---

Noble Metal‐Based Multimetallic Nanoparticles for Electrocatalytic Applications

Advanced Science, Journal Year: 2021, Volume and Issue: 9(1)

Published: Nov. 17, 2021

Noble metal-based multimetallic nanoparticles (NMMNs) have attracted great attention for their multifunctional and synergistic effects, which offer numerous catalytic applications. Combined experimental theoretical studies enabled formulation of various design principles tuning the electrocatalytic performance through controlling size, composition, morphology, crystal structure nanoparticles. Despite significant advancements in field, chemical synthesis NMMNs with ideal characteristics catalysis, including high activity, stability, product-selectivity, scalability is still challenging. This review provides an overview on structure-based classification general NMMN electrocatalysts. Furthermore, postsynthetic treatments, such as removal surfactants to optimize utilization onto suitable support practical applications are highlighted. In end, future direction challenges associated electrocatalysis covered.

Language: Английский

---