Ligand-Induced Activation of Single-Atom Palladium Heterogeneous Catalysts for Cross-Coupling Reactions

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

Published: Jan. 2, 2025

Single-atom heterogeneous catalysts (SACs) are potential, recoverable alternatives to soluble organometallic complexes for cross-coupling reactions in fine-chemical synthesis. When developing SACs these applications, it is often expected that the need ligands, which essential catalysts, can be bypassed. Contrary that, ligands remain almost always required palladium atoms stabilized on commonly used functionalized carbon and nitride supports, as otherwise show limited activity. Despite this, ligand optimization has received little attention, their role activating poorly understood. Here, we explore impact of structurally diverse phosphine performance nitrogen-doped supported single-atoms (Pd1@NC) Sonogashira–Hagihara (SH) reaction, using X-ray absorption spectroscopy density functional theory simulations rationalize observed trends. Compared ligand-free SAC, SH activity enhanced all ligand-assisted systems, with reactivity varying by up 8 orders magnitude depending choice. Distinct trends emerge based free volume class. Unlike molecular electronic effects less significant due modulating influence support. Instead, SAC-ligand systems governed a balance between deformation energy during coordination metal centers, resulting accessibility reagents. These findings offer key insights into optimizing Pd-SACs leveraging activate centers tailor 3D environment.

Language: Английский

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Palladium installed copper-organic framework for C–C coupling reactions

Science China Chemistry, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 3, 2025

Language: Английский

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A Universal In‐Situ Interfacial Growth Strategy for Various MXene‐Based van der Waals Heterostructures with Uniform Heterointerfaces: The Efficient Conversion from 3D Composite to 2D Heterostructures

Small, Journal Year: 2024, Volume and Issue: 20(45)

Published: July 27, 2024

Two-dimensional (2D) van der Waals heterostructures endow individual 2D material with the novel functional structures, intriguing compositions, and fantastic interfaces, which efficiently provide a feasible route to overcome intrinsic limitations of single components embrace distinct features different materials. However, construction uniform heterointerfaces still poses significant challenges. Herein, universal in-situ interfacial growth strategy is designed controllably prepare series MXene-based tin selenides/sulfides homogeneous heterostructures. Molten salt etching by-products that are usually recognized as undesirable impurities, reasonably utilized by us transform into nanostructures via growth. The obtained present sandwiched structures lamellar interlacing networks heterointerfaces, demonstrate efficient conversion from 3D composite Such significantly enhance charge transfer efficiency, chemical reversibility, overall structural stability in electrochemical process. Taking 2D-SnSe

Language: Английский

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Resolution of Selectivity Steps of CO Reduction Reaction on Copper by Quantum Monte Carlo

The Journal of Physical Chemistry Letters, Journal Year: 2025, Volume and Issue: unknown, P. 1494 - 1500

Published: Feb. 3, 2025

Electrochemical reduction of carbon monoxide to valuable fuels and chemicals on copper surfaces remains a challenging area in catalysis due limited understanding adsorption mechanisms reaction pathways. Although density functional theory (DFT)-based studies have investigated these processes, their accuracy varies across different functionals. Here, we present the application fixed-node diffusion Monte Carlo (FNDMC) benchmark energies CO*, H*, key CO (CORR) intermediates, COH* CHO* Cu(111) surface. Our results for CO* H* closely align with experimentally measured chemisorption reactions, highlighting limitations DFT providing site-specific energy comparisons that are often not available experimentally. Additionally, explore effect explicit solvation, demonstrating how water stabilizes over CHO*, thus suggesting critical role CORR. Finally, release our high-accuracy FNDMC benchmarks testing developing new functionals electrocatalysis. Overall, this study underscores potential detailed surface chemistry offers insights into catalytic processes.

Language: Английский

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Realizing High Stable Lithium Storage by Self-Healing Ga-Based Anode Designs

ACS Applied Electronic Materials, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 11, 2025

Language: Английский

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Revolutionizing heterogeneous catalysis: Dual-atom catalysts as the next frontier in green chemistry

Fuel, Journal Year: 2025, Volume and Issue: 396, P. 135262 - 135262

Published: April 8, 2025

Language: Английский

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Controllable preparation of carbon coating Ge nanospheres with a cubic hollow structure for high-performance lithium ion batteries

Journal of Colloid and Interface Science, Journal Year: 2024, Volume and Issue: 677, P. 655 - 664

Published: Aug. 3, 2024

Language: Английский

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Recent Advances on Non-noble Metal Catalysts toward N-ethylcarbazole Hydrogen Storage

Journal of Materials Chemistry A, Journal Year: 2024, Volume and Issue: unknown

Published: Jan. 1, 2024

This paper summarizes NEC non-noble metal hydrogenation catalysts' latest research, covering synthesis, structural features, hydrogen storage performance and development prospect. The aim is to boost catalyst research application.

Language: Английский

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