Rational Design of a Heterometallic Framework as a Highly Active Catalyst for Green Fixation of CO2 under Moderate Conditions DOI
Xinyu Tang,

Wenyu Ding,

Xin Zhang

et al.

Inorganic Chemistry, Journal Year: 2025, Volume and Issue: unknown

Published: May 22, 2025

Rational design of highly active noble-metal-free heterometallic catalysts for the green fixation CO2 into valuable chemicals is necessary and promising. Herein, a novel three-dimensional (3D) lanthanide-based copper-iodine cluster metal-organic framework has been harvested. Notably, benefiting from abundant Eu(III) [CuxIy] Lewis-acid sites (x = 4, y 3, 4), this compound reveals efficient catalytic performance (99%) cyclicity in carboxylative cyclization both propargylic alcohols amines with under extremely mild conditions (room temperature 1 bar) 6 or 1.5 h, respectively. Furthermore, simulated flue gas 13% large biological macromolecule substrates also can have good applicability, which may be attributed to synergistic effect between as well nucleophilic cocatalyst. DFT (density functional theory) further revealed activation Cu(I) on C≡C bonds amines, providing theoretical guidance preparation material conversion.

Language: Английский

Coordinated Ionic Self-Assembly of Highly Ordered Mesoporous Pt2Sn2S6 Networks for Boosted Hydrogen Evolution DOI

Sixing Yin,

Rongyao Li,

Hongfei Wu

et al.

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

Published: March 5, 2025

Metal sulfide materials, endowed with ordered mesoporosity, offer ample opportunities in a variety of renewable energy applications due to the integration intrinsic functional properties and enhanced reaction kinetics. Unfortunately, mesoporous metal sulfides have rarely been reported immense synthetic difficulties by conventional self-assembly approaches. Herein, we explore compatible coordinated ionic strategy for facile synthesis highly Pt2Sn2S6 networks templated mesopores at 4.2 nm hexagonal mesophase (space group p6mm) accessible surface area. The mechanism is further investigated, revealing role cationic surfactant anionic sulfur pair balancing suitable interaction utilized ammonia ligand retard fast precipitation source effective assembly. Owing combination porosity functionality, after crystallization exhibits excellent activity (overpotential 13 mV, Tafel slope 34 mV dec-1) long-term durability over 100 h electrochemical hydrogen evolution (HER) alkaline solution. Our study provides toolbox rational compositions as advanced model platforms future versatile technologies.

Language: Английский

Citations

0
Atomically Dispersed Tungsten Enhances CO Tolerance in Electrocatalytic Hydrogen Oxidation by Regulating the 5d-Orbital Electrons of Platinum DOI Creative Commons
Xu Zhang, Peng Yu, Di Shen

et al.

Advanced Powder Materials, Journal Year: 2025, Volume and Issue: unknown, P. 100288 - 100288

Published: March 1, 2025

Language: Английский

Citations

0
Reductive Supramolecular In Situ Construction of Nano‐Platinum Effectively Couples Cathodic Hydrogen Evolution and Anodic Alcohol Oxidation DOI Creative Commons
Rui Bai,

Qiao Ye,

Cuiyu Li

et al.

Advanced Science, Journal Year: 2025, Volume and Issue: unknown

Published: April 3, 2025

The deployment of high-performance catalysts and the acceleration anodic reaction kinetics are key measures to achieve maximum energy efficiency in overall water electrolysis hydrogen production systems. Here, an innovative strategy is developed by directly constructing a supramolecular framework embedded with boron clusters cucurbituril as reducing agent. This approach enabled situ conversion Pt⁴⁺ into highly dispersed, small-sized nano-platinum, which subsequently distributed on boron-carbon-nitrogen (BCN) matrix. resulting Pt/BNHCSs catalyst demonstrates ability facilitate electrocatalytic splitting for across multiple scenarios while simultaneously accelerating methanol oxidation kinetics, significantly outperforming commercial Pt/C various aspects. cathodic evolution-anodic coupling system constructed using greatly reduces consumption system. In attenuated total reflection Fourier transform infrared online differential electrochemical mass spectrometry reveals that interface enhances H₂O adsorption promotes CH₃OH→CO process, density functional theory calculations indicated BCN support facilitated evolution H₂ CH₃OH CO, elucidating mechanism promoted oxidation.

Language: Английский

Citations

0
Ce Clusters Enhance Ultrafine Pt Nanoparticles for Efficient Acidic Hydrogen Evolution Reaction DOI

Qiang Hu,

An‐Bang Wu,

Yongqin Shi

et al.

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

Published: April 10, 2025

Abstract Pt‐based catalysts have great potential for application in the hydrogen evolution reaction. However, developing cost‐effective, highly active, and durable electrocatalysts remains a challenge. Herein, we report facile strategy to synthesize ultrafine Pt nanoparticles (Pt‐CeCN) by Ce clusters pre‐anchored on nitrogen‐doped carbon (CN). The electronic structure of species is modulated doped Ce, which reinforces metal‐support interaction significantly enhances activity stability catalyst acidic electrolyte. resultant Pt‐CeCN exhibits overpotentials 16.3 35.6 mV at current densities 10 100 mA cm −2 , respectively. It worth noting that density reaches h under conditions. XPS analysis reveals shows lower valence state than Pt‐CN, indicating strong between atoms resulting electron‐rich nanoparticles.

Language: Английский

Citations

0
Rational Design of a Heterometallic Framework as a Highly Active Catalyst for Green Fixation of CO2 under Moderate Conditions DOI
Xinyu Tang,

Wenyu Ding,

Xin Zhang

et al.

Inorganic Chemistry, Journal Year: 2025, Volume and Issue: unknown

Published: May 22, 2025

Rational design of highly active noble-metal-free heterometallic catalysts for the green fixation CO2 into valuable chemicals is necessary and promising. Herein, a novel three-dimensional (3D) lanthanide-based copper-iodine cluster metal-organic framework has been harvested. Notably, benefiting from abundant Eu(III) [CuxIy] Lewis-acid sites (x = 4, y 3, 4), this compound reveals efficient catalytic performance (99%) cyclicity in carboxylative cyclization both propargylic alcohols amines with under extremely mild conditions (room temperature 1 bar) 6 or 1.5 h, respectively. Furthermore, simulated flue gas 13% large biological macromolecule substrates also can have good applicability, which may be attributed to synergistic effect between as well nucleophilic cocatalyst. DFT (density functional theory) further revealed activation Cu(I) on C≡C bonds amines, providing theoretical guidance preparation material conversion.

Language: Английский

Citations

0