Ultralow Pt Catalyst Loading Prepared by the Electroreduction of a Supramolecular Assembly for the Hydrogen Evolution Reaction

Abstract

The hydrogen evolution reaction (HER) from the electrocatalysis of water splitting is the most promising approach to producing green and renewable hydrogen energy for sustainable development. The precious metal platinum is the best electrocatalyst for HER. However, its scarcity and high cost still hinder the large-scale application. It is highly desirable to fabricate efficient Pt electrocatalysts with low Pt loading. Herein, we report an efficient ultralow Pt-loading HER catalyst, which was obtained by the electroreduction of a preprepared supramolecular self-assembly. Utilizing the strong hydrogen bonding formation ability of macrocyclic cucurbit[8]uril (CB[8]), a porous supramolecule (CB[8]-[PtCl6]) composed of [PtCl6]2– and CB[8] is obtained as the HER catalyst precursor. By the electroreduction of the as-prepared supramolecular compound, Pt nanoparticles (NPs) protected by CB[8] (CB[8]-Pt) exhibit high catalytic activity and excellent long-term stability toward HER with ultralow Pt loading. CB[8]-Pt with a Pt loading of only 1.2 μg/cm2 presents 23 times higher HER activity than commercial Pt/C. Moreover, CB[8]-Pt shows excellent stability under 10 000-cycle cyclic voltammetry (CV) and at least 120 h for chronopotentiometry at 10 mA/cm2 in 0.5 M H2SO4, which greatly outperforms commercial Pt/C. This work provides a strategy for the rational design of ultralow-loading Pt catalysts with good activity and stability for hydrogen production.

Robust Fluorine-Functionalized {Ln5}-Organic Frameworks for Excellent Catalytic Performance on Cycloaddition of CO2 with Epoxides and Knoevenagel Condensation

“…According to the experimental results, the structure characteristics of NUC-61Ho-a , and previous similar reports, − a plausible catalytic mechanism was proposed, as shown in Figure . First, the O atom on the epoxy compound is activated by the open Ho 3+ site in the [Ho 5 (μ 3 -OH) 6 (CO 2 ) 6 ] cluster.…”

Robust {Cd4}-Organic Framework for Efficiently Catalyzing CO2 Cycloaddition and Knoevenagel Condensation

“…Metal–organic frameworks (MOFs), as a kind of novel porous crystalline materials generated by the self-assembly of inorganic metal nodes or secondary building units (SBUs) and organic ligands through molecular self-assembly, have become one of the hotspots in the research field because of their great potential applications in catalysis, fluorescence detection, chemical sensing, gas separation-storage, proton conduction, etc., − which are decided by their high specific surface area, structural diversity, ligand modifiability, and adjustable surface properties. In recent years, research and application of nanostructured MOFs have provided a new perspective for the design of functional host frameworks, which have the following advantages: (i) the large volume cavities can accelerate mass transfer rates, thereby improving the reaction efficiency; (ii) the large specific surface area and high porosity can provide more catalytic active sites; and (iii) the tunable and easily functionalized pores can optimize the catalytic activity and selectivity. − In addition, cluster-based microporous materials constructed from polynuclear metal nodes and polydentate organic ligands are rapidly developing into research hotspots in coordination chemistry and supramolecular chemistry, not only because of their attractive structures with diverse ends but also because of their better performance in catalysis, magnetism, gas storage, and optics. − To date, although there are a great number of cluster-based microporous metal–organic host frameworks displayed by the Cambridge Structural Database, cadmium­(II)–cluster-based ones are still rarely reported, which should be attributed to the fact that the large ion radius makes the Cd 2+ ion more directionless when coordinating with organic ligands. , …”

Photocatalytic Synthesis of Ultrafine Pt Electrocatalysts with High Stability Using TiO2‐Decorated N‐Doped Carbon as Composite Support

“…Additional references cited within the Supporting Information. [30][31][32][33][34][35][36][37][38][39][40][41][42]…”