Facile Synthesis of Single Iron Atoms over MoS₂ Nanosheets via Spontaneous Reduction for Highly Efficient Selective Oxidation of Alcohols

Abstract

The facile creation of high‐performance single‐atom catalysts (SACs) is intriguing in heterogeneous catalysis, especially on 2D transition‐metal dichalcogenides. An efficient spontaneous reduction approach to access atomically dispersed iron atoms supported over defect‐containing MoS2 nanosheets is herein reported. Advanced characterization methods demonstrate that the isolated iron atoms situate atop of molybdenum atoms and coordinate with three neighboring sulfur atoms. This Fe SAC delivers exceptional catalytic efficiency (1 atm O2 @ 120 °C) in the selective oxidation of benzyl alcohol to benzaldehyde, with 99% selectivity under almost 100% conversion. The turnover frequency is calculated to be as high as 2105 h−1. Moreover, it shows admirable recyclability, storage stability, and substrate tolerance. Density functional theory calculations reveal that the high catalytic activity stems from the optimized electronic structure of single iron atoms over the MoS2 support.

Iron‐Based Nanocatalysts for Electrochemical Nitrate Reduction

“…When this catalyst is used to selectively oxidize benzyl alcohol to benzaldehyde, the formed structures, which are similar to natural iron-containing enzymes, can achieve 99% selectivity at nearly 100% conversion. [171] Interestingly, in nature, nitrate reductases that catalyze the reduction of nitrate ions to nitrite ions and nitrite reductases that degrade nitrite to NO or NH 3 exist. Electron donors and transporters are required to participate in the catalytic reaction process.…”

Cobalt and Aluminum Co-Optimized 1T Phase MoS2 with Rich Edges for Robust Hydrogen Evolution Activity

“…Some defects can also be seen, which are possibly caused by the stress during the ball milling process and the Co and Al modification. As shown in Figure d, there is structural configuration of the distorted 1T phase in CA-1T-MoS 2 due to the formation of a Co–S bond and lattice mismatch, indicating that at the basal plane Co and Al atoms are likely to be coordinated to three adjacent S atoms and located above the Mo atoms. − As seen in the elemental mappings of CA-1T-MoS 2 (Figure e-i), the Co and Al elements are evenly distributed on the basal plane and rich edges of 1T-MoS 2 .…”

A Review of Transition Metal Dichalcogenides-Based Biosensors

“…Of these methods, 2D-TMDCs nanosheets can be scaled up for production under mild conditions by liquid exfoliation while achieving modification ( Yim et al, 2018 ). For example, the addition of surfactants ( Li et al, 2022b ) in aqueous solution can not only reduce the surface energy of exfoliated 2D-TMDCs nanosheets through intermolecular interactions to achieve effective exfoliation and dispersion of 2D-TMDCs, but also functionalize the surface of 2D-TMDCs nanosheets ( Yim et al, 2018 ). Therefore, this is an approach for the simultaneous exfoliation and functionalization of TMDCs in aqueous solution.…”