Rational design of catalysts for heterogeneous selective hydrogenation of unsaturated aldehydes/ketones: From nanoparticles to single atoms

Deng, Mingyang; Wang, Dingsheng; Li, Yadong

doi:10.1016/j.apcata.2023.119423

Cited by 7 publications

(2 citation statements)

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“…24,25 Most researches focus on exploiting distinctive single-atom metal, coordination environment manipulation, and the underlying relationship between single-atom metal properties and catalytic reaction engineering. 26 To the best of our knowledge, studies of the effect of the curved support surface on the properties of single-atom catalysts and attendant performance are rare. Wang et al revealed that a single-atom Ni on a curved carbon surface possessed the enhanced density of states around Fermi level and improved catalytic activity for CO 2 electro-reduction reaction relative to that on a flat carbon surface.…”

Section: Introductionmentioning

confidence: 99%

“…Single-atom catalysts have drawn extensive attentions in the heterogeneous catalysis field of study due to the 100% atomic utilization efficiency, tunable coordination environment, and superior catalytic performance, bringing about the wide application in various reactions such as acetylene selective hydrogenation, alkane oxidation, and CO 2 reduction. − The catalytic performance of single-atom catalysts relies on a slew of structure factors, including the metal atom type, loading subject, coordination environment, and electronic structure. , Currently, graphitic carbon nitride (g-C 3 N 4 ) is recognized as the ideal support for anchoring and stabilizing metal species at the atomic level because of its enriched 6-fold cavities, lone-pair electrons in pyridinic nitrogen, controllable mesoporous structure, etc. , Most researches focus on exploiting distinctive single-atom metal, coordination environment manipulation, and the underlying relationship between single-atom metal properties and catalytic reaction engineering . To the best of our knowledge, studies of the effect of the curved support surface on the properties of single-atom catalysts and attendant performance are rare.…”

Section: Introductionmentioning

confidence: 99%

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Curved Surface of Graphitic Carbon Nitride Boosting Cyclohexane Oxidation over Single-Atom Catalysts

Xu,

Yu,

Shi

et al. 2024

ACS Appl. Nano Mater.

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Although single metal sites on graphitic carbon nitride (g-C3N4) are extensively employed in the catalysis field, the related study is based on the flat g-C3N4 surface model, which is far beyond the reality of the curved structure involved in g-C3N4. Herein, g-C3N4 nanorods with diameters of 9.0 and 7.0 nm are synthesized via the hard template approach to support single-atom Co for the catalytic oxidation of cyclohexane. Comprehensive characterizations, combined with theoretical calculations, find that the curved structure would broaden the space of g-C3N4 interlayers, modulate the electronic structure, and reduce the coordination number of atomic Co. The mechanism study reveals that compared with Co atoms on a flat g-C3N4 surface, the low-coordinated Co atoms anchored on a curved g-C3N4 surface are capable of enhancing the reactant adsorption and facilitating the oxygen dissociation, thereby boosting the catalytic cyclohexane oxidation. The cyclohexane conversion on resultant Co/g-C3N4-9 nm reaches up to 22.4% at the overall selectivity of above 95% under mild reaction conditions, outperforming state-of-the-art nonprecious metal-based catalysts. The present work not only offers a synthesis strategy of the effective single-atom metal catalysts for the cyclohexane oxidation but also sheds light on the origin of the enhanced catalytic performance of curved g-C3N4-based catalysts.

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Section: Introductionmentioning

confidence: 99%