Metal-Organic Framework-Derived Ni-S/C Catalysts for Selective Alkyne Hydrogenation.

Autor: Li N; State Key Laboratory of Chemical Resource Engineering, Beijing Engineering Center for Hierarchical Catalysts, Beijing University of Chemical Technology, Beijing 100029, China.; Quzhou Institute for Innovation in Resource Chemical Engineering, Quzhou 324000, China., Weng S; State Key Laboratory of Chemical Resource Engineering, Beijing Engineering Center for Hierarchical Catalysts, Beijing University of Chemical Technology, Beijing 100029, China.; Quzhou Institute for Innovation in Resource Chemical Engineering, Quzhou 324000, China., McCue AJ; Department of Chemistry, University of Aberdeen, Aberdeen AB24 3UE, U.K., Song Y; State Key Laboratory of Chemical Resource Engineering, Beijing Engineering Center for Hierarchical Catalysts, Beijing University of Chemical Technology, Beijing 100029, China.; Quzhou Institute for Innovation in Resource Chemical Engineering, Quzhou 324000, China., He Y; State Key Laboratory of Chemical Resource Engineering, Beijing Engineering Center for Hierarchical Catalysts, Beijing University of Chemical Technology, Beijing 100029, China.; Quzhou Institute for Innovation in Resource Chemical Engineering, Quzhou 324000, China., Liu Y; State Key Laboratory of Chemical Resource Engineering, Beijing Engineering Center for Hierarchical Catalysts, Beijing University of Chemical Technology, Beijing 100029, China.; Quzhou Institute for Innovation in Resource Chemical Engineering, Quzhou 324000, China., Feng J; State Key Laboratory of Chemical Resource Engineering, Beijing Engineering Center for Hierarchical Catalysts, Beijing University of Chemical Technology, Beijing 100029, China.; Quzhou Institute for Innovation in Resource Chemical Engineering, Quzhou 324000, China., Li D; State Key Laboratory of Chemical Resource Engineering, Beijing Engineering Center for Hierarchical Catalysts, Beijing University of Chemical Technology, Beijing 100029, China.; Quzhou Institute for Innovation in Resource Chemical Engineering, Quzhou 324000, China.
Jazyk: angličtina
Zdroj: ACS applied materials & interfaces [ACS Appl Mater Interfaces] 2023 Oct 18; Vol. 15 (41), pp. 48135-48146. Date of Electronic Publication: 2023 Oct 04.
DOI: 10.1021/acsami.3c09531
Abstrakt: A carbon matrix-supported Ni catalyst with surface/subsurface S species is prepared using a sacrificial metal-organic framework synthesis strategy. The resulting highly dispersed Ni-S/C catalyst contains surface discontinuous and electron-deficient Ni δ+ sites modified by p-block S elements. This catalyst proved to be extremely active and selective for alkyne hydrogenation. Specifically, high intrinsic activity (TOF = 0.0351 s -1 ) and superior selectivity (>90%) at complete conversion were achieved, whereas an analogous S-free sample prepared by the same synthetic route performed poorly. That is, the incorporation of S in Ni particles and the carbon matrix exerts a remarkable positive effect on catalytic behavior for alkyne hydrogenation, breaking the activity-selectivity trade-off. Through comprehensive experimental studies, enhanced performance of Ni-S/C was ascribed to the presence of discontinuous Ni ensembles, which promote desorption of weakly π-bonded ethylene and an optimized electronic structure modified via obvious p-d orbital hybridization.
Databáze: MEDLINE
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