Non-oxidative dehydrogenation of propane is a highly efficient approach for industrial preparation of propene that is commonly catalyzed by noble Pt or toxic Cr catalysts and suffers from coking. In this work, ferric catalyst confined in a zeolite framework was synthesized by a hydrothermal procedure. The isolated Fe in the framework formed distorted tetrahedra, which were beneficial for the selective dehydrogenation of propane and reached over 95 % propene selectivity and over 99 % total olefins selectivity. This catalyst had a silanol-free structure and was oxygen tolerant, hydrothermally stable, and coke free, with a deactivation constant of 0.01 h . This study provided guidance for the synthesis of structural heteroatomic zeolite and efficient propane non-oxidative dehydrogenation over early transition metals.
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http://dx.doi.org/10.1002/anie.202305915 | DOI Listing |
Nat Commun
December 2024
Key Laboratory of Urban Pollutant Conversion, Institute of Urban Environment, Chinese Academy of Sciences, Xiamen, China.
The emergence of single-atom catalysts offers exciting prospects for the green production of hydrogen peroxide; however, their optimal local structure and the underlying structure-activity relationships remain unclear. Here we show trace Fe, up to 278 mg/kg and derived from microbial protein, serve as precursors to synthesize a variety of Fe single-atom catalysts containing FeNO (1 ≤ x ≤ 4) moieties through controlled pyrolysis. These moieties resemble the structural features of nonheme Fe-dependent enzymes while being effectively confined on a microbe-derived, electrically conductive carbon support, enabling high-current density electrolysis.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
December 2024
Shenzhen University, Chemistry, Nanhai Ave 3688, 518060, Shenzhen, CHINA.
The high entropy alloy (HEA) possesses distinctive thermal stability and electronic characteristics, which exhibits substantial potential for diverse applications in electrocatalytic reactions. However, accurately controlling the size of HEA still remains a challenge, especially for the ultrasmall HEA nanoparticles. Herein, we firstly calculate and illustrate the size impact on the electronic structure of HEA and the adsorption energies of crucial intermediates in typical electrocatalytic reactions, such as the hydrogen evolution reaction (HER), oxygen reduction reaction (ORR), CO2 electroreduction (CO2RR) and NO3- electroreduction (NO3RR).
View Article and Find Full Text PDFAngew Chem Int Ed Engl
December 2024
Huazhong University of Science and Technology, School of Chemistry and Chemical Engineering, Luoyu Road 1037, 430074, Wuhan, CHINA.
Low-iridium acid-stabilized electrocatalysts for efficient oxygen evolution reaction (OER) are crucial for the market deployment of proton exchange membrane (PEM) water electrolysis. Manipulating the in situ reconstruction of Ir-based catalysts with favorable kinetics is highly desirable but remains elusive. Herein, we propose an atomic ordering strategy to modulate the dynamic surface restructuring of catalysts to break the activity/stability trade-off.
View Article and Find Full Text PDFSmall
December 2024
School of Chemistry, Dalian University of Technology, Dalian, 116024, China.
Confinement of metal species in porous supports is an effective strategy to optimize hydrogenation performance ascribing to tunable nanopore environments. However, only focusing on the electronic structure modulation for metal species has limited the design of improved catalysts. Herein, spatial confinement strategy is reported for constructing ultrasmall metal clusters in nitro-bonded COF (M@TpPa-NO, M = Pd, Pt, Ru, Rh, Ir).
View Article and Find Full Text PDFInorg Chem
December 2024
Guizhou Provincial Key Laboratory of Green Chemical and Clean Energy Technology, School of Chemistry and Chemical Engineering, Guizhou University, Guiyang, Guizhou 550025, China.
The combination of the electrocatalytic glycerol oxidation reaction (GOR) with the cathodic hydrogen evolution reaction serves to reduce the anodic overpotential, thereby facilitating the efficient production of hydrogen. However, the GOR is confined to a narrow potential range due to the competition of the oxygen evolution reaction (OER) at high potential. Therefore, it is necessary to develop a catalyst with a high Faraday efficiency of formate (FE) over a wide potential range.
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