Nano Research, Journal Year: 2024, Volume and Issue: 17(7), P. 5884 - 5896
Published: April 12, 2024
Language: Английский
Nano Research, Journal Year: 2024, Volume and Issue: 17(7), P. 5884 - 5896
Published: April 12, 2024
Language: Английский
Science, Journal Year: 2024, Volume and Issue: 383(6689), P. 1325 - 1331
Published: March 21, 2024
Propylene production through propane dehydrogenation (PDH) is endothermic, and high temperatures required to achieve acceptable conversions lead low selectivity severe carbon-induced deactivation of conventional catalysts. We developed a catalyst-membrane system that removes the hydrogen by-product can thus exceed equilibrium limits. In this codesigned system, silica/alumina (SiO
Language: Английский
Citations
29Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)
Published: Aug. 2, 2024
Designing highly active and stable catalytic sites is often challenging due to the complex synthesis procedure agglomeration of during high-temperature reactions. Here, we report a facile two-step method synthesize Pt clusters confined by In-modified ZSM-5 zeolite. In-situ characterization confirms that In located at extra-framework position as In+, are stabilized In-ZSM-5 The resulting in show excellent propane conversion, propylene selectivity, stability, outperforming monometallic Pt, In, bimetallic PtIn alloys. incorporation In+ neutralizes Brønsted acid inhibit side reactions, well tunes electronic properties facilitate activation desorption. strategy combining precious metal with cation-exchanged zeolites opens avenue develop heterogeneous catalysts for other reaction systems. procedures Here authors present ZSM-5, superior dehydrogenation performance.
Language: Английский
Citations
20Chemical Synthesis, Journal Year: 2025, Volume and Issue: 5(1)
Published: Jan. 11, 2025
Propane dehydrogenation (PDH) Pt-based catalysts are facing the serious challenge of coke deactivation. The locations would greatly influence formation, while detailed mechanism is not fully explored. Herein, mechanisms on different including Al2O3, Sn, Pt, and Pt-Sn sites were deeply investigated via in situ Fourier transform infrared spectroscopy (FTIR) technology, key factors triggering catalyst deactivation proposed. Excessive propyl species a crucial initial step formation coke, whether at metal or supports. These Al2O3 supports then cyclize to form monocyclic aromatic bicyclic species, those SnOx species. As for supported PtSn catalysts, strong function interaction between Pt trigger complex mechanism. surface with saturated coordination prone deposition, leading rapid stage reaction. However, low-coordination ultra-small size found be highly resistant PDH reaction, which selectively catalytic PDH. Owing metal-support interaction, extensive active hydrogen generated from can regulate precursors Furthermore, effect co-feed deposition also inhibits results higher H/C ratio (3.96) precursors. This study enhance understanding PDH, important designing efficient catalysts.
Language: Английский
Citations
4Chemical Engineering Journal, Journal Year: 2024, Volume and Issue: 484, P. 149369 - 149369
Published: Feb. 4, 2024
Language: Английский
Citations
15Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(35), P. 24358 - 24367
Published: Aug. 21, 2024
Crystalline zeolites have been proven to be excellent supports for confining subnanometric metal catalysts boost the propane dehydrogenation (PDH) reaction. However, introduced metallic species may suffer from severe sintering and limited stability during catalytic process, especially when utilizing an industrial impregnation method incorporation. In this study, we developed a new type of support based on amorphous protozeolite (PZ), taking advantage its adjustable silanol chemistry zeolitic microporous characteristic stabilizing atomically dispersed PtSn catalyst via simple, cost-effective coimpregnation process. The combination X-ray absorption spectroscopy, photoelectron in situ diffuse reflectance infrared Fourier transform spectroscopy under CO atmosphere, density functional theory calculations confirmed formation highly active Ptδ+-Ox-Sn PtSn/PZ. PtSn/PZ exhibited high conversion 45.4% propylene selectivity 99% (WHSV= 3.6 h–1, 550 °C), with apparent rate coefficient 565 molC3H6·gPt–1·h–1·bar–1 at WHSV 108 presenting top-level performance among state-of-the-art Pt-based prepared by synthesis methods. determined chemical state species, showing change sites alloy decreasing supports. This work provides general strategy using silanol-rich as various simple also offers effective way fine tailoring silanol-engineered approach.
Language: Английский
Citations
12Fuel, Journal Year: 2024, Volume and Issue: 366, P. 131429 - 131429
Published: March 11, 2024
Language: Английский
Citations
11Chemical Engineering Journal, Journal Year: 2024, Volume and Issue: 494, P. 152925 - 152925
Published: June 7, 2024
Language: Английский
Citations
10ACS Catalysis, Journal Year: 2025, Volume and Issue: unknown, P. 3215 - 3226
Published: Feb. 7, 2025
Structural transformation under in situ reaction conditions plays a vital role heterogeneous catalytic performance, especially caused by metal migration. However, the migration of active components often leads to irreversible structural disruption at high temperatures, which could be associated with deactivation catalysts. Here, we report low-melting-point Zn migration-mediated strategy synthesize ultrastable isolated PtFe3 sites anchored MFI zeolite for propane direct dehydrogenation. The optimized catalyst exhibited superior specific activity 36.5 mol C3H6 molPt–1 s–1 propylene selectivity above 99% 550 °C. Moreover, dehydrogenation remained stable after over 400 h on stream low rate constant 0.001 h–1 industrial 580 In characterizations demonstrated that Fe3+ species were conducive rearrangement electronic configuration unoccupied 5d states Pt atoms form electron-deficient sites. This afford insights into dynamic evolution preparation processes.
Language: Английский
Citations
2ACS Catalysis, Journal Year: 2023, Volume and Issue: 13(22), P. 14737 - 14745
Published: Nov. 1, 2023
Propane dehydrogenation (PDH) presents a promising alternative to naphtha steam cracking processes for propene production. However, the current commercial catalysts are plagued by toxicity of Cr (VI) and exorbitant cost Pt. We have developed an efficient, eco-friendly, cost-effective catalyst (CoOx@MFI) in which reduction-resistant CoOx clusters embedded situ into zeolite framework. This exhibits good catalytic performances (59.0% propane conversion 93.0% selectivity) PDH reactions, surpassing most Co-based competing with Pt-based ones. Crucially, both spectroscopy theoretical calculations demonstrate that MFI zeolite-stabilized Co–O moieties highly favorable C–H bond activation via O atom as Lewis base, can attach H generate [CoOH]+ intermediate remarkable efficiency.
Language: Английский
Citations
23Chemical Engineering Journal, Journal Year: 2023, Volume and Issue: 474, P. 145648 - 145648
Published: Aug. 25, 2023
Language: Английский
Citations
20