Chem Catalysis, Journal Year: 2024, Volume and Issue: 4(9), P. 101076 - 101076
Published: Aug. 20, 2024
Language: Английский
Nature Communications, Journal Year: 2023, Volume and Issue: 14(1)
Published: Nov. 6, 2023
Abstract The quest for efficient non-Pt/Pd catalysts has proved to be a formidable challenge auto-exhaust purification. Herein, we present an approach construct robust catalyst by embedding single-atom Ru sites onto the surface of CeO 2 through gas bubbling-assisted membrane deposition method. formed sites, which occupy lattice , can improve activation efficiency NO and O . Remarkably, 1 /CeO exhibits exceptional catalytic performance stability during carbon particle oxidation (soot), rivaling commercial Pt-based catalysts. turnover frequency (0.218 h −1 ) is nine-fold increase relative nanoparticle catalyst. We further show that strong interfacial charge transfer within atomically dispersed active site greatly enhances rate-determining step oxidation, resulting in substantial reduction apparent energy soot oxidation. represents toward reducing dependence on Pt/Pd-based
Language: Английский
Citations
47
Chemical Reviews, Journal Year: 2024, Volume and Issue: 124(16), P. 9457 - 9579
Published: Aug. 16, 2024
The large production volumes of commodity polyolefins (specifically, polyethylene, polypropylene, polystyrene, and poly(vinyl chloride)), in conjunction with their low unit values multitude short-term uses, have resulted a significant pressing waste management challenge. Only small fraction these is currently mechanically recycled, the rest being incinerated, accumulating landfills, or leaking into natural environment. Since are energy-rich materials, there considerable interest recouping some chemical value while simultaneously motivating more responsible end-of-life management. An emerging strategy catalytic depolymerization, which portion C-C bonds polyolefin backbone broken assistance catalyst and, cases, additional molecule reagents. When products molecules materials higher own right, as feedstocks, process called upcycling. This review summarizes recent progress for four major upcycling strategies: hydrogenolysis, (hydro)cracking, tandem processes involving metathesis, selective oxidation. Key considerations include macromolecular reaction mechanisms relative to mechanisms, design transformations, effect conditions on product selectivity. Metrics describing critically evaluated, an outlook future advances described.
Language: Английский
Citations
26
Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(15), P. 10655 - 10665
Published: April 2, 2024
While Ru-catalyzed hydrogenolysis holds significant promise in converting waste polyolefins into value-added alkane fuels, a major constraint is the high cost of noble metal catalysts. In this work, we propose, for first time, that Co-based catalysts derived from CoAl-layered double hydroxide (LDH) are alternatives efficient polyolefin hydrogenolysis. Leveraging chemical flexibility LDH platform, reveal metallic Co species serve as highly active sites Furthermore, introduced Ni framework to tackle issue restricted hydrogenation ability associated with contiguous Co–Co sites. In-situ analysis indicates integration induces electron transfer and facilitates hydrogen spillover. This dual effect synergistically enhances hydrogenation/desorption olefin intermediates, resulting reduction yield low-value CH4 27.1 12.6%. Through leveraging unique properties LDH, have developed cost-effective sustainable recycling valorization materials.
Language: Английский
Citations
22
JACS Au, Journal Year: 2024, Volume and Issue: 4(6), P. 2081 - 2098
Published: June 4, 2024
Single-use polyolefins are widely used in our daily life and industrial production due to their light weight, low cost, superior stability, durability. However, the rapid accumulation of plastic waste low-profit recycling methods resulted a global crisis. Catalytic hydrogenolysis is regarded as promising technique, which can effectively selectively convert polyolefin value-added products. In this perspective, we focus on design synthesis structurally well-defined catalysts across mesoscopic, nanoscopic, atomic scales, accompanied by insights into future directions catalyst for further enhancing catalytic performance. These principles also be applied depolymerization other polymers ultimately realize chemical upcycling plastics.
Language: Английский
Citations
9
Energy & Environmental Science, Journal Year: 2024, Volume and Issue: unknown
Published: Jan. 1, 2024
This review summarizes the research progress of single-atom catalysts (SACs) in hydrogen production and hydrogenation, proposes rational design principles SACs for hydrogenation firstly.
Language: Английский
Citations
9
Applied Catalysis B Environment and Energy, Journal Year: 2025, Volume and Issue: unknown, P. 125059 - 125059
Published: Jan. 1, 2025
Language: Английский
Citations
1
Applied Catalysis B Environment and Energy, Journal Year: 2024, Volume and Issue: 347, P. 123822 - 123822
Published: April 24, 2024
Language: Английский
Citations
8
Chemical Engineering Journal, Journal Year: 2024, Volume and Issue: 486, P. 150332 - 150332
Published: March 11, 2024
Language: Английский
Citations
7
Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(26)
Published: April 22, 2024
Catalytic upcycling of polyolefins into high-value chemicals represents the direction in end-of-life plastics valorization, but poses great challenges. Here, we report synthesis a tandem porous catalyst via micelle cascade assembly strategy for selectively catalytic cracking polyethylene olefins at low temperature. A hierarchically silica layer from mesopore to macropore is constructed on surface microporous ZSM-5 nanosheets through dynamic micelles. The outer arrays can adsorb bulky quickly by capillary and hydrophobic effects, enhancing diffusion access active sites. middle mesopores present nanoconfinement space, pre-cracking intermediates weak acid sites, which then transport zeolites micropores further strong Brønsted acidic structures, mimicking biomimetic protease clefts, ideally match steps polyolefins, thus suppressing coke formation facilitating product escape. As result, light hydrocarbons (C
Language: Английский
Citations
7
Nature Communications, Journal Year: 2023, Volume and Issue: 14(1)
Published: Aug. 29, 2023
Abstract The conversion of carbon-based solids, like non-recyclable plastics, biomass, and coal, into small molecules appears attractive from different points view. However, the strong carbon–carbon bonds in these substances pose a severe obstacle, thus—if such reactions are possible at all—high temperatures required 1–5 . Bergius process for coal to hydrocarbons requires above 450 °C 6 , pyrolysis polymers oil is also typically carried out similar 7,8 We have now discovered that efficient hydrogenation solid substrates with backbone light can be achieved room temperature by ball milling. This mechanocatalytic method surprisingly effective broad range carbon substrates, including even diamond. reaction found proceed via radical mechanism, as demonstrated presence scavengers. finding adds currently limited knowledge understanding mechanisms induced results, guided insight could induce more extended exploration broaden application scope help address problem plastic waste approach.
Language: Английский
Citations
15