New horizon in C1 chemistry: breaking the selectivity limitation in transformation of syngas and hydrogenation of CO₂into hydrocarbon chemicals and fuels

Chemical Society Reviews, Journal Year: 2019, Volume and Issue: 48(12), P. 3193 - 3228

Published: Jan. 1, 2019

Catalytic transformations of syngas (a mixture H2 and CO), which is one the most important C1-chemistry platforms, CO2, a greenhouse gas released from human industrial activities but also candidate abundant carbon feedstock, into chemicals fuels have attracted much attention in recent years. Fischer-Tropsch (FT) synthesis classic route chemistry, product selectivity FT limited by Anderson-Schulz-Flory (ASF) distribution. The hydrogenation CO2 C2+ hydrocarbons involving C-C bond formation encounters similar limitation. present article focuses on advances breaking limitation using reaction coupling strategy for both CO hydrocarbons, include key building-block chemicals, such as lower (C2-C4) olefins aromatics, liquid fuels, gasoline (C5-C11 hydrocarbons), jet fuel (C8-C16 hydrocarbons) diesel (C10-C20 hydrocarbons). design development novel bifunctional or multifunctional catalysts, are composed metal, metal carbide oxide nanoparticles zeolites, to beyond will be reviewed. factors controlling catalytic performances, catalyst component, acidity mesoporosity zeolite proximity between metal/metal carbide/metal zeolite, analysed provide insights designing efficient catalysts. mechanism, particular activation pathway intermediate, discussed deep understanding chemistry new C1 routes synthesis.

Language: Английский

---

Cooperative Coupling of Oxidative Organic Synthesis and Hydrogen Production over Semiconductor-Based Photocatalysts

Chemical Reviews, Journal Year: 2021, Volume and Issue: 121(21), P. 13051 - 13085

Published: Aug. 11, 2021

Merging hydrogen (H2) evolution with oxidative organic synthesis in a semiconductor-mediated photoredox reaction is extremely attractive because the clean H2 fuel and high-value chemicals can be coproduced under mild conditions using light as sole energy input. Following this dual-functional photocatalytic strategy, dreamlike pathway for constructing C–C/C–X (X = C, N, O, S) bonds from abundant readily available X–H bond-containing compounds concomitant release of fulfilled without need external chemical reagents, thus offering green fascinating synthetic strategy. In review, we begin by presenting concise overview on general background traditional production then focus fundamental principles cooperative coupling selective simultaneous utilization photoexcited electrons holes over semiconductor-based catalysts to meet economic sustainability goal. Thereafter, put dedicated emphasis recent key progress various transformations, including alcohol oxidation, methane conversion, amines coupling, cross-coupling, cyclic alkanes dehydrogenation, reforming lignocellulosic biomass, so on. Finally, remaining challenges future perspectives flourishing area have been critically discussed. It anticipated that review will provide enlightening guidance rational design such system, thereby stimulating development economical environmentally benign solar generation value-added fine chemicals.

Language: Английский

---

Hydrophobic zeolite modification for in situ peroxide formation in methane oxidation to methanol

Science, Journal Year: 2020, Volume and Issue: 367(6474), P. 193 - 197

Published: Jan. 10, 2020

Confining peroxide to make methanol In principle, hydrogen would be an efficient oxidant for the conversion of methane under mild conditions. practice, however, it is currently too expensive produce ahead time this purpose. Jin et al. report a catalyst system that generates and concentrates immediate reaction with methane. A hydrophobically coated zeolite keeps close gold palladium active site, where incoming then selectively oxidized methanol. Science , issue p. 193

Language: Английский

---

Electrocatalytic Refinery for Sustainable Production of Fuels and Chemicals

Angewandte Chemie International Edition, Journal Year: 2021, Volume and Issue: 60(36), P. 19572 - 19590

Published: Feb. 19, 2021

Abstract Compared to modern fossil‐fuel‐based refineries, the emerging electrocatalytic refinery (e‐refinery) is a more sustainable and environmentally benign strategy convert renewable feedstocks energy sources into transportable fuels value‐added chemicals. A crucial step in conducting e‐refinery processes development of appropriate reactions optimal electrocatalysts for efficient cleavage formation chemical bonds. However, compared well‐studied primary (e.g., O 2 reduction, water splitting), mechanistic aspects materials design complex are yet be settled. To address this challenge, herein, we first present fundamentals heterogeneous electrocatalysis some reactions, then implement these establish framework by coupling situ generated intermediates (integrated reactions) or products (tandem reactions). We also set principles strategies efficiently manipulate reaction pathways.

Language: Английский

---

Direct Methane Conversion under Mild Condition by Thermo-, Electro-, or Photocatalysis

Chem, Journal Year: 2019, Volume and Issue: 5(9), P. 2296 - 2325

Published: May 27, 2019

Language: Английский

---

Room-Temperature Methane Conversion by Graphene-Confined Single Iron Atoms

Chem, Journal Year: 2018, Volume and Issue: 4(8), P. 1902 - 1910

Published: June 19, 2018

Language: Английский

---

Selective Activation of Methane on Single-Atom Catalyst of Rhodium Dispersed on Zirconia for Direct Conversion

Journal of the American Chemical Society, Journal Year: 2017, Volume and Issue: 139(48), P. 17694 - 17699

Published: Nov. 10, 2017

Direct methane conversion into value-added products has become increasingly important. Because of inertness methane, cleaving the first C–H bond been very difficult, requiring high reaction temperature on heterogeneous catalysts. Once becomes activated, remaining bonds are successively dissociated metal surface, hindering direct chemicals. Here, a single-atom Rh catalyst dispersed ZrO2 surface synthesized and used for selective activation methane. The single atomic nature was confirmed by extended X-ray fine structure analysis, electron microscopy images, diffuse reflectance infrared Fourier transform spectroscopy. A model Rh/ZrO2 constructed density functional theory calculations, it shown that CH3 intermediates can be energetically stabilized catalyst. performed using H2O2 in aqueous solution or O2 gas phase as oxidants. Whereas nanoparticles produced CO2 only, methanol ethane phase.

Language: Английский

---

Metal-organic framework-based heterogeneous catalysts for the conversion of C1 chemistry: CO, CO2 and CH4

Coordination Chemistry Reviews, Journal Year: 2019, Volume and Issue: 387, P. 79 - 120

Published: Feb. 19, 2019

Language: Английский

---

Synergy of Single-Atom Ni₁ and Ru₁ Sites on CeO₂ for Dry Reforming of CH₄

Journal of the American Chemical Society, Journal Year: 2019, Volume and Issue: 141(18), P. 7283 - 7293

Published: April 25, 2019

Heterogeneous catalysis performs on specific sites of a catalyst surface even if many catalysts during could not be identified readily. Design by managing catalytic an atomic scale is significant for tuning performance and offering high activity selectivity at relatively low temperature. Here, we report synergy effect two sets single-atom (Ni1 Ru1) anchored the CeO2 nanorod, Ce0.95Ni0.025Ru0.025O2. The this catalyst, Ce0.95Ni0.025Ru0.025O2, consists which are highly active reforming CH4 using CO2 with turnover rate producing 73.6 H2 molecules each site per second 560 °C. Selectivity temperature 98.5%. Ni1 Ru1 Ce0.95Ni0.025Ru0.025O2 remain singly dispersed in cationic state up to 600 play synergistic role, evidenced lower apparent activation barrier higher production CO contrast Ce0.95Ni0.05O2 only Ce0.95Ru0.05O2 sites. Computational studies suggest molecular mechanism observed effects, originate (1) different roles terms activations form dissociation site, respectively (2) sequential role first forming H atoms through then coupling site. These effects same demonstrated new method designing

Language: Английский

---

Confinement Catalysis with 2D Materials for Energy Conversion

Advanced Materials, Journal Year: 2019, Volume and Issue: 31(50)

Published: Aug. 7, 2019

Abstract The unique electronic and structural properties of 2D materials have triggered wide research interest in catalysis. lattice the interface between covers other substrates provide intriguing confinement environments for active sites, which has stimulated a rising area “confinement catalysis with materials.” Fundamental understanding will favor rational design high‐performance nanocatalysts. Confinement found extensive applications energy‐related reaction processes, especially conversion small molecules such as O 2 , CH 4 CO, CO H O, 3 OH. Two representative strategies, i.e., lattice‐confined single atoms cover‐confined metals, been applied to construct catalytic systems superior activity stability. Herein, recent advances design, applications, structure–performance analysis two are summarized. different routes tuning states catalysts highlighted perspectives on toward energy utilization future provided.

Language: Английский

---