Engineering ZrO-Ru interface to boost Fischer-Tropsch synthesis to olefins.

Understanding the structures and reaction mechanisms of interfacial active sites in the Fisher-Tropsch synthesis reaction is highly desirable but challenging. Herein, we show that the ZrO-Ru interface could be engineered by loading the ZrO promoter onto silica-supported Ru nanoparticles (ZrRu/SiO), achieving 7.6 times higher intrinsic activity and ~45% reduction in the apparent activation energy compared with the unpromoted Ru/SiO catalyst.

Control of metal-support interaction for tunable CO hydrogenation performance over Ru/TiO nanocatalysts.

The catalytic behavior of CO hydrogenation can be modulated by metal-support interactions, while the role of the support remains elusive. Herein, we demonstrate that the presence of strong metal-support interactions (SMSI) depends strongly on the crystal phase of TiO (rutile or anatase) and the treatment conditions for the TiO support, which could critically control the activity and selectivity of Ru-based nanocatalysts for CO hydrogenation. High CO conversion and olefin selectivity were observed for Ru/rutile-TiO (Ru/r-TiO), while catalysts supported by anatase (a-TiO) showed almost no activity.

Effective SrWO /TiO Heterojunction with Enhanced Carriers Separation and Transfer for Photocatalytic Methane Oxidation.

Photocatalytic methane oxidation to oxygenates with promising performance remains as a grand challenge due to the low productivity and severe overoxidation. Herein, SrWO /TiO heterojunction was developed for photocatalytic methane oxidation with O to liquid oxygenates ( Please replace "oxygenates" with "oxygenated")products under mild reaction conditions. The optimized SrWO /TiO catalyst exhibited high productivity of 13365 μmol/g with high selectivity of 98.

Selective Oxidation of Methane to Oxygenates using Oxygen via Tandem Catalysis.

Selective oxidation of methane to oxygenates using low-cost and environment-friendly molecular oxygen (O ) under mild reaction conditions is a promising strategy but still remains grand challenge. It is of great importance to accelerate the activation of O to generate highly active oxygen species, such as hydroxyl peroxide and hydroxyl species to improve catalytic performance for selective oxidation of methane. Selective oxidation of methane using O by coupling with in situ generation of hydrogen peroxide via tandem catalysis ensures the easy formation of active oxygen species for methane activation, leading to high oxygenates productivity under mild conditions.

Direct production of olefins from syngas with ultrahigh carbon efficiency.

Syngas conversion serves as a competitive strategy to produce olefins chemicals from nonpetroleum resources. However, the goal to achieve desirable olefins selectivity with limited undesired C1 by-products remains a grand challenge. Herein, we present a non-classical Fischer-Tropsch to olefins process featuring high carbon efficiency that realizes 80.

Green Carbon Science: Keeping the Pace in Practice.

The concept of green carbon science is to promote the goal of achieving carbon neutrality, the importance and urgency of which have been well-recognized and received worldwide attention. Carbon neutrality has become the focus of research work in many fields, and correspondingly, a growing number of papers and publications have been published over the last few years. However, since carbon neutralization is a real problem that urgently requires technical solutions, the transition from fundamental research to practical applications must be accelerated.

Recent advances in CoC-based nanocatalysts for direct production of olefins from syngas conversion.

Syngas conversion provides an important platform for efficient utilization of various carbon-containing resources such as coal, natural gas, biomass, solid waste and even CO. Various value-added fuels and chemicals including paraffins, olefins and alcohols can be directly obtained from syngas conversion the Fischer-Tropsch Synthesis (FTS) route. However, the product selectivity control still remains a grand challenge for FTS due to the limitation of Anderson-Schulz-Flory (ASF) distribution.

Highly Selective Photocatalytic Aerobic Oxidation of Methane to Oxygenates with Water over W-doped TiO.

Highly selective conversion of methane to oxygenates with O as a green oxidant remains a great challenge. It is still difficult to suppress the generation of CO (x=1, 2) as undesired by-products due to unavoidable overoxidation reaction. Hence, tungsten-doped (W-doped) TiO photocatalysts were designed with a tunable band structure for photocatalytic oxidation of methane to C oxygenates using O at low temperature (30 °C).

Tandem Catalysis for Selective Oxidation of Methane to Oxygenates Using Oxygen over PdCu/Zeolite.

Selective oxidation of methane to oxygenates with O under mild conditions remains a great challenge. Here we report a ZSM-5 (Z-5) supported PdCu bimetallic catalyst (PdCu/Z-5) for methane conversion to oxygenates by reacting with O in the presence of H at low temperature (120 °C). Benefiting from the co-existence of PdO nanoparticles and Cu single atoms via tandem catalysis, the PdCu/Z-5 catalyst exhibited a high oxygenates yield of 1178 mmol g  h (mmol of oxygenates per gram Pd per hour) and at the same time high oxygenates selectivity of up to 95 %.

Catalytic cycle of the partial oxidation of methane to methanol over Cu-ZSM-5 revealed using DFT calculations.

Density functional theory (DFT) calculations were performed to investigate the catalytic cycle of methane conversion to methanol over both [Cu2(O2)]2+ and [Cu2(μ-O)]2+ active sites in the Cu-ZSM-5 catalyst. The [Cu2(O2)]2+ site is found to be active for the partial oxidation of methane to methanol, and although it has a higher energy barrier in the methane activation step, it involves a very low energy barrier in the methanol formation step (36.3 kJ mol-1) as well as a lower methanol desorption energy (52.

Cobalt Carbide Nanocatalysts for Efficient Syngas Conversion to Value-Added Chemicals with High Selectivity.

Syngas conversion is a key platform for efficient utilization of various carbon-containing resources including coal, natural gas, biomass, organic wastes, and even CO. One of the most classic routes for syngas conversion is Fischer-Tropsch synthesis (FTS), which is already available for commercial application. However, it still remains a grand challenge to tune the product distribution from paraffins to value-added chemicals such as olefins and higher alcohols.

Cu single-atoms embedded in porous carbon nitride for selective oxidation of methane to oxygenates.

Cu single atoms embedded in the CN (Cu-SAs/CN) matrix exhibited high activity with 95% oxygenate selectivity for the direct conversion of methane at ambient temperature. The presence of abundant anchoring sites in CN led to highly dispersed Cu-N moieties, which were suggested to be the underlying active sites for methane conversion.

Gamma-Ray Irradiation to Accelerate Crystallization of Mesoporous Zeolites.

Gamma-ray (γ-ray) irradiation was introduced into zeolite synthesis. The crystallization process of zeolite NaA, NaY, Silicalite-1, and ZSM-5 were greatly accelerated. The crystallization time of NaA zeolite was significantly decreased to 18 h under γ-ray irradiation at 20 °C, while more than 102 h was needed for the conventional process.

Enhancing CO methanation over a metal foam structured catalyst by electric internal heating.

We develop an electric internal heating method based on a Ni-foam structured catalyst for CO2 methanation, in which the Joule heat generated by electric current passing through the catalyst drives the reaction. Compared with the conventional external heating method, EIH significantly enhances the catalytic activity and anti-poisoning ability of the catalyst.

Selective Transformation of CO and H into Lower Olefins over In O -ZnZrO /SAPO-34 Bifunctional Catalysts.

Because lower olefins (C -C ) are important bulk petrochemicals, their direct production from CO hydrogenation is highly attractive. However, the selectivity towards C -C by the modified Fischer-Tropsch synthesis is restricted to 56.7 % with high undesired methane selectivity.

In situ XAFS study on the formation process of cobalt carbide by Fischer-Tropsch reaction.

Fischer-Tropsch (F-T) synthesis is an effective approach to convert the syngas of H and CO into lower olefin and other valuable products for the chemical industry. Cobalt carbide (CoC), which was regarded as the sign of activity loss in the past, has recently been recognized as a highly-active phase for F-T synthesis. However, systematic study on the formation process of CoC by F-T reaction is still lacking.

Direct Production of Higher Oxygenates by Syngas Conversion over a Multifunctional Catalyst.

Selective synthesis of higher oxygenates (linear α-alcohols and α-aldehydes, C OH) from syngas is highly attractive but remains challenging owing to the low C OH selectivity and low catalytic stability. Herein we introduce a multifunctional catalyst composed of CoMn and CuZnAlZr oxides that dramatically increased the oxygenates selectivity to 58.1 wt %, where more than 92.

Direct production of olefins syngas conversion over CoC-based catalyst in slurry bed reactor.

Direct production of olefins syngas conversion over a CoC-based catalyst was investigated in a slurry bed reactor (SBR). It was found that the total selectivities to olefins and oxygenates reached 88.8C% at a CO conversion of 29.

Direct conversion of CO into liquid fuels with high selectivity over a bifunctional catalyst.

Although considerable progress has been made in carbon dioxide (CO) hydrogenation to various C chemicals, it is still a great challenge to synthesize value-added products with two or more carbons, such as gasoline, directly from CO because of the extreme inertness of CO and a high C-C coupling barrier. Here we present a bifunctional catalyst composed of reducible indium oxides (InO) and zeolites that yields a high selectivity to gasoline-range hydrocarbons (78.6%) with a very low methane selectivity (1%).

Cobalt carbide nanoprisms for direct production of lower olefins from syngas.

Lower olefins-generally referring to ethylene, propylene and butylene-are basic carbon-based building blocks that are widely used in the chemical industry, and are traditionally produced through thermal or catalytic cracking of a range of hydrocarbon feedstocks, such as naphtha, gas oil, condensates and light alkanes. With the rapid depletion of the limited petroleum reserves that serve as the source of these hydrocarbons, there is an urgent need for processes that can produce lower olefins from alternative feedstocks. The 'Fischer-Tropsch to olefins' (FTO) process has long offered a way of producing lower olefins directly from syngas-a mixture of hydrogen and carbon monoxide that is readily derived from coal, biomass and natural gas.

Synthesis of Co-based bimetallic nanocrystals with one-dimensional structure for selective control on syngas conversion.

Co-based bimetallic nanocrystals with one-dimensional (1D) branches were synthesized by the heterogeneous nucleation of Co atoms onto prenucleated seeds, such as Pd or Cu, through a facile wet-chemical route. The peripheral branches (rod-like) of the Co-Pd and Co-Cu nanocrystals were outspread along the (001) direction and were enclosed by (101) facets. By switching the prenucleated metals to form robust Co-Pd or Co-Cu bimetallic nanocatalysts, the selectivity of CO hydrogenation could be adjusted purposely towards heavy paraffins, light olefins or oxygenates.

Hierarchically nanoporous ceria nanoparticles with a high-surface area: synthesis, characterization, and their catalytic activity.

A redox route based on ethylene glycol mediated process was developed to synthesize hierarchically nanoporpous ceria nanoparticles (ceria HNPNPs). The synthesized ceria HNPNPs are composed of building blocks fabricated with cubic ceria nanocrystals of several nanometers in diameter. Scanning electron microscopy was performed to investigate the evolution process of ceria precursor, and a two-step growth process was suggested for the morphology evolution.

Facile synthesis of nanoporous anatase spheres and their environmental applications.

Highly nanoporous TiO(2) (anatase) spheres with an excellent ability in environmental applications have been successfully prepared via in situ hydrolysis of titanium glycolate precursor spheres.