Electroreduction of acetonitrile to ethylamine by thin carbon-coated copper catalysts with rich active interphases.

Thin carbon-coated copper catalysts facilitate the electroreduction of acetonitrile to ethylamine, in which a faradaic selectivity of 98% and a partial current density of 117 mA cm towards ethylamine at -0.8 V can be achieved. The carbon shells benefit the formation of rich active interfaces and suppress copper agglomeration.

Selectively Deoxygenative Deuteration of Aldehydes by Superwetting Porous Carbon-Supported Palladium Catalysts.

We present a method of deoxygenative deuteration of aldehydes (DDA) over heterogeneously superwetting porous carbon-supported palladium catalyst (Pd/SPC), which is efficient for the synthesis of deuterated aromatic compounds with -CD group. Exemplified by the DDA reaction of 2-naphthaldehyde (2-NAL) to 2-methylnaphthalene (2-MNE), the total deuterium incorporation radio in the resultant aromatic hydrocarbons was higher than 95% and the selectivity toward 2-MNE-d reached 87%. The impressed catalytic activity was found relevant to the combined effect of surface wettability and the electron-rich properties of Pd species of this kind of heterogeneous Pd/SPC catalyst.

Anomalous enhancement of humid CO capture by local surface bound water in polar carbon nanopores.

Removal of confined space carbon dioxide (CO) that is in low concentration and with coexisting water is necessary but challenging by physical adsorption method. To make the removal process effective, rendering the nanopore surface hydrophobic to resist water is the popular way. Instead of preventing water from occupying the nanopores, in this work, we propose to utilize the guest water for the spatially selective formation of local surface bound water and further induce the preferential CO capture.

Revealing an Extended Adsorption/Insertion-Filling Sodium Storage Mechanism in Petroleum Coke-Derived Amorphous Carbon.

Amorphous carbon holds great promise as anode material for sodium-ion batteries due to its cost-effectiveness and good performance. However, its sodium storage mechanism, particularly the insertion process and origin of plateau capacity, remains controversial. Here, an extended adsorption/insertion-filling sodium storage mechanism is proposed using petroleum coke-derived amorphous carbon as a multi-microcrystalline model.

Balancing the Kinetic and Thermodynamic Synergetic Effect of Doped Carbon Molecular Sieves for Selective Separation of CH/CH.

Selective separation of ethylene and ethane (CH/CH) is a formidable challenge due to their close molecular size and boiling point. Compared to industry-used cryogenic distillation, adsorption separation would offer a more energy-efficient solution when an efficient adsorbent is available. Herein, a class of CH/CH separation adsorbents, doped carbon molecular sieves (d-CMSs) is reported which are prepared from the polymerization and subsequent carbonization of resorcinol, m-phenylenediamine, and formaldehyde in ethanol solution.

pH-Regulated Refinement of Pore Size in Carbon Spheres for Size-Sieving of Gaseous C , C and C Hydrocarbon Pairs.

Selective separation of industrial important C , C and C hydrocarbon pairs by physisorbents can greatly reduce the energy intensity related to the currently used cryogenic distillation techniques. The achievement of size-sieving based on carbonaceous materials is desirable, but commonly hindered by the random structure of carbons often with a broad pore size distribution. Herein, a pH-regulated pre-condensation strategy was introduced to control the carbon pore architecture by the sp /sp hybridization of precursor.

Boosting Selective Oxidation of Ethylene to Ethylene Glycol Assisted by In situ Generated H O from O Electroreduction.

Ethylene glycol is a useful organic compound and chemical intermediate for manufacturing various commodity chemicals of industrial importance. Nevertheless, the production of ethylene glycol in a green and safe manner is still a long-standing challenge. Here, we established an integrated, efficient pathway for oxidizing ethylene into ethylene glycol.

MOF-Derived Robust and Synergetic Acid Sites Inducing C-N Bond Disruption for Energy-Efficient CO Desorption.

Amine-based scrubbing technique is recognized as a promising method of capturing CO to alleviate climate change. However, the less stability and poor acidity of solid acid catalysts (SACs) limit their potential to further improve amine regeneration activity and reduce the energy penalty. To address these challenges, here, we introduce two-dimensional (2D) cobalt-nitrogen-doped carbon nanoflakes (Co-N-C NSs) driven by a layered metal-organic framework that work as SACs.

Beyond the Selectivity-Capacity Trade-Off: Ultrathin Carbon Nanoplates with Easily Accessible Ultramicropores for High-Efficiency Propylene/Propane Separation.

Rapid and highly efficient CH/CH separation over porous carbons is seriously hindered by the trade-off effect between adsorption capacity and selectivity. Here, we report a new type of porous carbon nanoplate (CNP) featuring an ultrathin thickness of around 8 nm and easily accessible ultramicropores (approximately 5.0 Å).

Recent Advances in Carbon-Based Adsorbents for Adsorptive Separation of Light Hydrocarbons.

Light hydrocarbons (LHs) separation is an important process in petrochemical industry. The current separation technology predominantly relies on cryogenic distillation, which results in considerable energy consumption. Adsorptive separation using porous solids has received widespread attention due to its lower energy footprint and higher efficiency.

Asymmetric heterojunctions between size different 2D flakes intensify the ionic diode behaviour.

Here we report on the facile formation of asymmetric heterojunctions between laterally size different 2D flakes, which leads to a prominent gradient in charge distribution at the nanocontact interface and triggers ionic diode-like transport behaviour with a rectification ratio of 110.

Construction of Confined Bifunctional 2D Material for Efficient Sulfur Resource Recovery and Hg Adsorption in Desulfurization.

Substantial energy penalty of valuable sulfate recovery restricts the efficiency of wet desulfurization and increases the risk of Hg reemission. Although the enhanced sulfite oxidation rate with cobalt-based materials can increase the energy efficiency, inactivation and poisoning of catalyst due to the competition of reactant must be addressed. Here we obtained a superwetting two-dimensional cobalt-nitrogen-doped carbon (2D Co-N-C) nanosheet featuring confined catalysis/adsorption sites for the energy-efficient sulfite oxidation and Hg adsorption.

Ion exchange in atomically thin clays and micas.

The physical properties of clays and micas can be controlled by exchanging ions in the crystal lattice. Atomically thin materials can have superior properties in a range of membrane applications, yet the ion-exchange process itself remains largely unexplored in few-layer crystals. Here we use atomic-resolution scanning transmission electron microscopy to study the dynamics of ion exchange and reveal individual ion binding sites in atomically thin and artificially restacked clays and micas.

Wiggling Mesopores Kinetically Amplify the Adsorptive Separation of Propylene/Propane.

Adsorptive separation is an appealing technology for propylene and propane separation; however, the challenge lies in the design of efficient adsorbents which can distinguish the two molecules having very similar properties. Here we report a kinetically amplified separation by creating wiggling mesopores in structurally robust carbon monoliths. The wiggling mesopores with alternating wide and narrow segments afford a surface area of 413 m  g and a tri-modal pore size distribution centered at 1.

Nitrogen and boron doped carbon layer coated multiwall carbon nanotubes as high performance anode materials for lithium ion batteries.

Lithium ion batteries (LIBs) are at present widely used as energy storage and conversion device in our daily life. However, due to the limited power density, the application of LIBs is still restricted in some areas such as commercial vehicles or heavy-duty trucks. An effective strategy to solve this problem is to increase energy density through the development of battery materials.

Self-Pillared Ultramicroporous Carbon Nanoplates for Selective Separation of CH /N.

There is growing evidence that pillaring up a densely packed ultramicroporous two-dimensional (2D) structure is an effective strategy to reduce their internal diffusion. Reliable pillaring paradigms, however, is rather challenging. Here we report a one-pot multi-component sequential assembly method for the preparation of a new self-pillared 2D polymer and ultramicroporous carbon with integrated surface protrusions.

Proton and Li-Ion Permeation through Graphene with Eight-Atom-Ring Defects.

Defect-free graphene is impermeable to gases and liquids but highly permeable to thermal protons. Atomic-scale defects such as vacancies, grain boundaries, and Stone-Wales defects are predicted to enhance graphene's proton permeability and may even allow small ions through, whereas larger species such as gas molecules should remain blocked. These expectations have so far remained untested in experiment.

An Asymmetric Supercapacitor-Diode (CAPode) for Unidirectional Energy Storage.

A new asymmetric capacitor concept is proposed providing high energy storage capacity for only one charging direction. Size-selective microporous carbons (w<0.9 nm) with narrow pore size distribution are demonstrated to exclusively electrosorb small anions (BF ) but size-exclude larger cations (TBA or TPA ), while the counter electrode, an ordered mesoporous carbon (w>2 nm), gives access to both ions.

Understanding activity and selectivity of metal-nitrogen-doped carbon catalysts for electrochemical reduction of CO.

Direct electrochemical reduction of CO to fuels and chemicals using renewable electricity has attracted significant attention partly due to the fundamental challenges related to reactivity and selectivity, and partly due to its importance for industrial CO-consuming gas diffusion cathodes. Here, we present advances in the understanding of trends in the CO to CO electrocatalysis of metal- and nitrogen-doped porous carbons containing catalytically active M-N moieties (M = Mn, Fe, Co, Ni, Cu). We investigate their intrinsic catalytic reactivity, CO turnover frequencies, CO faradaic efficiencies and demonstrate that Fe-N-C and especially Ni-N-C catalysts rival Au- and Ag-based catalysts.

Thermal Exfoliation of Layered Metal-Organic Frameworks into Ultrahydrophilic Graphene Stacks and Their Applications in Li-S Batteries.

2D nanocarbon-based materials with controllable pore structures and hydrophilic surface show great potential in electrochemical energy storage systems including lithium sulfur (Li-S) batteries. This paper reports a thermal exfoliation of metal-organic framework crystals with intrinsic 2D structure into multilayer graphene stacks. This family of nanocarbon stacks is composed of well-preserved 2D sheets with highly accessible interlayer macropores, narrowly distributed 7 Å micropores, and ever most polar pore walls.

Hydrophilic non-precious metal nitrogen-doped carbon electrocatalysts for enhanced efficiency in oxygen reduction reaction.

Exploring the role of surface hydrophilicity of non-precious metal N-doped carbon electrocatalysts in electrocatalysis is challenging. Herein we discover an ultra-hydrophilic non-precious carbon electrocatalyst, showing enhanced catalysis efficiency on both gravimetric and areal basis for oxygen reduction reaction due to a high dispersion of active centres.