ChemCatChem最新文献

To enhance the electrochemical synthesis of ammonia performance by accelerating the reaction kinetics of electrocatalytic Nitrate reduction reaction (NO₃⁻RR), it is crucial to develop electrocatalysts with high acitiity and selectivity of NO₃⁻RR. Herein, a Ru-doped Co-Ti₃C₂ catalyst was prepared for NO₃⁻RR in this work. In 0.1 M KOH & 0.1 M KNO₃ electrolyte, the Ru doped Co-Ti₃C₂ (nRu:nCo = 2:8, RuCo-Ti₃C₂-2:8) achieved a Faraday efficiency (FE) of 96.48% and an ammonia yield of 2261.99 µg cm⁻² h⁻¹ at −0.4 V vs. RHE. Compared with the Co-MXene catalyst and the Ru doped Co-Ti₃C₂ catalysts of other compositions, RuCo-Ti₃C₂-2:8 exhibited better ammonia yield and high FE. Moreover, the RuCo-Ti₃C₂-2:8 catalyst exhibited excellent stability of electrocatalytic NO₃⁻RR.

Electrification of chemical production requires the development of innovative solutions, with plasma catalysis being among them. This perspective summarizes many years of studies and discussions made in the frame of the ERC Synergy project SCOPE dedicated to the above aspects. However, it does not aim to overview the project results but rather use them in combination with literature indications to outline the emerging trends and present gaps to pass from a research area to a key technology to develop sustainable production and associated changes required in the modalities of production. The perspective thus aims to offer a vision of the future for plasma catalysis and its role in facing societal challenges.

The precision with which atoms can be positioned in 3D space through reticular chemistry imbues metal-organic frameworks (MOFs) with the potential to access catalytic performance beyond what is possible with classical heterogeneous manifolds. In this paper, we highlight illustrative examples in which MOF-based catalysts integrate adsorption and catalysis, optimize cooperation, bypass high-energy intermediates, bring about active site regeneration, stabilize unusual active sites or use extended environment effects in order to break new ground in catalyst design.

The removal of acetylene traces from ethylene streams coming from the steamcracker is carried out in the industry on an annual scale of several million tons using Pd-Ag/Al₂O₃ catalysts. The substitution of palladium containing catalysts with more abundant, cheap, and nontoxic materials is a first crucial step toward a more sustainable chemical industry. As iron is one of the most abundant metals and can be mined in almost all regions worldwide, it is an ideal catalyst material. In this work, we present the development of α-alumina supported iron catalysts with 1, 5, and 10 wt% iron loading and their application in the selective acetylene hydrogenation under industrially applied front-end conditions. The catalysts were prepared via simple incipient wetness-impregnation and were analyzed via XRD, XRF, TPR, TEM, and N₂-physisorption. The catalysts were subsequently calcined, reduced, and tested in the selective acetylene hydrogenation. After an activation phase, the catalysts show excellent activity and selectivity in the acetylene hydrogenation at 90 °C without significant ethylene hydrogenation. The excellent catalytic activity underline the great potential of iron based catalysts as an alternative to conventional Pd-containing materials.

The Cover Feature depicts the coupling reaction of CO₂ and n-C₁₆ to CO and gasoline at the bifunctional sites of a Ni/β catalyst. In their Research Article (DOI: 10.1002/cctc.202401546), F. Shi, X. Cui, and co-workers report a promising approach to CO₂ utilization—coupling transformation of CO₂ and n-C₁₆ to gasoline. The Brønsted acid was responsible for n-C₁₆ activation, and Ni catalyzed the RWGS reaction and captured the H₂ species produced during aromatization, thereby increasing the yield of aromatics and the octane value of gasoline.

The Front Cover illustrates symmetry (nature) and chirality (chemistry). Geometry, symmetry and chirality are definitions that are closely linked. In geometry, an object has symmetry if there is an operation or transformation that maps the object onto itself. In chemistry, a molecule (or ion) is called chiral if it is distinguishable from its mirror image. In their Review (DOI: 10.1002/cctc.202400019), A. Franco and E. Barath have summarized asymmetric hydrogenation reactions (of C<C═>C and C<C═>O double bonds) using heterogeneous metal catalysts.

Catalytic pyrolysis technology has been widely used in the conversion of lignin to aromatics, but the catalysts still suffer from poor stability and low product yields due to the lack of oxygen vacancy design. In this study, we report a multi-active site synergistic strategy to enhance the cleavage of lignin aryl carbon-oxygen bonds. Pt-MoO_x/TiO₂ has a large specific surface area and pore volume, showing a significant medium mesopore size, which was favorable for trapping macromolecular oxides. Meanwhile, a significant synergistic effect was found between hydrogen-activated metallic Pt and molybdenum oxide, which both inhibited the hydrogenation of the aryl ring and promoted the dissociation of hydrogen, thus providing more active sites. More importantly, the defective oxygen vacancies played a key role in the adsorption and activation of oxygen-containing groups, facilitating the absorption of active hydrogen formed by hydrogen spillover. Under the conditions of atmospheric pressure and 400 °C, the high efficiency conversion (100%) of m-cresol was achieved, and guaranteed a high yield of aromatics (98%) and high selectivity (98%). Extending to lignin, the yield of aromatics can reach 5 wt.%. The catalyst remained highly active after 6 h of continuous operation, and there was no significant decrease in yield after two regenerations.

The catalytic oxidation of ethylene glycol (EG) on the Co₃O₄ (001) surface is investigated by AIMD simulations in the presence of a water layer for the A- and B- terminations. In addition to the surface structure and composition, the chemical state of the aqueous environment plays a crucial role in the oxidation process. Specifically, it depends on the concentration of surface hydroxyl groups, which can act both as proton donors and acceptors. Reference surfaces, which are generated by bringing the unhydrogenated A- and B-terminated surfaces in contact with a stoichiometric water layer, show some spontaneous water dissociation, which produces a number of surface hydroxyl groups. On such an A-terminated reference surface, the EG molecule is barely reactive. This holds even in a more oxidative state. On the B-terminated surface, EG's decomposition into ethylenedioxy species occurs already in the reference state. Under the more oxidative hydrogen-deficient conditions obtained by removing eight hydrogen atoms, the reaction proceeds to the formation of the two-electron oxidation product glycolaldehyde. Removal of altogether 16 hydrogen atoms facilitates the formation of four-electron oxidation products, such as glycolic acid and glyoxal and the observation of a transient H₂O₂ species, which subsequently evolves to form dioxygen.

Graphite-based catalysts, with their abundant availability, low cost, excellent electrical conductivity, and chemical stability, serve as an ideal candidate for eletrocatalytical synthesis of hydrogen peroxide (H₂O₂). This review explores the fundamental principles of H₂O₂ production via the electrochemical oxygen reduction reaction (ORR) and the theoretical basis for evaluating catalyst selectivity. It summarizes the structural characteristics, classifications, and developmental history of graphite-based catalysts, with a focus on recent advancements. The discussion highlights strategies such as heteroatom doping, defect engineering, and surface oxygen functionalization, analyzing their effectiveness in designing novel high-performance catalysts. By rationally designing catalyst components and fine-tuning the microenvironment of active sites, it is possible to develop efficient and highly stable catalysts, narrowing the gap between experimental outcomes and theoretical predictions. This work aims to advance the scalable application of graphite-based materials in green chemistry and energy fields.

We present a decarboxylative cross-dehydrogenative coupling (CDC) reaction between tetrahydroisoquinoline (THIQ) derivatives and alkynoic acids using a carbon nanotube-supported copper/nickel oxide (CNT-CuO/Ni) catalyst. This catalyst leverages the catalytic properties of copper and magnetic recoverability of nickel to facilitate efficient carbon─carbon bond formation under mild conditions while allowing for easy separation and reuse. Under optimized conditions, the reaction produced various 1-alkynyl-2-aryl-1,2,3,4-tetrahydroisoquinoline derivatives in good yields. The CNT-CuO/Ni catalyst exhibited significant reusability, retaining high catalytic performance through 12 reaction cycles. Competition experiments revealed that the electronic properties of substituents on the phenyl propiolic acid and THIQ aryl groups had a minimal effect on the reaction outcome. This study underscores the potential of CNT-CuO/Ni as a recyclable catalyst for sustainable organic synthesis in decarboxylative CDC reactions.