Hierarchically Porous (Alumino)Silicates Prepared by an Imidazole-Based Surfactant and Their Application in Acid-Catalyzed Reactions.

In this work, we developed a novel strategy to synthesize porous (alumino)silicate materials using a single structure-directing agent composed of an imidazole unit with a hydrophobic tail, namely, 1,2-dimethyl-3-hexadecyl-1H-imidazol-3-ium bromide (CdMImz). A wide range of products such as ordered mesoporous silicas, layered silica-alumina, and hierarchically porous mordenite zeolite were obtained by varying synthesis parameters such as temperature and aluminum concentration. By changing crystallization temperature, we could control the degree of silica condensation and tune the textural and morphological properties of the final materials.

Unraveling the Role of Lithium in Enhancing the Hydrogen Evolution Activity of MoS: Intercalation versus Adsorption.

Molybdenum disulfide (MoS) is a highly promising catalyst for the hydrogen evolution reaction (HER) to realize large-scale artificial photosynthesis. The metallic 1T'-MoS phase, which is stabilized via the adsorption or intercalation of small molecules or cations such as Li, shows exceptionally high HER activity, comparable to that of noble metals, but the effect of cation adsorption on HER performance has not yet been resolved. Here we investigate in detail the effect of Li adsorption and intercalation on the proton reduction properties of MoS.

Enhancing the electrocatalytic activity of 2H-WS for hydrogen evolution via defect engineering.

Transition metal dichalcogenides (TMDs), such as MoS2 and WS2, are promising alternative non-noble metal catalysts to drive the electrocatalytic H2 evolution reaction (HER). However, their catalytic performance is inherently limited by the small number of active sites as well as their poor electrical conductivity. Here, we grow vertically aligned 2H-WS2 on different substrates to expose their edge sites for the HER and introduce a scalable approach to tune these active sites via defect engineering.

Reversible Restructuring of Silver Particles during Ethylene Epoxidation.

The restructuring of a silver catalyst during ethylene epoxidation under industrially relevant conditions was investigated without and with vinyl chloride (VC) promotion. During non-VC-promoted ethylene epoxidation, the silver particles grow and voids are formed at the surface and in the bulk. Electron tomography highlighted the presence of voids below the Ag surface.

In situ structural evolution of single particle model catalysts under ambient pressure reaction conditions.

The catalytic activity of metal nanoparticles can be altered by applying strain, which changes the crystalline lattice spacing and modifies the electronic properties of the metal. Understanding the role of elastic strain during catalytic reactions is thus crucial for catalyst design. Here, we show how single highly faceted Pt nanoparticles expand or contract upon interaction with different gas atmospheres using in situ nano-focused coherent X-ray diffraction imaging.

Development of Methods for the Determination of pKa Values.

The acid dissociation constant (pKa) is among the most frequently used physicochemical parameters, and its determination is of interest to a wide range of research fields. We present a brief introduction on the conceptual development of pKa as a physical parameter and its relationship to the concept of the pH of a solution. This is followed by a general summary of the historical development and current state of the techniques of pKa determination and an attempt to develop insight into future developments.