Publications

An entry from the Cambridge Structural Database, the world’s repository for small molecule crystal structures. The entry contains experimental data from a crystal diffraction study. The deposited dataset for this entry is freely available from the CCDC and typically includes 3D coordinates, cell parameters, space group, experimental conditions and quality measures.

An entry from the Inorganic Crystal Structure Database, the world’s repository for inorganic crystal structures. The entry contains experimental data from a crystal diffraction study. The deposited dataset for this entry is freely available from the joint CCDC and FIZ Karlsruhe Access Structures service and typically includes 3D coordinates, cell parameters, space group, experimental conditions and quality measures.

Here, we show that by incorporating the polyketide triacetic acid lactone (TAL) in polydiketoenamines (PDK), we increase the working temperature of these circular plastics, opening the door wider to applications where circularity is urgently needed.

Coordinative alignment of target small molecules onto a chiral metal-organic framework (MOF-520)provides a powerful method to determine the structures of small molecules through single-crystal X-ray diffraction (SXRD). In this work, the structures of 17 molecules with eight new coordinating functionalities and varying size have been determined by this method, four of which are complex molecules being crystallized for the first time. The chirality of the MOF backbone not only enables enantioselective crystallization of chiral small molecules from a racemic mixture but also imposes diastereoselective incorporation upon achiral molecules. Crystallographic studies assisted by density functional theory (DFT) calculations indicate that the stereoselectivity of MOF-520 not exclusively comes from the steric confinement of the chiral pore environment but also from asymmetric chemical bonding of the target molecules with the framework that is able to provide sufficient energy difference between possible coordination configurations.

Glucocorticoids are extremely effective anti-inflammatory therapies, but their clinical use is limited due to severe side effects, including osteoporosis, muscle wasting, fat redistribution, and skin thinning. Here we use heavy water labeling and mass spectrometry to measure fluxes through metabolic pathways impacted by glucocorticoids. We combine these methods with measurements of body composition in corticotropin-releasing hormone (CRH)-transgenic (Tg) + mice that have chronically elevated, endogenously produced corticosterone and a phenotype that closely mimics Cushing's disease in humans. CRH-Tg + mice had increased adipose mass, adipose triglyceride synthesis, and greatly increased triglyceride/fatty acid cycling in subcutaneous and abdominal fat depots and increased de novo lipogenesis in the abdominal depot. In bone, CRH-Tg + mice had decreased bone mass, absolute collagen synthesis rates, and collagen breakdown rate. In skin, CRH-Tg + mice had decreased skin thickness and absolute collagen synthesis rates but no decrease in the collagen breakdown rate. In muscle, CRH-Tg + mice had decreased muscle mass and absolute protein synthesis but no decrease in the protein breakdown rate. We conclude that chronic exposure to endogenous glucocorticoid excess in mice is associated with ongoing decreases in bone collagen, skin collagen, and muscle protein synthesis without compensatory reduction (coupling) of breakdown rates in skin and muscle. Both of these actions contribute to reduced protein pool sizes. We also conclude that increased cycling between triglycerides and free fatty acids occurs in both abdominal and subcutaneous fat depots in CRH-Tg + mice. CRH-Tg mice have both increased lipolysis and increased triglyceride synthesis in adipose tissue.

Synthesis prediction is a key accelerator for the rapid design of advanced materials. However, determining synthesis variables such as the choice of precursor materials is challenging for inorganic materials because the sequence of reactions during heating is not well understood. In this work, we use a knowledge base of 29,900 solid-state synthesis recipes, text-mined from the scientific literature, to automatically learn which precursors to recommend for the synthesis of a novel target material. The data-driven approach learns chemical similarity of materials and refers the synthesis of a new target to precedent synthesis procedures of similar materials, mimicking human synthesis design. When proposing five precursor sets for each of 2654 unseen test target materials, the recommendation strategy achieves a success rate of at least 82%. Our approach captures decades of heuristic synthesis data in a mathematical form, making it accessible for use in recommendation engines and autonomous laboratories.

Hollow nanocrystals can be synthesized through a mechanism analogous to the Kirkendall Effect, in which pores form because of the difference in diffusion rates between two components in a diffusion couple. Starting with cobalt nanocrystals, we show that their reaction in solution with oxygen and either sulfur or selenium leads to the formation of hollow nanocrystals of the resulting oxide and chalcogenides. This process provides a general route to the synthesis of hollow nanostructures of a large number of compounds. A simple extension of the process yielded platinum-cobalt oxide yolk-shell nanostructures, which may serve as nanoscale reactors in catalytic applications.

An entry from the Cambridge Structural Database, the world’s repository for small molecule crystal structures. The entry contains experimental data from a crystal diffraction study. The deposited dataset for this entry is freely available from the CCDC and typically includes 3D coordinates, cell parameters, space group, experimental conditions and quality measures.

These findings suggest that when primed by everyday worries and concerns, individuals prone to preoccupation may have their capacity to recall emotion-related interpersonal information compromised.