Articles in 2023

Therapeutic proteins have great potential for the treatment of various diseases, however, achieving high delivery efficiency remains challenging. Here, the authors develop a complex coacervate system formed via the phase separation of anionic metabolite NADPH with a short arginine-rich peptide, and apply it to the redox-responsive drug delivery of therapeutic proteins.

The binding interaction between the Shelterin complex protein TPP1 and the human telomerase enzyme can trigger telomerase maintenance, however, the conformational change of TPP1 functional for binding remains underexplored. Here, the authors characterize the structural properties of a group of amino acids named the TEL-patch within TPP1’s oligosaccharide/oligonucleotide-domain by molecular dynamics simulation, time-series analyses, and graph-based networks, revealing their conformational plasticity and allosteric communication networks.

Copalyl diphosphate synthases (CPSs) catalyze the crucial cyclization step in labdane diterpene biosynthesis to generate stereochemically distinct copalyl diphosphates (CPPs), however, the stereoselectivity within CPSs remains underexplored. Here, the authors report the 3D structure and oligomeric properties of syn-CPS from Oryza sativa, which originally produces syn-CPP but also ent-CPP after mutagenesis.

PUFA-plasmalogens show neuroprotective properties via the stimulation of CREB activation, however, their efficiency is limited by low bioavailabilities. Here, the authors develop PUFA-plasmalogen-loaded liquid crystalline lipid-peptide nanoparticles to achieve sustained CREB activation in an in vitro neurodegeneration model.

Polyurethanes find versatile applications in our daily lives, e.g., as coatings, foams and adhesives, but non-hazardous synthesis routes with renewable feedstocks are urgently needed. Here, the authors report an organocatalytic synthesis route towards non-isocyanate polyurethanes using terpenes as renewable starting materials.

Organic π-conjugated radicals have recently joined the ranks of high-efficiency light-emitting materials, however, their light-emission mechanism is still a matter of debate. Here, the authors highlight a recently proposed luminescent enhancement mechanism and record-breaking efficiency of a radical organic light-emitting diode.

Cathepsin D (CatD) is an aspartic acid protease involved in the immune response of macrophages to bacterial infection, and the development of pH insensitive CatD probes is vital in order to detect its activity across multiple cellular components. Here, the authors develop a water soluble and pH insensitive FRET-based fluorescent probe for the sensitive detection of CatD.

Single-atom catalysts (SACs) are highly promising materials for applications such as electrocatalytic water splitting, but coordination geometries around catalyst centers remain the subject of debate. Here, the authors use spin-polarized ab initio molecular dynamics simulations to compare the aqueous reactivities of iron porphyrin and iron pyridine SACs embedded in graphene, and predict the interfacial water dissociative adsorption mechanism under a moderate electric field for an iron porphyrin SAC.

Modelling the structural transitions of flexible metal-organic frameworks provides key insight into their breathing behaviours, but molecular dynamics simulations performed to date do not typically account for finite size and surface effects affecting the phase transition mechanism. Here, the authors present an approach that allows for the analysis and control of the volume of finite-size structures during molecular dynamics simulations, using a tetrahedral tessellation of nanocrystallite volume.

PAPP-A and PAPP-A2 are two isoforms of pregnancy-associated plasma protein A that cleave insulin-like growth factor binding proteins (IGFBPs) to modulate insulin-like growth factor signaling, however the structure and function of PAPP-A2 remain underexplored. Here, the authors report the cryo-EM structure of PAPP-A2, computational modeling of the PAPP-A2/IGFBP5 complex, and biochemical studies that reveal unique structural features and a lower IGFBP5 cleaving efficiency compared with PAPP-A.

To meet the rising demand for sustainable and simple polymer syntheses, organocatalytic polymerizations are a powerful tool. Here, the authors report the quasi-alternating polymerization of oxirane monomers at room temperature and in solvent-free conditions catalyzed by potassium acetate complexed by 18-crown-6 ether, leading to well-defined polyethers with varied comonomer content and low dispersity values.

Pupils with vision impairment face significant challenges in learning science. Here, the authors discuss the impact of an inaccessible curriculum and new ideas that can improve accessibility.

Traditional peptide synthesis iteratively elongates the chain from the C-terminus to the N-terminus (C-to-N), however, this process requires excess N-carbamate-protected amino acids and condensation reagents to minimize epimerization. Here, the authors report an alternative N-to-C elongation strategy by catalytic peptide thioacid formation and oxidative peptide bond formation without requiring condensation reagents and excessive protecting group manipulations.

Iron(III) molybdate is a commercial catalyst for selective oxidations such as oxidative dehydrogenation of methanol, but our understanding of the involved (sub)surface and bulk conversion processes remains limited. Here, the authors use modulation excitation IR, operando impedance, and multiwavelength Raman spectroscopy to show the mode of operation of this important catalyst.

Designing peptides that bind to specific protein targets is crucial for peptidic drug development, however, traditional computer-aided binder design is outperformed by AlphaFold2. Here, the authors develop a peptide binder designing tool by combining Foldseek, ESM-IF1 and AlphaFold2 to increase the success rate.

On-surface synthesis is a key tool to access low dimensional carbon-based nanomaterials with atomic precision. Here, the authors synthesize a nitrogen-doped nanographene structure with an [18]annulene pore on Ag(111) through sequential debromination, aryl–aryl coupling, cyclodehydrogenation and C–N coupling reactions from a 3,12-dibromo-7,8-diaza[5]helicene precursor.

Heterotopic ossification (HO) is the pathological formation of bone in soft tissues involving hydroxyapatite (HA) formation in vivo, however, the exact mechanism of HA formation remains debated. Here, the authors demonstrate the chemical mapping of human HO and the transformation of amorphous calcium carbonate in physiological conditions and reveal the role of ATP in bone mineralisation.

Dry reforming of methane (DRM) is a promising method for sustainable valorisation of methane and carbon dioxide, but its application is hampered by sintering of the active catalytic phase and coke formation. Here, the authors study DRM with non-noble metal atoms in supported gallium-rich liquid alloys which suppress both catalyst sintering and coke formation.

Volatile organic compounds are found on a majority of surfaces where they change surface properties and act as reactants, however, their diffusion flow rates remain undetermined. Here, the authors show that isoprene travels approximately 1 μm/s on zirconia under ultrahigh vacuum and is polymerized by an electron beam.

Networks of interacting DNA oligomers have various applications in molecular biology, chemistry and materials science, however, kinetic dispersions during DNA hybridization can be problematic for some applications. Here, the authors reveal that limiting unnecessary duplexes using in-silico optimization can reduce in-vitro kinetic dispersions by as much as 96%.