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The quantitative self-assembly of mechanically interlocked molecules in water, instead of organic solvents, opens up the possibility of such systems being used in a biological context where their functions can be interfaced with biomolecular systems.
Catalytic methods are among the most valuable tools for sustainable synthesis. Domino catalysis enables multiple reactions to be combined so that synthetic efficiency may begin to approach that of nature, but significant challenges remain before this promising approach can fulfil the needs of pharmaceutical and materials chemistry.
Vision is initiated by photoisomerization of 11-cis retinal in the visual pigment rhodopsin — a fast and efficient process. Spectroscopic studies now demonstrate that the transition from the reactant photoexcited-state to the ground-state photoproduct, which mediates this important reaction, occurs on a sub-50-fs timescale and is vibrationally coherent.
Racemic or enantiomerically pure alcohols can be converted with high yield into enantiopure chiral amines in a one-pot redox-neutral cascade process by the clever combination of an alcohol dehydrogenase and an appropriate amine dehydrogenase.
Synthetic vaccines offer one method to avoid the drawbacks associated with vaccines derived from whole organisms. This Perspective highlights the improvements and significant recent progress that has been achieved in developing well-defined synthetic vaccines using a variety of molecular antigens.
The self-assembly of building blocks is an enticing route towards functional materials, yet understanding and controlling the mechanisms at play has remained challenging. Now the different morphologies and emission colours of the aggregates of a platinum(II) compound has enabled its assembly pathways into different structures to be controlled and visualized in real time.
The structural order of supramolecular assemblies typically depends on the enantiomeric purity of their building blocks. Now, a perylene bisimide (PBI) derivative has been described that assembles into a single-handed supramolecular helix, which in turn packs into domains with an identical crystalline order irrespective of the PBI's chirality. A cogwheel mechanism is proposed.
Gels formed by metal–ligand coordination typically consist of single metal ions linked together by polymer chains. Now, metal–organic cages have been used as junctions instead. A gel was prepared that features a large number of polymer chains at each junction, including loops that further serve to functionalize the material.
The isomerization of the retinal chromophore of rhodopsin is the photochemical process that initiates the sense of vision. Now, heterodyne-detected transient grating spectroscopy has been used to resolve coherent vibrational dynamics during this process, helping to identify strictly local vibrational motions as the origin of the coherent surface crossing, which occurs on a sub-50-fs timescale.
The Sustainable Development Goals adopted at a UN summit in September 2015 address many of the great challenges that our planet faces this century. Chemistry can make pivotal contributions to help realize these ambitious goals, but first it must undergo major changes in its priorities, approaches and practices.
Purely organic molecules with complex interlocked architectures have proved difficult to prepare in water. Now, a three-dimensional organic [2]catenane has been obtained in a weakly acidic aqueous solution, through an almost quantitative self-assembly process relying on dynamic hydrazone linkages. The catenane is kinetically stable in neutral and weakly basic environments.
Copper is a transition metal ion essential for the regulation of cellular oxidative stress and ATP production. Now, the inhibition of copper-trafficking proteins by a small molecule has been shown to significantly reduce proliferation of cancer cells. The results indicate that copper-trafficking proteins could represent new anti-tumour therapeutic targets.
Tridecafullerenes with 120 peripheral carbohydrate groups have been made in one step from hexakis-adducts of [60]fullerene by using azide–alkyne click chemistry. This synthetic approach offers control over the size and multivalency of these ‘sugar superballs', which are shown to be potent inhibitors of cell infection by an artificial Ebola virus, with IC50 values in the sub-nanomolar range.
Amides have historically been considered stable and unreactive functional groups because of resonance stabilization. Here, it is demonstrated that Boc-activated amides can be employed in Suzuki–Miyaura couplings using non-precious-metal catalysis. The overall reaction is complementary to the widely employed Weinreb ketone synthesis.
[Fe]-hydrogenase has an iron-guanylylpyridinol cofactor and catalyses the reversible hydrogenation of a methenyl-tetrahydromethanopterin. Now, [Fe]-hydrogenase has been reconstituted using synthetic cofactor mimics. The enzyme containing a mimic with a 2-hydroxy-pyridine group was active, whereas one containing a 2-methoxy-pyridine group was inactive. This result, together with DFT computations, supports a catalytic mechanism involving the deprotonated pyridinol hydroxy group as a proton acceptor.
Synthetic anion transporters that replace the activity of defective anion channels have been proposed as treatments for cystic fibrosis; however, it remains uncertain whether such molecules are fundamentally toxic. A series of bis- and tris-(thio)ureas capable of transporting anions have now been tested in cells expressing halide-sensitive yellow fluorescent protein. One bis-urea compound proved especially effective while showing almost no toxicity.
