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The emergence of high-entropy materials affords opportunities to harmonize precision and disorder for materials design. This Review highlights the synthesis principles and strategies towards controllable and predictive fabrication of high-entropy materials with complex chemical compositions, engineered microstructures and tailored atomic configurations.
Simultaneous application of mechanical and chemical effects during materials synthesis can increase control of crystallization, but use of this strategy in preparing halide perovskite films is underexplored. Now, a method that integrates rapid chemical crystallization with mechanical shearing enables the fabrication of perovskite films with long-range crystalline order and enhanced optoelectronic properties.
Monodisperse perovskite nanocrystals are formed by using a diffusion-mediated growth mechanism that controls converted monomer concentration such that premature termination or secondary growth processes are prevented.
Grain boundary engineering, by electrodeposition and demoulding of elemental metal from a van der Waals gap, gives rise to nanosheets with high electrical anisotropy.
Inspired by pharmaceutical capsules, an extended-release shell to regulate catalyst surface reconstruction is developed, generating highly active sites and leading to enhanced CO2 electroreduction performance.
Two catalysts working together under light irradiation selectively dehydrogenate proteinogenic amino acids to yield intermediates that can be diversified into non-canonical amino acids.
Site-selective C–H bond functionalization of silanes is challenging because of the presence of multiple C–H bonds. Now, a photocatalytic method for the radical β-C(sp3)–H functionalization of silanes using the β-silicon effect is developed, enabling the aminoalkylation, alkylation and arylation of simple silanes to prepare more complex organosilicon compounds.
Digital workflow representations in automated and autonomous chemistry laboratories can achieve transferability by using abstract concepts. However, such abstractions must abide by certain rules to ensure reproducibility. Lessons learned from computer science for responsible abstraction are translated into an automated chemistry laboratory context to guide digital workflow development towards reproducibility.
Simultaneously achieving high energy and carbon efficiency in ethanol electrosynthesis is challenging. Now, an interfacial cation matrix (ICM) is developed that modifies the catalyst microenvironment to increase these performance metrics towards multicarbon products in the acidic CO2 reduction reaction. Furthermore, combining a tailored Cu–Ag catalyst with the ICM facilitates selective ethanol electrosynthesis.
Singly bonded, low-valent group 13 compounds are rare, and their reactions are typically limited to oxidative additions. Now, a compound with a singly bonded gallium(i) centre has been prepared using a sterically hindered ligand. This compound exhibits varied reactivity, undergoing both oxidative addition and redox-invariant carbometallation reactions.
Supramolecular peptide complexes with interlocking heterochiral linkers showcase a route for self-assembled nanostructures with exceptional mechanical stability.
Anisotropic gels made from supramolecular nanofibres are formed from mechanical or magnetic forces applied with orchestrated enzymatically-triggered pH changes.
Sulfur(vi) fluoride exchange and modular diazotransfer reactions have advanced click chemistry, but their mechanisms and reactivity profiles are not well understood. Now, a computational study of these reactions provides mechanistic insights and predictive reactivity models for modular diazotransfer, facilitating the development of an easy-to-prepare and -handle diazotransfer reagent with excellent reactivity.
Enantioenriched alkyl–alkyl bonds are produced from abundant alkenes in one step via Ni-catalysed asymmetric cross-hydrodimerization. This technique overcomes the reactivity and selectivity challenges associated with coupling between two similar nucleophiles.
A strategy is demonstrated for the hierarchical assembly of highly crystalline supramolecular nanotubes and tubular covalent organic frameworks (COFs), driven by cooperative dynamic covalent and coordination bonding. The pore size of the tubular COFs can be precisely controlled, and their reversible demetallation and remetallation could enable further tuning of the properties.
Aryl thianthrenium salts participate in Suzuki–Miyaura cross-coupling reactions with boronic acids. Notably, the reactions occur at low pH, facilitating the use of base-sensitive boronic acids or Lewis basic substrates.