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Extending carbon chemistry at high-pressure by synthesis of CaC2 and Ca3C7 with deprotonated polyacene- and para-poly(indenoindene)-like nanoribbons
The authors demonstrate that carbides with infinite chains of fused [C6] and [C5] rings are synthesized at deep planetary pressures and temperatures. Hydrolysis of these carbides may lead to polycyclic aromatic hydrocarbons in the Universe.
- Saiana Khandarkhaeva
- , Timofey Fedotenko
- & Leonid Dubrovinsky
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Stabilization of N6 and N8 anionic units and 2D polynitrogen layers in high-pressure scandium polynitrides
The authors discover high-pressure Sc2N6, Sc2N8, and ScN5 polynitrides, synthesized at high pressure and temperature conditions, featuring a unique nitrogen catenation and previously unknown N66− anions, N86− anions and anionic corrugated 2D-polynitrogen layers.
- Andrey Aslandukov
- , Alena Aslandukova
- & Leonid Dubrovinsky
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Article
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Mechanochemical synthesis of organoselenium compounds
While the reported methods for the synthesis of organoselenium compounds mainly employ preformed activated selenium reagents, the direct utilization of elemental selenium in the synthesis is a more attractive but challenging strategy. Here, the authors report the rapid synthesis of versatile organoselenium compounds via mechanical stimulation.
- Shanshan Chen
- , Chunying Fan
- & Xiaofeng Wei
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Article
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Total wash elimination for solid phase peptide synthesis
Peptide drug manufacturing commonly uses large amounts of hazardous solvents primarily due to multiple washings after each step. Here, the authors introduce the concept of a completely wash-free methodology that enables up to 95% waste reduction.
- Jonathan M. Collins
- , Sandeep K. Singh
- & Christopher L. Houser
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Suppression of alpha-carbon racemization in peptide synthesis based on a thiol-labile amino protecting group
During solid-phase peptide synthesis (SPPS) inherent side reactions of the protected amino acids such as α-C racemization generate by-products that are hard to remove. Here, the authors report thiol-labile amino protecting group for SPPS, DNPBS group, which suppresses the main side reactions observed during conventional SPPS.
- Yifei Zhou
- , Hongjun Li
- & Chuanzheng Zhou
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Li3TiCl6 as ionic conductive and compressible positive electrode active material for all-solid-state lithium-based batteries
An ideal positive electrode for all-solid-state Li batteries should be ionic conductive and compressible. However, this is not possible with state-of-the-art metal oxides. Here, the authors demonstrate the use of an ionic conductive metal chloride as compressible positive electrode active material.
- Kai Wang
- , Zhenqi Gu
- & Cheng Ma
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Thiocarbazate building blocks enable the construction of azapeptides for rapid development of therapeutic candidates
The rapid protease degradation of peptides is currently limiting their therapeutic utility. Here, the authors report functionalised thiocarbazate scaffolds as precursors of aza-amino acids that can be integrated in peptide sequences, extending their bioavailability, and demonstrate this on FSSE/P5779 and bradykinin.
- Ahmad Altiti
- , Mingzhu He
- & Yousef Al-Abed
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Self-regeneration of supported transition metals by a high entropy-driven principle
Sintering of supported transition metal catalysts is problematic for high-temperature catalysis. Here the authors report entropy-driven, self-regeneration of high entropy oxide nanoparticles, promoting better stability and in situ reversible exsolution-dissolution process in multi-redox cycles.
- Shengtai Hou
- , Xuefeng Ma
- & Sheng Dai
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Mechanochemical transformation of planar polyarenes to curved fused-ring systems
The transformation of planar aromatic molecules into non-planar structures is a challenging task and has not been realized by mechanochemistry before. Here, the authors demonstrate that mechanochemical forces can transform a planar polyarene into a curved geometry by creating new C-C bonds along the rim of the molecular structure.
- Teoh Yong
- , Gábor Báti
- & Mihaiela C. Stuparu
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Fully automated fast-flow synthesis of antisense phosphorodiamidate morpholino oligomers
PMOs (phosphorodiamidate morpholino oligomers) have huge potential for antisense therapy but complex and slow synthesis limits application. Here, the authors report the development of automated flow synthesis methods which reduce nucleobase coupling times from hours to minutes removing human errors and allow for high-throughput production.
- Chengxi Li
- , Alex J. Callahan
- & Bradley L. Pentelute
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A graph-based network for predicting chemical reaction pathways in solid-state materials synthesis
Predictive computational approaches are fundamental to accelerating solid-state inorganic synthesis. This work demonstrates a computational tractable approach constructed from available thermochemistry data and based on a graph-based network model for predicting solid-state inorganic reaction pathways.
- Matthew J. McDermott
- , Shyam S. Dwaraknath
- & Kristin A. Persson
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In situ microbeam surface X-ray scattering reveals alternating step kinetics during crystal growth
The basal-plane surfaces of hexagonal close-packed crystals typically exhibit an alternating sequence of A and B steps with different atomic structures and growth kinetics. Here the authors demonstrate a method to determine whether A or B steps have faster kinetics under specific growth conditions.
- Guangxu Ju
- , Dongwei Xu
- & G. Brian Stephenson
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A protein tertiary structure mimetic modulator of the Hippo signalling pathway
Targeting the interaction between transcription factor TEAD and its co-repressor VGL4 is an attractive strategy to chemically modulate Hippo signaling. Here, the authors develop a proteomimetic with stabilized tertiary structure that inhibits the TEAD:VGL4 interaction in vitro and in cells.
- Hélène Adihou
- , Ranganath Gopalakrishnan
- & Herbert Waldmann
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Discovery of gramicidin A analogues with altered activities by multidimensional screening of a one-bead-one-compound library
The strong hemolytic activity and mammalian cytotoxicity of gramicidin A, a peptide antibiotic, has hindered its non-topical clinical application. Here, the authors report a high-throughput strategy for the discovery of gramicidin A analogues with altered biological activity profiles.
- Yuri Takada
- , Hiroaki Itoh
- & Masayuki Inoue
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Mechanochemical synthesis of pillar[5]quinone derived multi-microporous organic polymers for radioactive organic iodide capture and storage
Incorporation of supramolecular macrocycles into porous organic polymers can increase uptake of guest molecules through host−guest interactions. Here the authors report a pillar[5]quinone derived multi-microporous organic polymer, which show a superior performance in radioactive iodomethane capture and storage.
- Kecheng Jie
- , Yujuan Zhou
- & Sheng Dai
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Prevention of aspartimide formation during peptide synthesis using cyanosulfurylides as carboxylic acid-protecting groups
Aspartimide formation is a frequently occurring problem during peptide synthesis. Here, the authors present cyanosulfurylides as a protection group that masks aspartic acid residues during solid phase peptide synthesis, thus preventing aspartimide formation, and can be removed with N-chlorosuccinimide.
- Kevin Neumann
- , Jakob Farnung
- & Jeffrey W. Bode
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Late-stage peptide C–H alkylation for bioorthogonal C–H activation featuring solid phase peptide synthesis
Palladium-catalyzed late-stage diversification of structurally complex peptides has major shortcomings. Here, the authors developed a ruthenium-catalyzed C–H alkylations of peptides allowing for fluorescence labeling, late-stage diversifications and peptide ligations by solid phase peptide synthesis.
- Alexandra Schischko
- , Nikolaos Kaplaneris
- & Lutz Ackermann
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Development of a high-throughput strategy for discovery of potent analogues of antibiotic lysocin E
The depsipeptide Lysocin E has antibacterial activity against methicillin-resistant Staphylococcus aureus. Here, the authors developed a high-throughput one-bead-on-compound method for the synthesis and screening lysocin E derivatives, with several hits being more active than the parent compound.
- Hiroaki Itoh
- , Kotaro Tokumoto
- & Masayuki Inoue
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Non-equilibrium crystallization pathways of manganese oxides in aqueous solution
Multistage crystallization of transition metal oxides often proceeds through a number of metastable intermediates. Here, the authors shed light on this phenomenon by extending Pourbaix diagrams to capture the metastable and nanoscale thermodynamics of manganese oxide nucleation.
- Wenhao Sun
- , Daniil A. Kitchaev
- & Gerbrand Ceder
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Olefin-accelerated solid-state C–N cross-coupling reactions using mechanochemistry
Cross-coupling reactions have been achieved in solution, yet tend to be inefficient in a solid state. Here, the authors report a solid-state palladium-catalyzed Buchwald-Hartwig cross-coupling using olefins as molecular dispersants, enabling reduction of solvent waste.
- Koji Kubota
- , Tamae Seo
- & Hajime Ito
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Rechargeable potassium-ion batteries with honeycomb-layered tellurates as high voltage cathodes and fast potassium-ion conductors
The development of potassium-ion batteries requires cathode materials that can maintain the structural stability during cycling. Here the authors have developed honeycomb-layered tellurates K2M2TeO6 that afford high ionic conductivity and reversible intercalation of large K ions at high voltages.
- Titus Masese
- , Kazuki Yoshii
- & Masahiro Shikano
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Realization of vertical metal semiconductor heterostructures via solution phase epitaxy
Controlling the composition and crystal phase of layered heterostructures is important. Here, the authors report the liquid-phase epitaxial growth of Sn0.5W0.5S2 nanosheets with 83% metallic phase on SnS2 nanoplates, which are used as 100 ppb level chemiresistive gas sensors at room temperature.
- Xiaoshan Wang
- , Zhiwei Wang
- & Wei Huang
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Fe-N system at high pressure reveals a compound featuring polymeric nitrogen chains
Owing to the energetic nature of N–N bonds, poly-nitrogen compounds are considered promising high energy density materials. Here, the authors synthesize three iron–nitrogen compounds at high pressure, including FeN4, which features polymeric nitrogen chains of [N42−]n units.
- M. Bykov
- , E. Bykova
- & L. Dubrovinsky
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The effect of crystallite size on pressure amplification in switchable porous solids
Pressure amplification phenomena have recently been observed in ordered mesoporous solids, but little is understood about this counter-intuitive behaviour. Here, Kaskel and colleagues demonstrate that crystal size can play an important role in modulating pressure amplification in metal-organic frameworks.
- Simon Krause
- , Volodymyr Bon
- & Stefan Kaskel
LaMg6Ga6S16: a chemical stable divalent lanthanide chalcogenide