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Today: 26 January 2021, Tuesday.

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#1

 
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Iron-catalysed synthesis and chemical recycling of telechelic 1,3-enchained oligocyclobutanes | Nature Chemistry
Description Closed-loop recycling offers the opportunity to mitigate plastic waste through reversible polymer construction and deconstruction. Although examples of chemical recycling of polymers are known, few have been applied to materials derived from abundant commodity olefinic monomers, which are the building blocks of ubiquitous plastic resins. Here we describe a [2+2] cycloaddition/oligomerization of 1,3-butadiene to yield a previously unrealized telechelic microstructure of (1,n′-divinyl)oligocyclobutane. This material is thermally stable, has stereoregular segments arising from chain-end control, and exhibits high crystallinity even at low molecular weight. Exposure of the oligocyclobutane to vacuum in the presence of the pyridine(diimine) iron precatalyst used to synthesize it resulted in deoligomerization to generate pristine butadiene, demonstrating a rare example of closed-loop chemical recycling of an oligomeric material derived from a commodity hydrocarbon feedstock. Iron-catalysed [2+2] cycloaddition/oligomerization of neat butadiene affords (1,n′-divinyl)oligocyclobutane—a telechelic, crystalline material consisting of 1,3-enchained cyclobutyl units. This oligocyclobutane can be chemically recycled to pure butadiene using the same iron catalyst employed in its synthesis, demonstrating design principles for next-generation plastic materials that can be returned to pristine monomer.

#Chemicals
Field # Chemicals
Updated 25 January 2021

#2

 
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Non-equilibrium metal oxides via reconversion chemistry in lithium-ion batteries | Nature Communications
Description Binary metal oxides are attractive anode materials for lithium-ion batteries. Despite sustained effort into nanomaterials synthesis and understanding the initial discharge mechanism, the fundamental chemistry underpinning the charge and subsequent cycles—thus the reversible capacity—remains poorly understood. Here, we use in operando X-ray pair distribution function analysis combining with our recently developed analytical approach employing Metropolis Monte Carlo simulations and non-negative matrix factorisation to study the charge reaction thermodynamics of a series of Fe- and Mn-oxides. As opposed to the commonly believed conversion chemistry forming rocksalt FeO and MnO, we reveal the two oxide series topotactically transform into non-native body-centred cubic FeO and zincblende MnO via displacement-like reactions whose kinetics are governed by the mobility differences between displaced species. These renewed mechanistic insights suggest avenues for the future design of metal oxide materials as well as new material synthesis routes using electrochemically-assisted methods. The charging of Fe and Mn oxide anodes in lithium-ion batteries are believed to form rocksalt phases via reconstructive conversion reactions. Here, the authors show that MxOy (M = Fe, Mn) transform into non-native body-centred cubic FeO and zincblende MnO via topotactic displacement-like pathways.

#Chemicals
Field # Chemicals
Updated 25 January 2021

#3

 
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Flowery endocytosis | Nature Chemical Biology
Description

#Chemicals
Field # Chemicals
Updated 22 January 2021

#4

 
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A recipe for execution | Nature Chemical Biology
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#Chemicals
Field # Chemicals
Updated 22 January 2021

#5

 
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The enemy of my enemy | Nature Chemical Biology
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#Chemicals
Field # Chemicals
Updated 22 January 2021

#6

 
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Demystifying the momilactone pathway | Nature Chemical Biology
Description Re-channeling metabolic routes in Nicotiana benthamiana allows elucidation and reconstitution of the biosynthesis of the natural products momilactones A and B. Insights into how plants make these and other natural crop protection chemicals promise future biotechnologies for sustainable agriculture.

#Chemicals
Field # Chemicals
Updated 22 January 2021

#7

 
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Bringing distant DNA together | Nature Chemical Biology
Description Yin Yang 1 (YY1) is a transcription factor involved in gene regulation. A recent study has revealed G-quadruplex structures as novel binding targets of YY1, and their interactions regulate DNA looping and gene expression.

#Chemicals
Field # Chemicals
Updated 22 January 2021

#8

 
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To protect and emit beauty | Nature Chemical Biology
Description The plant cuticle has long been considered a barrier to volatile organic compound emission. New research reveals the paradoxical role of the cuticle as a barrier and facilitator of volatile emissions in hybrid petunia.

#Chemicals
Field # Chemicals
Updated 22 January 2021

#9

 
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Towards more sustainable curricula | Nature Reviews Chemistry
Description If chemistry is to contribute effectively to the development of a more sustainable world, it is essential that it is taught within a broader socioeconomic and ecological context. If chemistry is to contribute effectively to the development of a more sustainable world, it is essential that it is taught within a broader socioeconomic and ecological context.

#Chemicals
Field # Chemicals
Updated 21 January 2021

#10

 
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Dope new organocatalysts for ATRP | Nature Reviews Chemistry
Description A re-evaluation of the design principles of organocatalysts for atom transfer radical polymerization has led to the development of heteroatom-doped polycyclic arenes as highly active photocatalysts.

#Chemicals
Field # Chemicals
Updated 21 January 2021

#11

 
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Intoxicating Chemicals in Catnip Don’t Just Give Cats Joy – They Help Repel Mosquitoes
Description TBD

#Chemicals
Field # Chemicals
Updated 20 January 2021

#12

 
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Chemists Invent Shape-Shifting Nanomaterial With Intriguing Biomedical Potential
Description TBD

#Chemicals
Field # Chemicals
Updated 19 January 2021

#13

 
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Single hydrogen atom manipulation for reversible deprotonation of water on a rutile TiO 2 (110) surface | Communications Chemistry
Description The discovery of hydrogen atoms on the TiO2 surface is crucial for many practical applications, including photocatalytic water splitting. Electronically activating interfacial hydrogen atoms on the TiO2 surface is a common way to control their reactivity. Modulating the potential landscape is another way, but dedicated studies for such an activation are limited. Here we show the single hydrogen atom manipulation, and on-surface facilitated water deprotonation process on a rutile TiO2 (110) surface using low temperature atomic force microscopy and Kelvin probe force spectroscopy. The configuration of the hydrogen atom is manipulated on this surface step by step using the local field. Furthermore, we quantify the force needed to relocate the hydrogen atom on this surface using force spectroscopy and density functional theory. Reliable control of hydrogen atoms provides a new mechanistic insight of the water molecules on a metal oxide surface. Rutile TiO2 is a prominent photocatalyst for overall water splitting, but the on-surface activation of hydrogen atoms is still not fully understood. Here, the authors use atomic force and kelvin probe force microscopy to study the lateral manipulation of hydrogen on a rutile (110) surface.

#Chemicals
Field # Chemicals
Updated 19 January 2021

#14

 
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Local structure and distortions of mixed methane-carbon dioxide hydrates | Communications Chemistry
Description A vast source of methane is found in gas hydrate deposits, which form naturally dispersed throughout ocean sediments and arctic permafrost. Methane may be obtained from hydrates by exchange with hydrocarbon byproduct carbon dioxide. It is imperative for the development of safe methane extraction and carbon dioxide sequestration to understand how methane and carbon dioxide co-occupy the same hydrate structure. Pair distribution functions (PDFs) provide atomic-scale structural insight into intermolecular interactions in methane and carbon dioxide hydrates. We present experimental neutron PDFs of methane, carbon dioxide and mixed methane-carbon dioxide hydrates at 10 K analyzed with complementing classical molecular dynamics simulations and Reverse Monte Carlo fitting. Mixed hydrate, which forms during the exchange process, is more locally disordered than methane or carbon dioxide hydrates. The behavior of mixed gas species cannot be interpolated from properties of pure compounds, and PDF measurements provide important understanding of how the guest composition impacts overall order in the hydrate structure. Natural gas can be collected from hydrate deposits by exchange with CO2, but the ensuing mixed hydrates and the path to a complete exchange are not fully understood. Here, computational analyses of neutron pair distribution functions of CH4, CO2 and mixed CH4-CO2 hydrates at 10 K reveal that the behavior of mixed gas species cannot be interpolated from properties of pure compounds.

#Chemicals
Field # Chemicals
Updated 19 January 2021

#15

 
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Washing with alkaline solutions in protein A purification improves physicochemical properties of monoclonal antibodies | Scientific Reports
Description Protein A affinity chromatography has been widely used for both laboratory scale purification and commercial manufacturing of monoclonal antibodies and Fc-fusion proteins. Protein A purification is specific and efficient. However, there still remain several issues to be addressed, such as incomplete clearance of impurities including host cell proteins, DNA, aggregates, etc. In addition, the effects of wash buffers in protein A purification on the physicochemical characteristics of antibodies have yet to be fully understood. Here we found a new purification protocol for monoclonal antibodies that can improve physicochemical properties of monoclonal antibodies simply by inserting an additional wash step with a basic buffer after the capture step to the conventional protein A purification. The effects of the alkaline wash on monoclonal antibodies were investigated in terms of physicochemical characteristics, yields, and impurity clearance. The simple insertion of an alkaline wash step resulted in protection of antibodies from irreversible aggregation, reduction in free thiols and impurities, an improvement in colloidal and storage stability, and enhanced yields. This new procedure is widely applicable to protein A affinity chromatography of monoclonal antibodies.

#Chemicals
Field # Chemicals
Updated 19 January 2021

#16

 
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Diagnostic performance of a faecal immunochemical test for patients with low-risk symptoms of colorectal cancer in primary care: an evaluation in the South West of England | British Journal of Cancer
Description The faecal immunochemical test (FIT) was introduced to triage patients with low-risk symptoms of possible colorectal cancer in English primary care in 2017, underpinned by little primary care evidence. All healthcare providers in the South West of England (population 4 million) participated in this evaluation. 3890 patients aged ≥50 years presenting in primary care with low-risk symptoms of colorectal cancer had a FIT from 01/06/2018 to 31/12/2018. A threshold of 10 μg Hb/g faeces defined a positive test. Six hundred and eighteen (15.9%) patients tested positive; 458 (74.1%) had an urgent referral to specialist lower gastrointestinal (GI) services within three months. Forty-three were diagnosed with colorectal cancer within 12 months. 3272 tested negative; 324 (9.9%) had an urgent referral within three months. Eight were diagnosed with colorectal cancer within 12 months. Positive predictive value was 7.0% (95% CI 5.1–9.3%). Negative predictive value was 99.8% (CI 99.5–99.9%). Sensitivity was 84.3% (CI 71.4–93.0%), specificity 85.0% (CI 83.8–86.1%). The area under the ROC curve was 0.92 (CI 0.86–0.96). A threshold of 37 μg Hb/g faeces would identify patients with an individual 3% risk of cancer. FIT performs exceptionally well to triage patients with low-risk symptoms of colorectal cancer in primary care; a higher threshold may be appropriate in the wake of the COVID-19 crisis.

#Chemicals
Field # Chemicals
Updated 19 January 2021

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