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"Dyson, Paul J."
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The Eagle has landed : 50 years of lunar science fiction
\"In celebration of the 50th anniversary of the Apollo 11 landing, the endlessly-mysterious moon is explored in this reprint short science fiction anthology from award-winning editor and anthologist Neil Clarke ... On July 20, 1969, mankind made what had only years earlier seemed like an impossible leap forward: when Apollo 11 became the first manned mission to land on the moon, and Neil Armstrong the first person to step foot on the lunar surface. While there have only been a handful of new missions since, the fascination with our planet's satellite continues, and generations of writers and artists have imagined the endless possibilities of lunar life. From adventures in the vast gulf of space between the earth and the moon, to journeys across the light face to the dark side, to the establishment of permanent residences on its surface, science fiction has for decades given readers bold and forward-thinking ideas about our nearest interstellar neighbor and what it might mean to humankind, both now and in our future. [This book] collects the best stories written in the fifty years since mankind first stepped foot on the lunar surface, serving as a shining reminder that the moon is and always has been our most visible and constant example of all the infinite possibility of the wider universe\"-- Provided by publisher.
BOOK
Direct synthesis of formic acid from carbon dioxide by hydrogenation in acidic media
The chemical transformation of carbon dioxide into useful products becomes increasingly important as CO
2
levels in the atmosphere continue to rise as a consequence of human activities. In this article we describe the direct hydrogenation of CO
2
into formic acid using a homogeneous ruthenium catalyst, in aqueous solution and in dimethyl sulphoxide (DMSO), without any additives. In water, at 40 °C, 0.2 M formic acid can be obtained under 200 bar, however, in DMSO the same catalyst affords 1.9 M formic acid. In both solvents the catalysts can be reused multiple times without a decrease in activity. Worldwide demand for formic acid continues to grow, especially in the context of a renewable energy hydrogen carrier, and its production from CO
2
without base, via the direct catalytic carbon dioxide hydrogenation, is considerably more sustainable than the existing routes.
The conversion of carbon dioxide into formic acid is attractive for energy storage and chemical production, but the typical use of bases or other additives make isolation of the free acid difficult. Here, the authors report the catalytic conversion of carbon dioxide into formic acid without the need for any additives.
Journal Article
Direct conversion of lignin to functionalized diaryl ethers via oxidative cross-coupling
Efficient valorization of lignin, a sustainable source of functionalized aromatic products, would reduce dependence on fossil-derived feedstocks. Oxidative depolymerization is frequently applied to lignin to generate phenolic monomers. However, due to the instability of phenolic intermediates, repolymerization and dearylation reactions lead to low selectivity and product yields. Here, a highly efficient strategy to extract the aromatic monomers from lignin affording functionalized diaryl ethers using oxidative cross-coupling reactions is described, which overcomes the limitations of oxidative methods and affords high-value specialty chemicals. Reaction of phenylboronic acids with lignin converts the reactive phenolic intermediates into stable diaryl ether products in near-theoretical maximum yields (92% for beech lignin and 95% for poplar lignin based on the content of β−O−4 linkages). This strategy suppresses side reactions typically encountered in oxidative depolymerization reactions of lignin and provides a new approach for the direct transformation of lignin into valuable functionalized diaryl ethers, including key intermediates in pharmaceutical and natural product synthesis.
Efficient valorization of lignin, a sustainable source of functionalized aromatic products, would reduce dependence on fossil-derived feedstocks. Here, the authors directly transform lignin into valuable functionalized diaryl ethers in near-theoretical-maximum yields, using oxidative cross coupling under copper catalysis.
Journal Article
Oriented nucleation in formamidinium perovskite for photovoltaics
The black phase of formamidinium lead iodide (FAPbI
3
) perovskite shows huge promise as an efficient photovoltaic, but it is not favoured energetically at room temperature, meaning that the undesirable yellow phases are always present alongside it during crystallization
1
–
4
. This problem has made it difficult to formulate the fast crystallization process of perovskite and develop guidelines governing the formation of black-phase FAPbI
3
(refs.
5
,
6
). Here we use in situ monitoring of the perovskite crystallization process to report an oriented nucleation mechanism that can help to avoid the presence of undesirable phases and improve the performance of photovoltaic devices in different film-processing scenarios. The resulting device has a demonstrated power-conversion efficiency of 25.4% (certified 25.0%) and the module, which has an area of 27.83 cm
2
, has achieved an impressive certified aperture efficiency of 21.4%.
The black phase of formamidinium lead iodide perovskite is used to make highly efficient solar cells, and a technique to improve its purity and stability by controlling crystal nucleation could make them even better.
Journal Article
Dopant-additive synergism enhances perovskite solar modules
Perovskite solar cells (PSCs) are among the most promising photovoltaic technologies owing to their exceptional optoelectronic properties
1
,
2
. However, the lower efficiency, poor stability and reproducibility issues of large-area PSCs compared with laboratory-scale PSCs are notable drawbacks that hinder their commercialization
3
. Here we report a synergistic dopant-additive combination strategy using methylammonium chloride (MACl) as the dopant and a Lewis-basic ionic-liquid additive, 1,3-bis(cyanomethyl)imidazolium chloride ([Bcmim]Cl). This strategy effectively inhibits the degradation of the perovskite precursor solution (PPS), suppresses the aggregation of MACl and results in phase-homogeneous and stable perovskite films with high crystallinity and fewer defects. This approach enabled the fabrication of perovskite solar modules (PSMs) that achieved a certified efficiency of 23.30% and ultimately stabilized at 22.97% over a 27.22-cm
2
aperture area, marking the highest certified PSM performance. Furthermore, the PSMs showed long-term operational stability, maintaining 94.66% of the initial efficiency after 1,000 h under continuous one-sun illumination at room temperature. The interaction between [Bcmim]Cl and MACl was extensively studied to unravel the mechanism leading to an enhancement of device properties. Our approach holds substantial promise for bridging the benchtop-to-rooftop gap and advancing the production and commercialization of large-area perovskite photovoltaics.
A synergistic dopant-additive combination strategy using methylammonium chloride as the dopant and a Lewis-basic ionic-liquid additive is shown to enable the fabrication of perovskite solar modules achieving record certified performance and long-term operational stability.
Journal Article
Mechanistic classification and benchmarking of polyolefin depolymerization over silica-alumina-based catalysts
Carbon-carbon bond cleavage mechanisms play a key role in the selective deconstruction of alkanes and polyolefins. Here, we show that the product distribution, which encompasses carbon range and formation of unsaturated and isomerization products, serves as a distinctive feature that allows the reaction pathways of different catalysts to be classified. Co, Ni, or Ru nanoparticles immobilized on amorphous silica-alumina, Zeo-Y and ZSM-5, were evaluated as catalysts in the deconstruction of
n
-hexadecane model substrate with hydrogen to delineate between different mechanisms, i.e., monofunctional- (acid site dominated) or bifunctional-hydrocracking (acid site & metal site) versus hydrogenolysis (metal site dominated), established from the product distributions. The ZSM-5-based catalysts were further studied in the depolymerization of polyethylene. Based on these studies, the catalysts are plotted on an activity-mechanism map that functions as an expandable basis to benchmark catalytic activity and to identify optimal catalysts that afford specific product distributions. The systematic approach reported here should facilitate the acceleration of catalyst discovery for polyolefin depolymerization.
Product distributions have been used to classify the depolymerization pathways of polyolefins catalyzed by silica-alumina-based catalysts to construct an activity-mechanism map as a benchmarking tool to facilitate catalyst discovery.
Journal Article
N-formylation and N-methylation of amines using metal-free N-heterocyclic carbene catalysts and CO2 as carbon source
This protocol describes the environmentally benign
N
-formylation and
N
-methylation of primary and secondary amines using carbon dioxide as the carbon source, hydrosilanes as reductants and
N
-heterocyclic carbenes as catalysts.
N
-formylation and
N
-methylation of amines are important reactions that are used to produce a wide range of key intermediates and compounds. This protocol describes the environmentally benign
N
-formylation and
N
-methylation of primary and secondary amines using carbon dioxide (CO
2
) as the carbon source, hydrosilanes as reductants and
N
-heterocyclic carbenes (NHCs) as catalysts. Using CO
2
as a reagent has the advantage of low cost and negligible toxicity. However, the catalyst is air-sensitive and must be generated fresh before use; consequently, the techniques used to prepare and manipulate the catalyst are described. The synthetic approach described in this protocol does not use any toxic reagents; using the appropriate catalyst,
N
-formylated or
N
-methylated products can be obtained with high selectivity. The overall time for catalyst preparation and for conducting several catalytic reactions in parallel is 15–48 h, depending on the nature of the substrates.
Journal Article
Tuning structural isomers of phenylenediammonium to afford efficient and stable perovskite solar cells and modules
Organic halide salt passivation is considered to be an essential strategy to reduce defects in state-of-the-art perovskite solar cells (PSCs). This strategy, however, suffers from the inevitable formation of in-plane favored two-dimensional (2D) perovskite layers with impaired charge transport, especially under thermal conditions, impeding photovoltaic performance and device scale-up. To overcome this limitation, we studied the energy barrier of 2D perovskite formation from
ortho-
,
meta-
and
para-
isomers of (phenylene)di(ethylammonium) iodide (PDEAI
2
) that were designed for tailored defect passivation. Treatment with the most sterically hindered
ortho
-isomer not only prevents the formation of surficial 2D perovskite film, even at elevated temperatures, but also maximizes the passivation effect on both shallow- and deep-level defects. The ensuing PSCs achieve an efficiency of 23.9% with long-term operational stability (over 1000 h). Importantly, a record efficiency of 21.4% for the perovskite module with an active area of 26 cm
2
was achieved.
Salt passivation of perovskite often results in formation of 2D perovskite layers, which impaired charge transport behaviour. Here, the authors study the energy barrier of 2D perovskite formation upon passivation by different iodide salt, and provide insight how to manipulate this to maximise device performance.
Journal Article
Repositioning approved drugs for the treatment of problematic cancers using a screening approach
Advances in treatment strategies together with an earlier diagnosis have considerably increased the average survival of cancer patients over the last four decades. Nevertheless, despite the growing number of new antineoplastic agents introduced each year, there is still no adequate therapy for problematic malignancies such as pancreatic, lung and stomach cancers. Consequently, it is important to ensure that existing drugs used to treat other types of cancers, and potentially other diseases, are not overlooked when searching for new chemotherapy regimens for these problematic cancer types. We describe a screening approach that identifies chemotherapeutics for the treatment of lung and pancreatic cancers, based on drugs already approved for other applications. Initially, the 1280 chemically and pharmacologically diverse compounds from the Prestwick Chemical Library® (PCL) were screened against A549 (lung cancer) and PANC-1 (pancreatic carcinoma) cells using the PrestoBlue fluorescent-based cell viability assay. More than 100 compounds from the PCL were identified as hits in one or both cell lines (80 of them, being drugs used to treat diseases other than cancer). Selected PCL hits were further evaluated in a dose-response manner. Promising candidates for repositioning emanating from this study include antiparasitics, cardiac glycosides, as well as the anticancer drugs vorinostat and topotecan.
Journal Article
Symbiont-mediated RNA interference in insects
RNA interference (RNAi) methods for insects are often limited by problems with double-stranded (ds) RNA delivery, which restricts reverse genetics studies and the development of RNAi-based biocides. We therefore delegated to insect symbiotic bacteria the task of: (i) constitutive dsRNA synthesis and (ii) trauma-free delivery. RNaseIII-deficient, dsRNA-expressing bacterial strains were created from the symbionts of two very diverse pest species: a long-lived blood-sucking bug, Rhodnius prolixus, and a short-lived globally invasive polyphagous agricultural pest, western flower thrips (Frankliniella occidentalis). When ingested, the manipulated bacteria colonized the insects, successfully competed with the wild-type microflora, and sustainably mediated systemic knockdown phenotypes that were horizontally transmissible. This represents a significant advance in the ability to deliver RNAi, potentially to a large range of non-model insects.
Journal Article