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Alzheimer's disease (AD) patients admitted to intensive care units (ICUs) exhibit varying survival outcomes due to the unique challenges in managing AD patients. Stratifying patient mortality risk and understanding the criticality of nursing care are important to improve the clinical outcomes of AD patients. This study aimed to leverage machine learning (ML) and electronic health records (EHRs) only consisting of demographics, disease history, and routine lab tests, with a focus on nursing care, to facilitate the optimization of nursing practices for AD patients. We utilized Medical Information Mart for Intensive Care III, an open-source EHR dataset, and AD patients were identified based on the International Classification of Diseases, Ninth Revision codes. From a cohort of 453 patients, a total of 60 features, encompassing demographics, laboratory tests, disease history, and number of nursing events, were extracted. ML models, including XGBoost, random forest, logistic regression, and multi-layer perceptron, were trained to predict the 30-day mortality risk. In addition, the influence of nursing care was analyzed in terms of feature importance using values calculated from both the inherent XGBoost module and the SHapley Additive exPlanations (SHAP) library. XGBoost emerged as the lead model with a high accuracy of 0.730, area under the curve (AUC) of 0.750, sensitivity of 0.688, and specificity of 0.740. Feature importance analyses using inherent XGBoost module or SHAP both indicated the number of nursing care within 14 days post-admission as an important denominator for 30-day mortality risk. When nursing care events were excluded as a feature, stratifying patient mortality risk was also possible but the model's AUC of receiver operating characteristic curve was reduced to 0.68. Nursing care plays a pivotal role in the survival outcomes of AD patients in ICUs. ML models can be effectively employed to predict mortality risks and underscore the importance of specific features, including nursing care, in patient outcomes. Early identification of high-risk AD patients can aid in prioritizing intensive nursing care, potentially improving survival rates., Competing Interests: Declaration of Conflicting InterestsThe author(s) declared no potential conflicts of interest with respect to the research, authorship, and/or publication of this article.

The synthesis of value-added products via CO 2 electroreduction (CO 2 ER) is of great significance, but the development of efficient and versatile strategies for the controllable selectivity tuning is extremely challenging. Herein, the tuning of CO 2 ER selectivity through the modulation of CO 2 adsorption behavior is proposed. Using the constructed zeolitic MOF (SNNU-339), CO 2 adsorption behavior is controllably changed from *CO 2 to CO 2 * via the precise ligand-to-metal charge donation (LTMCD) regulation. It is confirmed that the high electronegativity of the coordinate ligand directly restricts the LTMCD, reduces the charge density on the metal sites, lowers the Gibbs free energy for CO 2 * adsorption, and leads to the transformation of CO 2 adsorption mode from *CO 2 to CO 2 *. Owing to the modulated CO 2 adsorption behavior and regulated kinetics, SNNU-339 exhibits superior HCOOH selectivity (≈330% promotion, 85.6% Faradaic efficiency) and high CO 2 ER activity. The wide applicability of the proposed approach sheds light on the efficient CO 2 ER. This study provides a competitive strategy for rational catalyst design and underscores the significance of adsorption behavior tuning in electrocatalysis., (© 2024 Wiley‐VCH GmbH.)

Developing catalysts with excellent CO 2 capture capability and electrochemical CO 2 reduction reaction (CO 2 RR) at a wide potential range simultaneously is significant but remains a formidable challenge. Here, two novel InMg defective trinuclear cluster-based MOFs (SNNU-41 and SNNU-42) with abundant p -block unsaturated coordinated sites were reported and exhibited good CO 2 capture and CO 2 RR performance simultaneously. Due to the suitable micropores, SNNU-41 showed higher CO 2 capture ability at different adsorption pressure conditions. On account of the rigid framework and the closer p band center to Fermi level, SNNU-42 accelerated the conversion of CO 2 molecule to C1 efficiency. Notably, via adjusting the ratio of p -block metal (In) in the SNNU-42 framework, the performance of the CO 2 RR was promoted drastically. SNNU-42 with the InMg (1:1.8) mixed cluster delivered an excellent Faradaic efficiency of 91.3% for C1 products and high selectivity of 72.0% for HCOOH at -2.5 V (vs Ag/Ag + ) with a total current density of 77.2 mA cm -2 . This work provides a possibility for efficient CO 2 capture and CO 2 RR electrocatalysts through the modulation of electronic structures and composition in MOFs.

Recovery of light alkanes from natural gas is of great significance in petrochemical production. Herein, a promising strategy utilizing two types of size-complementary aromatic ring-confined nanotraps (called bi-nanotraps here) is proposed to efficiently trap ethane (C 2 H 6 ) and propane (C 3 H 8 ) selectively at their respective sites. Two isostructural metal-organic frameworks (MOFs, SNNU-185/186), each containing bi-nanotraps decorated with six aromatic rings, are selected to demonstrate the feasibility of this method. The smaller nanotrap acts as adsorption sites tailored for C 2 H 6 while the larger one is optimized in size for C 3 H 8 . The separation is further facilitated by the large channels, which serve as mass transfer pathways. These advanced features give rise to multiple C-H⋯π interactions and size/shape-selective interaction sites, enabling SNNU-185/186 to achieve high C 2 H 6 adsorption enthalpy (43.5/48.8 kJ mol -1 ) and a very large thermodynamic interaction difference between C 2 H 6 and CH 4 . Benefiting from the bi-nanotrap effect, SNNU-185/186 exhibits benchmark experimental natural gas upgrade performance with top-level CH 4 productivity (6.85/6.10 mmol g -1 ), ultra-high purity and first-class capture capacity for C 2 H 6 (1.23/0.90 mmol g -1 ) and C 3 H 8 (2.33/2.15 mmol g -1 )., Competing Interests: There are no conflicts to declare., (This journal is © The Royal Society of Chemistry.)

Evolutionary rescue occurs when populations survive lethal environmental stresses through the rising and fixation of tolerant genotypes. Temperature has long been believed to determine the evolutionary speed of populations and species. Here, we suggest that warmer temperatures can facilitate evolutionary rescue. Moreover, with dispersal among habitats, the advantage in evolutionary rescue for warmer populations may cause a bias in habitat colonization dynamics towards the warm-to-cold direction. We experimentally tested these hypotheses with a model microbial system. Our first experiment showed that bacterial populations at warmer temperatures had a greater chance to evolve resistance and escape the fate of extinction under an antibiotic treatment. In the second experiment, metapopulations that consisted of warm and cold habitats were exposed to the antibiotic stress; local populations that went extinct might be recolonized, and such recolonization events were biased to the warm-to-cold direction. We also examined possible mechanisms underlying the temperature effect on the rapid evolution of resistance in our study system. Our results may help to understand the mechanisms of maintenance of biodiversity and patterns of gene flow among climatic regions, particularly in pest species subject to chemical control treatments.

Ultramicroporous metal-organic frameworks (MOFs) are demonstrated to be advantageous for the separation and purification of light hydrocarbons such as C 2 H 2 , C 2 H 4 , and CH 4 . The introduction of transition metal sites with strong π-complexation affinity into MOFs is more effective than other adsorption sites for the selective adsorption of π-electron-rich unsaturated hydrocarbon gases from their mixtures. However, lower coordination numbers make it challenging to produce robust MOFs directly utilizing metal ions with π-coordination activity, such as Cu + , Ag + , and Pd 2+ . Herein, a series of novel π-complexing MOFs (SNNU-33s) with a pore size of 4.6 Å are precisely constructed by cleverly introducing symmetrically matched C 3 -type [Cu(pyz) 3 ] (pyz = pyrazine) coordinated fragments into 1D hexagonal channels of MIL-88 prototype frameworks. Benifit from the spatial confinement combined with π-complex-active Cu + of [Cu(pyz) 3 ], pore-space-partitioned SNNU-33 MOFs all present excellent C 2 H 2 /CH 4 , C 2 H 4 /CH 4 , and CO 2 /CH 4 separation ability. Notably, the optimized SNNU-33b adsorbent demonstrates top-level IAST selectivity values for C 2 H 2 /CH 4 (597.4) and C 2 H 4 /CH 4 (69.8), as well as excellent breakthrough performance. Theoretical calculations further reveal that such benchmark light hydrocarbon separation and purification ability is mainly ascribed to the extra-strong binding affinity between Cu + and π-electron donor molecules via a spatially confined π-complexation process., (© 2024 Wiley‐VCH GmbH.)

Pillar-layered metal-organic frameworks (PLMOFs) are promising gas adsorbents due to their high designability. In this work, high CO 2 storage capacity as well as controllable C 2 H 2 /CO 2 separation ability are acquired by rationally manipulating the interlayer stacking in pillar-layered MOF materials. The rational construction of pillar-layered MOFs started from the 2D Ni-BTC-pyridine layer, an isomorphic structure of pioneering MOF-1 reported in 1995. The replacement of terminal pyridine groups by bridging pyrazine linkers under optimized solvothermal conditions led to three 3D PLMOFs with different stacking types between adjacent Ni-BTC layers, named PLMOF 1 (ABAB stacking), PLMOF 2 (AABB stacking), and PLMOF 3 (AAAA stacking). Regulated by the layer arrangements, CO 2 and C 2 H 2 adsorption capacities (273 K and 1 bar) of PLMOFs 1-3 vary from 173.0/153.3, 185.0/162.4, to 203.5/159.5 cm 3 g -1 , respectively, which surpass the values of most MOF adsorbents. Dynamic breakthrough experiments further indicate that PLMOFs 1-3 have controllable C 2 H 2 /CO 2 separation performance, which can successfully overcome the C 2 H 2 /CO 2 separation challenge. Specially, PLMOFs 1-3 can remove trace CO 2 (3%) from the C 2 H 2 /CO 2 mixture and produce high-purity ethylene (99.9%) in one step with the C 2 H 2 productivities of 1.68, 2.45, and 3.30 mmol g -1 , respectively. GCMC simulations indicate that the superior CO 2 adsorption and unique C 2 H 2 /CO 2 separation performance are mainly ascribed to different degrees of CO 2 agglomeration in the ultramicropores of these PLMOFs.

Interspecific competition can hinder populations from evolutionarily adapting to abiotic environments, particularly by reducing population size and niche space; and feedback may arise between competitive ability and evolutionary adaptation. Here we studied populations of two model bacterial species, Escherichia coli and Pseudomonas fluorescens, that evolved in monocultures and cocultures for approximately 2400 generations at three temperatures. The two species showed a reversal in competitive dominance in cocultures along the temperature gradient. Populations from cocultures where they had been competitively dominant showed the same magnitude of fitness gain as those in monocultures. However, competitively inferior populations in cocultures showed limited abiotic adaptation compared with those in monocultures. The inferior populations in cocultures were also more likely to evolve weaker interspecific competitive ability, or go extinct. The possible competitive ability-adaptation feedback may have crucial consequences for population persistence., (© 2024 John Wiley & Sons Ltd.)

Populations may survive environmental deterioration by evolutionary adaptation. However, such evolutionary rescue events may be associated with ecological costs, such as reduction in growth performance and loss of ecologically important genetic diversity. Those negative ecological consequences may be mitigated by additional adaptive evolution. Both the ecological costs and the opportunities for additional evolution are contingent on the severity of environmental deterioration. Here, we hypothesize that populations evolutionarily rescued from faster, relative to slow, environmental deterioration suffer more severe long-term fitness decline and diversity loss. An experiment with the model adaptive radiation of bacterium Pseudomonas fluorescens exposed to abruptly or gradually increased antibiotic stress supported our hypothesis. The effect of additional adaptive evolution in recovering population size and ecological diversity was far from perfect. Cautions are therefore needed in predicting the role of rapid evolution for mitigating the impacts of environmental changes, in particular very fast environmental deterioration. We also found that bacterial populations rescued from gradually increased antibiotic stress evolved higher levels of antibiotic resistance, lending more support to aggressive chemotherapy in pathogen control., (© The Author(s) 2023. Published by Oxford University Press on behalf of The Society for the Study of Evolution (SSE). All rights reserved. For permissions, please e-mail: journals.permissions@oup.com.)

Developing efficient adsorbents for acetylene purification from multicomponent mixtures is of critical significance in the chemical industry, but the trade-off between regenerability and selectivity significantly restricts practical industrial applications. Here, we report ultramicroporous metal-organic frameworks with acetylene-affinity channels to enhance electrostatic interaction between C 2 H 2 and frameworks for the efficient one-step purification of C 2 H 2 from C 2 H 2 /CO 2 /C 2 H 4 mixtures, in which the electrostatic interaction led to high regenerability. The obtained SNNU-277 exhibits significantly higher adsorption capacity for C 2 H 2 than that for both C 2 H 4 and CO 2 at 298 K and 0.1 bar, while an ultrahigh selectivity of C 2 H 2 /C 2 H 4 (100.6 at 298 K) and C 2 H 2 /CO 2 (32.8 at 298 K) were achieved at 1 bar. Breakthrough experiments validated that SNNU-277 can efficiently separate C 2 H 2 from C 2 H 2 /C 2 H 4 /CO 2 mixtures. CO 2 and C 2 H 4 broke through the adsorption column at 4 and 14.8 min g -1 , whereas C 2 H 2 was detected until 177.6 min g -1 at 298 K. Theoretical calculations suggest that the framework is electrostatically compatible with C 2 H 2 and electrostatically repels C 2 H 4 and CO 2 in the mixed components. This work highlights the importance of rational pore engineering for maximizing the electrostatic effect with the preferentially absorbed guest molecule for efficient multicomponent separation.

The precise design of low-cost, efficient, and definite electrocatalysts is the key to sustainable renewable energy. The urea oxidation reaction (UOR) offers a promising alternative to the oxygen evolution reaction for energy-saving hydrogen generation. In this study, by tuning the lattice expansion, a series of M-FeNi layered double hydroxides (M-FeNi LDHs, M: Mo, Mn, V) with excellent UOR performance are synthesized. The hydrolytic transformation of Fe-MIL-88A is assisted by urea, Ni 2+ and high-valence metals, to form a hollow M-FeNi LDH. Owing to the large atomic radius of the high-valence metal, lattice expansion is induced, and the electronic structure of the FeNi-LDH is regulated. Doping with high-valence metal is more favorable for the formation of the high-valence active species, NiOOH, for the UOR. Moreover, the hollow spindle structure promoted mass transport. Thus, the optimal Mo-FeNi LDH showed outstanding UOR electrocatalytic activity, with 1.32 V at 10 mA cm -2 . Remarkably, the Pt/C||Mo-FeNi LDH catalyst required a cell voltage of 1.38 V at 10 mA·cm -2 in urea-assisted water electrolysis. This study suggests a new direction for constructing nanostructures and modulating electronic structures, which is expected to ultimately lead to the development of a class of auxiliary electrocatalysts., (© 2023 Wiley-VCH GmbH.)

Comprehensive understanding of substituent groups located on the pore surface of metal-organic frameworks (which we call substituent engineering herein) can help to promote gas adsorption and catalytic performance through ligand functionalization. In this work, pore-space-partitioned metal-organic frameworks (PSP MOFs) were selected as a platform to evaluate the effect of organic functional groups on CO 2 adsorption, separation, and catalytic conversion. Twelve partitioned acs metal-organic frameworks (pacs-MOFs, named SNNU-25-R n here) containing different functional groups were synthesized, which can be classified into electron-donor groups (-OH, -NH 2 , -CH 3 , and -OCH 3 ) and electron-acceptor groups (-NO 2 , -F, -Cl, and -Br). The experimental results showed that SNNU-25-R n with electron donors usually perform better than those with electron acceptors for the comprehensive utilization of CO 2 . The CO 2 uptake of the 12 SNNU-25-R n MOFs ranged from 30.9 to 183.6 cm 3 g -1 at 273 K and 1 bar, depending on the organic functional groups. In particular, SNNU-25-OH showed the highest CO 2 adsorption, SNNU-25-CH 3 had the highest IAST of CO 2 /CH 4 (36.1), and SNNU-25-(OH) 2 showed the best catalytic activity for the CO 2 cycloaddition reaction. The -OH functionalized MOFs with excellent performance may be attributed to the Lewis acid-base and hydrogen-bonding interactions between -OH groups and the CO 2 molecules. This work modulated the effect of the microenvironment of MOFs on CO 2 adsorption, separation, and catalysis in terms of substituents, providing valuable information for the precise design of porous MOFs with a comprehensive utilization of CO 2 .

Fitness effects of mutations may generally depend on temperature that influences all rate-limiting biophysical and biochemical processes. Earlier studies suggested that high temperatures may increase the availability of beneficial mutations ('more beneficial mutations'), or allow beneficial mutations to show stronger fitness effects ('stronger beneficial mutation effects'). The 'more beneficial mutations' scenario would inevitably be associated with increased proportion of conditionally beneficial mutations at higher temperatures. This in turn predicts that populations in warm environments show faster evolutionary adaptation but suffer fitness loss when faced with cold conditions, and those evolving in cold environments become thermal-niche generalists ('hotter is narrower'). Under the 'stronger beneficial mutation effects' scenario, populations evolving in warm environments would show faster adaptation without fitness costs in cold environments, leading to a 'hotter is (universally) better' pattern in thermal niche adaptation. We tested predictions of the two competing hypotheses using an experimental evolution study in which populations of two model bacterial species, Escherichia coli and Pseudomonas fluorescens, evolved for 2400 generations at three experimental temperatures. Results of reciprocal transplant experiments with our P. fluorescens populations were largely consistent with the 'hotter is narrower' prediction. Results from the E. coli populations clearly suggested stronger beneficial mutation effects at higher assay temperatures, but failed to detect faster adaptation in populations evolving in warmer experimental environments (presumably because of limitation in the supply of genetic variation). Our results suggest that the influence of temperature on mutational effects may provide insight into the patterns of thermal niche adaptation and population diversification across thermal conditions., (© 2023 European Society for Evolutionary Biology.)

The potential for artificial selection at the community level to improve ecosystem functions has received much attention in applied microbiology. However, we do not yet understand what conditions in general allow for successful artificial community selection. Here we propose six hypotheses about factors that determine the effectiveness of artificial microbial community selection, based on previous studies in this field and those on multilevel selection. In particular, we emphasize selection strategies that increase the variance among communities. We then report a meta-analysis of published artificial microbial community selection experiments. The reported responses to community selection were highly variable among experiments; and the overall effect size was not significantly different from zero. The effectiveness of artificial community selection was greater when there was no migration among communities, and when the number of replicated communities subjected to selection was larger. The meta-analysis also suggests that the success of artificial community selection may be contingent on multiple necessary conditions. We argue that artificial community selection can be a promising approach, and suggest some strategies for improving the performance of artificial community selection programs., Competing Interests: The authors declare that the research was conducted in the absence of any commercial or financial relationships that could be construed as a potential conflict of interest., (Copyright © 2023 Yu, Zhang and Zhang.)

Metal-organic frameworks (MOFs) have attracted extensive attention in methane (CH 4 ) purification and storage. Specially, multinuclear cluster-based MOFs usually have prominent performance because of large cluster size and abundant open metal sites. However, compared to diverse combinations of organic linkers, one MOF with two or more multinuclear clusters is difficult to achieve. In this paper, we demonstrate a mixed multinuclear cluster strategy, which successfully led to three new heterometallic MOFs (SNNU-328-330) with the same common H 3 TATB [2,4,6-tris(4-carboxyphenyl)-1,3,5-triazine] tritopic linker and six types of multinuclear clusters ([YCd(COO) 4 (μ 2 -H 2 O)], [YCd 2 (COO) 8 ], [In 3 (COO) 6 (μ 3 -OH)], [In 3 Eu 2 (COO) 9 (μ 3 -OH) 3 (μ 4 -O)], [Y 9 (COO) 12 (μ 3 -OH) 14 ] and [Y 2 Cd 8 (COO) 16 (μ 2 -H 2 O) 4 (μ 3 -OH) 8 ]). Three MOF adsorbents all show great potentials to remove the impurities (CO 2 and C 2 -hydrocarbons) in natural gas and show prominent high-pressure methane storage capacity. Among them, the ideal adsorbed solution theory separation ratios of equimolar C 2 H 2 /CH 4 , C 2 H 4 /CH 4 , C 2 H 6 /CH 4 , and CO 2 /CH 4 at 298 K for SNNU-328 reach to 29.7-16.0, 19.1-8.2, 33.2-10.3, and 74.3-8.5, which have surpassed many famous MOF adsorbents. Dynamic breakthrough experiments conducted at 273 and 298 K showed that SNNU-330 can separate CH 4 from C 2 H 2 /CH 4 , C 2 H 4 /CH 4 , C 2 H 6 /CH 4 , and CO 2 /CH 4 mixtures with the breakthrough interval times of about 48.2, 17.9, 37.2, and 17.1 min g -1 (273 K, 1 bar, v / v = 50/50, 2 mL min -1 ), respectively. Remarkably, SNNU-329 exhibits extremely high methane storage performance at 298 K with the total uptake and working capacity of 192 cm 3 cm -3 (95 bar) and 171 cm 3 cm -3 (65 bar) due to the synergistic effects of high surface area, suitable pore sizes, and multiple open metal sites.

Natural enemies are critical drivers of species biogeography, and they may often limit the evolutionary adaptation and persistence of victim populations in sink habitats. Source-sink migration is also a major determinant of adaptation in sink habitats. Here, we specifically suggest that source-sink migration of enemies reduces evolutionary adaptation of victim populations in sink habitats. The underlying mechanisms may include depressed population size (which limits the supply of genetic variation) and enforced resistance evolution in victims (which shows a trade-off with growth performance). We experimentally tested this hypothesis using a model microbial system, bacterium Pseudomonas fluorescens (victim) and its lytic bacteriophage (enemy). The ancestral bacterial strain had lower growth performance at a cold temperature (10 °C, considered as sink habitat) than at its optimal temperature (28 °C, source habitat). Evolutionary adaptation took place in bacterial populations that evolved alone in the cold environment. When phages were present, no significant abiotic adaptation was observed. Crucially, phage immigration from source populations caused maladaptation, i.e., decreased growth performance relative to the ancestral genotype, although this was not the case when there was simultaneous immigration of phage and bacteria. Therefore, enemy-mediated intraspecific apparent competition could lead to prosperity in core habitats causing hardship in edge habitats., (© The Author(s) 2023. Published by Oxford University Press on behalf of The Society for the Study of Evolution (SSE). All rights reserved. For permissions, please e-mail: journals.permissions@oup.com.)

Grain boundary engineering (GBE) is considered to be an attractive approach to microstructure control, which significantly enhances the grain-boundary-related properties of face-centered cubic (FCC) metals. During the twinning-related GBE, the microstructures are characterized as abundant special twin boundaries that sufficiently disrupt the connectivity of the random boundary network. However, controlling the grain boundary character distribution (GBCD) is an extremely difficult issue, as it strongly depends on diverse processing parameters. This article provides a comprehensive review of controlling GBCD during the twinning-related GBE of FCC materials. To commence, this review elaborates on the theory of twinning-related GBE, the microscopic mechanisms used in the optimization of GBCD, and the optimization objectives of GBCD. Aiming to achieve control over the GBCD, the influence of the initial microstructure, thermo-mechanical processing (TMP) routes, and thermal deformation parameters on the twinning-related microstructures and associated evolution mechanisms are discussed thoroughly. Especially, the development of twinning-related kinetics models for predicting the evolution of twin density is highlighted. Furthermore, this review addresses the applications of twinning-related GBE in enhancing the mechanical properties and corrosion resistance of FCC materials. Finally, future prospects in terms of controlling the GBCD during twinning-related GBE are proposed. This study will contribute to optimizing the GBCD and designing GBE routes for better grain-boundary-related properties in terms of FCC materials.

Due to the trade-off barrier between high storage capacity and high selectivity, the controllable and systematic design of metal-organic frameworks (MOFs) aiming at performance optimization is still challenging. Herein, considering the effectiveness of alkoxy group functionalization and a pore-space partition strategy, a series of rigid Mg-pacs-MOFs ( SNNU-10- n , n = 1-6 ) with flexible side chains are built for the first time, realizing systematic pore environmental modification. The steric hindrance effects, electron-donating ability, and the flexibility of alkoxy groups are considered as key factors, which lead to a regular change of gas adsorption capacity and selectivity. Notably, methoxy-modified SNNU-10-1 with moderately high storage capacities of C 2 H 2 (139.4 cm 3 g -1 ), C 2 H 4 (100.4 cm 3 g -1 ), CO 2 (105.0 cm 3 g -1 ), and high selectivity values for equimolar C 2 H 2 /CH 4 (431.8), C 2 H 4 /CH 4 (164.2), and CO 2 /CH 4 (16.1) mixture separation at 273 K and 100 kPa achieves an ideal gas uptake-selectivity balance. Breakthrough experiments verified that it could effectively separate the above-mentioned mixtures under ambient conditions, and GCMC simulation provides a deep understanding of methoxy group functionalization. Undoubtedly, this work not only realizes controllable regulation of gas adsorption behavior but also proves the validity of improving selectivity by alkoxy groups in those platforms with high gas-uptake potential to overcome the trade-off barrier.

Drug rotation (cycling), in which multiple drugs are administrated alternatively, has the potential for limiting resistance evolution in pathogens. The frequency of drug alternation could be a major factor to determine the effectiveness of drug rotation. Drug rotation practices often have low frequency of drug alternation, with an expectation of resistance reversion. Here we, based on evolutionary rescue and compensatory evolution theories, suggest that fast drug rotation can limit resistance evolution in the first place. This is because fast drug rotation would give little time for the evolutionarily rescued populations to recover in population size and genetic diversity, and thus decrease the chance of future evolutionary rescue under alternate environmental stresses. We experimentally tested this hypothesis using the bacterium Pseudomonas fluorescens and two antibiotics (chloramphenicol and rifampin). Increasing drug rotation frequency reduced the chance of evolutionary rescue, and most of the finally surviving bacterial populations were resistant to both drugs. Drug resistance incurred significant fitness costs, which did not differ among the drug treatment histories. A link between population sizes during the early stages of drug treatment and the end-point fates of populations (extinction vs survival) suggested that population size recovery and compensatory evolution before drug shift increase the chance of population survival. Our results therefore advocate fast drug rotation as a promising approach to reduce bacterial resistance evolution, which in particular could be a substitute for drug combination when the latter has safety risks., (© 2023 European Society for Evolutionary Biology.)

The syntheses and magnetic properties of organometallic heterometallic compounds [K(THF) 6 ]{Co I [(μ 3 -HAN)RE 2 Cp* 4 ] 2 } (1-RE) and [K(Crypt)] 2 {Co I [(μ 3 -HAN)RE 2 Cp* 4 ] 2 } (2-RE) containing hexaazatrinaphthylene radicals (HAN⋅ 3- ) and four rare earth (RE) ions are reported. 1-RE shows isolable species with ligand-based mixed valency as revealed by cyclic voltammetry (CV) thus leading to the isolation of 2-RE via one-electron chemical reduction. Strong electronic communication in mixed-valency supports stronger overall ferromagnetic behaviors in 2-RE than 1-RE containing Gd and Dy ions. Ac magnetic susceptibility data reveal 1-Dy and 2-Dy both exhibit slow magnetic relaxation. Importantly, larger coercive field was observed in the hysteresis of 2-Dy at 2.0 K, indicating the enhanced SMM behavior compared with 1-Dy. Ligand-based mixed-valency strategy has been used for the first time to improve the magnetic coupling in lanthanide (Ln) SMMs, thus opening up new ways to construct strongly coupled Ln-SMMs., (© 2023 Wiley-VCH GmbH.)

An ideal adsorbent for separation requires optimizing both storage capacity and selectivity, but maximizing both or achieving a desired balance remain challenging. Herein, a de-linker strategy is proposed to address this issue for metal-organic frameworks (MOFs). Broadly speaking, the de-linker idea targets a class of materials that may be viewed as being intermediate between zeolites and MOFs. Its feasibility is shown here by a series of ultra-microporous MOFs (SNNU-98-M, M=Mn, Co, Ni, Zn). SNNU-98 exhibit high volumetric C 2 H 2 uptake capacity under low and ambient pressures (175.3 cm 3  cm -3 @ 0.1 bar, 222.9 cm 3  cm -3 @ 1 bar, 298 K), as well as extraordinary selectivity (2405.7 for C 2 H 2 /C 2 H 4 , 22.7 for C 2 H 2 /CO 2 ). Remarkably, SNNU-98-Mn can efficiently separate C 2 H 2 from C 2 H 2 /CO 2 and C 2 H 2 /C 2 H 4 mixtures with a benchmark C 2 H 2 /C 2 H 4 (1/99) breakthrough time of 2325 min g -1 , and produce 99.9999 % C 2 H 4 with a productivity up to 64.6 mmol g -1 , surpassing values of reported MOF adsorbents., (© 2023 Wiley-VCH GmbH.)

Precise design of low-cost, efficient and definite electrocatalysts is the key to sustainable renewable energy. Herein, this work develops a targeted-anchored and subsequent spontaneous-redox strategy to synthesize nickel-iron layered double hydroxide (LDH) nanosheets anchored with monodispersed platinum (Pt) sites (Pt@LDH). Intermediate metal-organic frameworks (MOF)/LDH heterostructure not only provides numerous confine points to guarantee the stability of Pt sites, but also excites the spontaneous reduction for Pt II . Electronic structure, charge transfer ability and reaction kinetics of Pt@LDH can be effectively facilitated by the monodispersed Pt moieties. As a result, the optimized Pt@LDH that with the 5% ultra-low content Pt exhibits the significant increment in electrochemical water splitting performance in alkaline media, which only afford low overpotentials of 58 mV at 10 mA cm -2 for hydrogen evolution reaction (HER) and 239 mV at 10 mA cm -2 for oxygen evolution reaction (OER), respectively. In a real device, Pt@LDH can drive an overall water-splitting at low cell voltage of 1.49 V at 10 mA cm -2 , which can be superior to most reported similar LDH-based catalysts. Moreover, the versatility of the method is extended to other MOF precursors and noble metals for the design of ultrathin LDH supported monodispersed noble metal electrocatalysts promoting research interest in material design., (© 2023 Wiley-VCH GmbH.)

Simple, fast, and sensitive detection of trace water in organic solvents is an urgent requirement for chemical industries. Herein, combining the unusual excited-state intramolecular proton transfer (ESIPT) mechanism with the effective strategy of pore space partition, for the first time, we construct a powerful fluorescent metal-organic framework (SNNU-301) probe with excellent water stability. The SNNU-301 probe shows a remarkable performance for turn-on ESIPT-based fluorescence response to water in nine common organic solvents, exhibiting wide linear ranges, low limit of detection values, and ultrafast response, especially in dimethyl sulfoxide (0-5.2%; 0.011%, v/v; 110 s). The typical ESIPT-sensitive linker 2,5-dihydroxyterephthalate (DHBDC) imparts it with discriminative detection properties via enol-keto tautomerism, and light-responsive triangular tri(pyridin-4-yl)-amine (TPA) realizes pore space partition. The theoretical calculation gives an in-depth explanation about the proton transfer mechanism. Comparative experiments and GCMC simulation provide evidence that the synergy of the ESIPT process and TPA of the framework further boosts its performance effectively. Definitely, this work not only offers a promising candidate with fast detection speed, high sensitivity, excellent universality, and visual observation for the determination of water in organic solvents but also provides valuable guidance for the design of high-performance fluorescent probes.

It is well known that the introduction of exposed fluorine (F) sites into metal-organic frameworks (MOFs) can effectively promote acetylene (C 2 H 2 ) adsorption via C-H⋯F hydrogen bonds. However, such super strong hydrogen bonding interactions usually lead to very high acetylene adsorption enthalpy and thus require more energy during the adsorbent regeneration process. As the same group elements, chlorine (Cl), bromine (Br) and iodine (I) also can act as hydrogen bond acceptors but with relatively weak forces. So, it is speculated that the decoration of Cl, Br or I sites on the pore surface of MOF adsorbents may enhance acetylene adsorption but with lower energy consumption. Herein, ultra-microporous MOFs constructed by Cu 4 X 4 (X = Cl, Br, I) motifs and 1,2,4-triazolate linkers, namely, [Cu 8 X 4 (TRZ) 4 ] n (TRZ = 3,5-diethyl-1,2,4-triazole or detrz for SNNU-313-X, and 3,5-dipropyl-1,2,4-triazole or dptrz for SNNU-314-X), provide an ideal platform to investigate the effect of C-H⋯X (X = Cl, Br, I) hydrogen bonding on C 2 H 2 adsorption and purification performance. Benefiting from the small pore size and pore environment, the C 2 H 2 uptake and separation properties of this series of MOFs are systematically regulated. Detailed gas adsorption results show that with the same organic linker, the C 2 H 2 uptake and separation (C 2 H 2 /C 2 H 4 and C 2 H 2 /CO 2 ) performance decrease clearly with the electronegativity of halogen ions (SNNU-313-Cl > SNNU-313-Br > SNNU-313-I). With the same halogen ion, the gas adsorption decreases with the bulk of decorated alkyl groups (SNNU-313-Cl > SNNU-314-Cl). Remarkably, SNNU-313/314 series MOF adsorbents exhibit moderate C 2 H 2 uptake capacity and high separation ability, but the C 2 H 2 adsorption enthalpies are much lower than those of MOF materials with exposed F sites. Dynamic fixed-bed column breakthrough experiments and Grand Canonical Monte Carlo (GCMC) simulations further indicate the critical effects of halogen hydrogen bonds on acetylene adsorption and separation. Overall, this work demonstrated an effective regulation of acetylene adsorption and separation by rational C-H⋯X hydrogen bonding, which may provide a new route for the exploration of energy-efficient acetylene adsorbent materials.

The spatiotemporal phase transformation during hot stamping would considerably effect the microstructure and mechanical properties of steels. In order to manufacture hot-stamping components of ultra-high-strength steel with tailored mechanical properties, the effect of the quenching time and the temperature of the die on the phase-transformation characteristics and mechanical property of ultra-high-strength steel was deeply studied. A finite element (FE) model coupled with a thermomechanical phase was employed to perform a succession of simulations for hot stamping corresponding to different quenching times and the temperatures of die, and the corresponding hot stamping experiments were performed. The 3D mapping surfaces of the temperature; quenching time; and three microstructures, namely austenite, bainite, and martensite, were constructed, and the mapping relationships in such surfaces were further explained by microstructural observations. Subsequently, based on the test results of the mechanical properties, the relationship curves of hardness and tensile strength, hardness, and elongation at break were fitted respectively, and then the 3D mapping surfaces were constructed for hardness, tensile strength, and elongation at break, which varied with the temperature die and quenching time. Finally, the quenching parameters of the automobile B-pillar were designed according to the constructed mapping relationship, and the hot-stamping FE simulation of the automobile B-pillar was developed. The result shows that those constructed mapping surfaces are helpful for adjusting the local mechanical property of the steels by designing the parameters.

Within the grain boundary engineering (GBE) of alloys, a mixed grain boundary network with random grain boundaries interrupted by twin boundaries, contributes to enhancing the overall grain boundary-related properties. The higher density of twin boundaries is pursued herein. Furthermore, a two-stage deformation method, i.e., prior cold deformation followed by thermal deformation, was proposed for improving the mixed grain boundary network in the thermal deformation of Ni80A superalloy. The influence of prior cold deformation on the mixed grain boundary network was investigated through a series of two-stage deformation experiments. The analysis of the stress-strain curves shows that the critical strain for dynamic recrystallization (DRX) and peak strains decrease significantly under the effect of prior cold deformation. In comparison to the necklace-like microstructures that occur after a single thermal deformation, the microstructures apparent after a two-stage deformation are characterized by finer DRX grains with abundant Σ3 n twin boundaries, with a significantly improved density of the Σ3 n twin boundaries (BLD Σ3 n ) by a factor of around nine. With increasing prior cold strain, the grain size, after a two-stage deformation, decreases continuously, while the BLD Σ3 n increases firstly and then decreases. The mechanisms for improving the mixed grain boundary network via two-stage deformation were uncovered. The sub-grain boundaries formed in prior cold deformation stimulate the nucleation of DRX grains and twins; meanwhile, the driving force for grain boundary migration is enhanced due to prior stored energy. Then, DRX is activated in advance and occurs more completely, thereby promoting the formation of Σ3 n twin boundaries.

Electric upsetting has been widely employed to manufacture the preformed workpiece of large-scale exhaust valves. The temperature field in the electric upsetting process plays an important role in microstructure evolution and defect formation. In order to uncover the temperature evolution in a larger-scale electric upsetting process, the electric-thermal-mechanical multi-field coupling finite element model was developed to simulate the electric upsetting forming process of Ni80A superalloy. The temperature distribution characteristics and their formation mechanisms under different stages were analyzed systematically. Results indicate that at the preheating stage, the billet temperature increases from 20 °C to 516.7 °C, and the higher temperature region firstly appears at the contact surface between billet and anvil due to the combined effects of contact resistance and volume resistance. With increasing preheating time, the higher temperature region is transferred to the interior of the billet because the contact resistance is reduced with increasing temperature. As for the forming process, the billet is gradually deformed into an onion shape. The highest billet temperature increases to 1150 °C and keeps relatively constant. The high temperature region always appears at the neck of the onion due to the relatively higher current density at this place. It enlarges continuously in the primary stage and intermediate stage, and then decreases at the stable deformation stage. The low temperature regions lie in the contact surface and the outer surface of the onion because a lot of heat is lost to the anvil and surroundings through thermal conduction and radiation. Finally, the established finite element model was verified by an actual electric upsetting experiment. The average relative error between simulated temperatures and experimental ones was estimated as 7.54%. The longitudinal and radial errors between simulated onion shape and the experimental one were calculated as 1.38% and 2.70%, respectively.

The capture and fixation of CO 2 under mild conditions is a cost-effective route to reduce greenhouse gases, but it is challenging because of the low conversion and selectivity issues. Metal-organic frameworks (MOFs) are promising in the fields of adsorption and catalysis because of their structural tunability and variability. However, the precise structural design of MOFs is always pursued and elusive. In this work, a metal-mixed MOF (SNNU-97-InV) was designed by precisely introducing single vanadium site into the isostructural In-MOF (SNNU-97-In). The single V sites clearly change the interactions between the MOF framework and CO 2 molecules, leading to a 71.3% improvement in the CO 2 adsorption capacity. At the same time, the enhanced light absorption enables SNNU-97-InV to efficiently convert CO 2 into cyclic carbonates (CCs) with epoxides under illumination. Controlled experiments showed that the promoted performance of SNNU-97-InV may be that the V═O site can more easily combine with CO 2 and convert them into an intermediate state under illumination, and the possible mechanism was thus speculated.

Describing the dynamic recrystallization (DRX) behaviors and grain evolution mechanisms in the hot forming process contributes to controlling microstructures and enhancing mechanical properties of materials. Here, the isothermal compression experiments for SAE 5137H steel were conducted under temperatures of 1123-1483 K and strain rates of 0.01-10 s -1 . The DRX kinetics models, including DRX volume fraction and grain size models, and the meso-scale cellular automaton (CA) models, were established based on the obtained true stress-strain curves and microstructure observation results. In order to dynamically reveal DRX behaviors and grain morphology evolution, a multi-field and multi-scale coupling finite element (FE) model for the hot compression process was developed by embedding the solved DRX kinetics models and CA models. Results show that the DRX volume fraction and grain size increase with temperature increasing and strain rate decreasing. The DRX grains are easier to nucleate at the initial grain boundaries. As strain increases, DRX grains grow up by devouring the matrix grains until DRX occurs completely. The microstructures after compression are composed of equiaxed DRX grains. Finally, the comparisons of grain size between experimental results and simulation results were performed. The mean relative errors between experimental results and predicted results from DRX kinetics models, and between experimental results and predicted results from CA models, were evaluated as 6.5% and 6.0%, respectively. It proves that the developed FE model can well describe the microstructure evolution in the hot deformation process of SAE 5137H steel., Competing Interests: The authors declare no conflicts of interest.

The development of paraffin-selective adsorbents is desirable but extremely challenging because adsorbents usually prefer olefin over paraffin. Herein, a new pore-window-partition strategy is proposed for the rational design of highly efficient paraffin-preferred metal-organic framework (MOF) adsorbents. The power of this strategy is demonstrated by stepwise installations of linear bidentate N-donor linkers into a prototype MOF (SNNU-201) to produce a series of partitional MOF adsorbents (SNNU-202-204). With continuous pore-window partitions from SNNU-201 to SNNU-204, the isosteric heat of adsorption can be tuned from -34.4 to -19.4 kJ mol -1 for ethylene and from -25.5 to -20.7 kJ mol -1 for ethane. Accordingly, partitional MOFs exhibit much higher ethane adsorption capacities, especially for SNNU-204 (104.6 cm 3 g -1 ), representing nearly 4 times as much ethane as the prototypical counterpart (SNNU-201; 27.5 cm 3 g -1 ) under ambient conditions. The C 2 H 6 /C 2 H 4 ideal adsorbed solution theory selectivity, dynamic breakthrough experiments, and theoretical simulations further indicate that pore-window partition is a promising and universal strategy for the exploration of highly efficient paraffin-selective MOF adsorbents.

In thermal deformation of materials, grain refinement induced by dynamic recrystallization (DRX) is often pursued to obtain excellent mechanical properties. Here, the thermal deformation behaviors of SAE 5137H steel were investigated and characterized at temperature and strain rate range of 1123-1483 K and 0.01-10 s -1 . Meanwhile, a design approach in speed-loading paths for grain refinement during current-heating compression was proposed, and these paths are linked to a typical three-dimensional (3D) response surface. Depending on the acquired stress-strain curves, the flow behaviors of this steel were analyzed and the typical 3D processing map was constructed to clarify the stable processing parameter domains during the continuous deformation process. Then, by the typical 3D processing map and microstructure observation, the 3D deformation mechanism map was constructed to connect the processing parameters and microstructural mechanisms. Subsequently, the 3D activation energy map was constructed to evaluate these deformation mechanisms, and the enhanced deformation mechanism map was constructed. Eventually, based on the enhanced deformation mechanism map, the speed-loading paths for SAE 5137H steel during current-heating compression were designed and they are mapped in a 3D response surface.

Rational exploration of efficient, inexpensive, and robust electrocatalysts is critical for the efficient water splitting. Conjugated conductive metal-organic frameworks (cMOFs) with multicomponent layered double hydroxides (LDHs) to construct bifunctional heterostructure catalysts are considered as an efficient but complicated strategy. Here, the fabrication of a cMOF/LDH hetero-nanotree array catalyst (CoNiRu-NT) coupled with monodispersed ruthenium (Ru) sites via a controllable grafted-growth strategy is reported. Rich-amino hexaiminotriphenylene linkers coordinate with the LDH nanotrunk to form cMOF nanobranches, providing numerous anchoring sites to precisely confine and stabilize RuN 4 sites. Moreover, monodispersed and reduced Ru moieties facilitate H 2 O adsorption and dissociation, and the heterointerface between the cMOF and the LDH further modifies the chemical and electronic structures. Optimized CoNiRu-NT displays a significant increase in electrochemical water-splitting properties in alkaline media, affording low overpotentials of 22 mV at 10 mA cm -2 and 255 mV at 20 mA cm -2 for the hydrogen evolution reaction and oxygen evolution reaction, respectively. In an actual electrochemical system, CoNiRu-NT drives an overall water splitting at a low cell voltage of 1.47 V to reach 10 mA cm -2 . This performance is comparable to that of pure noble-metal-based materials and superior to most reported MOF-based catalysts., (© 2022 Wiley-VCH GmbH.)

High storage capacity, high separation selectivity, and high structure stability are essential for an idea gas adsorbent. However, it is not easy to achieve all three at the same time, even for the promising metal-organic framework (MOF) adsorbents. We demonstrate herein that robust [Sc 3 O]-organic frameworks could be regulated by a micropore combination strategy for high-performance acetylene adsorption. Under the same solvent system with formic acid as a modulator, similar tritopic ligands extend [Sc 3 O(COO) 6 ] trigonal-prismatic clusters to generate SNNU-5-Sc and SNNU-150-Sc adsorbents. Notably, the two Sc-MOFs can keep their architectures over 24 h in water at different pH values (2-12) or at 90 °C. Modulated by the linker symmetry, the final stacking metal-organic polyhedral cages produce open window sizes of about 10 Å for SNNU-5-Sc and 5 Å + 7 Å for SNNU-150-Sc. Due to such micropore combinations, SNNU-5-Sc exhibits a top-level C 2 H 2 uptake of 211.2 cm 3 g -1 (1 atm and 273 K) and SNNU-150-Sc shows high C 2 H 2 /CH 4 , C 2 H 2 /C 2 H 4 , and C 2 H 2 /CO 2 selectivities of 80.65, 4.03, and 8.19, respectively, under ambient conditions. Dynamic breakthrough curves obtained on a fixed-bed column and grand canonical Monte Carlo (GCMC) simulations further support their prominent acetylene storage and purification performance. High framework stability, storage capacity, and separation selectivity make SNNU-5-Sc and SNNU-150-Sc ideal acetylene adsorbents in practical applications.

Objectives: To study the phenomenon of pulmonary hypostasis in corpses of various causes of death, and to explore the potential value of this phenomenon in assisting forensic pathological diagnosis of drowning., Methods: A total of 235 cases with clear cause of death through systematic autopsy were collected from January 2011 to June 2021 in Guangzhou. According to the location of body discovery, the cases were divided into the water body group (97 cases) and the non - water body group (138 cases), and the water body group was further divided into the water drowning group (90 cases) and the water non - drowning group (7 cases). Non-water body group was further divided into the non - water drowning group (1 case) and the non - water non - drowning group (137 cases). Three senior forensic pathologists independently reviewed autopsy photos to determine whether there was hypostasis in the lungs. The detection rate of pulmonary hypostasis was calculated., Results: The detection rate of pulmonary hypostasis in the water drowning group (90 cases) was 0, and the negative rate was 100%. The detection rate of pulmonary hypostasis in the water non - drowning group (7 cases) was 100% and the negative rate was 0. The detection rate of pulmonary hypostasis in the water body group and in the non - water body group (after excluding 2 cases, 136 cases were calculated) was 7.22% and 87.50%, respectively. There were statistically significant differences in the detection rate of pulmonary hypostasis between water body group and non - water body group, and between water drowning group and water non - drowning group ( P <0.05)., Conclusions: The disappearance of pulmonary hypostasis can be used as a specific cadaveric sign to assist in the forensic pathological diagnosis of drowning.

Bi 5 O 7 I belongs to the family of bismuth oxyhalides (BiOX, X = Cl, Br, I), having a unique layered structure with an internal electrostatic field that promotes the separation and transfer of photo-generated charge carriers. Interestingly, Bi 5 O 7 I exhibits higher thermal stability compared to its other BiOX member compounds and absorption spectrum extended to the visible region. Bi 5 O 7 I has demonstrated applications in diverse fields such as photocatalytic degradation of various organic pollutants, marine antifouling, etc. Unfortunately, owing to its wide band gap of ∼2.9 eV, its absorption lies mainly in the ultraviolet region, and a tiny portion of absorption lies in the visible region. Due to limited absorption, the photocatalytic performance of pure Bi 5 O 7 I is still facing challenges. In order to reduce the band gap and increase the light absorption capability of Bi 5 O 7 I, doping and formation of heterostructure strategies have been employed, which showed promising results in the photocatalytic performance. In addition, the plasmonic heterostructures of Bi 5 O 7 I were also developed to further boost the efficiency of Bi 5 O 7 I as a photocatalyst. Here, in this review article, we present such recent efforts made for the advanced development of Bi 5 O 7 I regarding its synthesis, properties and applications. The strategies for photocatalytic performance enhancement have been discussed in detail. Moreover, in the conclusion section, we have presented the current challenges and discussed possible prospective developments in this field., (Copyright © 2021 Elsevier Ltd. All rights reserved.)

In this study, the reaction mechanism underlying the green synthesis of glutaric acid was studied via joint test technology. Density functional theory calculations were used to verify the mechanism. Quantitative analysis of glutaric acid via infrared spectroscopy and HPLC was established. The linear correlation between the two methods was good, from 0.01 to 0.25 g mL -1 . The analysis results of the two methods were consistent as the reaction progressed., Competing Interests: There are no conflicts to declare., (This journal is © The Royal Society of Chemistry.)

Refined microstructures achieved by cyclic heat treatment significantly contribute to improving the wear resistance of steels. To acquire the refined microstructures of 65Mn low-alloy steel, first, the specimens were solid solution-treated; then, they were subjected to cyclic heat treatment at cyclic quenching temperatures of 790-870 °C and quenching times of 1-4 with a fixed holding time of 5 min. The mechanical properties of 65Mn low-alloy steel in terms of hardness, tensile strength, elongation and wear resistance were characterized. Afterwards, the effect of cyclic heat treatment on microstructure evolution and the relationships between grain refinement and mechanical properties' improvement were discussed. The results show that the average grain size firstly decreased and then increased with the increase in the quenching temperature. Hardness increased with grain refinement when the temperature was lower than 830 °C. Once the temperature exceeded 830 °C, hardness increased with the temperature increase owing to the enrichment of carbon content in the martensite. With the increase in cyclic quenching times, hardness continuously increased with grain refinement strengthening. In addition, both tensile strength and elongation could be significantly improved through grain refinement. The relationships among wear loss, hardness and average grain size showed that wear resistance was affected by the synthesis reaction of grain refinement and hardness. Higher hardness and refined grain size contributed to improving the wear resistance of 65Mn low-alloy steel.

By employing a tetraphenylethylene (TPE)-based tetracarboxylate linker, tetrakis(4-carboxyphenyl)ethylene (H 4 TCPE), we herein constructed a novel luminescent Mn-MOF based on a rare [Mn 4 (μ 3 -OH) 2 ] cluster (SQNU-55). Interestingly, the TPE-based SQNU-55 not only provides a good material for the blue LED device, but also has a better luminescent molecular thermometer for low-temperature detection.

Acetylene (C 2 H 2 ) purification is of great importance for many chemical synthesis and processes. Metal-organic frameworks (MOFs) are widely used for gas adsorption and separation due to their variable structure and porosity. However, the exploitation of ideal MOF adsorbents for C 2 H 2 keeps a challenging task. Herein, a combination of open metal sites (OMSs) and Lewis basic sites (LBSs) in robust MOFs is demonstrated to effectively promote the C 2 H 2 purification performance. Accordingly, SNNU-37(Fe/Sc), two isostructural MOFs constituted by [Fe 3 O(COO) 6 ] or [Sc 3 O(COO) 6 ] trinuclear clusters and amide-functionalized tricarboxylate linkers, were designed with extra-stable 3,6-connected new architectures. Derived from the coexistence of high-density OMSs and LBSs, the C 2 H 2 adsorption amounts of SNNU-37(Fe/Sc) are much higher than those values for C 2 H 4 and CO 2 . Theoretical IAST selectivity values of SNNU-37(Fe) are 2.4 for C 2 H 2 /C 2 H 4 (50/50, v/v) and 9.9 for C 2 H 2 /CO 2 (50/50, v/v) at 298 K and 1 bar, indicating an excellent C 2 H 2 separation ability. Experimental breakthrough curves also revealed that SNNU-37(Fe) could effectively separate C 2 H 2 /C 2 H 4 and C 2 H 2 /CO 2 under ambient conditions. GCMC simulations further indicate that open Fe or Sc sites and amide groups mainly contribute to stronger adsorption sites for C 2 H 2 molecules.

In order to obtain the desired mechanical properties of products, an innovative method of loading parameter designs for acquiring the desired grain refinement is proposed, and it has been applied in the compression process of Ni80A superalloy. The deformation mechanism maps derived from processing maps based on the Dynamic Materials Model (DMM) theory were constructed, since the critical indicator values corresponding to dynamic recrystallization (DRX) and dynamic recovery (DRV) mechanisms were determined. The processing-parameter domains with DRX mechanisms were separated from the deformation mechanism map, while such domains were chaotic and difficult to apply in innovative parameter loading path design. The speed-loading path derived from strain rate-loading path in a compression process was pursued. The grain refinement domains are discretized into a finite series of sub-domains with clear processing parameters, and the optimal strain rate of each sub-domain is determined by step-by-step finite element simulation. A 3D response surface of the innovative optimal loading path of strain rate was fitted by interpolating methods. Finally, the isothermal compression experiments for Ni80A superalloy were conducted, and the microstructure observations indicated that the desired grain refinement was achieved. This innovative method of parameter loading path design contributes to the microstructure adjustment of the alloys with DRX mechanism.

High-quality CoP nanorings (CoP NRs) are easily achieved using a phosphorating treatment of CoOOH nanorings, and reveal high activity towards the hydrogen evolution reaction and the nitrate electrocatalytic reduction reaction due to substantial coordinately unsaturated active sites, a high surface area, and available mass transfer pathways. Consequently, the CoP NRs can achieve a faradaic efficiency of 97.1% towards NO 3 - -to-NH 3 conversion and provide an NH 3 yield of 30.1 mg h -1 mg -1 cat at a -0.5 V potential.

Acyclovir (ACV) is an effective and selective antiviral drug, and the study of its toxicology and the use of appropriate detection techniques to control its toxicity at safe levels are extremely important for medicine efforts and human health. This review discusses the mechanism driving ACV's ability to inhibit viral coding, starting from its development and pharmacology. A comprehensive summary of the existing preparation methods and synthetic materials, such as 5-aminoimidazole-4-carboxamide, guanine and its derivatives, and other purine derivatives, is presented to elucidate the preparation of ACV in detail. In addition, it presents valuable analytical procedures for the toxicological studies of ACV, which are essential for human use and dosing. Analytical methods, including spectrophotometry, high performance liquid chromatography (HPLC), liquid chromatography/tandem mass spectrometry (LC-MS/MS), electrochemical sensors, molecularly imprinted polymers (MIPs), and flow injection-chemiluminescence (FI-CL) are also highlighted. A brief description of the characteristics of each of these methods is also presented. Finally, insight is provided for the development of ACV to drive further innovation of ACV in pharmaceutical applications. This review provides a comprehensive summary of the past life and future challenges of ACV.

Intraspecific competition for limited niches has been recognized as a driving force for adaptive radiation, but results for the role of interspecific competition have been mixed. Here, we report the adaptive diversification of the model bacteria Pseudomonas fluorescens in the presence of different numbers and combinations of four competing bacterial species. Increasing the diversity of competitive community increased the morphological diversity of focal species, which is caused by impeding the domination of a single morphotype. Specifically, this pattern was driven by more diverse communities being more likely to contain key species that occupy the same niche as otherwise competitively superior morphotype, and thus preventing competitive exclusion within the focal species. Our results suggest that sympatric adaptive radiation is driven by the presence or absence of niche-specific competitors., (Copyright © 2021 Chu, Zhang, Buckling and Castledine.)

Since the discovery of liquid-phase-exfoliated black phosphorus (BP) as a field-effect transistor in 2014, BP, with its 2D layered structure, has attracted significant attention, owing to its anisotropic electroconductivity, tunable direct bandgap, extraordinary surface activity, moderate switching ratio, high hole mobility, good biocompatibility, and biodegradability. Several pioneering research efforts have explored the application of BP in different types of electrochemical sensors. This review summarizes the latest synthesis methods, protection strategies, and electrochemical sensing applications of BP and its derivatives. The typical synthesis methods for BP-based crystals, nanosheets, and quantum dots are discussed in detail; the degradation of BP under ambient conditions is introduced; and state-of-the-art protection methodologies for enhancing BP stability are explored. Various electrochemical sensing applications, including chemically modified electrodes, electrochemiluminescence sensors, enzyme electrodes, electrochemical aptasensors, electrochemical immunosensors, and ion-selective electrodes are discussed in detail, along with the mechanisms of BP functionalization, sensing strategies, and sensing properties. Finally, the major challenges in this field are outlined and future research avenues for BP-based electrochemical sensors are highlighted., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2021 Elsevier B.V. All rights reserved.)

The use of lytic bacteriophages for treating harmful bacteria (phage therapy) is faced with the challenge of bacterial resistance evolution. Phage strains with certain traits, for example, rapid growth and relatively broad infectivity ranges, may enjoy an advantage in slowing bacterial resistance evolution. Here, we show the possibility for laboratory selection programs ("evolutionary training") to yield phage genotypes with both high growth rate and broad infectivity, traits between which a trade-off has been assumed. We worked with a lytic phage that infects the bacterium Pseudomonas fluorescens and adopted three types of training strategies: evolution on susceptible bacteria, coevolution with bacteria, and rotation between evolution and coevolution phases. Overall, there was a trade-off between growth rate and infectivity range in the evolved phage isolates, including those from the rotation training programs. A small number of phages had both high growth rate and broad infectivity, and those trade-off-overcoming phages could slow or even completely prevent resistance evolution in initially susceptible bacterial populations. Our findings show the promise of well-designed evolutionary training programs, in particular an evolution/coevolution rotation selection regime, for obtaining therapeutically useful phage materials., Competing Interests: None declared., (© 2021 The Authors. Evolutionary Applications published by John Wiley & Sons Ltd.)

Biological populations may survive lethal environmental stress through evolutionary rescue. The rescued populations typically suffer a reduction in growth performance and harbor very low genetic diversity compared with their parental populations. The present study addresses how population size and within-population diversity may recover through compensatory evolution, using the experimental adaptive radiation of bacterium Pseudomonas fluorescens . We exposed bacterial populations to an antibiotic treatment and then imposed a one-individual-size population bottleneck on those surviving the antibiotic stress. During the subsequent compensatory evolution, population size increased and leveled off very rapidly. The increase of diversity was of slower paces and persisted longer. In the very early stage of compensatory evolution, populations of large sizes had a greater chance to diversify; however, this productivity-diversification relationship was not observed in later stages. Population size and diversity from the end of the compensatory evolution was not contingent on initial population growth performance. We discussed the possibility that our results be explained by the emergence of a "holey" fitness landscape under the antibiotic stress., Competing Interests: None declared., (© 2021 The Authors. Ecology and Evolution published by John Wiley & Sons Ltd.)

Background: Mutation accumulation (MA) has profound ecological and evolutionary consequences. One example is that accumulation of conditionally neutral mutations leads to fitness trade-offs among heterogenous habitats which cause population divergence. Here we suggest that temperature, which controls the rates of all biochemical and biophysical processes, should play a crucial role for determining mutational effects. Particularly, warmer temperatures may mitigate the effects of some, not all, deleterious mutations and cause stronger environmental dependence in MA effects., Results: We experimentally tested the above hypothesis by measuring the growth performance of ten Escherichia coli genotypes on six carbon resources across ten temperatures, where the ten genotypes were derived from a single ancestral strain and accumulated spontaneous mutations. We analyzed resource dependence of MA consequences for growth yields. The MA genotypes typically showed reduced growth yields relative to the ancestral type; and the magnitude of reduction was smaller at intermediate temperatures. Stronger resource dependence in MA consequences for growth performance was observed at higher temperatures. Specifically, the MA genotypes were more likely to show impaired growth performance on all the six carbon resources when grown at lower temperatures; but suffered growth performance loss only on some, not all the six, carbon substrates at higher temperatures., Conclusions: Higher temperatures increase the chance that MA causes conditionally neutral fitness effects while MA is more likely to cause fitness loss regardless of available resources at lower temperatures. This finding has implications for understanding how geographic patterns in population divergence may emerge, and how conservation practices, particularly protection of diverse microhabitats, may mitigate the impacts of global warming.

As one of the most powerful natural antioxidants, astaxanthin (Ax) has begun to be applied to the field of reproductive biology. Here we used porcine oocyte as a model to explore how Ax improves the oocyte potential during in vitro maturation (IVM), and we also investigated the cytoprotective effects of Ax on the vitrified oocytes. Ax supplementation (final concentration of 2.5 μM) was subjected for immature oocytes during vitrification and subsequent IVM; fresh oocytes were also matured in vitro in the presence or absence of 2.5 μM Ax. Our results showed that Ax significantly increased the survival rate of vitrified oocytes, and promoted the blastocyst yield of both fresh and vitrified oocytes after parthenogenetic activation and somatic cell nuclear transfer. The oocytes treated with Ax displayed significantly lower reactive oxygen species generation and higher glutathione level. Vitrification of oocytes had no impact on caspase-3, cathepsin B and autophagic activities; Ax significantly decreased the cathepsin B activity in both fresh and vitrified oocytes. Moreover, the relative fluorescence intensity of lysosomes was significantly increased in vitrified oocytes, which was recovered by Ax treatment. The mitochondrial activity did not differ between fresh and vitrified oocytes, and was significantly enhanced in Ax-treated oocytes. Furthermore, Ax significantly restored the decreased expression of BMP15, ZAR1, POU5F1, GPX4 and LAMP2 genes in vitrified oocytes. Both fresh and vitrified oocytes treated with Ax showed significantly higher mRNA levels of GDF9, POU5F1, SOD2, NRF2 and ATG5. Taken together, this study provides new perspectives in understanding the mechanisms by which Ax improves the developmental competence of both fresh and vitrified porcine oocytes., Competing Interests: Declaration of competing interest The authors declare no conflict of interest in the publication of this research article., (Copyright © 2021 Elsevier Inc. All rights reserved.)

We report a new sensing mechanism based on an indium-dihydroxyterephthalic acid metal-organic framework (MOF, SNNU-153), in which the spatially fitted analyte-MOF hydrogen-bond (H-bond) formation provides selective recognition while the analyte-H-bond assisted excited-state intramolecular proton transfer (ESIPT) and the resulting ratiometric emission act as a superior signal transducer with ultrafast response. The synergy of ESIPT signal transduction and confined MOF pore enables the SNNU-153 sensor selectively sensing hydrazine even among nitrogen-containing hydride analogs such as NH 3 , NH 2 OH, and (Me) 2 NNH 2 . The key of H-bond and associated ESIPT was further counter evidenced by an indium-2,5-dimethoxyterephthalic acid MOF (SNNU-152), where the hydroxyl protons were removed by methylation, showing near inertness to N 2 H 4 . The new molecular recognition concept thus makes SNNU-153 a powerful N 2 H 4 sensor, which should be far-reaching to other sensing elements.