Due to the intricate structure of catalysts, traditional catalyst design relies on iterative trial-and-error experiments. We have systematically established a catalyst design strategy to evaluate the performance of NH3-SCO reactions from the perspective of DFT calculations. Specifically, we used the catalyst formation energy as a stability descriptor and the adsorption energies of NH3, NH2, and O p-band center as performance descriptors, we identified the four most promising catalysts among 45 kinds of doped SnO2 catalysts. Subsequently, experimental validation was performed to demonstrate the outstanding consistency between the DFT-driven descriptors and the stability and catalytic performance of the catalyst. Particularly, the Ce doping resulted in a 175 °C reduction in the T90 compared to the SnO2 catalyst. It is noteworthy that Ce doping promotes the cycling between oxygen vacancies and lattice oxygen, which contributes primarily to the enhancement of O2 activation capability and, consequently, the improvement in catalytic activity.

Developing flame retardant and UV-blocking polylactide (PLA) with reinforced mechanical properties is important but challenging. Herein, bio-derived phytic acid was decorated on halloysite nanotube though silane grafting, ring-opening reaction with melamine and then electrostatic interactions with phytic acid. The obtained phopsphorous-nitrogen-silicon decorated halloysite nanotube (PNSiHNT) was incorporated into PLA to prepare PLA composites. The surface modification significantly improved the compatibility between PNSiHNT and PLA, and the flame retardant, UV-shielding and mechanical properties of the composites were enhanced. At 5% mass loading, the peak heat release and total heat release were reduced by 18% and 12% compared to pure PLA, respectively, superior to most phytic acid-based flame retardants. The relevant mechanism analysis showed that PNSiHNT can restrain the emission of combustible volatiles and promote the formation of protective char layer. Moreover, the flame-retardant PLA showed excellent UV-shielding ability with an ultraviolet protection factor (UPF) value of around 120. Due to the reinforcing effect of PNSiHNT and the strong interfacial interactions between PNSiHNT and PLA matrix, the PLA/PNSiHNT showed 77% and 116% increase in tensile strength and elongation at break compared to the bulk PLA. This study provides a strategy for designing bio-derived organic/inorganic systems for enhancing flame retardant, UV-blocking and reinforced PLA.

Artificial photosynthetic diluted CO2 reduction directly driven by natural sunlight is a challenging, but promising way to realize carbon-resources recycling utilization. Herein, a three-in-one photocatalytic system of CO2 enrichment, CO2 reduction and H2 O oxidation sites is designed for diluted CO2 reduction. A Zn-Salen-based covalent organic framework (Zn-S-COF) with oxidation and reductive sites is synthesized; then, ionic liquids (ILs) are loaded into the pores. As a result, [Emim]BF4 @Zn-S-COF shows a visible-light-driven CO2 -to-CO conversion rate of 105.88µmol g-1 h-1 under diluted CO2 (15%) atmosphere, even superior than most photocatalysts in high concentrations CO2 . Moreover, natural sunlight driven diluted CO2 reduction rate also reaches 126.51µmol g-1 in 5h. Further experiments and theoretical calculations reveal that the triazine ring in the Zn-S-COF promotes the activity of H2 O oxidation and CO2 reduction sites, and the loaded ILs provide an enriched CO2 atmosphere, realizing the efficient photocatalytic activity in diluted CO2 reduction.

AbstractThe purpose of model transfer is to solve the problem that multivariate calibration models cannot be shared among different near‐infrared spectrometers. Taking gasoline as the research object, the transfer analysis of its octane number model was carried out. The gasoline samples collected by two near‐infrared spectrometers of the same type were used as the research object. The screening wavelengths with consistent and stable signals (SWCSS) combined with competitive adaptive reweighted sampling (CARS), uninformative variable elimination (UVE), and successive projections algorithm (SPA) were used to reduce the adverse effects of invalid wavelengths in the SWCSS method; therefore, the analysis ability of the master model to the slave samples was improved. Partial least squares regression (PLSR) models based on SWCSS‐UVE, SWCSS‐CARS, and SWCSS‐SPA algorithms were established, and comparison was made between their analytical capabilities for slave samples and those of SWCSS, direct standardization (DS) algorithm , piecewise direct standardization (PDS) algorithm, and slope/bias (S/B) algorithm. The results shown that the SWCSS‐UVE and SWCSS‐CARS methods can be used to establish models from the 231 and 6 wavelengths selected from the consistent wavelengths, respectively. The root mean square error of prediction (RMSEP) of the gasoline octane number (RON) content of the direct analysis of the spectrum measured by the slave machine was reduced from 5.7490 to 0.3226 and 0.3250, respectively, which was better than the single SWCSS and DS, PDS, and SWCSS‐SPA methods, and was close to the model transfer accuracy of the S/B algorithm. The transfer accuracy of SWCSS‐UVE and SWCSS‐CARS was not much different, but the wavelength variable involved in the model transfer of the latter was much smaller than that of the former, and the AIC value of SWCSS‐CARS was −59.59, which was much smaller than the akaike information criterion (AIC) value of SWCSS‐UVE 398.42.

Various risk factors of Alzheimer’s disease (AD) are known, such as advanced age, possession of certain genetic variants, accumulation of toxic amyloid-β (Aβ) peptides, and unhealthy lifestyle. An estimate of heritability of AD ranges from 0.13 to 0.25, indicating that its phenotypic variation is accounted for mostly by non-genetic factors. DNA methylation is regarded as an epigenetic mechanism that interfaces the genome with non-genetic factors. The Tg2576 mouse model has been insightful in AD research. These transgenic mice express a mutant form of human amyloid precursor protein linked to familial AD. At 9–13 months of age, these mice show elevated levels of Aβ peptides and cognitive impairment. The current literature lacks integrative multiomics of the animal model. We applied transcriptomics and DNA methylomics to the same brain samples from ~ 11-month-old transgenic mice. We found that genes involved in extracellular matrix structures and functions are transcriptionally upregulated, and genes involved in extracellular protein secretion and localization are differentially methylated in the transgenic mice. Integrative analysis found enrichment of GO terms related to memory and synaptic functionability. Our results indicate a possibility of transcriptional modulation by DNA methylation underlying AD neuropathology.

Histamine plays pivotal role in normal physiology and dysregulated production of histamine or signaling through histamine receptors (HRH) can promote pathology. Previously, we showed that Bordetella pertussis or pertussis toxin can induce histamine sensitization in laboratory inbred mice and is genetically controlled by Hrh1/HRH1. HRH1 allotypes differ at three amino acid residues with P263-V313-L331 and L263-M313-S331, imparting sensitization and resistance respectively. Unexpectedly, we found several wild-derived inbred strains that carry the resistant HRH1 allotype (L263-M313-S331) but exhibit histamine sensitization. This suggests the existence of a locus modifying pertussis-dependent histamine sensitization. Congenic mapping identified the location of this modifier locus on mouse chromosome 6 within a functional linkage disequilibrium domain encoding multiple loci controlling sensitization to histamine. We utilized interval-specific single-nucleotide polymorphism (SNP) based association testing across laboratory and wild-derived inbred mouse strains and functional prioritization analyses to identify candidate genes for this modifier locus. Atg7, Plxnd1, Tmcc1, Mkrn2, Il17re, Pparg, Lhfpl4, Vgll4, Rho and Syn2 are candidate genes within this modifier locus, which we named Bphse, enhancer of Bordetella pertussis induced histamine sensitization. Taken together, these results identify, using the evolutionarily significant diversity of wild-derived inbred mice, additional genetic mechanisms controlling histamine sensitization.

The effect of the solvent environment is important for the activity and selectivity of a catalytic reaction conducted in the liquid phase. One must carefully consider the potential interactions between the solvent molecules and the reacting species as these interactions can alter mass transfer rates, reaction kinetics, product selectivity, and catalyst stability as well as the properties of the solvent including density and viscosity. As a result, these so-called solvation effects can induce a significant change in the catalytic performance. However, finding the perfect “marriage” between the solvent, reaction, and catalyst is difficult as only a few solvents can deliver the desired performance. Essentially, the best solvents to stabilize the reactants and products in the bulk might not be the optimal solvation environment for the catalyst. A promising approach could be to decouple the local reaction environment of the active sites from that of the solvent in the bulk. This can be achieved with a polymer coating that can induce a solvation effect near the active site. In this thesis, a thermal-responsive polymer (p-NIPAM) that has a lower critical solution temperature (LCST) has been employed as polymer coating on a model Pd/SiO2 catalyst to validate this concept. The effect of the solvent and polymer-induced solvation effects on the reaction selectivity and activity have been studied using the nitrite and nitrobenzene hydrogenation reactions as probe chemistries.