科研成果

Covalent organic frameworks (COFs) have great application potentials in photocatalytic water treatment. By using p-phenylenediamine with different numbers and locations of heterocyclic nitrogen atoms as a precursor, five types of COFs with different nitrogen positions were synthesized. We found that Cr(VI) photoreduction,Escherichia coli inactivation, and paracetamol degradation by COFs were heterocyclic nitrogen location-dependent. Particularly, the photocatalytic performance for all three tested pollutants by five types of COFs followed the order of the best performance for COF-PDZ with two ortho position heterocyclic N atoms, medium for COF-PMD with two meta position heterocyclic N atoms, and COF-PZ with two para position heterocyclic N atoms, and COF-PD with a single heterocyclic N atom, the worst performance for COF-1 without a heterocyclic N atom. Compared to the other COFs, COF-PDZ contained improved quantum efficiency and thus enhanced generation of electrons. The lower energy barriers and larger energy gaps of COF-PDZ contributed to its improved quantum efficiencies. The stronger affinity to Cr(VI) with lower adsorption energy of COF-PDZ also contributed to its excellent Cr(VI) reduction performance. By transferring into a more stable keto form, COF-PDZ showed great stability through five regeneration and reuse cycles. Overall, this study provided an insight into the synthesis of high-performance structure-dependent COF-based photocatalysts.

Covalent organic frameworks (COFs) have great application potentials in photocatalytic water treatment. By using p-phenylenediamine with different numbers and locations of heterocyclic nitrogen atoms as a precursor, five types of COFs with different nitrogen positions were synthesized. We found that Cr(VI) photoreduction,Escherichia coli inactivation, and paracetamol degradation by COFs were heterocyclic nitrogen location-dependent. Particularly, the photocatalytic performance for all three tested pollutants by five types of COFs followed the order of the best performance for COF-PDZ with two ortho position heterocyclic N atoms, medium for COF-PMD with two meta position heterocyclic N atoms, and COF-PZ with two para position heterocyclic N atoms, and COF-PD with a single heterocyclic N atom, the worst performance for COF-1 without a heterocyclic N atom. Compared to the other COFs, COF-PDZ contained improved quantum efficiency and thus enhanced generation of electrons. The lower energy barriers and larger energy gaps of COF-PDZ contributed to its improved quantum efficiencies. The stronger affinity to Cr(VI) with lower adsorption energy of COF-PDZ also contributed to its excellent Cr(VI) reduction performance. By transferring into a more stable keto form, COF-PDZ showed great stability through five regeneration and reuse cycles. Overall, this study provided an insight into the synthesis of high-performance structure-dependent COF-based photocatalysts. © 2021 American Chemical Society.

The gas adsorption hysteresis effects have strong implications for the characterization of the micropore structure, which is one of the most important properties of shales. This study describes one of the first investigations of low-pressure CO2 adsorption hysteresis illustrated on the Antrim Shale samples, Michigan Basin. A total of 23 samples were characterized by using a combination of X-Ray diffraction (XRD), Rock-Eval pyrolysis, scanning electron microscope (SEM) imaging and CO2 adsorption. The partial least linear regression (PLS) was employed to study the influence of rock composition on the micropore structures and hysteresis index (HI). The results showed that the micropore parameters (surface area and volume) are positively correlated to the amount of organic matter and clay minerals, and have a negative correlation to non-clay minerals. In the Antrim Shale samples, the CO2 adsorption hysteresis seen under low pressure appears to be controlled mainly by the pore network effect caused by the presence of ink-bottle shaped pores, rather than by the swelling of clays and organic matter.

Understanding the creep behavior of shale is essential to precisely predict borehole instability issues and model fracturing of unconventional shale reservoirs. In this study, the creep behavior of shale in micron scale is investigated by integrating the nano-dynamic mechanical analysis (nano-DMA) grid nanoindentation (15 × 15 indents) and data clustering techniques. The results showed that the creep displacement, the creep rate, and hardness, both can be related through a logarithmic function with creep time. Furthermore, contact creep modulus increased as the hardness or Young’s modulus increased. The clustering analysis revealed that three separate phases are present in the samples where Phase 1(clay/organic matter) has the smallest contact creep modulus and Phase 3 (quartz) the largest. While creep is in progress, the creep displacement, hardness and contact creep modulus of all three phases obey the logarithmic function. Under the same creep time, reduction in the contact creep modulus of Phase 3 appears to be faster than Phase 1 while the creep rate of Phase 3 is much less than Phase 1. Ultimately, contact creep modulus is better correlated with hardness than Young’s modulus.

This chapter assesses the 1926-1927 Uprising in Indonesia across several interconnected geographic and institutional scales: In the Comintern, where exiled leaders of the Partai Komunis Indonesia conferred with Comintern representatives about the situation at home; in the highest levels of the Politburo, where disagreements over revolutionary tactics in China exacerbated the power struggle between Stalin and Trotsky; and in Indonesia itself, where colonial repression inspired the abortive uprising. In so doing, this chapter shows how the Uprising demonstrated the limits of internationalism. As PKI leaders were unable to maintain effective contact with the movement in Indonesia, gaps in information undermined decision-making and led to conflict over the applicability of Russian models to the Indonesian context. Debates over Moscow’s China policy diverted attention from other territories and drew PKI members into the Stalin-Trotsky feud. Comintern support for the Uprising, therefore, did not materialize, further undermining the communist movement in Indonesia.

Traditional models of retinal system identification analyze the neural response to artificial stimuli using models consisting of predefined components. The model design is limited to prior knowledge, and the artificial stimuli are too simple to be compared with stimuli processed by the retina. To fill in this gap with an explainable model that reveals how a population of neurons work together to encode the larger field of natural scenes, here we used a deep-learning model for identifying the computational elements of the retinal circuit that contribute to learning the dynamics of natural scenes. Experimental results verify that the recurrent connection plays a key role in encoding complex dynamic visual scenes while learning biological computational underpinnings of the retinal circuit. In addition, the proposed models reveal both the shapes and the locations of the spatiotemporal receptive fields of ganglion cells.

The potential exposure of titanate nanotubes (TNTs) to wildlife and humans may occur as a result of increased use and application as functional nanomaterials. However, there is a dearth of knowledge regarding the pathways of uptake and excretion of TNTs and their toxicity in cells. In this study, three strains of the Tetrahymena genus of free-living ciliates, including a wild type strain (SB210) and two mutant strains (SB255: mucocyst-deficient; NP1: temperature-sensitive “mouthless’’), were used to study the pathways of uptake and excretion and evaluate the cytotoxicity of TNTs. The three Tetrahymena strains were separately exposed to 0, 0.01, 0.1, 1 or 10 mg/L of TNTs, and cells were collected at different time points for quantification of intracellular TNTs (e.g., 5, 10, 20, 40, 60, 90 and 120 min) and evaluation of cytotoxicity (12 and 24 h). TNT contents in NP1 and SB255 were greater or comparable to the contents in SB210 while exposure to 10 mg/L TNTs in 120 min. Furthermore, exposure to 10 mg/L TNTs for 24 h caused greater decreases in cell density of NP1 (38.2 %) and SB255 (36.8 %) compared with SB210 (26.5 %) and upregulated the expression of caspase 15 in SB210. Taken together, our results suggested that TNT uptake by pinocytosis and excretion by exocytosis in Tetrahymena, and the exposure could cause cytotoxicity which can offer novel insights into the accumulation kinetics of nanotubes and even nanomaterials in single cell.

Abstract Despite the recent decrease in pollution events in Chinese urban areas, the World Health Organization air quality guideline values are still exceeded. Observations from monitoring networks show a stronger decrease of organic aerosol directly emitted to the atmosphere relative to secondary organic aerosol (SOA) generated from oxidation processes. Here, the uptake of water-soluble gas-phase oxidation products is reported as a major SOA contribution to particulate pollution in Beijing, triggered by the increase of aerosol liquid water. In pollution episodes, this pathway is enough to explain the increase in SOA mass, with formaldehyde, acetaldehyde, glycolaldehyde, formic, and acetic acid alone explaining 15 to 25% of the SOA increase. Future mitigation strategies to reduce non-methane volatile organic compound emissions should be considered to reduce organic particulate pollution in China.

Abstract Despite the recent decrease in pollution events in Chinese urban areas, the World Health Organization air quality guideline values are still exceeded. Observations from monitoring networks show a stronger decrease of organic aerosol directly emitted to the atmosphere relative to secondary organic aerosol (SOA) generated from oxidation processes. Here, the uptake of water-soluble gas-phase oxidation products is reported as a major SOA contribution to particulate pollution in Beijing, triggered by the increase of aerosol liquid water. In pollution episodes, this pathway is enough to explain the increase in SOA mass, with formaldehyde, acetaldehyde, glycolaldehyde, formic acid, and acetic acid alone explaining 15%–25% of the SOA increase. Future mitigation strategies to reduce non-methane volatile organic compound emissions should be considered to reduce organic particulate pollution in China.