Latest ArticlesAs key biomarkers, amyloid-β (Aβ) plaques are frequently used to diagnose Alzheimer's disease (AD). Although fluorescence imaging has proven to be effective in detecting these plaques, the gold standard probe thioflavin T (ThT), used for Aβ aggregates, cannot be applied in vivo owing to its invasive nature. Therefore, the development of novel fluorescent probes capable of identifying Aβ plaques in situ is necessary. Based on the ThT structure, two π-conjugated heterocyclic D-π-A probes were designed bearing the hydroxytricyanopyrrole acceptor and N,N-dimethylaminophenyl donor. These probes exhibited red to near-infrared fluorescence emission (λmax = 732 nm), large Stokes shifts (>100 nm), exceptional signal-to-noise ratio, rapid response (<30 s), and high binding affinity (NT-HTCP = 33.32 nmol/L; NF-HTCP = 53.35 nmol/L) for Aβ aggregates. As the best candidate, NT-HTCP was used for in situ imaging of Aβ plaques in AD mouse models. Furthermore, in vivo research demonstrated that NT-HTCP could cross the blood–brain barrier and continue imaging the Aβ plaques with a good signal-to-noise ratio. Additionally, the outcomes of the docking computations helped guide the development of the Aβ probes. This study expands the family of N,N-dimethylaminophenyl-based Aβ-sensitive fluorophores, with NT-HTCP emerging as a highly promising imaging agent.
Mechanochromophores based on bichromic molecular switches, such as bis-naphthopyanes, allow multimodal mechanochromic behavior beyond the typical binary response from single chromophores, which is important for distinguishing between multiple stress states through discrete changes in color. Spontaneously generated persistent and distinguishable multi-colors from activated bis-naphthopyanes remain challenging. And the versatility of bis-mechanophore design for advanced optical molecular systems and the fundamental insights into the corresponding mechano-reactivity are not enough. Here, we identify a dihydroanthracene bridged bis-naphthopyrans as a multimodal mechanochromophore in polymers. Bridging two pyrans with the sterically constrained dihydroanthracene is helpful to control the steric effect for the favorable formation of a distinctly appreciable bis-merocyanine (bis-MC) product. By varying the length of the polymer chains, the force delivered to the mechanophore is modulated, resulting in a gradient change in the relative distribution of two distinctly colored MC products and a multicolor mechanochromism. Mechanical activation of this bis-naphthopyanes proceeds via a mechanistically distinct pathway compared to the photochemical process. In addition, the bulk films can also achieve pronounced color changes when subjected to mechanical force. This study thus further expands the molecular diversity of mechanochromophores and tune the multimodal switch properties of bis-naphthopyrans based polymers.
The dynamic RNA modifications have been viewed as new posttranscriptional regulator in modulating gene expression as well as in a broad range of physiological processes. N1-methyladenosine (m1A) is one of the most prevalent modifications existing in multiple types of RNAs. In-depth investigation of the functions of m1A requires the site-specific assessment of m1A stoichiometry in RNA. Herein, we established a demethylase-assisted method (DA-m1A) for the site-specific detection and quantification of m1A in RNA. N1-methyl group in m1A could result in the stalling of reverse transcription at m1A site, thus producing the truncated cDNA. E. coli AlkB is a demethylase that can demethylate m1A to produce adenine in RNA, thus generating full-length cDNA from AlkB-treated RNA. Evaluation of the produced amounts of full-length cDNA by quantitative real-time PCR can achieve the site-specific detection and quantification of m1A in RNA. With the DA-m1A method, we examined and successfully confirmed the previously well-characterized m1A sites in various types of RNAs with low false positive rate. In addition, we found that the level of m1A was significantly decreased at the bromodomain containing 2 (BRD2) mRNA position 1674 and CST telomere replication complex component 1 (CTC1) mRNA position 5643 in human hepatocellular carcinoma tissues. The results suggest that these two m1A sites in mRNA may be involved in liver tumorigenesis. Taken together, the DA-m1A method is simple and enables the rapid, cost-effective, and site-specific detection and quantification of m1A in RNA, which provides a valuable tool to decipher the functions of m1A in human diseases.
Integrated CO2 capture and conversion of (ICCC) is one of the most effective solutions to reduce anthropogenic CO2 emissions, which has attracted extensive public attention. Dual functional materials (DFMs), including adsorbent and catalyst, are the key components to achieve ICCC. Magnesium oxide (MgO) is an ideal adsorbent for ICCC, since it is characterized by high theoretical adsorption capacity, low cost, low energy consumption and extensive sources. It can also be used as DFMs in combination with the Ni catalysts. MgO not only can act as an adsorbent in DFMs but also enhance the catalytic performance of Ni. This review summarizes the advantages and modification methods of MgO as adsorbent and the influence of its adsorption conditions on the adsorption performance. Moreover, the important role of MgO in facilitating the catalytic conversion of CO2 is highlighted. Future research focuses are proposed for the development of MgO based DFMs with high adsorption capacity, high stability, conversion, and selectivity as well as low cost and energy consumption.
The present study reported fabrication of novel carbon quantum dots-MnFe2O4@ZIF-8 (CQDs-MFO@ZIF-8) by using co-precipitation hydrothermal method for activation of peroxydisulfate (PDS) to degrade bisphenol A (BPA), one of important emerging organic pollutants in water environment. CQDs-MFO@ZIF-8 served as a highly efficient thermal activated PDS catalyst with high catalytic degradation efficiency, reusability and stability. The catalyst achieved almost completely removal of 20.0 mg/L BPA within 5.0 min, and the degradation efficiency remained higher than 83% after 5 consecutive cycles. Free radicals (•OH, SO4•− and •O2−) and non-free radicals (1O2) were generated in the thermal PDS-activation system, in which singlet oxygen (1O2) played a dominant role in the degradation of BPA. The potential toxicity of BPA degradation intermediates was analyzed upon the culture of E. coli and Chlorella sorokiniana by using Ecological Structure-Activity Relationship Model (ECOSAR) program. The catalytic performances of BPA degradation by CQDs-MFO@ZIF-8 were evaluated for treatment of different practical water samples to further verify the feasibility of practical applications. This study provides proof-in-concept demonstration of new nanomaterials for enhanced catalytic water decontamination.
As the most common pathological type of nephrotic syndrome, membranous nephropathy (MN) presents diversity in progression trends, facing severe complications. The precise discrimination of MN from healthy people, other types of nephrotic syndrome or those with therapeutic remission has always been huge challenge in clinics, not to mention comprehensive individualized monitoring relied on minimally invasive molecular detection means. Herein, we construct a functionalized pore architecture to couple with machine learning to aid all-round peptidome enrichment and data profiling from hundreds of human serum samples, and finally establish a set of defined peptide panel consisting of 12 specific feature signals. In addition to the realization of above-mentioned precise discrimination with more than 97% of sensitivity, 88% of accuracy and f1 score, the simultaneously comprehensive individualized monitoring for MN can also be achieved, including conventionally screening diagnosis, congeneric distinction and prognostic evaluation. This work greatly advances the development of peptidome data-driven individualized monitoring means for complex diseases and undoubtedly inspire more devotion into molecular detection field.
Borylation of 1,3-enynes with bis(boronate) compounds often ends up with the formation of hydroborylated products, leaving the diborylation of 1,3-enynes for the formation of 1,4-diborylated allenes to be challenging. Herein, a copper-catalyzed chemo-, regio-, and stereo-selective diborylation of 1,3-enynes for the efficient construction of 1,4-diborylated allenes under base-free conditions was reported. A wide range of 1,3-enynes bearing various functional groups can participant in the reaction and afforded the corresponding 1,4-diborylated allenes in good to excellent yields, which was enabled by the protocol of Bpin to BF3K conversion. the borylcopper species was supposed to selectively attack the C–C triple bond of the 1,3-enynes.
In September 2018, we proposed the cutting-edge concept of "Beyond Limits Manufacturing" (BLM). BLM technology is based on the three-dimensional inner engraving or precise outer engraving of ultra-fast laser, to invent micro/nano scale flow chips or devices, which makes it possible for the microform, integration, economy, safety, high efficiency, green and intelligence of research, development and manufacturing process, so as to realize transformational manufacturing in the era of Industry 4.0. In this paper, we reviewed the representative results we made in the field of micro/nano flow chemistry during the implementation of the BLM major project (December 2019 to August 2023), and discussed its application prospects in micro/nano flow chemistry.
Thin-film composite (TFC) reverse osmosis (RO) membranes have attracted considerable attention in water treatment and desalination processes due to their specific separation advantages. Nevertheless, the trade-off effect between water flux and salt rejection poses huge challenges to further improvement in TFC RO membrane performance. Numerous research works have been dedicated to optimizing membrane fabrication and modification for addressing this issue. In the meantime, several reviews summarized these approaches. However, the existing reviews seldom analyzed these methods from a theoretical perspective and thus failed to offer effective optimization directions for the RO process from the root cause. In this review, we first propose a mass transfer model to facilitate a better understanding of the entire process of how water and solute permeate through RO membranes in detail, namely the migration process outside the membrane, the dissolution process on the membrane surface, and the diffusion process within the membrane. Thereafter, the water and salt mass transfer behaviors obtained from model deduction are comprehensively analyzed to provide potential guidelines for alleviating the trade-off effect between water flux and salt rejection in the RO process. Finally, inspired by the theoretical analysis and the accurate identification of existing bottlenecks, several promising strategies for both regulating RO membranes and optimizing operational conditions are proposed to further exploit the potential of RO membrane performance. This review is expected to guide the development of high-performance RO membranes from a mass transfer theory standpoint.
The virtual cocrystal screening approach based on molecular electrostatic potential surface (MEPS) maps is a fast and feasible computational method to estimate the probability of cocrystal formation by calculating the difference in the interaction site pairing energies of monomers and that of their assemblies prior to experimental screening. In this paper, we report 12 cocrystal forms of temozolomide with mono-, di-, and trihydroxy benzoic acids, namely, 3-hydroxy-, 2,4-dihydroxy-, 2,5-dihydroxy-, 2,6-dihydroxy-, 3,4-dihydroxy-, and 3,4,5-trihydroxy-benzoic acids, as well as benzoic acid, as pharmaceutical coformers for the first time. 10 single crystals out of the 12 cocrystal forms were obtained and unequivocally determined by single-crystal X-ray diffraction, which clarified spatial arrangements, molecular conformations, and supramolecular synthons. MEPS further gains some insights into the sites of hydrogen bonding interactions for exploring combination patterns in these assemblies. Modulated stability of TMZ was successfully achieved by cocrystallization with these acids.
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