Two-Dimensional Nanoarchitectonics of End-on Oligomers with Versatile Structures and Tunable Negative Differential Resistance.

Maximizing the molecular information density requires simultaneously functionalizing distinct monomers and their coupling connections. However, current synthesis generally focuses on distinct monomers rather than coupling reactions because the multistep reactions significantly escalate the synthetic complexity in an exponential increase. Here, we report the two-dimensional nanoarchitectures (2DNs) of end-on oligomers, with versatile molecular structures and negative differential resistance (NDR), synthesized by programmed and surface-initiated step electrosynthesis based on the simultaneous utilization of six reactions including cross- and homocouplings.

Correction: Polydopamine-capped AgNPs as a novel matrix overcoming the ion suppression of phosphatidylcholine for MALDI MS comprehensive imaging of glycerophospholipids and sphingolipids in impact-induced injured brain.

Correction for 'Polydopamine-capped AgNPs as a novel matrix overcoming the ion suppression of phosphatidylcholine for MALDI MS comprehensive imaging of glycerophospholipids and sphingolipids in impact-induced injured brain' by Chao Han , , 2019, , 6304-6312, https://doi.org/10.1039/C9AN01361J.

Correction: Open-flow microperfusion combined with mass spectrometry for liver lipidomic analysis.

Correction for 'Open-flow microperfusion combined with mass spectrometry for liver lipidomic analysis' by Tuo Li , , 2021, , 1915-1923, https://doi.org/10.1039/D0AN02189J.

Nanoarchitectonics on Electrosynthesis and Assembly of Conjugated Metallopolymers.

In contrast to edge-on and face-on orientations, end-on uniaxial conjugated polymers have the theoretical possibility of providing a macroscopic crystalline film. However, their fabrication is insurmountable due to sluggishly thermodynamic equilibrium states. Herein, we report the programmatic pathway to fabricate nanoarchitectonics on end-on uniaxial conjugated metallopolymers by surface-initiated simultaneous electrosynthesis and assembly.

Measurement of degree of hydrolysis and molecular weight distribution of protein hydrolysates by liquid chromatography-mass spectrometry.

Enzymatic hydrolysis of milk protein is an effective way to improve protein digestibility, to reduce their allergenicity and to produce peptides with better functionalities. Among the process, the degree of hydrolysis (DH) and molecular weight distribution (MWD) of protein hydrolysates are two important parameters that need to be monitored. In this work, a new method based on liquid chromatography-mass spectrometry (LC-MS) was developed for the first time to accurately detect the DH and the MWD of proteolytic peptides.

Composition and sequence-controlled conductance of crystalline unimolecular monolayers.

Understanding how the charge travels through sequence-controlled molecules has been a formidable challenge because of simultaneous requirements in well-controlled synthesis and well-manipulated orientation. Here, we report electrically driven simultaneous synthesis and crystallization as a general strategy to study the conductance of composition and sequence-controlled unioligomer and unipolymer monolayers. The structural disorder of molecules and conductance variations on random positions can be extremely minimized, by uniform synthesis of monolayers unidirectionally sandwiched between electrodes, as an important prerequisite for the reproducible measurement on the micrometer scale.

Liposomes embedded with PEGylated iron oxide nanoparticles enable ferroptosis and combination therapy in cancer.

Ferroptosis, an iron-dependent regulated cell death process driven by excessive lipid peroxides, can enhance cancer vulnerability to chemotherapy, targeted therapy and immunotherapy. As an essential upstream process for ferroptosis activation, lipid peroxidation of biological membranes is expected to be primarily induced by intrabilayer reactive oxygen species (ROS), indicating a promising strategy to initiate peroxidation by improving the local content of diffusion-limited ROS in the lipid bilayer. Herein, liposomes embedded with PEG-coated 3 nm γ-FeO nanoparticles in the bilayer (abbreviated as Lp-IO) were constructed to promote the intrabilayer generation of hydroxyl radicals (•OH) from hydrogen peroxide (HO), and the integration of amphiphilic PEG moieties with liposomal bilayer improved lipid membrane permeability to HO and •OH, resulting in efficient initiation of lipid peroxidation and thus ferroptosis in cancer cells.

Crystalline Unipolymer Monolayer with High Modulus and Conductivity.

The synthesis of crystalline polymer with a well-defined orientated state and a two-dimensional crystalline size beyond a micrometer will be essential to achieve the highest physical feature of polymer material but remain challenging. Herein, we show the synthesis of the crystalline unipolymer monolayer with an unusual ultrahigh modulus that is higher than the ITO substrate and high conductance by simultaneous electrosynthesis and manipulation. We find that the polymer monolayer has fully extended in the vertical and unidirectional orientation, which is proposed to approach their theoretically highest density, modulus, and conductivity among all aggregation formations of the current polymer.

Abplatin inhibited tumor growth on a patient derived cancer model of hepatocellular carcinoma and its comparative multi-omics study with cisplatin.

Background: Cisplatin, the alkylating agent of platinum(II) (Pt(II)), is the most common antitumor drug in clinic; however, it has many side effects, therefore it is higly desired to develop low toxicity platinum(IV) (Pt(IV)) drugs. Multi-omics analysis, as a powerful tool, has been frequently employed for the mechanism study of a certain therapy at the molecular level, which might be helpful for elucidating the mechanism of platinum drugs and facilitating their clinical application.

Methods: Strating form cisplatin, a hydrophobic Pt(IV) prodrug (CisPt(IV)) with two hydrophobic aliphatic chains was synthesized, and further encapsulated with a drug carrier, human serum albumin (HSA), to form nanoparticles, namely AbPlatin.

Real-time analysis of metabolites in vivo by online extraction electrospray ionization mass spectrometry coupled to microdialysis.

In vivo and real-time analysis could reflect a more real biological state, which was of great significance to the study of complex life processes. In this work, we constructed an online extraction electrospray ionization (OE-ESI) ion source as the interface of microdialysis and mass spectrometry, which realized real-time analysis of metabolites in vivo without sample pretreatment process. The ion source was consisted of three coaxial capillaries, and the parameters of the ion source were optimized.

Quantitative Lipidomics and Spatial MS-Imaging Uncovered Neurological and Systemic Lipid Metabolic Pathways Underlying Troglomorphic Adaptations in Cave-Dwelling Fish.

Sinocyclocheilus represents a rare, freshwater teleost genus endemic to China that comprises the river-dwelling surface fish and the cave-dwelling cavefish. Using a combinatorial approach of quantitative lipidomics and mass-spectrometry imaging (MSI), we demonstrated that neural compartmentalization of lipid distribution and lipid metabolism is associated with the evolution of troglomorphic traits in Sinocyclocheilus. Attenuated docosahexaenoic acid (DHA) biosynthesis via the Δ4 desaturase pathway led to reductions in DHA-phospholipids in cavefish cerebellum.

A dual-mode strategy combining SERS with MALDI FTICR MS based on core-shell silver nanoparticles for dye identification and semi-quantification in unearthed silks from Tang Dynasty.

Silk, as one of the representative artifacts of China, profoundly affects the communication between eastern and western civilizations, and dyes, as the color support of silks, reflected crucial historical, cultural and technological information. Surface enhanced Raman spectroscopy (SERS) characterized by vibrational information has been extensively employed in dye analysis. However, since natural plants with complex coloring compositions in ancient China were broadly applied in dying textiles, the existing SERS methods often misinterpret results in dye analysis.

Design and Application of Near-Infrared Nanomaterial-Liposome Hybrid Nanocarriers for Cancer Photothermal Therapy.

Liposomes are attractive carriers for targeted and controlled drug delivery receiving increasing attention in cancer photothermal therapy. However, the field of creating near-infrared nanomaterial-liposome hybrid nanocarriers (NIRN-Lips) is relatively little understood. The hybrid nanocarriers combine the dual superiority of nanomaterials and liposomes, with more stable particles, enhanced photoluminescence, higher tumor permeability, better tumor-targeted drug delivery, stimulus-responsive drug release, and thus exhibiting better anti-tumor efficacy.

An Integrated Transcriptomics and Proteomics Analysis Implicates lncRNA MALAT1 in the Regulation of Lipid Metabolism.

Long noncoding RNA metastasis-associated lung adenocarcinoma transcript 1 (MALAT1) is upregulated in various cancers, and its overexpression is associated with tumor growth and metastasis. MALAT1 has been recognized as a key player in the regulation of RNA splicing and transcription; however, the landscape of gene expression regulated by MALAT1 remains unclear. In this study, we employed an integrated transcriptomics and proteomics strategy to characterize the alterations in gene expression induced by MALAT1 knockdown in hepatocellular carcinoma (HCC) cells and identified 2662 differentially expressed transcripts and 1149 differentially expressed proteins.

Distribution of perfluorooctane sulfonate in mice and its effect on liver lipidomic.

Perfluorooctane sulfonate (PFOS) is an emerging persistent organic pollutant (POP), and the harm caused by the enrichment of PFOS in living organism has attracted more and more attention. In this work, animal exposure model to PFOS was established. Mass spectrometry (MS), mass spectrometry imaging (MSI), hematoxylin and eosin (H&E) staining and lipidomics were combined for the study of the organ targeting of PFOS, the toxicity and possible mechanism caused by PFOS.

Open-flow microperfusion combined with mass spectrometry for in vivo liver lipidomic analysis.

At present, conventional microdialysis (MD) techniques cannot efficiently sample lipids in vivo, possibly due to the high mass transfer resistance and/or the serious adsorption of lipids onto the semi-permeable membrane of a MD probe. The in vivo monitoring of lipids could be of great significance for the study of disease development and mechanisms. In this work, an open-flow microperfusion (OFM) probe was fabricated, and the conditions for sampling lipids via OFM were optimized.

Neutral Human Milk Oligosaccharides Are Associated with Multiple Fixed and Modifiable Maternal and Infant Characteristics.

We aimed to identify if maternal and infant factors were associated with neutral human milk oligosaccharides (HMOs) variability and examined the associations between HMOs concentration and infant growth and disease status in healthy Chinese mothers over a 6-month lactation period. We recruited mothers and their full-term infants as our subjects. At 1-5 days, 8-14 days, 4 weeks, and 6 months postpartum, all participants were interviewed to collect breast milk samples, obtain follow-up data and measure infant length and weight at their local hospital.

Co-Incorporated Mesoporous Carbon Material-Assisted Laser Desorption/Ionization Ion Source as an Online Interface of In Vivo Microdialysis Coupled with Mass Spectrometry.

The combination of microdialysis and mass spectrometry (MS) provides the potential for rapidly monitoring diverse metabolites in vivo. Unfortunately, the high concentration of salt in biological microdialysates hindered the sensitive and online detection of these small molecular compounds. In this study, we synthesized Co-incorporated mesoporous carbon material (Co-NC) and developed a Co-NC-assisted laser desorption/ionization (LDI) ion source as an online interface of in vivo microdialysis coupled with MS for the direct analysis of diverse metabolites in microdialysates.

Developing IR-780 as a Novel Matrix for Enhanced MALDI MS Imaging of Endogenous High-Molecular-Weight Lipids in Brain Tissues.

The matrix plays a prominent role in expanding the ability of matrix assisted laser desorption/ionization mass spectrometry (MALDI MS). However, on account of the unclarity of necessary properties of the matrix in MALDI MS, development of a new matrix is still in the exploratory stage and lacks systematic theoretical guidance. Meanwhile, most of the existing matrices are unable to simultaneously detect various high-molecular-weight (high-MW) lipids including (poly-)phosphoinositides, cardiolipins, and gangliosides.

Polydopamine-capped AgNPs as a novel matrix overcoming the ion suppression of phosphatidylcholine for MALDI MS comprehensive imaging of glycerophospholipids and sphingolipids in impact-induced injured brain.

Matrix-assisted laser desorption/ionization mass spectrometry imaging (MALDI MSI) is a powerful tool for the characterization and localization of analytes without the need for extraction, purification, separation or labeling of samples. However, in tissue sections the most abundant lipids, phosphatidylcholines (PCs), could suppress the signals of other classes of coexisting lipids. In this work, polydopamine (PDA)-capped AgNPs (AgNPs@PDA) were synthesized as a matrix of MALDI MSI to analyze lipids in both positive and negative ion modes.

Combination of electrospray deposition technology of TiO nanoparticles and MALDI FTICR MSI for identification of fingerprint morphology and latent components.

In fingerprint recognition, besides the physical shape information afforded by fingerprint enhancement techniques (FET), in recent years, more and more efforts are focused on researching the chemical composition of a fingerprint residue. In this work, electrospray deposition method was elaborately used to softly and homogenously deposit the physical enhancers of FET, TiO nanoparticles (TiO NPs), onto fingerprints. The results showed that this type of deposition was nondestructive to the fingerprint morphology and provided the physical shape information containing all level features.