It is challenging to remove polar organic micropollutants from water through adsorption‐mediated processes. Macrocycle‐crosslinked polymers were recently shown to be effective adsorbents for nonpolar ...or charged organic micropollutants through specific host–guest binding, but are rarely used for the treatment of neutral and polar organic micropollutants. This is due to the challenge of recognizing polar molecules in water by macrocyclic hosts. In this research, we report two amide naphthotube‐crosslinked polymers which can effectively and rapidly adsorb a wide scope of polar organic micropollutants from water through biomimetic molecular recognition. Amide naphthotubes possess hydrogen bonding sites in their deep hydrophobic cavities and can effectively bind polar organic micropollutants in water through the hydrophobic effects and shielded hydrogen bonds. The cross‐linked polymers containing amide naphthotubes are even able to remove a complex mixture of organic micropollutants from water and the used materials can be easily regenerated through washing with MeOH or EtOH. This research provides a solution for the treatment of polar organic micropollutants by using biomimetic molecular recognition in water.
The cross‐linked polymers containing the biomimetic macrocyclic hosts, amide naphthotubes, are able to effectively and rapidly adsorb polar organic micropollutants from water by employing host–guest binding. The polymers can be readily regenerated through washing with MeOH or EtOH at room temperature.
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SBCE, SBMB, UL, UM, UPUK
Cuproptosis, a newly identified form of regulated cell death that is copper‐dependent, offers great opportunities for exploring the use of copper‐based nanomaterials inducing cuproptosis for cancer ...treatment. Here, a glucose oxidase (GOx)‐engineered nonporous copper(I) 1,2,4‐triazolate (Cu(tz)) coordination polymer (CP) nanoplatform, denoted as GOx@Cu(tz), for starvation‐augmented cuproptosis and photodynamic synergistic therapy is developed. Importantly, the catalytic activity of GOx is shielded in the nonporous scaffold but can be “turned on” for efficient glucose depletion only upon glutathione (GSH) stimulation in cancer cells, thereby proceeding cancer starvation therapy. The depletion of glucose and GSH sensitizes cancer cells to the GOx@Cu(tz)‐mediated cuproptosis, producing aggregation of lipoylated mitochondrial proteins, the target of copper‐induced toxicity. The increased intracellular hydrogen peroxide (H2O2) levels, due to the oxidation of glucose, activates the type I photodynamic therapy (PDT) efficacy of GOx@Cu(tz). The in vivo experimental results indicate that GOx@Cu(tz) produces negligible systemic toxicity and inhibits tumor growth by 92.4% in athymic mice bearing 5637 bladder tumors. This is thought to be the first report of a cupreous nanomaterial capable of inducing cuproptosis and cuproptosis‐based synergistic therapy in bladder cancer, which should invigorate studies pursuing rational design of efficacious cancer therapy strategies based on cuproptosis.
An enzyme‐engineered cupreous nanomaterial capable of inducing cuproptosis and cuproptosis‐based synergistic therapy in cancer cells is reported, which may invigorate studies pursuing rational design of effective cancer therapy strategies based on cuproptosis.
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SBCE, SBMB, UL, UM, UPUK
Although clinical studies have shown promise for targeting programmed cell death protein-1 (PD-1) and ligand (PD-L1) signaling in non-small cell lung cancer (NSCLC), the factors that predict which ...subtype patients will be responsive to checkpoint blockade are not fully understood.
We performed an integrated analysis on the multiple-dimensional data types including genomic, transcriptomic, proteomic, and clinical data from cohorts of lung adenocarcinoma public (discovery set) and internal (validation set) database and immunotherapeutic patients. Gene set enrichment analysis (GSEA) was used to determine potentially relevant gene expression signatures between specific subgroups.
We observed that
mutation significantly increased expression of immune checkpoints and activated T-effector and interferon-γ signature. More importantly, the
comutated subgroup manifested exclusive increased expression of PD-L1 and a highest proportion of
Meanwhile,
or
-mutated tumors showed prominently increased mutation burden and specifically enriched in the transversion-high (TH) cohort. Further analysis focused on the potential molecular mechanism revealed that
or
mutation altered a group of genes involved in cell-cycle regulating, DNA replication and damage repair. Finally, immunotherapeutic analysis from public clinical trial and prospective observation in our center were further confirmed that
or
mutation patients, especially those with co-occurring
mutations, showed remarkable clinical benefit to PD-1 inhibitors.
This work provides evidence that
and
mutation in lung adenocarcinoma may be served as a pair of potential predictive factors in guiding anti-PD-1/PD-L1 immunotherapy.
.
Research on biomarker-driven therapy and immune check-point blockade in non-small cell lung cancer (NSCLC) is rapidly evolving. The width and depth of clinical trials have also dramatically improved ...in an unprecedented speed. The personalized treatment paradigm evolved every year. In this review, we summarize the promising agents that have shifted the treatment paradigm for NSCLC patients across all stages, including targeted therapy and immunotherapy using checkpoint inhibitors. Based on recent evidence, we propose treatment algorithms for NSCLC and propose several unsolved clinical issues, which are being explored in ongoing clinical trials. The results of these trials are likely to impact future clinical practice.
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IZUM, KILJ, NUK, PILJ, PNG, SAZU, UL, UM, UPUK
Harnessing data to discover the underlying governing laws or equations that describe the behavior of complex physical systems can significantly advance our modeling, simulation and understanding of ...such systems in various science and engineering disciplines. This work introduces a novel approach called physics-informed neural network with sparse regression to discover governing partial differential equations from scarce and noisy data for nonlinear spatiotemporal systems. In particular, this discovery approach seamlessly integrates the strengths of deep neural networks for rich representation learning, physics embedding, automatic differentiation and sparse regression to approximate the solution of system variables, compute essential derivatives, as well as identify the key derivative terms and parameters that form the structure and explicit expression of the equations. The efficacy and robustness of this method are demonstrated, both numerically and experimentally, on discovering a variety of partial differential equation systems with different levels of data scarcity and noise accounting for different initial/boundary conditions. The resulting computational framework shows the potential for closed-form model discovery in practical applications where large and accurate datasets are intractable to capture.
Currently, developing nonprecious‐metal catalysts to replace Pt‐based electrocatalysts in fuel cells has become a hot topic because the oxygen reduction reaction (ORR) in fuel cells often requires ...platinum, a precious metal, as a catalyst, which is one of the major hurdles for commercialization of the fuel cells. Recently, the newly emerging metal‐organic frameworks (MOFs) have been widely used as self‐sacrificed precursors/templates to fabricate heteroatom‐doped porous carbons. Here, the recent progress of MOF‐derived, heteroatom‐doped porous carbon catalysts for ORR in fuel cells is systematically reviewed, and the synthesis strategies for using different MOF precursors to prepare heteroatom‐doped porous carbon catalysts, including the direct carbonization of MOFs, MOF and heteroatom source mixture carbonization, and MOF‐based composite carbonization are summarized. The emphasis is placed on the precursor design of MOF‐derived metal‐free catalysts and transition‐metal‐doped carbon catalysts because the MOF precursors often determine the microstructures of the derived porous carbon catalysts. The discussion provides a useful strategy for in situ synthesis of heteroatom‐doped carbon ORR electrocatalysts by rationally designing MOF precursors. Due to the versatility of MOF structures, MOF‐derived porous carbons not only provide chances to develop highly efficient ORR electrocatalysts, but also broaden the family of nanoporous carbons for applications in supercapacitors and batteries.
Metal‐organic frameworks (MOFs) have emerged as promising precursors to synthesize metal‐free or nonprecious‐metal‐doped porous carbon catalysts for the oxygen reduction reaction (ORR) due to their unique advantages. Here, the recent progress of MOF‐derived carbon catalysts in ORR applications is systematically reviewed and the strategies to develop highly efficient carbon electrocatalysts by rationally designing MOF precursors are summarized.
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SBCE, SBMB, UL, UM, UPUK
Non-precious metal and nitrogen codoped carbon catalysts have emerged as promising candidates to replace noble platinum (Pt)-based catalysts in the processes of the oxygen reduction reaction (ORR) ...and the hydrogen evolution reaction (HER). Herein, we use a 1D/2D hybrid strategy to synthesize a Co,N-codoped carbon nanotube (CNT)/graphene heterostructure bifunctional catalyst (Co/NCNT/NG). The Co/NCNT/NG heterostructure catalyst shows not only a positive half-wave potential of 0.85 V ( versus RHE) and long-term stability for the ORR, but also a low overpotential of 123 mV at a current density of 10 mA cm −2 and ultrahigh stability in 0.5 M H 2 SO 4 for the HER. The superior performance of the Co/NCNT/NG catalyst is attributed to the inimitable 1D/2D CNT/graphene heterostructure, in which 1D and 2D structures provide different catalytically active sites (including metallic Co, CoN 2 and N–C) for the HER and ORR, respectively. Moreover, the catalyst also exhibits similar discharge performance and robust durability as an air electrode in Zn–air batteries to the Pt-based one. This work provides a new approach for the in situ synthesis of bifunctional and multifunctional catalysts by integrating 1D/2D/3D materials with different catalytically active sites into one heterostructure.
Carbon dots (CDs) are photoluminescent nanomaterials with wide-ranging applications. Despite their photoactivity, it remains unknown whether CDs degrade under illumination and whether such ...photodegradation poses any cytotoxic effects. Here, we show laboratory-synthesized CDs irradiated with light degrade into molecules that are toxic to both normal (HEK-293) and cancerous (HeLa and HepG2) human cells. Eight days of irradiation photolyzes 28.6-59.8% of the CDs to <3 kilo Dalton molecules, 1431 of which are detected by high-throughput, non-target high-performance liquid chromatography-quadrupole time-of-flight mass spectrometry. Molecular network and community analysis further reveal 499 cytotoxicity-related molecules, 212 of which contain polyethylene glycol, glucose, or benzene-related structures. Photo-induced production of hydroxyl and alkyl radicals play important roles in CD degradation as affected by temperature, pH, light intensity and wavelength. Commercial CDs show similar photodegraded products and cytotoxicity profiles, demonstrating that photodegradation-induced cytotoxicity is likely common to CDs regardless of their chemical composition. Our results highlight the importance of light in cytocompatibility studies of CDs.
Although biomimetic designs are expected to play a key role in exploring future structural materials, facile fabrication of bulk biomimetic materials under ambient conditions remains a major ...challenge. Here, we describe a mesoscale "assembly-and-mineralization" approach inspired by the natural process in mollusks to fabricate bulk synthetic nacre that highly resembles both the chemical composition and the hierarchical structure of natural nacre. The millimeter-thick synthetic nacre consists of alternating organic layers and aragonite platelet layers (91 weight percent) and exhibits good ultimate strength and fracture toughness. This predesigned matrix-directed mineralization method represents a rational strategy for the preparation of robust composite materials with hierarchically ordered structures, where various constituents are adaptable, including brittle and heat-labile materials.
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