Latest ArticlesAs one of the most promising adoptive T-cell therapies, chimeric antigen receptor T-cell (CAR-T) therapy has acquired Food and Drug Administration (FDA) approval for a variety of products and has been used successfully in the treatment of malignant hematological tumors. CAR-T therapy, on the other hand, faces a number of obstacles in the field of solid tumor therapy that limit its widespread clinical implementation. Significant advances in nanoparticle research in cancer therapy and immunotherapy have been made in recent years, providing novel strategies to address the challenges encountered by CAR-T therapy in the treatment of solid tumors. This review commences with a comprehensive explanation of the basic framework of CAR-T therapy as well as the challenges it faces in the treatment of solid tumors. Subsequently, we encapsulate a summary of the developmental research combining nanoparticles with CAR-T cells for the treatment of solid tumors, which includes gene transfection, cell activation and expansion, targeted infiltration, immune escape inhibition, and combination with other therapies. Coupled with the overview of the research progress, a discussion has been initiated on the challenges and perspectives of CAR-T based on nanoparticles.
Water contamination by tetracycline (TC) has emerged as an environmental concern owing to its widespread use and antibiotic resistance. Application of peracetic acid (PAA) in the water and wastewater treatment has recently been proposed and demonstrated to be effective for TC abatement, yet the underlying reaction kinetics between the PAA and TC are not yet clear. To explore the reaction kinetics, the effect of solution pH on TC abatement by PAA is studied and the species-specific rate constants are calculated. The ability to donate and accept electrons for different species of TC and PAA is evaluated via density functional theory (DFT) calculations. The pH-dependent apparent second-order rate constants of TC abatement by PAA exhibits the parabolic shape with the maximum at pH 8.5 (9.75 L mol−1 s−1). This phenomenon is closely related to the speciation of TC and PAA, in which the reaction between PAAH and TTC2− possesses the highest species-specific rate constants according to the kinetic simulation. Further DFT calculations suggest that the HOMO of TTCH+, TTC, TTC−, TTC2− and the LUMO of PAAH and PAA− are –6.40, –6.26, –5.10, –4.94 eV and –0.24, 0.60 eV, respectively. According to the DFT calculations, deprotonation of TC and PAA leads to an increase of the HOMO value of TC and the LUMO value of PAA. Furthermore, the HOMOTC–LUMOPAA values is in good agreement with the trend of species-specific rate constants, which can be used to evaluate the reactivity between PAA and TC with different species. This study provides the kinetic data and theoretical basis for the reaction of PAA and TC, which is critical for the application of PAA in the treatment of water and wastewater.
Environmental endocrine disruptors, represented by bisphenol A (BPA), have been widely detected in the environment, bringing potential health risks to human beings. Nitrogen-containing biocarbon catalyst can activate peroxymonosulfate (PMS) to degrade BPA in water, but its active sites remain opaque. Herein, in this work, nitrogen-containing biochar, i.e., CNedge, enriched with graphitic-N defects at the edges was prepared by one-pot co-pyrolysis of chitosan and potassium carbonate. The results showed that the CNedge/PMS system can effectively degrade 98% of BPA (50 mg/L). The electron transfer based non-radical oxidation mechanism was responsible for BPA degradation. Edge graphitic-N doping endows biochar with strong electron transfer ability. The catalyst had good recovery and reuse performance. This catalytic oxidation was also feasible for other refractory pollutants removal and worked well for treating practical wastewater. This work may provide valuable information in unraveling the N doping configuration-activity relationship during activating PMS by biochar.
Maximizing solar energy utilization is a persistent challenge in photo catalysis, which determines sustainable solar-driven photocatalytic process. Photo thermal-coupled photo catalysis is considered as a promising solution to tackle the issues of sustainable energy scarcity and environmental pollution by harvesting the full-spectrum solar energy. Herein, a highly efficient photo thermal-accelerated photo catalysis system is elaborately established, in which the assembled carbonized stick/Nb2C MXene evaporator can heat water into vapor and the integrated g-C3N4 photocatalyst further enables high-efficiency photocatalytic hydrogen production. The designed hyperboloid wood-based architecture possesses a multiphase interface of water steam/catalyst/hydrogen to reduce the transport resistance of hydrogen gas in liquid and ultimately maximize the output of hydrogen energy. Consequently, this coupled photothermal-photocatalytic system achieves a stable solar evaporation rate of 2.16 kg m-1 h-1 under one sun irradiation and highly efficient hydrogen-evolving rate of 3096 µmol g-1 h-1. This work paves a way to explore the improvement of photocatalytic hydrogen production by synergic photothermal effect for potential applications in renewable solar energy utilization and hydrogen production.
Tryptophan (Trp) is an essential amino acid that plays a critical role in human physiology. The increasing demand for Trp has created a highly promising market, underscoring the urgent necessity for the development of efficient strategies for the simultaneous detection and uptake of tryptophan. Herein, we report an expanded "Texas-sized" molecular box (An-TxSB), which incorporates luminescent anthracene bridging subunits and molecular recognition motifs. This luminescent molecular box demonstrates exceptional sensitivity to Trp in water, permitting its precise quantification with a notably low limit of detection (LOD) of 0.42 µmol/L. Moreover, An-TxSB facilitates the proficient uptake of Trp from simulated water samples, thereby revealing an impressive Trp adsorption capacity of up to 226.0 µmol/g.
An efficient and scalable electrochemical asymmetric protocol with metal-free catalysts and even without additional oxidants for the cross-dehydrogenative coupling reaction (CDC) of two C(sp3)-H bonds is reported. A series of aldehydes including natural products and various substrates containing C(sp3)-H bonds including xanthenes, acridines, cycloheptatrienes and even diarylmethane have been shown to undergo asymmetric CDC to afford a series of carbon-carbon bond coupling products with up to 94% yield and 98% ee. Mechanistic studies such as radical clock experiment suggest that the reaction proceeds via nucleophilic attack by enamine under electrochemical conditions.
We describe a versatile electrophile addition/SPR sequence of readily available cyclopropyl carbinols that affords multi-substituted carbonylated cyclopropanes with high stereo-fidelity. This approach tolerates various heteroatom electrophiles, migration of carbon moiety of all possible hybridization states, facile ring reorganization and natural compound valorization. The examples represent an unprecedented version of SPR wherein migration to a non-benzylic bulky tertiary carbo-cation is realized with promising enantiocontrol.
Covalently bonded bridging between different semiconductors is a remarkable approach to improve the transfer of charge carriers at interfaces. In this study, we designed a ternary heterojunction (MBG) combining of molybdenum diselenide (MoSe2), black phosphorus nanosheets (Bpn) and graphitic carbon nitride (GCN). Among this MBG of MoSe2/Bpn/GCN, (ⅰ) the covalently bonded bridging effect between Bpn/GCN facilitates directional charge carrier transfer, meanwhile (ⅱ) a Z-scheme heterojunction is formed between MoSe2/GCN to enhance the separation of photogenerated carriers. Furthermore, (ⅲ) this composite exhibits an increased absorption for visible light. Using this MBG, photocatalytic degradation of over 98% of moxifloxacin is achieved within 20 min, with O2•− confirmed as the primary photocatalytic active species. These findings provide novel insights into the construction of efficient heterojunction by covalently bonded bridging.
Nitrogen-doped carbon loaded single-atom catalysts (SACs) are promising candidates for electrocatalytic conversion of CO2 into high-valuable chemicals, and the modification of catalysts by heteroatom-doping strategy is an effective approach to enhance the CO2 reduction performance. However, the large difference exists in atomic radius between nitrogen atoms and the doped heteroatoms may lead to the poor stability of active sites. In this study, we have synthesized a Ni single atom catalyst with S doping at the second-shell on the ultrathin carbon nanosheets support (Ni-N4-SC) by solid-phase pyrolysis. The S atom in the second-shell contributes to the higher efficiency of CO2 conversion at lower potentials while the Ni-N4-SC can be more stable. The experimental results and theoretical calculations indicate that the S atom in second-shell breaks the uniform charge distribution and reduces the free energy of hydrogenation, which can increase the adsorption of CO2, accelerate charge transfer, and reduce the reaction energy barrier. This work reveals the close relationship between the second-shell and the electrocatalytic activity of single atom sites, which also provides a new perspective to design efficient single atom catalysts.
Single-atom catalysts were widely used to treat atmospheric pollution and alleviate energy crises through photocatalysis. However, how to prevent the aggregation of single atoms during the preparation and catalytic processes remained a great challenge. Herein, a novel ultrathin two-dimensional porphyrin-based single-atom photocatalyst Ti-MOF (abbreviated as TMPd) obtained through a simple hydrothermal synthesis strategy was used for photocatalytic hydrogen evolution and NO removal, in which the single-atom Pd tightly anchored in the center of porphyrin to ensure single-atom Pd stable existence. Compared with most reported MOFs-based photocatalysts, the TMPd showed an excellent hydrogen evolution rate (1.32 mmol g−1 h−1) and the NO removal efficiency (62%) under visible light irradiation. Aberration-corrected high-angle annular dark-field scanning transmission electron microscope (HAADF-STEM) and synchrotron-radiation-based X-ray absorption fine-structure spectroscopy (XAFS) proved that pd in TMPd existed in an isolated state, and the atomic force microscope (AFM) proved the ultrathin morphology of TMPd. DFT calculations had demonstrated that single-atom Pd could serve as the active center and more effectively achieve electron transfer, indicating that single-atom Pd played a vital role in photocatalytic hydrogen evolution. In addition, a possible photocatalytic pathway of NO removal was proposed based on ESR and in-situ infrared spectra, in which the catalysts anchored with single-atom Pd could produce more active substances and more effectively oxidize NO to NO2− or NO3−. The results suggested that coordinating single-atom metal species as the active site in the center of porphyrin could be a feasible strategy to obtain various ultrathin porphyrin-based single-atom photocatalysts to acquire excellent photocatalytic performance further.
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