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BACKGROUND: Two-dimensional (2D) - shear wave elastography (SWE) has made promising advances in the diagnostic of breast lesions. However, few studies have assessed whether the diagnostic effectiveness of different platforms employing 2D-SWE is equal or different. OBJECTIVE: To compare the diagnostic effectiveness of 2D-SWE techniques from two different systems in differentiating malignant breast lesions from benign ones. METHODS: A total of 84 breast lesions were retrospectively analyzed by experienced radiologists using 2D-SWE on two ultrasound systems, i.e. system-1 (LOGIQ E9 system, GE Healthcare, Wauwatosa, WI, USA), and system-2 (Aixplorer US system, SuperSonic Imagine, Aix-en-Provence, France). Qualitative and quantitative parameters including color sign, the maximum elasticity modulus values (E-max), the mean elasticity modulus values (E-mean) and standard deviation (E-sd) of elasticity modulus values in two 2D-SWE systems were analyzed. The diagnostic performance between system-1 and system-2 were evaluated in terms of the areas under the receiver operating characteristic curves (AUROCs). RESULTS: Among the 84 lesions in this study, 66 (78.6%) were benign and 18 (21.4%) were malignant. E-max in system-1 showed the best diagnostic performance with a cut-off value of 174.5 kPa with the associated sensitivity and specificity of 100.0% and 80.3% respectively. Meanwhile, E-sd in system-2 displayed the best diagnostic performance with a cut-off value of 12.7 kPa, with the associated sensitivity and specificity of 94.4% and 80.3% respectively. The diagnostic performance of the two 2D-SWE systems was not statistically different according to receiver operating characteristic curve (ROC) analysis of E-max, E-mean, and E-sd. CONCLUSION: For identifying breast lesions, system-1 and system-2 appear to be similar in diagnostic performance. However, different cut-off values for different parameters might be selected to obtain the best diagnostic performance for the two 2D-SWE systems.

Sonodynamic therapy (SDT), relying on the generation of reactive oxygen species (ROS), is a promising clinical therapeutic modality for the treatment of hepatocellular carcinoma (HCC) due to its noninvasiveness and high tissue-penetration depth, whereas the oxidative stress and antioxidative defense system in cancer cells significantly restrict the prevalence of SDT. Herein, we initially identified that NFE2L2 was immediately activated during SDT, which further inhibited SDT efficacy. To address this intractable issue, an ultrasound remote control of the cluster regularly interspaced short palindromic repeat (CRISPR)/CRISPR-associated protein 9 (Cas9) release system (HMME@Lip-Cas9) was meticulously designed and constructed, which precisely knocks down NFE2L2 to alleviate the adverse effects and augment the therapeutic efficiency of SDT. The hematoporphyrin monomethyl ether (HMME) in this system yielded abundant ROS to damage cancer cells under ultrasound irradiation, and meanwhile the generated ROS could induce lysosomal rupture to release Cas9/single guide RNA ribonucleoprotein (RNP) and destroy the oxidative stress-defensing system, significantly promoting tumor cell apoptosis. This study provides a new paradigm for HCC management and lays the foundation for the widespread application of CRISPR/Cas9 with promising clinical translation, meanwhile developing a synergistic therapeutic modality in the combination of SDT with gene editing., An ultrasound-controlled CRISPR/Cas9 nanosystem has been constructed for delivery of hematoporphyrin monomethyl ether and Cas9/sgRNA, which controls CRISPR/Cas9 release for precisely knocking down NFE2L2 to implement tumor-specific gene editing.

Reprogramming the tumor immunosuppressive microenvironment is a promising strategy for improving tumor immunotherapy efficacy. The clustered regularly interspaced short palindromic repeat (CRISPR)/CRISPR-associated protein 9 system can be used to knockdown tumor immunosuppression-related genes. Therefore, here, a self-driven multifunctional delivery vector is constructed to efficiently deliver the CRISPR-Cas9 nanosystem for indoleamine 2,3-dioxygenase-1 (IDO1) knockdown in order to amplify immunogenic cell death (ICD) and then reverse tumor immunosuppression. Lactobacillus rhamnosus GG (LGG) is a self-driven safety probiotic that can penetrate the hypoxia tumor center, allowing efficient delivery of the CRISPR/Cas9 system to the tumor region. While LGG efficiently colonizes the tumor area, it also stimulates the organism to activate the immune system. The CRISPR/Cas9 nanosystem can generate abundant reactive oxygen species (ROS) under the ultrasound irradiation, resulting in ICD, while the produced ROS can induce endosomal/lysosomal rupture and then releasing Cas9/sgRNA to knock down the IDO1 gene to lift immunosuppression. The system generates immune responses that effectively attack tumor cells in mice, contributing to the inhibition of tumor re-challenge in vivo. In addition, this strategy provides an immunological memory effect which offers protection against lung metastasis.

Featured with an exposed active facet, favorable ion diffusion pathway, and tailorable interfacial properties, low-dimensional structures are extensively explored as alternative electroactive materials with game-changing redox properties. Through a stepwise "proton exchange-insertion-exfoliation" procedure, in this article, we develop Na

The dynamically unstable interfacial properties and the low Li-utilization degree hinder the practical use of metallic lithium anodes in energy-dense battery construction with limited cation sources (lean electrolyte in the anode-free/anode-less model). Herein, an ultrathin interfacial layer of atomic Zn-doped N-doped carbon was prepared by a stepwise pyrolysis process and is proposed to regulate the reversible metallic plating/stripping process toward Cu foil. The ultrathin (similar to 2 mu m) and lightweight (0.25 mg cm(-2)) carbonaceous interfacial layer contained porous Zn-doped N-doped carbon sheets derived from metal-organic frameworks (MOFs) as a storage unit and interweaved carbon nanotubes (CNTs) as the structural support (denoted as the Zn-NC-CNT interfacial layer). The Zn-NC-CNT interfacial layer could effectively modify the Cu deposition substrate, maximizing the Li-utilization degree in both the symmetric cells and in a 2 mA h full battery prototype when integrated with the commercial NMC-811 (LiNi0.8Mn0.1Co0.1O2) cathode. This ultrathin layer interfacial modification strategy provides a feasible routine to construct the quasi-anode-free configuration without excessive Li abuse toward balanced energy/power densities and good cycling endurance.

The purpose of this study was to develop, validate and test a prediction model for discriminating malignant from benign breast lesions using conventional ultrasound (US), US elastography of strain elastography and contrast-enhanced ultrasound (CEUS). The study included 454 patients with breast imaging-reporting and data system (BI-RADS) category 4 breast lesions identified on histologic examinations. Firstly, 228 breast lesions (cohort 1) were analyzed by logistic regression analysis to identify the risk factors, and a breast malignancy prediction model was created. Secondly, the prediction model was validated in cohort 2 (84 patients) and tested in cohort 3 (142 patients) by using analysis of the area under the receiver operating characteristic curve (AUC). Univariate regression indicated that age ≥40 y, taller than wide shape on US, early hyperenhancement on CEUS and enlargement of enhancement area on CEUS were independent risk factors for breast malignancy (all p0.05). The logistic regression equation was established as follows: p = 1/1+Exp∑[-5.066 + 3.125 x (if age ≥40 y) + 1.943 x (if taller than wide shape) + 1.479 x (if early hyperenhancement) + 4.167 x (if enlargement of enhancement area). The prediction model showed good discrimination performance with an AUC of 0.967 in cohort 1, 0.948 in cohort 2 and 0.920 in cohort 3. By using the prediction model to selectively downgrade category 4a lesions, the re-rated BI-RADS yield an AUC of 0.880 (95% confidence interval [CI], 0.794-0.965) in cohort 2 and 0.870 (95% CI, 0.801-0.939) in cohort 3. The specificity increased from 0.0% (0/35) to 80.0% (28/35) without loss of sensitivity (from 100.0% to 95.9%, p = 0.153) in cohort 2. Similarly, the specificity increased from 0.0% (0/58) to 77.6% (45/58) without loss of sensitivity (from 100.0% to 96.4%, p = 0.081) in cohort 3. Multimodal US showed good diagnostic performance in predicting breast malignancy of BI-RADS category 4 lesions. Although the loss of sensitivity was existing, the addition of multimodal US to US BI-RADS could improve the specificity in BI-RADS category 4 lesions, which reduced unnecessary biopsies.

Density functional theory calculations (DFT), coupled with microkinetic modelling, have been used to simulate Temperature Programmed Desorption (TPD) experiments for calcined ceria nanopowders with the aim to gain insight into the chemistry governing their high redox activity. Our simulations consider two main nanoparticle models. One is a perfect ceria octahedron supercharged with adsorbed oxygen molecules turned into superoxide ions, as has previously been used to explain the enhanced oxygen storage capacity (OSC) in nanoceria. The other model is a variant where we have introduced oxygen vacancies under ridge Ce ions, thereby reducing their coordination numbers to five. The results from our microkinetic modelling suggest that including such five-coordinated Ce adsorption sites results in a TPD spectrum that better matches the experimental counterpart in terms of both peak position and width. In addition, this new structural model allows for the co-existence of Ce 3 + ions, superoxide ions and O2 molecules, as seen in experiments in the literature.

Although lorlatinib, the third generation of echinoderm microtubule protein 4-anaplastic lymphoma kinase (EML4-ALK) tyrosine kinase inhibitor (TKI), overcame the previous generation ALK-TKIs' drug resistance problems, but the mechanism of lorlatinib resistance remained unclear. Furthermore, optimal chemotherapy for lorlatinib-resistant non-small cell lung cancer (NSCLC) patients was still unknown.A lorlatinib-resistant NSCLC cell line SNU-2535LR was generated by gradually increasing dose of lorlatinib to crizotinib-resistant cell line SNU-2535 in vitro. To study the resistance mechanism of SNU-2535LR cells, we applied CCK-8 assay to detect the sensitivity of crizotinib and the reverse effect of APR-246, a p53 activator, on lorlatinib-induced resistance and different chemotherapy drugs to SNU-2535LR cells. We also detected the expressions of EML4-ALK-related proteins of SNU-2535LR cells via western blot.Please confirm that author names have been identified correctly and are presented in the right order.Dear Editor: I have carefully confirmed that the author names have been identified correctly and are presented in right order.Thank you very much! Your sincerely BoXie RESULTS: The sensitivity of SNU-2535LR cells to lorlatinib was decreased significantly than that of SNU-2535 cells. EML4-ALK fusion was decreased both at protein level and DNA level in SNU-2535LR cells. More interesting, the crizotinib-resistant mutation ALK p.G1269A disappeared, while new TP53 mutation emerged in SNU-2535LR cells. APR-246 can reverse the lorlatinib resistance in SNU-2535LR cells, with a reversal index of 4.768. Compared with SNU-2535 cells, the sensitivity of SNU-2535LR cells to gemcitabine, docetaxel and paclitaxel was significantly increased (P 0.05), but decreased to cisplatin (P 0.05).This study demonstrated that the combination of p53 protein agonist and lorlatinib may provide a new therapeutic strategy for NSCLC patients with lorlatinib resistance and TP53 mutation. Furthermore, the results also provide guidance for selecting optimal chemo-regimens for NSCLC patients after ALK-TKIs failure.

Intratumoral or intestinal microbiota correlates with tumorigenesis and progression, and microbiota regulation for reinforcing various anti-tumor approaches is of significant importance, which, however, suffers from no precise regulation method and unclear underlying mechanism. Herein, a microbiome metabolism-engineered phototherapy strategy is established, wherein Nb

MXenes, a new class of two-dimensional (2D) nanomaterials, have shown enormous potential for biological applications. Notably, the development of 2D MXenes in nanomedicine is still in its infancy. Herein, a distinct W1.33 C i-MXene with multiple theranostic functionalities, fast biodegradation, and satisfactory biocompatibility is explored. By designing a parent bulk laminate in-plane ordered (W2/3 Y1/3 )2 AlC ceramic and optionally etching aluminum (Al) and yttrium (Y) elements, 2D W1.33 C i-MXene nanosheets with ordered divacancies are efficiently fabricated. Especially, theoretical simulations reveal that W1.33 C i-MXene possesses a strong predominance of near-infrared (NIR) absorbance. The constructed ultrathin W1.33 C nanosheets feature excellent photothermal-conversion effectiveness (32.5% at NIR I and 49.3% at NIR II) with desirable biocompatibility and fast degradation in normal tissue rather than in tumor tissue. Importantly, the multimodal-imaging properties and photothermal-ablation performance of W1.33 C-BSA nanosheets are systematically revealed and demonstrated both in vitro and in vivo. The underlying mechanism and regulation factors for the W1.33 C-BSA nanosheets-induced hyperthermia ablation are also revealed by transcriptome and proteome sequencing. This work offers a paradigm that i-MXenes achieve the tailoring biomedical applications through composition and structure design on the atomic scale.

MXenes, a new class of two‐dimensional (2D) nanomaterials, have shown enormous potential for biological applications. Notably, the development of 2D MXenes in nanomedicine is still in its infancy. Herein, a distinct W1.33C i‐MXene with multiple theranostic functionalities, fast biodegradation, and satisfactory biocompatibility is explored. By designing a parent bulk laminate in‐plane ordered (W2/3Y1/3)2AlC ceramic and optionally etching aluminum (Al) and yttrium (Y) elements, 2D W1.33C i‐MXene nanosheets with ordered divacancies are efficiently fabricated. Especially, theoretical simulations reveal that W1.33C i‐MXene possesses a strong predominance of near‐infrared (NIR) absorbance. The constructed ultrathin W1.33C nanosheets feature excellent photothermal‐conversion effectiveness (32.5% at NIR I and 49.3% at NIR II) with desirable biocompatibility and fast degradation in normal tissue rather than in tumor tissue. Importantly, the multimodal‐imaging properties and photothermal‐ablation performance of W1.33C‐BSA nanosheets are systematically revealed and demonstrated both in vitro and in vivo. The underlying mechanism and regulation factors for the W1.33C‐BSA nanosheets‐induced hyperthermia ablation are also revealed by transcriptome and proteome sequencing. This work offers a paradigm that i‐MXenes achieve the tailoring biomedical applications through composition and structure design on the atomic scale., A distinct two dimensional W1.33C i‐MXene with multiple theranostic functionalities, fast biodegradation, and satisfactory biocompatibilityhas been demonstrated. The underlying mechanism and regulation factors for the engineered W1.33C‐BSA nanosheetsinduced photothermal hyperthermia are revealed via genomics and proteomics. This work significantly expands the biomedical applications of i‐MXene‐based nanomedicines with the desirable biological effect and excellent theranostics performance.

The potential of the cluster regularly interspaced short palindromic repeat (CRISPR)-associated protein 9 (Cas9)-based therapeutic genome editing is severely hampered by the difficulties in precise regulation of the in vivo activity of the CRISPR-Cas9 system. Herein, sono-controllable and reactive oxygen species (ROS)-sensitive sonosensitizer-integrated metal-organic frameworks (MOFs), denoted as P/M@CasMTH1, are developed for augmented sonodynamic therapy (SDT) efficacy using the genome-editing technology. P/M@CasMTH1 nanoparticles comprise singlet oxygen (1 O2 )-generating MOF structures anchored with CRISPR-Cas9 systems via 1 O2 -cleavable linkers, which serve not only as a delivery vector of CRISPR-Cas9 targeting MTH1, but also as a sonoregulator to spatiotemporally activate the genome editing. P/M@CasMTH1 escapes from the lysosomes, harvests the ultrasound (US) energy and converts it into abundant 1 O2 to induce SDT. The generated ROS subsequently trigger cleavage of ROS-responsive thioether bonds, thus inducing controllable release of the CRISPR-Cas9 system and initiation of genome editing. The genomic disruption of MTH1 conspicuously augments the therapeutic efficacy of SDT by destroying the self-defense system in tumor cells, thereby causing cellular apoptosis and tumor suppression. This therapeutic strategy for synergistic MTH1 disruption and abundant 1 O2 generation provides a paradigm for augmenting SDT efficacy based on the emerging nanomedicine-enabled genome-editing technology.

Despite the efficacy of current starvation therapies, they are often associated with some intrinsic drawbacks such as poor persistence, facile tumor metastasis and recurrence. Herein, we establish an extravascular gelation shrinkage-derived internal stress strategy for squeezing and narrowing blood vessels, occluding blood & nutrition supply, reducing vascular density, inducing hypoxia and apoptosis and eventually realizing starvation therapy of malignancies. To this end, a biocompatible composite hydrogel consisting of gold nanorods (GNRs) and thermal-sensitive hydrogel mixture was engineered, wherein GRNs can strengthen the structural property of hydrogel mixture and enable robust gelation shrinkage-induced internal stresses. Systematic experiments demonstrate that this starvation therapy can suppress the growths of PANC-1 pancreatic cancer and 4T1 breast cancer. More significantly, this starvation strategy can suppress tumor metastasis and tumor recurrence via reducing vascular density and blood supply and occluding tumor migration passages, which thus provides a promising avenue to comprehensive cancer therapy., The efficacy of tumour starvation therapy is limited by lack of persistent tumour suppression, tumour metastasis and recurrence. Here, the authors report biocompatible gold nanorods and thermal-sensitive hydrogel to promote narrowing of blood vessels and show this to reduce tumour growth and metastasis.

Graphene and transition metal dichalcogenides have been intensively investigated in recent years. Germanium selenide (GeSe) has emerged lately as a new low-symmetry two-dimensional material due to its extraordinary in-plane anisotropic electrical, optical, and optoelectronic properties. However, the controlled synthesis of large-scale GeSe flakes is still a significant challenge because of its strong interlayer coupling and low lattice symmetry. In this work, we have achieved the synthesis of rectangular GeSe microflakes (MFs) with lateral sizes up to 0.33 mm on the glass substrate via a vapor phase deposition technique. The lateral size, thickness, and growth mode of GeSe MFs can be effectively tuned based on space-confined and substrate engineering strategies. Germanium (Ge) MFs with triangular and hexagonal morphologies were simultaneously fabricated in the high-temperature zone. Our experimental results demonstrated that the growth temperature plays an important role in the selective growth of GeSe and Ge MFs. A corresponding growth mechanism has been discussed in detail based on systematic characterizations. Our work provides a new route for the controlled growth of large-size GeSe and Ge MFs, which promotes a promising future in the fields of novel optoelectronic devices.

The first layer of atoms on an oxide catalyst provides the first sites for adsorption of reactants and the last sites before products or oxygen are desorbed. We employ a unique combination of morphological, structural, and chemical analyses of a model ceria catalyst with different surface terminations under an H2 environment to unequivocally establish the effect of the last layer of atoms on surface reduction. (111) and (100) terminated epitaxial islands of ceria are simultaneously studied in situ allowing for a direct investigation of the structure–reducibility relationship under identical conditions. Kinetic rate constants of Ce4+ to Ce3+ transformation and equilibrium concentrations are extracted for both surface terminations. Unlike the kinetic rate constants, which are practically the same for both types of islands, more pronounced oxygen release, and overall higher reducibility were observed for (100) islands compared to (111) ones. The findings are in agreement with coordination-limited oxygen vacancy formation energies calculated by density functional theory. The results point out the important aspect of surface terminations in redox processes, with particular impact on the catalytic reactions of a variety of catalysts.

Cloud platforms allow users to execute tasks directly from their web browser and are a key enabling technology not only for commerce but also for computational science. Research software is often developed by scientists with limited experience in (and time for) user interface design, which can make research software difficult to install and use for novices. When combined with the increasing complexity of scientific workflows (involving many steps and software packages), setting up a computational research environment becomes a major entry barrier. AiiDAlab is a web platform that enables computational scientists to package scientific workflows and computational environments and share them with their collaborators and peers. By leveraging the AiiDA workflow manager and its plugin ecosystem, developers get access to a growing range of simulation codes through a python API, coupled with automatic provenance tracking of simulations for full reproducibility. Computational workflows can be bundled together with user-friendly graphical interfaces and made available through the AiiDAlab app store. Being fully compatible with open-science principles, AiiDAlab provides a complete infrastructure for automated workflows and provenance tracking, where incorporating new capabilities becomes intuitive, requiring only Python knowledge., Comment: Manuscript: 25 pages, 6 figures. Supplementary information: 15 pages, 10 figures

Prequenching and selective activation of photosensitizer (PS) are highly desired in photodynamic therapy (PDT) to avoid off-target effect due to nonspecific activation and poor targeting selectivity of PS. In this study, nanographene materials as a unique π-conjugated planar system for electronic transfer were employed as the robust platform for temporarily quenching of PS. Photosensitizer chlorin e6 (Ce6) was integrated onto planar structure of graphene quantum dot (GQD) or graphene oxide (GO) via a reduction cleavable disulfide linker. The formed hybrid nanosystem displayed considerable fluorescence quenching and slight phototoxicity, even under the condition of light irradiation, while the photoactivity of PS could be selectively recovered in the presence of the reducing agent. Compared with graphene oxide system with larger size (around 200 nm), GQD nanosystem exhibited significantly improved tumor accumulation via enhanced permeation and retention effect (EPR effect). The in vivo study demonstrated extremely effective suppression of tumor growth for the group treated with the GQD nanosystem with cleavable linker, revealing the promising application of the presented novel strategy.

In photodynamic therapy (PDT), selective activation of the photosensitiser in tumor-relevant conditions is highly desirable to avoid side effects. In this study, a graphene quantum dot (GQD) nanosystem, composed of a redox-triggered cleavable PEG shell, was designed and developed for selective recovery of photoactive chlorine e6 (Ce6) in tumor-relevant conditions. In this unique system, the planar π conjugated structure of GQD enables efficient quenching of the photochemical properties of Ce6 in terms of fluorescence and singlet oxygen generation. Once exposed to tumor relevant glutathione (GSH), the disulfide-linked PEG shell undergoes reductive cleavage and subsequent detachment from the GQD scaffold, leading to accelerated release of Ce6 with recovered photoactivity. MTT study against HeLa cells demonstrated the high PDT efficacy of Ce6, regulated by elevated GSH concentration. The studies on in vivo/ex vivo imaging and photodynamic efficacy demonstrated superior biocompatibility of the GQD nanosystem compared with the widely reported graphene oxide (GO)-based nanovehicle. Intravenously injected GQD–SS–PEG/Ce6 showed effective suppression of tumor growth.

Magnetically induced current densities and integrated ring-current strength susceptibilities have been calculated at the density functional theory (DFT) level for a test set consisting of 17 ring-shaped molecules using the gauge-including magnetically induced current (GIMIC) method. Reliable values for the ring-current strengths have been obtained by performing numerical integration of the current-density susceptibility passing a cut plane perpendicularly to the molecular ring. The current densities and ring current strengths were calculated at the DFT level using the B3LYP functional and def2-TZVP basis sets. Current densities and ring-current strengths have also been calculated at the Hartree-Fock self-consistent field (HF-SCF) level using Dunning’s aug-cc-pVTZ basis sets, which allow a direct comparison with ring-current strengths that have previously been estimated using ring-current models based on magnetic shielding calculations. Current density calculations at both levels of theory show that the magnetic shielding based ring-current models are not a very accurate means to estimate the magnetically induced ring current strengths, whereas they provide qualitatively the correct aromaticity trends for the studied molecules.

We investigate how the redox properties of ceria are affected by the fraction of Fock exchange in screened HSE06-based hybrid density functionals, and we compare with $\mathrm{PBE}+U$ results, and with experiments when available. We find that using $\ensuremath{\sim}15%$ Fock exchange yields a good compromise with respect to structure, electronic structure, and calculated reduction energies, and represents a significant improvement over the $\mathrm{PBE}+U$ results. We also investigate the possibility to use a computationally cheaper HSE06//$\mathrm{PBE}+U$ protocol consisting of structure optimization with $\mathrm{PBE}+U$, a subsequent lattice parameter rescaling step, and, finally, a single-point full hybrid calculation. We find that such a composite computational protocol works very well and yields results in close agreement with those where HSE06 was used also for the structure optimization.

Studies have shown the potential of nanomaterials for the accurate and early detection of cancer. The aim of the present study was to design and evaluate the value of prostate-specific membrane antigen (PSA)-targeted manganese oxide–mesoporous silica nanoparticles (Mn–Msns) for the detection of prostate cancer. Mn–Msns were prepared, and then conjugated with the PSA antibody and Cy7 to create the multimodality PSA-Mn-Msn-Cy7. Their particle size, zeta potential, stability and magnetic resonance imaging (MRI) features of the nanoparticles were characterized. Optical and MR imaging were evaluated in cell and tumor-bearing mouse models. The Mn in tissues was measured by inductively coupled plasma mass spectrometry. The fabricated nanoparticles were stable and showed good T1relaxivity. The targeted nanoparticles accumulated to a great extent in prostate cancer cells in vitro but not in noncancerous cells. In vivo studies further demonstrated a targeted distribution of PSA-Mn-Msn-Cy7 to cancer tissues as shown by high optical and T1 signals. The targeted distribution was also confirmed by determining the Mn content in the cancer tissues. Our data demonstrate that PSA targeted fluorescence and MR dual-functional nanoparticle can visualize prostate cancer and can be used as NIRF/MR contrast agents.

Several studies have reported a dramatically increased oxygen storage capacity (OSC) for small ceria nanoparticles (∼5 nm). Both experiments and theory have correlated this effect with superoxide ion formation. In previous studies, density functional theory (DFT) calculations with the PBE+U density functional have been used, and the obtained results were only in qualitative agreement with the experimental observations. One severe problem is the underbinding of the O2 molecule upon superoxide ion formation, which suggests that such species should not exist above room temperature. In this work, we use hybrid DFT functional to resolve this problem. We find that the discrepancy between theory and experiment originates from an incorrect estimate of the energy associated with the localized f-electrons with respect to the oxygen p-levels. By using average O2 adsorption energies from hybrid DFT calculations, extrapolated to large nanoparticles (3−10 nm), in conjunction with first-order desorption kinetics, we fin...

Fluorescent hydrogel demonstrates great potential in biomedical field as chemo/biosensor and bioimaging agent Herein, a labeling strategy based on coordination bond between lanthanide and bisphosphonate (BP) is reported to form fluorescent hydrogel. Specifically, BP-acrylamide compound was synthesized as organic "antenna" to stabilize lanthanide fluorescent signal. The coordination chemical structure and interaction energy between lanthanide (Eu3+) and BP-acrylamide ligand were obtained using density functional theory (DFT) calculations, indicating strong binding of Eu3+ ions with phosphonic oxygen atoms. Additionally, the lanthanide center dot BP complex could be chemically incorporated through acrylamide group into poly(ethylene glycol) diacrylate network to fabricate fluorescent hydrogels. The dynamic inherent properties of lanthanide center dot BP coordination bonds imparted the presented hydrogel's multistimuli-responsive properties against pH value and metal ions. The animal experiments revealed lanthanide-BP fluorescent hydrogel of great biocompatibilities and long-term structure stabilities in vivo. Therefore, we provide a facile coordination labeling strategy to develop biocompatible fluorescent hydrogel that presents potential for biomedical sensing and imaging applications.

Rechargeable sodium (Na) metal batteries (SMBs) provide an alternative energy-dense, low-cost energy storage system beyond prevailing Li‐ion technologies. However, their practical deployment requires the performance evaluation of Na anodes on the device level and mitigation of safety hazards, i.e., mechanical stress, electrode pulverization and dynamic interfacial properties. Here, we propose a lightweight N-doped carbon nanofiber substrate with SnSb nanocrystallites monodispersed within the mesopores (SnSb@NCNF). The alloying-induced Na15Sn4 and Na3Sb intermediates act as the heterogeneous sodiophilic “magnets” to homogenize Na ion flux and confine Na deposits within the nanospace. Additionally, the nucleation theory of metal solidification bridges the density functional theory calculations, elucidating the oriented Na propagation that maximizes the anode utilization. With the proper Na plating regulation, the SnSb@NCNF substrate (pre-stored 1 × excess Na) integrates with the NaVPO4F cathode in 5 mA h single-layer pouch cell, the prototype of which exhibits the cycling endurance (96.3% capacity retention for 500 cycles) and high specific energy/power densities even upon the repetitive mechanical flexing scenarios. The nanoconfinement of the heterogeneous nucleation process affords a feasible approach to mitigate the dendrite formation upon the geometry deformation or high areal-capacity loading, which enlightens the further exploration of the energy-dense, mechanical flexible battery system.

The technological barriers of the dimensional engineering and interfacial instability seriously hinder the scalable production of metallic (1T) transition metal dichalcogenides (TMD) monolayers. In this article, a facile and fast electron injection strategy is developed to modulate the d orbits of Mo center in trigonal prismatic 2H phases (MoS2 and MoSe2); meanwhile various cations (Li+, Na+, and K+) reinforce the in-plane 1T-atomic arrangement and expand the out-of-plane spacing for easy exfoliation. Theoretical and experimental evaluations further elucidate the decisive electron-donating capability and suitable ionic radius in stabilizing 1T coordination. The as-tailored 1T-MoS2/MoSe2 anodes can achieve the robust Na+ storage in the half cells (5000 cycles at 5 A g(-1)) and extreme power output of 3134.9 W kg(-1) in the full cell. This phase-engineering approach enables the precise dimensional manipulation of the 1T TMDs, which further extends their application horizons as the cation host for the power-oriented battery systems.

Metal-organic framework (MOF) is an exciting class of porous biomaterials that have been considered as a carrier to store and deliver therapeutic drugs. However, similar to other nanomaterials, the application of MOF in clinical settings is still limited because of premature diffusion of their payloads and tissue off-targeting behavior. To overcome these challenges, we designed an MOF-based hydrogel with structurally dynamic properties, i.e. , self-healing and shear-thinning, as an injectable localized drug delivery platform. The drug-encapsulating MOF hydrogel is formed through a dynamic coordination bond cross-linkage between a doxorubicin-loaded MOF (MOF@DOX) particle and a homemade bisphosphonatemodified hyaluronic acid (HA-BP) polymeric binder. The HA-BP middotMOF@DOX hydrogel demonstrates pHand ATP-responsive drug release characteristic and efficiently kills cancer cells in vitro . The animal experiments reveal that the HA-BP middotMOF@DOX hydrogel has enhanced capability in terms of tumor growth suppression as compared to the MOF@DOX group, which can be attributed to drug localization in hydrogel superstructure and sustained release at the tumor site. The presented injectable dynamic MOF-based hydrogel is a promising in vivo localized drug delivery system for cancer treatment. Herein, we report the self-healing and shear-thinning of MOF-based drug carrier cross-linked by coordinate bonds for the first time and provide new insights and a facile chemical strategy for designing and fabricating MOF-based biomaterials by using bisphosphonate-zinc interaction. Statement of significance Bisphosphonate-zinc interaction is a facile chemical strategy to cross-link metal-organic framework (MOF)-based hydrogel. The presented MOF-based hydrogel demonstrates structurally dynamic properties, including smooth injectability, self-healing, and shear-thinning. The developed MOF-based hydrogel pos-sesses pH-and ATP-responsive drug release characteristic and kills cancer cells in vitro efficiently. The dynamic MOF-based hydrogel shows enhanced in vivo anticancer activity as compared to pure MOF par-ticles. Self-healing and shear-thinning of metal-ligand cross-linked MOF-based drug delivery system are reported for the first time, thus providing new insights for the design and fabrication of MOF-based bio-materials. (c) 2022 Acta Materialia Inc. Published by Elsevier Ltd. All rights reserved.