Modulating the electronic structure of VS2via Ru decoration for an efficient pH-universal electrocatalytic hydrogen evolution reaction.

High-efficiency water electrolysis over a broad pH range is desirable but challenging. Herein, Ru-decorated VS2 on carbon cloth (Ru-VS2/CC) has been in situ synthesized, which features the regulated electronic structure of VS2 by introducing Ru. It is remarkable that the optimal Ru-VS2/CC displays excellent electrocatalytic hydrogen evolution activity with overpotentials of 89 and 87 mV at -10 mA cm-2 in 0.5 M H2SO4 and 1.0 M KOH, respectively. Theoretical calculations and electrocatalytic measurements have demonstrated that introducing Ru induces an enhanced charge density around the Fermi level, facilitating charge transfer and speeding up the electrocatalytic HER kinetics. The Gibbs free energy of the hydrogen intermediate (ΔGH*) of Ru-VS2/CC (0.23 eV) is much closer to zero than that of pure VS2 (0.51 eV) and Ru (-0.37 eV), demonstrating an easier hydrogen adsorption and desorption process for Ru-VS2/CC. The more favorable ΔGH*, differential charge density and the d-band center endow Ru-VS2 with enhanced intrinsic electrocatalytic activity. This study presents a feasible strategy for enhancing electrocatalytic HER activity by the regulation of the electronic structure and the rational integration of dual active components.

Solution-Processable Large-Area Black Phosphorus/Reduced Graphene Oxide Schottky Junction for High-Temperature Broadband Photodetectors.

2D materials-based broadband photodetectors have extensive applications in security monitoring and remote sensing fields, especially in supersonic aircraft that require reliable performance under extreme high-temperature conditions. However, the integration of large-area heterostructures with 2D materials often involves high-temperature deposition methods, and also limited options and size of substrates. Herein, a liquid-phase spin-coating method is presented based on the interface engineering to prepare larger-area Van der Waals heterojunctions of black phosphorus (BP)/reduced graphene oxide (RGO) films at room temperature on arbitrary substrates of any required size. Importantly, this method avoids the common requirement of high-temperature, and prevents the curling or stacking in 2D materials during the liquid-phase film formation. The BP/RGO films-based devices exhibit a wide spectral photo-response, ranging from the visible of 532 nm to infrared range of 2200 nm. Additionally, due to Van der Waals interface of Schottky junction, the array devices provide infrared detection at temperatures up to 400 K, with an outstanding photoresponsivity (R) of 12 A W-1 and a specific detectivity (D*) of ≈2.4 × 109 Jones. This work offers an efficient approach to fabricate large-area 2D Schottky junction films by solution-coating for high-temperature infrared photodetectors.

All-Covalent Organic Framework Nanofilms Assembled Lithium-Ion Capacitor to Solve the Imbalanced Charge Storage Kinetics.

Free-standing covalent organic framework (COFs) nanofilms exhibit a remarkable ability to rapidly intercalate/de-intercalate Li+ in lithium-ion batteries, while simultaneously exposing affluent active sites in supercapacitors. The development of these nanofilms offers a promising solution to address the persistent challenge of imbalanced charge storage kinetics between battery-type anode and capacitor-type cathode in lithium-ion capacitors (LICs). Herein, for the first time, custom-made COFBTMB-TP and COFTAPB-BPY nanofilms are synthesized as the anode and cathode, respectively, for an all-COF nanofilm-structured LIC. The COFBTMB-TP nanofilm with strong electronegative-CF3 groups enables tuning the partial electron cloud density for Li+ migration to ensure the rapid anode kinetic process. The thickness-regulated cathodic COFTAPB-BPY nanofilm can fit the anodic COF nanofilm in the capacity. Due to the aligned 1D channel, 2D aromatic skeleton and accessible active sites of COF nanofilms, the whole COFTAPB-BPY//COFBTMB-TP LIC demonstrates a high energy density of 318 mWh cm-3 at a high-power density of 6 W cm-3, excellent rate capability, good cycle stability with the capacity retention rate of 77% after 5000-cycle. The COFTAPB-BPY//COFBTMB-TP LIC represents a new benchmark for currently reported film-type LICs and even film-type supercapacitors. After being comprehensively explored via ex situ XPS, 7Li solid-state NMR analyses, and DFT calculation, it is found that the COFBTMB-TP nanofilm facilitates the reversible conversion of semi-ionic to ionic C-F bonds during lithium storage. COFBTMB-TP exhibits a strong interaction with Li+ due to the C-F, C=O, and C-N bonds, facilitating Li+ desolation and absorption from the electrolyte. This work addresses the challenge of imbalanced charge storage kinetics and capacity between the anode and cathode and also pave the way for future miniaturized and wearable LIC devices.

Resolidified Chalcogen-Assisted Growth of Bilayer Semiconductors with Controlled Stacking Orders.

Bilayer semiconductors have attracted much attention due to their stacking-order-dependent properties. However, as both 3R- and 2H-stacking are energetically stable at high temperatures, most of the high-temperature grown bilayer materials have random 3R- or 2H-stacking orders, leading to non-uniformity in optical and electrical properties. Here, a chemical vapor deposition method is developed to grow bilayer semiconductors with controlled stacking order by modulating the resolidified chalcogen precursors supply kinetics. Taking tungsten disulfide (WS2 ) as an example, pure 3R-stacking (100%) and 2H-stacking dominated (87.6%) bilayer WS2 are grown by using this method and both show high structural and optical quality and good uniformity. Importantly, the bilayer 3R-stacking WS2 shows higher field effect mobility than 2H-stacking samples, due to the difference in stacking order-dependent surface potentials. This method is universal for growing other bilayer semiconductors with controlled stacking orders including molybdenum disulfide and tungsten diselenide, paving the way to exploit stacking-order-dependent properties of these family of emerging bilayer materials.

Multiple Helicenes Defected by Heteroatoms and Heptagons with Narrow Emissions and Superior Photoluminescence Quantum Yields.

The incorporation of heteroatoms and/or heptagons as the defects into helicenes expands the variety of chiroptical materials with novel properties. However, it is still challenging to construct novel boron-doped heptagon-containing helicenes with high photoluminescence quantum yields (PLQYs) and narrow full-width-at-half-maximum (FWHM) values. We report an efficient and scalable synthesis of a quadruple helicene 4Cz-NBN with two nitrogen-boron-nitrogen (NBN) units and a double helicene 4Cz-NBN-P1 bearing two NBN-doped heptagons, the latter could be formed via a two-fold Scholl reaction of the former. The helicenes 4Cz-NBN and 4Cz-NBN-P1 exhibit excellent PLQYs up to 99 % and 65 % with narrow FWHM of 24 nm and 22 nm, respectively. The emission wavelengths are tunable via stepwise titration experiments of 4Cz-NBN-P1 toward fluoride, enabling distinguished circularly polarized luminescence (CPL) from green, orange (4Cz-NBN-P1-F1) to yellow (trans/cis-4Cz-NBN-P1-F2) with near-unity PLQYs and broader circular dichroism (CD) ranges. The five structures of the aforementioned four helicenes were confirmed by single crystal X-ray diffraction analysis. This work provides a novel design strategy for construction of non-benzenoid multiple helicenes exhibiting narrow emissions with superior PLQYs.

Large-Area Black Phosphorus/PtSe2 Schottky Junction for High Operating Temperature Broadband Photodetectors.

High operating temperature (HOT) broadband photodetectors are urgently necessary for extreme condition applications in infrared-guided missiles, infrared night vision, fire safety imaging, and space exploration sensing. However, conventional photodetectors show dramatic carrier mobility decreases and carrier losses with low photoresponsivity at HOT due to the increased carrier scattering in channels at high temperatures. Herein, the HOT broadband photodetectors from room temperature to 470 K are developed for the first time by large-area black phosphorus (BP)/PtSe2 films device arrays via a depletion-enhanced photocarrier dynamics strategy. Attributed to the 2D Schottky junction at BP/PtSe2 interface and resulting in full depleted working channels, the BP/PtSe2 photodetector arrays exhibit high tolerance to carrier mobility decrease during the increasing operating temperature in a wide wavelength range from 532 to 2200 nm. Thus, the photodetector shows a state-of-the-art operating temperature at 470 K with the photo-responsivity (R) and specific detectivity (D*) of 25 A W-1 and 6.4 × 1011 Jones under 1850 nm illumination, respectively. Moreover, BP/PtSe2 photodetector arrays show high-uniformity photo-response in a large area. This work provides new strategies for high-performance broadband photodetector arrays with HOT by Schottky junction of large-area BP/PtSe2 films.

A multifunctional integrated carbon nanotubes/polyphenylene sulfide composite: preparation, properties and applications.

Although great progress has been achieved in polyphenylene sulfide (PPS) composites by the use of carbon nanotubes (CNTs), the development of cost-efficient, well dispersive and multifunctional integrated PPS composites has yet to be achieved because of the strong solvent resistance of PPS. In this work, a CNTs-PPS/PVA composite material has been prepared by mucus dispersion-annealing, which employed polyvinyl alcohol (PVA) to disperse PPS particles and CNTs at room temperature. Dispersion and scanning electron microscopy observations revealed that PVA mucus can uniformly suspend and disperse micron-sized PPS particles, promoting the interpenetration of the micro-nano scale between PPS and CNTs. During the annealing process, PPS particles deformed and then crosslinked with CNTs and PVA to form a CNTs-PPS/PVA composite. The as-prepared CNTs-PPS/PVA composite possesses outstanding versatility, including excellent heat stability with resistant temperatures up to 350 °C, corrosion resistance against strong acids and alkalis for up to 30 days, and distinguished electrical conductivity with 2941 S m-1. Besides, a well-dispersed CNTs-PPS/PVA suspension could be used to 3D print microcircuits. Hence, such multifunctional integrated composites will be highly promising in the future of new materials. This research also develops a simple and meaningful method to construct composites for solvent resistant polymers.

Bending Resistance Covalent Organic Framework Superlattice: "Nano-Hourglass"-Induced Charge Accumulation for Flexible In-Plane Micro-Supercapacitors.

Covalent organic framework (COF) film with highly exposed active sites is considered as the promising flexible self-supported electrode for in-plane micro-supercapacitor (MSC). Superlattice configuration assembled alternately by different nanofilms based on van der Waals force can integrate the advantages of each isolated layer to exhibit unexpected performances as MSC film electrodes, which may be a novel option to ensure energy output. Herein, a mesoporous free-standing A-COF nanofilm (pore size is 3.9 nm, averaged thickness is 4.1 nm) with imine bond linkage and a microporous B-COF nanofilm (pore size is 1.5 nm, averaged thickness is 9.3 nm) with ß-keto-enamine-linkages are prepared, and for the first time, we assembly the two lattice matching films into sandwich-type superlattices via layer-by-layer transfer, in which ABA-COF superlattice stacking into a "nano-hourglass" steric configuration that can accelerate the dynamic charge transportation/accumulation and promote the sufficient redox reactions to energy storage. The fabricated flexible MSC-ABA-COF exhibits the highest intrinsic CV of 927.9 F cm-3 at 10 mV s-1 than reported two-dimensional alloy, graphite-like carbon and undoped COF-based MSC devices so far, and shows a bending-resistant energy density of 63.2 mWh cm-3 even after high-angle and repeat arbitrary bending from 0 to 180°. This work provides a feasible way to meet the demand for future miniaturization and wearable electronics.

Modulating the Band Structure of Metal Coordinated Salen COFs and an In Situ Constructed Charge Transfer Heterostructure for Electrocatalysis Hydrogen Evolution.

A series of crystalline, stable Metal (Metal = Zn, Cu, Ni, Co, Fe, and Mn)-Salen covalent organic framework (COF)EDA complex are prepared to continuously tune the band structure of Metal-Salen COFEDA , with the purpose of optimizing the free energy intermediate species during the hydrogen evolution reaction (HER) process. The conductive macromolecular poly(3,4-ethylenedioxythiophene) (PEDOT) is subsequently integrated into the one-dimensional (1D) channel arrays of Metal-Salen COFEDA to form heterostructure PEDOT@Metal-Salen COFEDA via the in situ solid-state polymerization method. Among the Metal-Salen COFEDA and PEDOT@Metal-Salen COFEDA complexes, the optimized PEDOT@Mn-Salen COFEDA displays prominent electrochemical activity with an overpotential of 150 mV and a Tafel slope of 43 mV dec-1 . The experimental results and density of states data show that the continuous energy band structure modulation in Metal-Salen COFEDA has the ability to make the metal d-orbital interact better with the s-orbital of H, which is conducive to electron transport in the HER process. Moreover, the calculated charge density difference indicates that the heterostructures composed of PEDOT and Metal-Salen COFEDA induce an intramolecular charge transfer and construct highly active interfacial sites.

Microwave ablation treatment for medically inoperable stage I non-small cell lung cancers: long-term results.

OBJECTIVES: In the present study, we aim to show the results of microwave ablation (MWA) for medically inoperable stage I non-small cell lung cancers (NSCLCs) with long-term follow-up. METHODS: From Feb 2011 to Mar 2016, patients with histologically proven clinical stage I NSCLC were treated with CT-guided MWA and retrospectively analyzed. The primary end point was overall survival (OS). Secondary end points included disease-free survival (DFS), cancer-specific survival (CSS), and complications. RESULTS: A total of 105 patients with 105 lesions underwent MWA. The mean age was 70.7 years (range: 40-86 years), and the mean diameter of all lesions was 2.40 cm (range: 0.9-4.0 cm). Adenocarcinoma was the most common histological type (77, 73.3%), followed by squamous cell carcinomas (21, 20%) and undefined NSCLC (7, 6.7%). With a median follow-up of 54.8 months, the median DFS was 36.0 months, and 1-, 3-, and 5-year DFS rates were 89.5%, 49.4%, and 42.7%, respectively. The median CSS and OS were 89.8 and 64.2 months, respectively. The OS rate was 99% at 1 year, 75.6% at 3 years, and 54.1% at 5 years, while the CSS rates were 99%, 78.9%, and 60.9%, respectively. Patients with stage IB lesions had significant shorter DFS (22.3 months vs. undefined, HR: 11.5, 95%CI: 5.85-22.40) and OS (37.3 vs. 89.8 months, HR: 8.64, 95% CI: 4.49-16.60) than IA disease. CONCLUSION: MWA is a safe, effective, and potentially curative therapy for medically inoperable stage I NSCLC patients. KEY POINTS: • In this multicenter retrospective study which included 105 patients, we found the median overall survival (OS) was 64.2 months. The OS rate was 99% at 1 year, 75.6% at 3 years, and 54.1% at 5 years. • Procedures were technically successful and well tolerated in all patients. Most MWA complications were mild or moderate.

Ultrasensitive Photodetectors Promoted by Interfacial Charge Transfer from Layered Perovskites to Chemical Vapor Deposition-Grown MoS2.

Heterostructures for charge-carrier manipulation have laid the foundation of modern optoelectronic devices, such as photovoltaics and photodetectors. High-performance heterostructure devices usually impose stringent requirements on the material quality to sustain efficient carrier transport and charge transfer, thus leading to sophisticated fabrication processes. Here, a simple yet efficient strategy is proposed to develop ultrasensitive photodetectors based on heterostructures of chemical vapor deposition-grown MoS2 and polycrystalline-layered perovskites. The layered perovskites possess pure crystallographic orientation with conductive edges in contact with MoS2 , which gives rise to efficient light absorption, exciton diffusion, and interfacial charge transfer. In dark state, the mismatch of work functions of two materials facilitates low dark currents by the depletion of electrons in MoS2 . Under light irradiation, efficient exciton diffusion and interfacial charge transfer are realized in the heterostructures with type-II band alignment, which produces drifting electrons in MoS2 and leaves trapped holes in layered perovskites. The photodetectors present suppress noises and boost photocurrents, yielding a champion device with a responsivity of 2.5 × 104  A W-1 , and a specific detectivity of 4.1 × 1014  Jones. The results demonstrate a scalable approach for the integration of high-performance devices with high tolerance to defects.

Electrochemical Delamination of Ultralarge Few-Layer Black Phosphorus with a Hydrogen-Free Intercalation Mechanism.

Due to strong interlayer interaction and ease of oxidation issues of black phosphorus (BP), the domain size of artificial synthesized few-layer black phosphorus (FL-BP) crystals is often below 10 µm, which extremely limits its further applications in large-area thin-film devices and integrated circuits. Herein, a hydrogen-free electrochemical delamination strategy through weak Lewis acid intercalation enabled exfoliation is developed to produce ultralarge FL-BP single-crystalline domains with high quality. The interaction between the weak Lewis acid tetra-n-butylammonium acetate (CH3 COOTBA) and P atoms promotes the average domain size of FL-BP crystal up to 77.6 ± 15.0 µm and the largest domain size is found to be as large as 119 µm. The presence of H+ and H2 O is found to sharply decrease the size of as-exfoliated FL-BP flakes. The electronic transport measurements show that the delaminated FL-BP crystals exhibit a high hole mobility of 76 cm2 V-1 s-1 and an on/off ratio of 103 at 298 K. A broadband photoresponse from 532 to 1850 nm with ultrahigh responsivity is achieved. This work provides a scalable, simple, and low-cost approach for large-area BP films that meet industrial requirements for nanodevices applications.

Use of contrast-enhanced ultrasound in evaluating the efficacy and application value of microwave ablation for adenomyosis.

AIM: This study aims to assess the use of contrast-enhanced ultrasonography (CEUS) and dynamic contrast-enhanced magnetic resonance imaging (DCE-MRI) in the evaluation of percutaneous microwave ablation (PMWA) of localized adenomyosis. MATERIALS AND METHODS: Sixty-six patients with single-onset adenomyosis who underwent PMWA at the Liaocheng Tumor Hospital of Shandong Province from January 2013 to February 2019 were enrolled. Venous CEUS and DCE-MRI examinations were performed before and 1-2 days after the surgery. The ablation rates calculated by CEUS and DCE-MRI were compared and analyzed for accuracy. RESULTS: After microwave ablation (MWA), CEUS showed that the volume and ablation rate of the ablated zone were 52.03 ± 28.39 cm3 and 90.90% ±6.61%, respectively. By DCE-MRI, the ablation volume and ablation rate of adenomyosis were 52.20 ± 28.65 cm3 and 90.88% ±6.32%, respectively. Dysmenorrhea was significantly relieved within 3 months of the operation, and nonmenstrual hemoglobin levels were significantly improved at 3 and 6 months after the operation (P < 0.05). All 66 cases of adenomyosis were treated using PMWA. Postoperatively, 17 patients reported a change in vaginal fluid; however, no special treatment was required as this disappeared 2-11 days after surgery. CONCLUSIONS: CEUS can accurately evaluate the ablation rate of localized adenomyosis treated with MWA, which is consistent with DCE-MRI. It is convenient and easy to perform ablation of adenomyomas, with incomplete ablation and angiography, and is a method worthy of clinical promotion.

Diagnosis of triple negative breast cancer based on radiomics signatures extracted from preoperative contrast-enhanced chest computed tomography.

BACKGROUND: To explore the diagnostic value of radiomics features of preoperative computed tomography (CT) for triple negative breast cancer (TNBC) for better treatment of patients with breast cancer. METHODS: A total of 890 patients with breast cancer admitted to our hospital from June 2016 to January 2018 were analyzed. They were diagnosed by surgery and pathology to have mass and invasive breast cancer and had contrast-enhanced chest CT examination before operation. 300 patients were randomly selected for the study, including 100 TNBC and 200 non-TNBC (NTNBC) patients. Among them 180 were used in discovery group and 120 were used in validation group. The molecular subtypes of breast cancer in the patients were determined immunohistochemistrially. Radiomics features were extracted from three dimensional CT-images. The LASSO logistic method was used to select image features and calculate radiomics scores. Receiver operating characteristic (ROC) curve analysis was performed to evaluate the diagnostic value of radiomics scores for TNBC. RESULTS: Five image features were found to be related to TNBC subtype (P < 0.001). These image features based-radiomic signatures had good predictive values for TNBC with the areas under ROC curve (AUC) of 0.881 (95% CI: 0.781-0.921) in the discovery group and 0.851 (95% CI: 0.761-0.961) in the validation group, respectively. The sensitivities and specificities were 0.767, and 0.873 in the discovery group and 0.785 and 0.915 in the validation group. CONCLUSIONS: Radiomic signature based on preoperative CT is capable of distinguishing patients with TNBC and NTNBC. It adds additional value for conventional chest contrast-enhanced CT and helps plan the strategy for clinical treatment of the patients.

Comparative uptake and assimilation of nitrate, ammonium, and urea by dinoflagellate Karenia mikimotoi and diatom Skeletonema costatum s.l. in the coastal waters of the East China Sea.

The nitrogen uptake kinetics and physiological growth of Karenia mikimotoi and Skeletonema costatum sensu lato grown on different N substrates and concentrations were compared in the laboratory. In the presence of three N substrates, both species preferred to take up NH4+. K. mikimotoi and S. costatum s.l. showed the highest substrate affinities for urea and NO3-, respectively. Both species grew well on three N substrates, and the growth parameters were comparable among the different N substrates. However, K. mikimotoi assimilated urea more efficiently than it assimilated either NO3- or NH4+. Different with S. costatum s.l., K. mikimotoi grew slowly and steady and the physiological and growth activities in N-depleted conditions were higher than those in N-replete conditions. Our results suggested that K. mikimotoi shows a greater readiness for uptake and assimilation of urea, and that this species is more competitive in an N-depleted environment when compared with S. costatum s.l.

Controlled growth of large-scale uniform 1T' MoTe2 crystals with tunable thickness and their photodetector applications.

The monoclinic-phase 1T' MoTe2 crystal exhibits inversion symmetry as an anisotropic semi-metal, dictating its interesting quantum transport phenomenon and other novel physical properties. However, large-scale controllable growth of uniform MoTe2 crystals still remains a great challenge, hindering its further fundamental research and applications for novel devices. Herein, we report a modified growth method for synthesizing few-layer 1T' MoTe2 crystals with large-scale uniformity with the assistance of molecular sieves. The theoretical simulations demonstrated that due to the temperature-dependent formation energies of different edges, the edge of (010) orientation shows a higher thermodynamic stability than that of (100) orientation, and results in the anisotropic growth behavior of 1T' MoTe2 crystals while the temperature changes. The photoresponse of tri-layer 1T' MoTe2-based devices shows a broad-spectrum response from 532 nm to 1550 nm. The photo-response time of 1T' MoTe2 crystals demonstrates that it supposes to be the synergistic mechanism of photo-conductive and photo-radiation effects. Our findings not only provide a method for the controllable growth of anisotropic two-dimensional materials at a wafer scale, but also explore a broad-spectrum photodetector with the MoTe2-based device.

Microwave ablation plus chemotherapy versus chemotherapy in advanced non-small cell lung cancer: a multicenter, randomized, controlled, phase III clinical trial.

OBJECTIVES: This prospective trial was performed to verify whether microwave ablation (MWA) in combination with chemotherapy could provide superior survival benefit compared with chemotherapy alone. MATERIALS AND METHODS: From March 1, 2015, to June 20, 2017, treatment-naïve patients with pathologically verified advanced or recurrent non-small cell lung cancer (NSCLC) were randomly assigned to MWA plus chemotherapy group or chemotherapy group. The primary endpoint was progression-free survival (PFS), while the secondary endpoints included overall survival (OS), time to local progression (TTLP), and objective response rate (ORR). The complications and adverse events were also reported. RESULTS: A total of 293 patients were randomly assigned into the two groups. One hundred forty-eight patients with 117 stage IV tumors were included in the MWA plus chemotherapy group. One hundred forty-five patients with 113 stage IV tumors were included in the chemotherapy group. The median follow-up period was 13.1 months and 12.4 months, respectively. Median PFS was 10.3 months (95% CI 8.0-13.0) in the MWA plus chemotherapy group and 4.9 months (95% CI 4.2-5.7) in the chemotherapy group (HR = 0.44, 95% CI 0.28-0.53; p < 0.0001). Median OS was not reached in the MWA plus chemotherapy group and 12.6 months (95% CI 10.6-14.6) in the chemotherapy group (HR = 0.38, 95% CI 0.27-0.53; p < 0.0001) using Kaplan-Meier analyses with log-rank test. The median TTLP was 24.5 months, and the ORR was 32% in both groups. The adverse event rate was not significantly different in the two groups. CONCLUSIONS: In patients with advanced NSCLC, longer PFS and OS can be achieved with the treatment of combined MWA and chemotherapy than chemotherapy alone. KEY POINTS: • Patients treated with MWA plus chemotherapy had superior PFS and OS over those treated with chemotherapy alone. • The ORR of patients treated with MWA plus chemotherapy was similar to that of those treated with chemotherapy alone. • Complications associated with MWA were common but tolerable and manageable.

Alkaline phosphatase activities and regulation in three harmful Prorocentrum species from the coastal waters of the East China Sea.

Harmful blooms of Prorocentrum donghaiense occur annually in the phosphorus-scarce coastal waters of the East China Sea (ECS). The enzymatic activities of alkaline phosphatase (AP) and its regulation by external phosphorus were studied during a P. donghaiense bloom in this area. The AP characteristics of P. donghaiense was further compared with Prorocentrum minimum and Prorocentrum micans in monocultures with both bulk and single-cell enzyme-labeled fluorescence AP assays. Concentrations of dissolved inorganic phosphorus (DIP) varied between 0.04 and 0.73 µmol l-1, with more than half recording stations registering concentrations below 0.10 µmol l-1. Concentrations of dissolved organic phosphorus (DOP) were comparable or even higher than those of DIP. P. donghaiense suffered phosphorus stress and expressed abundant AP, especially when DIP was lower than 0.10 µmol l-1. The AP activities showed a negative correlation with DIP but a positive correlation with DOP. The AP activities were also regulated by internal phosphorus pool. The sharp increase in AP activities was observed until cellular phosphorus was exhausted. Most AP of P. donghaiense was located on the cell surface and some were released into the water with time. Compared with P. minimum and P. micans, P. donghaiense showed a higher AP affinity for organic phosphorus substrates, a more efficient and energy-saving AP expression quantity as a response to phosphorus deficiency. The unique AP characteristic of P. donghaiense suggests that it benefits from the efficient utilization of DOP, and outcompete other species in the phosphorus-scarce ECS.

Unsaturated Single Atoms on Monolayer Transition Metal Dichalcogenides for Ultrafast Hydrogen Evolution.

Large-scale implementation of electrochemical water splitting for hydrogen evolution requires cheap and efficient catalysts to replace expensive platinum. However, catalysts that work well at high current densities with ultrafast intrinsic activities is still the central challenge for hydrogen evolution. An ideal case is to use single atoms on monolayer two-dimensional (2D) materials, which simplifies the system and in turn benefits the mechanism study, but is a grand challenge to synthesize. Here, we report a universal cold hydrogen plasma reduction method for synthesizing different single atoms sitting on 2D monolayers. In the case of molybdenum disulfide, we design and identify a type of active site, i.e., unsaturated Mo single atoms on cogenetic monolayer molybdenum disulfide. The catalyst shows exceptional intrinsic activity with a Tafel slope of 36.4 mV dec-1 in 0.5 M H2SO4 and superior performance at a high current density of 400 mA cm-2 with an overpotential of ∼260 mV, based on single flake microcell measurements. Theoretical studies indicate that coordinately unsaturated Mo single atoms sitting on molybdenum disulfide increase the bond strength between adsorbed hydrogen atoms and the substrates through hybridization, leading to fast hydrogen adsorption/desorption kinetics and superior hydrogen evolution activity. This work shines fresh light on preparing highly efficient electrocatalysts for water splitting and other electrochemical processes, as well as provides a general method to synthesize single atoms on two-dimensional monolayers.

Safety and clinical outcomes of computed tomography-guided percutaneous microwave ablation in patients aged 80 years and older with early-stage non-small cell lung cancer: A multicenter retrospective study.

BACKGROUND: Previous studies have documented the therapeutic value of computed tomography (CT)-guided percutaneous microwave ablation (MWA) for early-stage non-small cell lung cancer (NSCLC). However, few studies have focused on patients aged 80 years and older. This retrospective study aimed to evaluate the safety and clinical outcomes of CT-guided percutaneous MWA in patients aged 80 years and older with early-stage peripheral NSCLC. METHODS: A retrospective analysis of 63 patients aged 80 years and older with cT1a-2bN0M0 peripheral NSCLC who underwent CT-guided percutaneous MWA was performed between January 2008 and January 2018 at 11 hospitals in Shandong Province, China. RESULTS: The median follow-up time was 21.0 months. The overall median survival time was 50 months. The cancer-specific median survival time was not reached in five years. The one-, two-, three-, four-, and five-year overall survival rates were 97.1%, 92.6%, 63.4%, 54.4%, and 32.6%, respectively. The one-, two-, and three-year cancer-specific survival (CSS) rates were 97.9%, 97.9%, and 69.4%, respectively. The four- and five-year CSS rates were not achieved. A total of 14 patients (22.2%) had local progression. The one-, two-, three-, four-, and five-year local control rates were 88.8%, 78.8%, 70.3%, 63.9%, and 63.9%, respectively. The mortality rate was 0% within 30 days after the procedure. Major complications included pneumothorax requiring drainage (21.1%), pulmonary infection (4.2%), and pleural effusions requiring drainage (2.8%). CONCLUSIONS: CT-guided percutaneous MWA is a safe and effective modality for treating patients aged 80 years and older with early-stage peripheral NSCLC.