Multifunctional catalytic sites regulation of atomic-scale iridium on orthorhombic-CoSe_(2)for high efficiency dual-functional alkaline hydrogen evolution and organic degradation

The earth-abundant and high-performance catalysts are crucial for commercial implementation of hydrogen evolution reaction(HER).Herein,a multifunctional site strategy to construct excellent HER catalysts by incorporating iridium(Ir)ions on the atomic scale into orthorhombic-CoSe2(Ir-CoSe_(2))was reported.Outstanding hydrogen evolution activity in alkaline media such as a low overpotential of 48.7 mV at a current density of 10 mA cm^(-2)and better performance than commercial Pt/C catalysts at high current densities were found in the Ir-CoSe_(2) samples.In the experiments and theoretical calculations,it was revealed that Ir enabled CoSe_(2)to form multifunctional sites to synergistically catalyze alkaline HER by promoting the adsorption and dissociation of H_(2)O(Ir sites)and optimizing the binding energy for H^(*)on Co sites.It was noticeable that the electrolytic system comprising the Ir-CoSe_(2)electrode not only produced hydrogen efficiently via HER,but also degraded organic pollutants(Methylene blue).The cell voltage of the dual-function electrolytic system was 1.58 V at the benchmark current density of 50 mA cm^(-2),which was significantly lower than the conventional water splitting voltage.It was indicated that this method was a novel strategy for designing advanced HER electrocatalysts by constructing multifunctional catalytic sites for hydrogen production and organic degradation.

Therapeutic Effectiveness of Leukocyte-and Platelet-rich Fibrin for Diabetic Foot Ulcers:A Retrospective Study

Objective Diabetic foot ulcer(DFU)is one of the most serious complications of diabetes.Leukocyte-and platelet-rich fibrin(L-PRF)is a second-generation autologous platelet-rich plasma.This study aims to investigate the clinical effects of L-PRF in patients with diabetes in real clinical practice.Methods Patients with DFU who received L-PRF treatment and standard of care(SOC)from 2018 to 2019 in Tongji Hospital were enrolled.The clinical information including patient characteristics,wound evaluation(area,severity,infection,blood supply),SOC of DFU,and images of ulcers was retrospectively extracted and analyzed.L-PRF treatment was performed every 7±2 days until the ulcer exhibited complete epithelialization or an overall percent volume reduction(PVR)greater than 80%.Therapeutic effectiveness,including overall PVR and the overall and weekly healing rates,was evaluated.Results Totally,26 patients with DFU were enrolled,and they had an ulcer duration of 47.0(35.0,72.3)days.The severity and infection of ulcers varied,as indicated by the Site,Ischemia,Neuropathy,Bacterial Infection,and Depth(SINBAD)scores of 2–6,Wagner grades of 1–4,and the Perfusion,Extent,Depth,Infection and Sensation(PEDIS)scores of 2–4.The initial ulcer volume before L-PRF treatment was 4.94(1.50,13.83)cm3,and the final ulcer volume was 0.35(0.03,1.76)cm3.The median number of L-PRF doses was 3(2,5).A total of 11 patients achieved complete epithelialization after the fifth week of treatment,and 19 patients achieved at least an 80%volume reduction after the seventh week.The overall wound-healing rate was 1.47(0.63,3.29)cm3/week,and the healing rate was faster in the first 2 weeks than in the remaining weeks.Concurrent treatment did not change the percentage of complete epithelialization or healing rate.Conclusion Adding L-PRF to SOC significantly improved wound healing in patients with DFU independent of the ankle brachial index,SINBAD score,or Wagner grade,indicating that this method is appropriate for DFU treatment under different clinical conditions.

Interaction between circulating cancer cells and platelets:clinical implication

Metastasis is the main cause of cancer-associated mortality. During this complicated process, some cancer cells, also called circulating tumor cells （CTCs）, detach from primary sites, enter bloodstream and extravasate at metastatic site. Thrombocytosis is frequently observed in patients with metastatic cancers suggesting the important role of platelets in metastasis. Therefore this review focuses on how platelets facilitate the generation of CTCs, protect them from various host attacks, such as immune assaults, apoptosis and shear stress, and regulate CTCs intravasation/extravasation. Platelet-derived cytokines and receptors are involved in this cascade. Identification the mechanisms underlie platelet-CTCs interactions could lead to the development of new platelet-targeted therapeutic strategy to reduce metastasis.

Expert Consensus on Cognitive Dysfunction in Diabetes

The incidence of diabetes is gradually increasing in China,and diabetes and associated complications,such as cognitive dysfunction have gained much attention in recent time.However,the concepts,clinical treatment,and prevention of cognitive dysfunction in patients with diabetes remain unclear.The Chinese Society of Endocrinology investigated the current national and overseas situation of cognitive dysfunction associated with diabetes.Based on research both in China and other countries worldwide,the Expert Consensus on Cognitive Dysfunction in Diabetes was established to guide physicians in the comprehensive standardized management of cognitive dysfunction in diabetes and to improve clinical outcomes in Chinese patients.This consensus presents an overview,definition and classification,epidemiology and pathogenesis,risk factors,screening,diagnosis,differential diagnosis,treatment,and prevention of cognitive dysfunction in patients with diabetes.

Changing trends of clinicopathologic features and survival duration after surgery for gastric cancer in Northeast China

BACKGROUND Through analyzing the data from a single institution in Northeast China,this study revealed the possible clinicopathologic characteristics that influence the prognosis of patients with gastric cancer(GC).AIM To evaluate the changing trends of clinicopathologic features and survival duration after surgery in patients with GC in Northeast China,which is a highprevalence area of GC.METHODS The study analyzed the difference in clinicopathologic features and survival duration after surgery of 5887 patients who were histologically diagnosed with GC at the Harbin Medical University Cancer Hospital.The study mainly analyzed the data in three periods,2000 to 2004(Phase 1),2005 to 2009(Phase 2),and 2010 to 2014(Phase 3).RESULTS Over time,the postoperative survival rate significantly increased from 2000 to 2014.In the past 15 years,compared with Phases 1 and 2,the tumor size was smaller in Phase 3(P<0.001),but the proportion of high-medium differentiated tumors increased(P<0.001).The proportion of early GC gradually increased from 3.9%to 14.4%(P<0.001).A surprising improvement was observed in the mean number of retrieved lymph nodes,ranging from 11.4 to 27.5(P<0.001).The overall 5-year survival rate increased from 24%in Phase 1 to 43.8%in Phase 3.Through multivariate analysis,it was found that age,tumor size,histologic type,tumor-node-metastasis stage,depth of invasion,lymph node metastasis,surgical approach,local infiltration,radical extent,number of retrieved lymph nodes,and age group were independent risk factors that influenced the prognosis of patients with GC.CONCLUSION The clinical features of GC in Northeast China changed during the observation period.The increasing detection of early GC and more standardized surgical treatment effectively prolonged lifetimes.

Prognostic significance of Borrmann type combined with vessel invasion status in advanced gastric cancer

BACKGROUND Borrmann classification(types I-IV)for the detection of advanced gastric cancer has been accepted worldwide,and lymphatic and/or blood vessel invasion(LBVI)status is related to the poor prognosis after gastric cancer.AIM To evaluate the significance of Borrmann type combined with LBVI status in predicting the prognosis of advanced gastric cancer.METHODS We retrospectively studied the clinicopathological characteristics and long-term survival data of 2604 patients who were diagnosed with advanced gastric adenocarcinoma at Harbin Medical University Cancer Hospital from January 2009 to December 2013.Categorical variables were evaluated by the Pearson’sχ^2 test,the Kaplan-Meier method was used to identify differences in cumulative survival rates,and the Cox proportional hazards model was used for multivariate prognostic analysis.RESULTS A total of 2604 patients were included in this study.The presence of LVBI[LBVI(+)]and Borrmann type(P=0.001),tumor location(P<0.001),tumor size(P<0.001),histological type(P<0.001),tumor invasion depth(P<0.001),number of metastatic lymph nodes(P<0.001),and surgical method(P<0.001)were significantly correlated with survival.When analyzing the combination of the Borrmann classification and LBVI status,we found that patients with Borrmann type Ⅲ disease and LBVI(+)had a similar 5-year survival rate to those with Borrmann IV+LBVI(-)(16.4%vs 13.1%,P=0.065)and those with Borrmann IV+LBVI(+)(16.4%vs 11.2%,P=0.112).Subgroup analysis showed that the above results were true for any pT stage and any tumor location.Multivariate Cox regression analysis showed that Borrmann classification(P=0.023),vascular infiltration(P<0.001),tumor size(P=0.012),pT stage(P<0.001),pN stage(P<0.001),and extent of radical surgery(P<0.001)were independent prognostic factors for survival.CONCLUSION Since patients with Borrmann Ⅲ disease and LBVI(+)have the same poor prognosis as those with Borrmann IV disease,more attention should be paid to patients with Borrmann Ⅲ disease and LBVI(+)during diagnosis and treatment,regardless of the pT stage and tumor location,to obtain better survival results.

Deep gold mineralization features of Jiaojia metallogenic belt,Jiaodong gold Province:Based on the breakthrough of 3000 m exploration drilling

Recently,continuous breakthroughs have been made about deep gold prospecting in the Jiaodong gold province area of China.Approximately 5000 t of cumulative gold resources have been explored in Jiaodong,which has thus become an internationally noteworthy gold ore cluster.The gold exploration depth has been increased to about 2000 m from the previous<1000 m.To further explore the mineralization potential of the Jiaodong area at a depth of about 3000 m,the Shandong Institute of Geological Sciences has drilled an exploratory drillhole named“Deep drillhole ZK01”to a depth of 3266 m.Hence,as reported herein,the mineralization characteristics of the Jiaojia metallogenic belt have been successfully documented.ZK01 is,to date,the deepest borehole with an gold intersect in China,and constitutes a significant advance in deep gold prospecting in China.The findings of this study further indicate that the depth interval of 2000 m to 4000 m below the ground surface in the Wuyi Village area incorporates 912 t of inferred gold resources,while the depth interval of 2000 m to 4000 m below the surface across the Jiaodong area possesses about 4000 t of inferred gold resources.The Jiaojia Fault Belt tends to gently dip downward,having dip angles of about 25°and about 20°at vertical depths of 2000 m and 2850 m,respectively.The deep part of the Jiaojia metallogenic belt differs from the shallow and moderately deep parts about fracturing,alteration,mineralization,and tectonic type.The deep zones can generally be categorized from inside outward as cataclastic granite,granitic cataclasite,weakly beresitized granitic cataclasite,beresitized cataclasite,and gouge.These zones exhibit a gradual transitional relation or occur alternately and repeatedly.The mineralization degree of the pyritized cataclastic granite-type ore in the deep part of the Jiaojia metallogenic belt is closely related to the degree of pyrite vein development;that is,the higher the pyrite content,the wider the veins and the higher the gold grade.Compared to the shallow gold ores,the deep-seated gold ores have higher fineness and contain joseite,tetradymite,and native bismuth,suggesting that the deep gold mineralization temperature is higher and that mantle-sourced material may have contributed to this mineralization.ZK01 has also revealed that the deep-seated ore bodies in the Jiaojia metallogenic belt are principally situated above the main fracture plane(gouge)and hosted within the Linglong Granite,contradicting previous findings indicating that the moderately shallow gold ore bodies are usually hosted in the contact zone between the Linglong Granite and Jiaodong Group or meta-gabbro.These new discoveries are particularly significant because they can help correct mineralization prospecting models,determine favorable positions for deep prospecting,and improve metallogenic prediction and resource potential evaluation.

Subsurface intercalation activating basal plane of black phosphorus for nitrogen reduction

Ammonia(NH3)is not only an important chemical in many fields,but also provides a promising intermediate for energy stor-age[1,2].To produce NH3 from naturally abundant N2,the strong N≡N bond in the inert N2 molecules must be broken firstly.

High Temperature Seedless Synthesis of Au NRs Using BDAC/CTAB Co-surfactant

Au nanorods have been successfully synthesized at 90 ℃ by using hexadecyltrimethylammonium bromide （CTAB） and benzyldimethylammoniumchloride hydrate （BDAC） co-surfactant. At 90 ℃, the reaction time was less than 10 s, and the longitudinal surface plasmon absorption band could vary between 680 and 770 nm by adjusting the molar ratio of BDAC to CTAB from 2 to 0.5. At 90 ℃, nanorods with a longitudinal surface plasmon absorption peak of 770 nm can be obtained when the molar ratio of BDAC to CTAB was 3：2.

Bias Dependence of Radiation-Induced Narrow-Width Channel Effects in 65 nm NMOSFETs

The bias dependence of radiation-induced narrow-width channel effects（RINCEs） in 65-nm n-type metal-oxidesemiconductor field-effect transistors（NMOSFETs） is investigated. The threshold voltage of the narrow-width65 nm NMOSFET is negatively shifted by total ionizing dose irradiation, due to the RINCE. The experimental results show that the 65 nm narrow-channel NMOSFET has a larger threshold shift when the gate terminal is kept in the ground, which is contrary to the conclusion obtained in the old generation devices. Depending on the three-dimensional simulation, we conclude that electric field distribution alteration caused by shallow trench isolation scaling is responsible for the anomalous RINCE bias dependence in 65 nm technology.

Engineering the axial coordination of cobalt single atom catalysts for efficient photocatalytic hydrogen evolution

Improving the catalytic activity of non-noble metal single atom catalysts(SACs)has attracted considerable attention in materials science.Although optimizing the local electronic structure of single atom can greatly improve their catalytic activity,it often involves in-plane modulation and requires high temperatures.Herein,we report a novel strategy to manipulate the local electronic structure of SACs via the modulation of axial Co-S bond anchored onto graphitic carbon nitride(C_(3)N_(4))at room temperature(RT).Each Co atom is bonded to four N atoms and one S atom(Co-(N,S)/C_(3)N_(4)).Owing to the greater electronegativity of S in the Co-S bond,the local electronic structure of the Co atoms is available to be controlled at a relatively moderate level.Consequently,when employed for the photocatalytic hydrogen evolution reaction,the adsorption energy of intermediate hydrogen(H*)on the Co atoms is remarkably low.In the presence of the Co-(N,S)/C_(3)N_(4)SACs,the hydrogen evolution rates reach up to 10 mmol/(g·h),which is nearly 10 and 2.5 times greater than the rates in the presence of previously reported transition metal/C_(3)N_(4)and noble platinum nanoparticles(PtNPs)/C_(3)N_(4)catalysts,respectively.Attributed to the tailorable axial Co-S bond in the SAC,the local electronic structure of the Co atoms can be further optimized for other photocatalytic reactions.This axial coordination engineering strategy is universal in catalyst designing and can be used for a variety of photocatalytic applications.

Intercalator-assisted plasma-liquid technology:an efficient exfoliation method for few-layer two-dimensional materials

本工作提出了一种插层剂辅助的等离子体液相技术用于高效地剥离高质量少层二维材料.采用氯化锂为插层剂可快速剥离石墨纸,形成具有小D峰/G峰比(0.02)以及大碳氧比(31.5)的石墨烯产物.并且,这种方法可以拓展至高质量少层2H相二硫化钼的制备.和传统的插层剂辅助电化学方法相比,等离子体诱导产生的大量活性粒子以及快速的电子转移,使得插层剂辅助的等离子体液相技术剥离的产物缺陷少且不会引入额外的基团.这种可控的快速剥离方法在制备其他各种类型的高质量二维材料方面都具有巨大潜力.

Understanding angle-resolved polarized Raman scattering from black phosphorus at normal and oblique laser incidences

The selection rule for angle-resolved polarized Raman(ARPR)intensity of phonons from standard grouptheoretical method in isotropic materials would break down in anisotropic layered materials(ALMs)due to birefringence and linear dichroism effects.The two effects result in depth-dependent polarization and intensity of incident laser and scattered signal inside ALMs and thus make a challenge to predict ARPR intensity at any laser incidence direction.Herein,taking in-plane anisotropic black phosphorus as a prototype,we developed a so-called birefringence-linear-dichroism(BLD)model to quantitatively understand its ARPR intensity at both normal and oblique laser incidences by the same set of real Raman tensors for certain laser excitation.No fitting parameter is needed,once the birefringence and linear dichroism effects are considered with the complex refractive indexes.An approach was proposed to experimentally determine real Raman tensor and complex refractive indexes,respectively,from the relative Raman intensity along its principle axes and incident-angle resolved reflectivity by Fresnel’s law.The results suggest that the previously reported ARPR intensity of ultrathin ALM flakes deposited on a multilayered substrate at normal laser incidence can be also understood based on the BLD model by considering the depth-dependent polarization and intensity of incident laser and scattered Raman signal induced by both birefringence and linear dichroism effects within ALM flakes and the interference effects in the multilayered structures,which are dependent on the excitation wavelength,thickness of ALM flakes and dielectric layers of the substrate.This work can be generally applicable to any opaque anisotropic crystals,offering a promising route to predict and manipulate the polarized behaviors of related phonons.

Mapping the elastic properties of two-dimensional MoS_(2) via bimodal atomic force microscopy and finite element simulation

Elasticity is a fundamental mechanical property of two-dimensional(2D)materials,and is critical for their application as well as for strain engineering.However,accurate measurement of the elastic modulus of 2D materials remains a challenge,and the conventional suspension method suffers from a number of drawbacks.In this work,we demonstrate a method to map the in-plane Young’s modulus of mono-and bi-layer MoS_(2) on a substrate with high spatial resolution.Bimodal atomic force microscopy is used to accurately map the effective spring constant between the microscope tip and sample,and a finite element method is developed to quantitatively account for the effect of substrate stiffness on deformation.Using these methods,the in-plane Young’s modulus of monolayer MoS_(2) can be decoupled from the substrate and determined as 265±13 GPa,broadly consistent with previous reports though with substantially smaller uncertainty.It is also found that the elasticity of mono-and bi-layer MoS_(2) cannot be differentiated,which is confirmed by the first principles calculations.This method provides a convenient,robust and accurate means to map the in-plane Young’s modulus of 2D materials on a substrate.

Data-driven structural descriptor for predicting platinum-based alloys as oxygen reduction electrocatalysts

Owing to increasing global demand for carbon neutral and fossil-free energy systems,extensive research is being conducted on efficient and inexpensive electrocatalysts for catalyzing the kinetically sluggish oxygen reduction reaction(ORR)at the cathode of fuel cells.Platinum(Pt)-based alloys are considered promising candidates for replacing expensive Pt catalysts.However,the current screening process of Pt-based alloys is time-consuming and labor-intensive,and the descriptor for predicting the activity of Pt-based catalysts is generally inaccurate.This study proposed a strategy by combining high-throughput first-principles calculations and machine learning to explore the descriptor used for screening Pt-based alloy catalysts with high Pt utilization and low Pt consump-tion.Among the 77 prescreened candidates,we identified 5 potential candidates for catalyzing ORR with low overpotential.Furthermore,during the second and third rounds of active learning,more Pt-based alloys ORR candidates are identi-fied based on the relationship between structural features of Pt-based alloys and their activity.In addition,we highlighted the role of structural features in Pt-based alloys and found that the difference between the electronegativity of Pt and heteroatom,the valence electrons number of the heteroatom,and the ratio of heteroatoms around Pt are the main factors that affect the activity of ORR.More importantly,the combination of those structural features can be used as structural descriptor for predicting the activity of Pt-based alloys.We believe the findings of this study will provide new insight for predicting ORR activ-ity and contribute to exploring Pt-based electrocatalysts with high Pt utiliza-tion and low Pt consumption experimentally.

Black Phosphorus: An Effective Feedstock for the Synthesis of Phosphorus-Based Chemicals

We propose and demonstrate the novel concept of synthesizing organophosphorus compounds directly from black phosphorus(BP)nanoparticles as the feedstock.Compounds such as alkyl phosphines,alkyl phosphine oxides,phosphine sulfide,and hexafluorophosphate anion are prepared with good isolation yields under mild conditions.Selective synthesis of primary,secondary,and tertiary organophosphorus compounds is also demonstrated utilizing this one-pot approach.Reaction mechanisms are proposed and discussed.Compared with traditional white phosphorus(P 4)-based methods,the new synthetic concept and process utilizing elemental phosphorus are more efficient and environmentally friendly.

CsPbBr_(3)-DMSO merged perovskite micro-bricks for efficient X-ray detection

Inorganic perovskite wafers with good stability and adjustable sizes are promising in X-ray detection but the high synthetic temperature is a hindrance.Herein,dimethyl sulfoxide(DMSO)is used to prepare the CsPbBr_(3)micro-bricks powder at room temperature.The CsPbBr_(3)powder has a cubic shape with few crystal defects,small charge trap density,and high crystallinity.A trace amount of DMSO attaches to the surface of the CsPbBr_(3)micro-bricks via Pb-O bonding,forming the CsPbBr_(3)-DMSO adduct.During hot isostatic processing,the released DMSO vapor merges the CsPbBr_(3)micro-bricks,producing a compact and dense CsPbBr_(3)wafer with minimized grain boundaries and excellent charge transport properties.The CsPbBr_(3)wafer shows a large mobility-lifetime(μτ)product of 5.16×10^(-4)cm^(2)·V^(-1),high sensitivity of 14,430μC·Gyair^(-1)·cm^(-2),low detection limit of 564 nGyair·s^(-1),as well as robust stability in X-ray detection.The results reveal a novel strategy with immense practical potential pertaining to high-contrast X-ray detection.