The development of highly active,stable and inexpensive electrocatalysts for hydrogen production by defects and morphology engineering remains a great challenge.Herein,S vacancies-rich Ni_(3)S_(2)@Cu_(2)S nan-otube he...The development of highly active,stable and inexpensive electrocatalysts for hydrogen production by defects and morphology engineering remains a great challenge.Herein,S vacancies-rich Ni_(3)S_(2)@Cu_(2)S nan-otube heterojunction arrays were in-situ grown on copper foam(V_(s)-Ni_(3)S_(2)@V_(s)-Cu_(2)S NHAs/CF)for efficient electrocatalytic overall water splitting.With the merits of nanotube arrays and efficient electronic mod-ulation drived by the OD vacancy defect and 2D heterojunction defect,the resultant V_(s)-Ni_(3)S_(2)@V_(s)-Cu_(2)S NHAs/CF electrocatalyst exhibits excellent electrocatalytic activity with a low overpotential of 47 mV for the hydrogen evolution reaction(HER)at 10 mA cm^(-2) current density,and 263 mV for the oxygen evolution reaction(OER)at 50 mA cm^(-2) current density,as well as a cell voltage of 1.48 V at 10 mA cm^(-2).Moreover,the nanotube heterojunction arrays endows V_(s)-Ni_(3)S_(2)@V_(s)-Cu_(2)S NHAs/CF with outstanding stability in long-term catalytic processes,as confirmed by the continuous chronopotentiom-etry tests at current densities of 10 mA cm^(-2) for 100 h.展开更多
Designing efficient and long-lasting non-metal electrocatalysts is an urgent task for addressing the issue of kinetic hysteresis in electrochemical oxidation reactions.The bimetallic hydroxides,catalyzing the oxygen e...Designing efficient and long-lasting non-metal electrocatalysts is an urgent task for addressing the issue of kinetic hysteresis in electrochemical oxidation reactions.The bimetallic hydroxides,catalyzing the oxygen evolution reaction(OER),have significant research potential because hydroxide reconstruction to generate an active phase is a remarkable advantage.Herein,the complete reconstruction of ultrathin CoNi(OH)_(2) nanosheets was achieved by embedding Ag nanoparticles into the hydroxide to induce a spontaneous redox reaction(SRR),forming heterojunction Ag@CoNi(OH)_(2) for bifunctional hydrolysis.Theoretical calculations and in situ Raman and ex situ characterizations revealed that the inductive effect of the Ag cation redistributed the charge to promote phase transformation to highly activate Ag-modified hydroxides.The Co-Ni dual sites in Co/NiOOH serve as novel active sites for optimizing the intermediates,thereby weakening the barrier formed by OOH^*.Ag@CoNi(OH)_(2) required a potential of 1.55 V to drive water splitting at a current density of 10 mA cm^(-2),with nearly 98.6% Faraday efficiency.Through ion induction and triggering of electron regulation in the OER via the synergistic action of the heterogeneous interface and surface reconstruction,this strategic design can overcome the limited capacity of bimetallic hydroxides and bridge the gap between the basic theory and industrialization of water decomposition.展开更多
Urea oxidation reaction(UOR)is proposed as an exemplary half-reaction in renewable energy applications because of its low thermodynamical potential.However,challenges persist due to sluggish reaction kinetics and comp...Urea oxidation reaction(UOR)is proposed as an exemplary half-reaction in renewable energy applications because of its low thermodynamical potential.However,challenges persist due to sluggish reaction kinetics and complex by-products separation.To this end,we introduce the lattice oxygen oxidation mechanism(LOM),propelling a novel UOR route using a modified CoFe layered double hydroxide(LDH)catalyst termed CFRO-7.Theoretical calculations and in-situ characterizations highlight the activated lattice oxygen(O_(L))within CFRO-7 as pivotal sites for UOR,optimizing the reaction pathway and accelerating the kinetics.For the urea overall electrolysis application,the LOM route only requires a low voltage of 1.54 V to offer a high current of 100 mA cm^(-2) for long-term utilization(>48 h).Importantly,the by-product NCO^(-)−is significantly suppressed,while the CO_(2)2/N_(2) separation is efficiently achieved.This work proposed a pioneering paradigm,invoking the LOM pathway in urea electrolysis to expedite reaction dynamics and enhance product selectivity.展开更多
The overall photocatalytic CO_(2) reduction reaction(OPCRR)that can directly convert CO_(2) and H_(2)O into fuels represents a promising renewable energy conversion technology.As a typical redox reaction,the OPCRR inv...The overall photocatalytic CO_(2) reduction reaction(OPCRR)that can directly convert CO_(2) and H_(2)O into fuels represents a promising renewable energy conversion technology.As a typical redox reaction,the OPCRR involves two half-reactions:the CO_(2) reduction half-reaction(CRHR)and the water oxidation half-reaction(WOHR).Generally,both half-reactions can be promoted by adjusting the wettability of catalysts.However,there is a contradiction in wettability requirements for the two half-reactions.Specifically,CRHR prefers a hydrophobic surface that can accumulate more CO_(2) molecules on the active sites,ensuring the appropriate ratio of gas-phase(CO_(2))to liquid-phase(H_(2)O)reactants.Conversely,the WOHR prefers a hydrophilic surface that can promote the departure of the gaseous product(O_(2))from the catalyst surface,preventing isolation between active sites and the reactant(H_(2)O).Here,we successfully reconciled the contradictory wettability requirements for the CRHR and WOHR by creating an alternately hydrophobic catalyst.This was achieved through a selectively hydrophobic modification method and a charge-transfer-control strategy.Consequently,the collaboratively promoted CRHR and WOHR led to a significantly enhanced OPCRR with a solar-to-fuel conversion efficiency of 0.186%.Notably,in ethanol production,the catalyst exhibited a 10.64-fold increase in generation rate(271.44μmol g^(-1)h~(-1))and a 4-fold increase in selectivity(55.77%)compared to the benchmark catalyst.This innovative approach holds great potential for application in universal overall reactions involving gas participation.展开更多
Electrocatalytic water splitting is crucial for H2generation via hydrogen evolution reaction(HER)but subject to the sluggish dynamics of oxygen evolution reaction(OER).In this work,single Fe atomdoped MoS_(2)nanosheet...Electrocatalytic water splitting is crucial for H2generation via hydrogen evolution reaction(HER)but subject to the sluggish dynamics of oxygen evolution reaction(OER).In this work,single Fe atomdoped MoS_(2)nanosheets(SFe-DMNs)were prepared based on the high-throughput density functional theory(DFT)calculation screening.Due to the synergistic effect between Fe atom and MoS_(2)and optimized intermediate binding energy,the SFe-DMNs could deliver outstanding activity for both HER and OER.When assembled into a two-electrode electrolytic cell,the SFe-DMNs could achieve the current density of 50 mA cm^(-2)at a low cell voltage of 1.55 V under neutral condition.These results not only confirmed the effectiveness of high-throughput screening,but also revealed the excellent activity and thus the potential applications in fuel cells of SFe-DMNs.展开更多
Electrocatalytic overall water splitting(OWS),a pivotal approach in addressing the global energy crisis,aims to produce hydrogen and oxygen.However,most of the catalysts in powder form are adhesively bounding to the e...Electrocatalytic overall water splitting(OWS),a pivotal approach in addressing the global energy crisis,aims to produce hydrogen and oxygen.However,most of the catalysts in powder form are adhesively bounding to the electrodes,resulting in catalyst detachment by bubble generation and other uncertain interference,and eventually reducing the OWS performance.To surmount this challenge,we synthesized a hybrid material of Co_(3)S_(4)-pyrolysis lotus fiber(labeled as Co_(3)S_(4)-p LF)textile by hydrothermal and hightemperature pyrolysis processes for electrocatalytic OWS.Owing to the natural LF textile exposing the uniformly distributed functional groups(AOH,ANH_(2),etc.)to anchor Co_(3)S_(4)nanoparticles with hierarchical porous structure and outstanding hydrophily,the hybrid Co_(3)S_(4)-p LF catalyst shows low overpotentials at 10 m A cm^(-2)(η_(10,HER)=100 m Vη_(10,OER)=240 mV)alongside prolonged operational stability during electrocatalytic reactions.Theoretical calculations reveal that the electron transfer from p LF to Co_(3)S_(4)in the hybrid Co_(3)S_(4)-p LF is beneficial to the electrocatalytic process.This work will shed light on the development of nature-inspired carbon-based materials in hybrid electrocatalysts for OWS.展开更多
BACKGROUND Gastric cancer(GC)is prevalent and aggressive,especially when patients have distant lung metastases,which often places patients into advanced stages.By identifying prognostic variables for lung metastasis i...BACKGROUND Gastric cancer(GC)is prevalent and aggressive,especially when patients have distant lung metastases,which often places patients into advanced stages.By identifying prognostic variables for lung metastasis in GC patients,it may be po-ssible to construct a good prediction model for both overall survival(OS)and the cumulative incidence prediction(CIP)plot of the tumour.AIM To investigate the predictors of GC with lung metastasis(GCLM)to produce nomograms for OS and generate CIP by using cancer-specific survival(CSS)data.METHODS Data from January 2000 to December 2020 involving 1652 patients with GCLM were obtained from the Surveillance,epidemiology,and end results program database.The major observational endpoint was OS;hence,patients were se-parated into training and validation groups.Correlation analysis determined va-rious connections.Univariate and multivariate Cox analyses validated the independent predictive factors.Nomogram distinction and calibration were performed with the time-dependent area under the curve(AUC)and calibration curves.To evaluate the accuracy and clinical usefulness of the nomograms,decision curve analysis(DCA)was performed.The clinical utility of the novel prognostic model was compared to that of the 7th edition of the American Joint Committee on Cancer(AJCC)staging system by utilizing Net Reclassification Improvement(NRI)and Integrated Discrimination Improvement(IDI).Finally,the OS prognostic model and Cox-AJCC risk stratification model modified for the AJCC system were compared.RESULTS For the purpose of creating the OS nomogram,a CIP plot based on CSS was generated.Cox multivariate regression analysis identified eleven significant prognostic factors(P<0.05)related to liver metastasis,bone metastasis,primary site,surgery,regional surgery,treatment sequence,chemotherapy,radiotherapy,positive lymph node count,N staging,and time from diagnosis to treatment.It was clear from the DCA(net benefit>0),time-de-pendent ROC curve(training/validation set AUC>0.7),and calibration curve(reliability slope closer to 45 degrees)results that the OS nomogram demonstrated a high level of predictive efficiency.The OS prediction model(New Model AUC=0.83)also performed much better than the old Cox-AJCC model(AUC difference between the new model and the old model greater than 0)in terms of risk stratification(P<0.0001)and verification using the IDI and NRI.CONCLUSION The OS nomogram for GCLM successfully predicts 1-and 3-year OS.Moreover,this approach can help to ap-propriately classify patients into high-risk and low-risk groups,thereby guiding treatment.展开更多
The sluggish kinetics of both hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)generate the large overpotential in water electrolysis and thus high-cost hydrogen production.Here,multidimensional nanop...The sluggish kinetics of both hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)generate the large overpotential in water electrolysis and thus high-cost hydrogen production.Here,multidimensional nanoporous interpenetrating-phase FeNiZn alloy and FeNi_(3)intermetallic heterostructure is in situ constructed on NiFe foam(FeNiZn/FeNi_(3)@NiFe)by dealloying protocol.Coupling with the eminent synergism among specific constituents and the highly efficient mass transport from integrated porous backbone,FeNiZn/FeNi_(3)@NiFe depicts exceptional bifunctional activities for water splitting with extremely low overpotentials toward OER and HER(η_(1000)=367/245 mV)as well as the robust durability during the 400 h testing in alkaline solution.The as-built water electrolyzer with FeNiZn/FeNi_(3)@NiFe as both anode and cathode exhibits record-high performances for sustainable hydrogen output in terms of much lower cell voltage of 1.759 and 1.919 V to deliver the current density of 500 and 1000 mA cm^(-2)as well long working lives.Density functional theory calculations disclose that the interface interaction between FeNiZn alloy and FeNi_(3)intermetallic generates the modulated electron structure state and optimized intermediate chemisorption,thus diminishing the energy barriers for hydrogen production in water splitting.With the merits of fine performances,scalable fabrication,and low cost,FeNiZn/FeNi_(3)@NiFe holds prospective application potential as the bifunctional electrocatalyst for water splitting.展开更多
Electrocatalytic oxygen evolution reaction(OER)has been recognized as the bottleneck of overall water splitting,which is a promising approach for sustainable production of H_(2).Transition metal(TM)hydroxides are the ...Electrocatalytic oxygen evolution reaction(OER)has been recognized as the bottleneck of overall water splitting,which is a promising approach for sustainable production of H_(2).Transition metal(TM)hydroxides are the most conventional and classical non-noble metal-based electrocatalysts for OER,while TM basic salts[M^(2+)(OH)_(2-x)(A_(m^(-))_(x/m),A=CO_(3)^(2−),NO_(3)^(−),F^(−),Cl^(−)]consisting of OH−and another anion have drawn extensive research interest due to its higher catalytic activity in the past decade.In this review,we summarize the recent advances of TM basic salts and their application in OER and further overall water splitting.We categorize TM basic salt-based OER pre-catalysts into four types(CO_(3)^(2−),NO_(3)^(−),F^(−),Cl^(−)according to the anion,which is a key factor for their outstanding performance towards OER.We highlight experimental and theoretical methods for understanding the structure evolution during OER and the effect of anion on catalytic performance.To develop bifunctional TM basic salts as catalyst for the practical electrolysis application,we also review the present strategies for enhancing its hydrogen evolution reaction activity and thereby improving its overall water splitting performance.Finally,we conclude this review with a summary and perspective about the remaining challenges and future opportunities of TM basic salts as catalysts for water electrolysis.展开更多
Transition-metal phosphides(TMPs)with high catalytic activity are widely used in the design of electrodes for water splitting.However,a major challenge is how to achieve the trade-off between activity and stability of...Transition-metal phosphides(TMPs)with high catalytic activity are widely used in the design of electrodes for water splitting.However,a major challenge is how to achieve the trade-off between activity and stability of TMPs.Herein,a novel method for synthesizing CoP nanoparticles encapsu-lated in a rich-defect carbon shell(CoP/DCS)is developed through the self-assembly of modified polycyclic aromatic molecules.The graft and removal of high-activity C-N bonds of aromatic molecules render the controllable design of crystallite defects of carbon shell.The density functional theory calculation indicates that the carbon defects with unpaired electrons could effectively tailor the band structure of CoP.Benefiting from the improved activity and corrosion resistance,the CoP/DCS delivers outstanding difunctional hydrogen evolution reaction(88 mV)and oxygen evolution reaction(251 mV)performances at 10 mA cm^(−2)current density.Furthermore,the coupled water electrolyzer with CoP/DCS as both the cathode and anode presents ultralow cell voltages of 1.49 V to achieve 10 mA cm^(−2)with long-time stability.This strategy to improve TMPs electrocatalyst with rich-DCS and heterogeneous structure will inspire the design of other transition metal compound electrocatalysts for water splitting.展开更多
The electronic structures and properties of electrocatalysts,which depend on the physicochemical structure and metallic element components,could significantly affect their electrocatalytic performance and their future...The electronic structures and properties of electrocatalysts,which depend on the physicochemical structure and metallic element components,could significantly affect their electrocatalytic performance and their future applications in Zn-air battery(ZAB)and overall water splitting(OWS).Here,by combining vacancies and heterogeneous interfacial engineering,three-dimensional(3D)core-shell NiCoP/NiO heterostructures with dominated oxygen vacancies have been controllably in-situ grown on carbon cloth for using as highly efficient electrocatalysts toward hydrogen and oxygen electrochemical reactions.Theoretical calculation and electrochemical results manifest that the hybridization of NiCoP core with NiO shell produces a strong synergistic electronic coupling effect.The oxygen vacancy can enable the emergence of new electronic states within the band gap,crossing the Fermi levels of the two spin components and optimizing the local electronic structure.Besides,the hierarchical core-shell NiCoP/NiO nanoarrays also endow the catalysts with multiple exposed active sites,faster mass transfer behavior,optimized electronic strutures and improved electrochemical performance during ZAB and OWS applications.展开更多
BACKGROUND Preoperative anemia is associated with increased postoperative morbidity and mortality and increased perioperative transfusion risk.For surgical patients,this affects physical and cognitive ability and qual...BACKGROUND Preoperative anemia is associated with increased postoperative morbidity and mortality and increased perioperative transfusion risk.For surgical patients,this affects physical and cognitive ability and quality of life,but it is an important and modifiable risk factor.AIM To determine the effect of preoperative anemia on the prognosis of gastric cancer(GC)patients and generate a prognostic nomogram to predict the postoperative overall survival(OS)of GC patients with preoperative anemia.METHODS Clinicopathological and follow-up data of GC patients treated at Zhejiang Provincial People's Hospital(China)from 2010 to 2015 were collected.Independent prognostic factors were screened by univariate and multivariate Cox regression analyses.Then,these factors were used to construct a nomogram to predict 1-,3-,and 5-year postoperative OS in preoperative anemic GC patients.The nomogram was assessed by calibration curves,receiver operating characteristic(ROC)curves,and decision curve analysis(DCA).RESULTS Nine hundred and sixty GC patients were divided into two groups(preoper atively anemic and nonanemic),and postoperative survival analysis was performed on both groups,yielding a shorter postoperative survival for preoperatively anemic patients than for nonanemic patients.A total of 347 GC patients with preoperative anemia were included.Age,preoperative alpha-fetoprotein level,monocyte count,lymphocyte count,clinicopathological stage,liver metastasis,and GC type were identified as independent prognostic factors for OS.The area under the ROC curve(AUC)of the nomogram for predicting 1-,3-,and 5-year OS was 0.831,0.845,and 0.840,respectively,for the training cohort,and the corresponding AUC values in the validation cohort were 0.827,0.829,and 0.812,respectively.Calibration curves and DCA indicated good performance of the nomogram.CONCLUSION In all,we have successfully produced and verified a useful nomogram for predicting OS in GC patients with preoperative anemia.This nomogram based on a variety of clinicopathological indices can provide an effective prognostic assessment and help clinicians choose an appropriate treatment strategy for GC patients with preoperative anemia.展开更多
Improving catalytic activity and durabilty through the structural and compositional development of bifunctional electrocatalysts with low cost,high activity and stability is a challenging issue in electrochemical wate...Improving catalytic activity and durabilty through the structural and compositional development of bifunctional electrocatalysts with low cost,high activity and stability is a challenging issue in electrochemical water splitting.Herein,we report the fabrication of heterostructured P-CoMoO_(4)@NiCoP on a Ni foam substrate through interface engineering,by adjusting its composition and architecture.Benefitting from the tailored electronic structure and exposed active sites,the heterostructured P-CoMoO_(4)@NiCoP/NF arrays can be coordinated to boost the overall water splitting.In addition,the superhydrophilic and superaerophobic properties of P-CoMoO_(4)@NiCoP/NF make it conducive to water dissociation and bubble separation in the electrocatalytic process.The heterostructured PCoMoO_(4)@NiCoP/NF exhibits excellent bifunctional electrocatalysis activity with a low overpotential of 66 mV at 10 mA cm^(-2) for HER and 252 mV at 100 mA cm^(-2) for OER.Only 1.62 V potential is required to deliver 20 mA cm^(-2) in a two-electrode electrolysis system,providing a decent overall water splitting performance.The rational construction of the heterostructure makes it possible to regulate the electronic structures and active sites of the electrocatalysts to promote their catalytic activity.展开更多
Simultaneously realizing improved activity and stability of acidic oxygen evolution reaction(OER) electrocatalysts is highly promising for developing cost-effective sustainable energy in the splitting of water techniq...Simultaneously realizing improved activity and stability of acidic oxygen evolution reaction(OER) electrocatalysts is highly promising for developing cost-effective sustainable energy in the splitting of water technique.Herein,we report iridium nanocrystals embedded into 3D conductive clothes(Ir-NCT/CC) as a low iridium electrocatalyst realizing ultrahigh acidic OER activity and robust stability.The well-designed Ir-NCT/CC requires a low overpotential of 202 mV to reach the current density of 10 mA cm^(-2)with a high mass activity of 1754 A g^(-1).Importantly,in acidic overall water splitting,Ir-NCT/CC merely delivers a cell voltage of 1.469 V at a typical current density of 10 mA cm^(-2)and also maintains robust durability under continuous operation.We identify that a low working voltage drives the formation of a highly stable amorphous IrOxactive phase over the surface of Ir nanocrystals(surface heterojunction IrOx/Ir-NCT) during operating conditions,which contributes to an effective and durable OER process.展开更多
BACKGROUND Fibrinogen-to-albumin ratio(FAR)has been found to be of prognostic significance for several types of malignant tumors.However,less is known about the association between FAR and survival outcomes in hepatoc...BACKGROUND Fibrinogen-to-albumin ratio(FAR)has been found to be of prognostic significance for several types of malignant tumors.However,less is known about the association between FAR and survival outcomes in hepatocellular carcinoma(HCC)patients.AIM To explore the association between FAR and prognosis and survival in patients with HCC.METHODS A total of 366 histologically confirmed HCC patients diagnosed between 2013 and 2018 in a provincial cancer hospital in southwestern China were retrospectively selected.Relevant data were extracted from the hospital information system.The optimal cutoff for baseline serum FAR measured upon disease diagnosis was established using the receiver operating characteristic(ROC)curve.Univariate and multivariate Cox proportional hazards models were used to determine the crude and adjusted associations between FAR and the overall survival(OS)of the HCC patients while controlling for various covariates.The restricted cubic spline(RCS)was applied to estimate the dose-response trend in the FAR-OS association.RESULTS The optimal cutoff value for baseline FAR determined by the ROC was 0.081.Multivariate Cox proportional hazards model revealed that a lower baseline serum FAR level was associated with an adjusted hazard ratio of 2.43(95%confidence interval:1.87–3.15)in the OS of HCC patients,with identifiable dose-response trend in the RCS.Subgroup analysis showed that this FAR-OS association was more prominent in HCC patients with a lower baseline serum aspartate aminotransferase or carbohydrate antigen 125 level.CONCLUSION Serum FAR is a prominent prognostic indicator for HCC.Intervention measures aimed at reducing FAR might result in survival benefit for HCC patients.展开更多
The overall carbonation of MgO-admixed soil provides not only an efficient and environmentally friendly technique for improving soft ground but also a permanently safe solution for CO_(2) sequestration.To evaluate the...The overall carbonation of MgO-admixed soil provides not only an efficient and environmentally friendly technique for improving soft ground but also a permanently safe solution for CO_(2) sequestration.To evaluate the carbon sequestration potential and promote the carbonation application in soil improvement,a laboratory-scale model investigation is designed under pressurized carbonation considering the influences of MgO dosage and CO_(2) ventilation mode(way).The temperature,dynamic resilience modulus,and dynamic cone penetration(DCP)were tested to assess the carbonation treatment effect.The physical,strength,and microscopic tests were also undertaken to reveal the evolution mechanisms of CO_(2) migration in the MgO-carbonated foundation.The results indicate that the temperature peaks of MgO-treated foundation emerge at w20 h during hydration,but occur at a distance of 0e25 cm from the gas source within 6 h during carbonation.The dynamic resilience moduli of the model foundation increase by more than two times after carbonation and the DCP indices reduce dramatically.As the distance from the gas inlet increases,the bearing capacity,strength,and carbon sequestration decrease,whereas the moisture content increases.Compared to the end ventilation,the middle ventilation produces a higher carbonation degree and a wider carbonation area.The cementation and filling of nesquehonite and dypingite/hydromagnesite are verified to be critical factors for carbonation evolution and enhancing mechanical performances.Finally,the overall carbonation model is described schematically in three stages of CO_(2) migration.The outcomes would help to facilitate the practical application of CO_(2) sequestration in soil treatment.展开更多
MXene,the two-dimensional transition metal carbide or nitride material,was first discovered in 2011.They possess superior characteristics such as stability,electric conductivity,and electrochemical properties,that mak...MXene,the two-dimensional transition metal carbide or nitride material,was first discovered in 2011.They possess superior characteristics such as stability,electric conductivity,and electrochemical properties,that make them attract the attention of the energy engineering field.Overall water splitting which generates hydrogen and oxygen,not only serves as a clean energy supply technology but also demonstrates the capacity for redistribution and integration of renewable energy.MXene based non-noble metal has demonstrated significant potential in terms of cost-effectiveness.Therefore,the current focus is implementing targeted regulation at the micro level to render it effective comparable to the precious metals.In this context,the mechanisms of the hydrogen evolution reaction(HER) and the oxygen evolution reaction(OER) under the influence of MXene can be elucidated in terms of electron and ion transfer processes,hydrogen coverage,and regulation of terminal groups.Certainly,the composition,structure,synthesis,and stability strategies of MXene are the subjects of comprehensive investigation from both theoretical calculations using density functional theory(DFT) and experimental perspectives.In addition,this review provides a comprehensive summary of MXene based non-noble metal and various modification methods.These methods encompass doping,vacancy engineering,hybrid structures,heterojunction formation,multi-scale engineering,surface engineering,and phase engineering.The review also presents suggestions for designing high-performance MXene based on non-noble metals.It offers guidance on employing construction strategies for electrocatalysts.By leveraging the unique properties and tunability of MXene and implementing these modification methods,researchers can enhance the catalytic activity,stability,selectivity,and efficiency of MXene based non-noble metal catalysts.展开更多
BACKGROUND Increasingly extranodal marginal B-cell lymphoma of mucosa-associated lymphoid tissue,known as mucosa-associated lymphoid tissue(MALT)lymphoma,is a type of non-Hodgkin’s lymphoma.The prognosis of primary g...BACKGROUND Increasingly extranodal marginal B-cell lymphoma of mucosa-associated lymphoid tissue,known as mucosa-associated lymphoid tissue(MALT)lymphoma,is a type of non-Hodgkin’s lymphoma.The prognosis of primary gastric MALT(GML)patients can be affected by many factors.Clinical risk factors,including age,type of therapy,sex,stage and family hematologic malignancy history,also have significant effects on the development of the disease.The available data are mainly focused on epidemiology;in contrast,few studies have investigated the prognostic variables for overall survival(OS)in patients with primary GML.Based on the realities above,we searched a large amount of data on patients diagnosed with primary GML in the Surveillance,Epidemiology and End Results(SEER)database.The aim was to develop and verify a survival nomogram model that can predict the overall survival prognosis of primary GML by com-bining prognostic and determinant variables.AIM To create an effective survival nomogram for patients with primary gastric GML.METHODS All data of patients with primary GML from 2004 to 2015 were collected from the SEER database.The primary endpoint was OS.Based on the LASSO and COX regression,we created and further verified the accuracy and effectiveness of the survival nomogram model by the concordance index(C-index),calibration curve and timedependent receiver operating characteristic(td-ROC)curves.RESULTS A total of 2604 patients diagnosed with primary GML were selected for this study.A total of 1823 and 781 people were randomly distributed into the training and testing sets at a ratio of 7:3.The median follow-up of all patients was 71 mo,and the 3-and 5-year OS rates were 87.2%and 79.8%,respectively.Age,sex,race,Ann Arbor stage and radiation were independent risk factors for OS of primary GML(all P<0.05).The C-index values of the nomogram were 0.751(95%CI:0.729-0.773)and 0.718(95%CI:0.680-0.757)in the training and testing cohorts,respectively,showing the good discrimination ability of the nomogram model.Td-ROC curves and calibration plots also indicated satisfactory predictive power and good agreement of the model.Overall,the nomogram shows favorable performance in discriminating and predicting the OS of patients with primary GML.CONCLUSION A nomogram was developed and validated to have good survival predictive performance based on five clinical independent risk factors for OS for patients with primary GML.Nomograms are a low-cost and convenient clinical tool in assessing individualized prognosis and treatment for patients with primary GML.展开更多
The development of high-efficiency and cost-effective bifunctional electrocatalysts for overall water splitting remains a formidable challenge.Herein,FeNi-Nd_(2)O_(3) nanoparticles anchored on N-doped carbon nanotubes...The development of high-efficiency and cost-effective bifunctional electrocatalysts for overall water splitting remains a formidable challenge.Herein,FeNi-Nd_(2)O_(3) nanoparticles anchored on N-doped carbon nanotubes(FeNi-Nd_(2)O_(3)/NCN) are designed for highly effective overall water splitting via a facile two-step hydrothermal approach.The synthetic FeNi-Nd_(2)O_(3) hetero-trimers(Fe 2p-Ni 2p-Nd 3d orbital coupling)on NCN achieve excellent oxygen evolution reaction(OER) and hydrogen evolution reaction(HER) activities with overpotentials of 270 and 120 mV at 10 mA cm^(-2) in 1 M KOH solution.Moreover,a small voltage of 1.52 V at 10 mA cm^(-2) is achieved when FeNi-Nd_(2)O_(3)/NCN is assessed as bifunctional catalyst for overall water splitting,which is superior to the typically integrated Pt/C and RuO_(2) counterparts(1.54 V at 10 mA cm^(-2)).The related characterizations including X-ray absorption fine structure(XAFS)spectroscopy show that the remarkably improved activity is originated from Nd_(2)O_(3)-induced FeNi bimetallic lattice contraction.Furthermore,density functional theory(DFT) calculations indicate that the lattice contraction reduces binding energies of intermediates by downshifting the position of FeNi bimetallic d-band center relative to the Fermi level to optimize catalytic performance.Therefore,the Nd_(2)O_(3)-induced FeNi bimetallic lattice contraction may provide a new perspective for designing and synthesizing innovative catalytic systems.展开更多
The efficiency of photocatalytic overall water splitting was mainly limited by the slow reaction kinetics of water oxidation.How to design effective surface active site to overcome the slow water oxidation reaction wa...The efficiency of photocatalytic overall water splitting was mainly limited by the slow reaction kinetics of water oxidation.How to design effective surface active site to overcome the slow water oxidation reaction was a major challenge.Here,we propose a strategy to accelerate surface water oxidation through the fabrication spatially separated double active sites.FeCoPi/Bi_(4)NbO_(8)Cl-OVs photocatalyst with spatially separated double active site was prepared by hydrogen reduction photoanode deposition method.Due to the high matching of the spatial loading positions of FeCoPi and OVs with the photogenerated charge distribution of Bi_(4)NbO_(8)Cl and corresponding reaction mechanisms of substrate,the FeCoPi and OVs on the(001)and(010)crystal planes of Bi_(4)NbO_(8)Cl photocatalyst provided surface active site for water oxidation reaction and electron shuttle reaction(Fe^(3+)/Fe^(2+)),respectively.Under visible light irradiation,the evolution O_(2)rate of FeCoPi/Bi_(4)NbO_(8)Cl OVs was 16.8μmol h^(-1),as 32.9 times as Bi_(4)NbO_(8)Cl.Furthermore,a hydrogen evolution co-catalyst PtRu@Cr_(2)O_(3)was prepared by sequential photodeposition method.Due to the introduction of Ru,the Schottky barrier between PbTiO_(3)and Pt was effectively reduced,which promoted the transfer of photogenerated electrons to PtRu@Cr_(2)O_(3)thermodynamically,the evolution H_(2)rate on PtRu@Cr_(2)O_(3)/PbTiO_(3)increased to 664.8 times.On based of the synchronous enhancement of the water oxidation performance on FeCoPi/Bi_(4)NbO_(8)Cl-OVs and water reduction performance on PtRu@Cr_(2)O_(3)/PbTiO_(3),a novel Z-Scheme photocatalytic overall water splitting system(FeCoPi/Bi_(4)NbO_(8)Cl-OVs)mediated by Fe^(3+)/Fe^(2+)had successfully constructed.Under visible light irradiation,the evolution rates of H_(2)and O_(2)were 2.5 and 1.3μmol h^(-1),respectively.This work can provide some reference for the design of active site and the controllable synthesis of OVs spatial position.On the other hand,the hydrogen evolution co catalyst(PtRu@Cr_(2)O_(3))and the co catalyst FeCoPi for oxygen evolution contributed to the construction of an overall water splitting system.展开更多
基金supported by the National Natural Science Foundation of China under Grant No.52072196,52002200,52102106,52202262,22379081,22379080Major Basic Research Program of Natural Science Foundation of Shandong Province under Grant No.ZR2020zD09the Natural Science Foundation of Shandong Province under Grant No.ZR2020QE063,ZR202108180009,ZR2023QE059.
文摘The development of highly active,stable and inexpensive electrocatalysts for hydrogen production by defects and morphology engineering remains a great challenge.Herein,S vacancies-rich Ni_(3)S_(2)@Cu_(2)S nan-otube heterojunction arrays were in-situ grown on copper foam(V_(s)-Ni_(3)S_(2)@V_(s)-Cu_(2)S NHAs/CF)for efficient electrocatalytic overall water splitting.With the merits of nanotube arrays and efficient electronic mod-ulation drived by the OD vacancy defect and 2D heterojunction defect,the resultant V_(s)-Ni_(3)S_(2)@V_(s)-Cu_(2)S NHAs/CF electrocatalyst exhibits excellent electrocatalytic activity with a low overpotential of 47 mV for the hydrogen evolution reaction(HER)at 10 mA cm^(-2) current density,and 263 mV for the oxygen evolution reaction(OER)at 50 mA cm^(-2) current density,as well as a cell voltage of 1.48 V at 10 mA cm^(-2).Moreover,the nanotube heterojunction arrays endows V_(s)-Ni_(3)S_(2)@V_(s)-Cu_(2)S NHAs/CF with outstanding stability in long-term catalytic processes,as confirmed by the continuous chronopotentiom-etry tests at current densities of 10 mA cm^(-2) for 100 h.
基金supported by the Inner Mongolia R&D Program Plan(2021ZD0042,2021EEDSCXSFQZD006)the National Natural Science Foundation of China(21902123)the Natural Science Basic Research Program of Shaanxi(2023-JC-ZD-22)。
文摘Designing efficient and long-lasting non-metal electrocatalysts is an urgent task for addressing the issue of kinetic hysteresis in electrochemical oxidation reactions.The bimetallic hydroxides,catalyzing the oxygen evolution reaction(OER),have significant research potential because hydroxide reconstruction to generate an active phase is a remarkable advantage.Herein,the complete reconstruction of ultrathin CoNi(OH)_(2) nanosheets was achieved by embedding Ag nanoparticles into the hydroxide to induce a spontaneous redox reaction(SRR),forming heterojunction Ag@CoNi(OH)_(2) for bifunctional hydrolysis.Theoretical calculations and in situ Raman and ex situ characterizations revealed that the inductive effect of the Ag cation redistributed the charge to promote phase transformation to highly activate Ag-modified hydroxides.The Co-Ni dual sites in Co/NiOOH serve as novel active sites for optimizing the intermediates,thereby weakening the barrier formed by OOH^*.Ag@CoNi(OH)_(2) required a potential of 1.55 V to drive water splitting at a current density of 10 mA cm^(-2),with nearly 98.6% Faraday efficiency.Through ion induction and triggering of electron regulation in the OER via the synergistic action of the heterogeneous interface and surface reconstruction,this strategic design can overcome the limited capacity of bimetallic hydroxides and bridge the gap between the basic theory and industrialization of water decomposition.
基金supported by Fundamental Research Funds for the Central Universities(B220202062)supported by Key Program of National Natural Science Foundation of China(92047201,92047303,52102237)+1 种基金National Science Funds for Creative Research Groups of China(51421006)supported by Postdoctoral Science Foundations of China and Jiangsu Province(2021M690861,2022T150183,2021K065A)。
文摘Urea oxidation reaction(UOR)is proposed as an exemplary half-reaction in renewable energy applications because of its low thermodynamical potential.However,challenges persist due to sluggish reaction kinetics and complex by-products separation.To this end,we introduce the lattice oxygen oxidation mechanism(LOM),propelling a novel UOR route using a modified CoFe layered double hydroxide(LDH)catalyst termed CFRO-7.Theoretical calculations and in-situ characterizations highlight the activated lattice oxygen(O_(L))within CFRO-7 as pivotal sites for UOR,optimizing the reaction pathway and accelerating the kinetics.For the urea overall electrolysis application,the LOM route only requires a low voltage of 1.54 V to offer a high current of 100 mA cm^(-2) for long-term utilization(>48 h).Importantly,the by-product NCO^(-)−is significantly suppressed,while the CO_(2)2/N_(2) separation is efficiently achieved.This work proposed a pioneering paradigm,invoking the LOM pathway in urea electrolysis to expedite reaction dynamics and enhance product selectivity.
基金financially supported by the National Natural Science Foundation of China(22378204,22008121,51790492)the National Outstanding Youth Science Fund Project of National Natural Science Foundation of China(T2125004)+1 种基金the Funding of NJUST(No.TSXK2022D002)the Postgraduate Research&Practice Innovation Program of Jiangsu Province(KYCX23_0454)。
文摘The overall photocatalytic CO_(2) reduction reaction(OPCRR)that can directly convert CO_(2) and H_(2)O into fuels represents a promising renewable energy conversion technology.As a typical redox reaction,the OPCRR involves two half-reactions:the CO_(2) reduction half-reaction(CRHR)and the water oxidation half-reaction(WOHR).Generally,both half-reactions can be promoted by adjusting the wettability of catalysts.However,there is a contradiction in wettability requirements for the two half-reactions.Specifically,CRHR prefers a hydrophobic surface that can accumulate more CO_(2) molecules on the active sites,ensuring the appropriate ratio of gas-phase(CO_(2))to liquid-phase(H_(2)O)reactants.Conversely,the WOHR prefers a hydrophilic surface that can promote the departure of the gaseous product(O_(2))from the catalyst surface,preventing isolation between active sites and the reactant(H_(2)O).Here,we successfully reconciled the contradictory wettability requirements for the CRHR and WOHR by creating an alternately hydrophobic catalyst.This was achieved through a selectively hydrophobic modification method and a charge-transfer-control strategy.Consequently,the collaboratively promoted CRHR and WOHR led to a significantly enhanced OPCRR with a solar-to-fuel conversion efficiency of 0.186%.Notably,in ethanol production,the catalyst exhibited a 10.64-fold increase in generation rate(271.44μmol g^(-1)h~(-1))and a 4-fold increase in selectivity(55.77%)compared to the benchmark catalyst.This innovative approach holds great potential for application in universal overall reactions involving gas participation.
基金supported by the Research Funds of Institute of Zhejiang University-Quzhou(IZQ2023RCZX032)the Natural Science Foundation of Guangdong Province(2022A1515010185)+1 种基金the Fundamental Research Funds for the Central Universities(FRF-TP-20-005A3)partially supported by the Special Funds for Postdoctoral Research at Tsinghua University(100415017)。
文摘Electrocatalytic water splitting is crucial for H2generation via hydrogen evolution reaction(HER)but subject to the sluggish dynamics of oxygen evolution reaction(OER).In this work,single Fe atomdoped MoS_(2)nanosheets(SFe-DMNs)were prepared based on the high-throughput density functional theory(DFT)calculation screening.Due to the synergistic effect between Fe atom and MoS_(2)and optimized intermediate binding energy,the SFe-DMNs could deliver outstanding activity for both HER and OER.When assembled into a two-electrode electrolytic cell,the SFe-DMNs could achieve the current density of 50 mA cm^(-2)at a low cell voltage of 1.55 V under neutral condition.These results not only confirmed the effectiveness of high-throughput screening,but also revealed the excellent activity and thus the potential applications in fuel cells of SFe-DMNs.
基金supported by the Scientific Research Foundation of Hunan Provincial Education Department,China(22B0893)the Scientific Research Foundation of Hunan Provincial Education Department,China(20A060)。
文摘Electrocatalytic overall water splitting(OWS),a pivotal approach in addressing the global energy crisis,aims to produce hydrogen and oxygen.However,most of the catalysts in powder form are adhesively bounding to the electrodes,resulting in catalyst detachment by bubble generation and other uncertain interference,and eventually reducing the OWS performance.To surmount this challenge,we synthesized a hybrid material of Co_(3)S_(4)-pyrolysis lotus fiber(labeled as Co_(3)S_(4)-p LF)textile by hydrothermal and hightemperature pyrolysis processes for electrocatalytic OWS.Owing to the natural LF textile exposing the uniformly distributed functional groups(AOH,ANH_(2),etc.)to anchor Co_(3)S_(4)nanoparticles with hierarchical porous structure and outstanding hydrophily,the hybrid Co_(3)S_(4)-p LF catalyst shows low overpotentials at 10 m A cm^(-2)(η_(10,HER)=100 m Vη_(10,OER)=240 mV)alongside prolonged operational stability during electrocatalytic reactions.Theoretical calculations reveal that the electron transfer from p LF to Co_(3)S_(4)in the hybrid Co_(3)S_(4)-p LF is beneficial to the electrocatalytic process.This work will shed light on the development of nature-inspired carbon-based materials in hybrid electrocatalysts for OWS.
基金Supported by Peng-Cheng Talent-Medical Young Reserve Talent Training Program,No.XWRCHT20220002Xuzhou City Health and Health Commission Technology Project Contract,No.XWKYHT20230081and Key Research and Development Plan Project of Xuzhou City,No.KC22179.
文摘BACKGROUND Gastric cancer(GC)is prevalent and aggressive,especially when patients have distant lung metastases,which often places patients into advanced stages.By identifying prognostic variables for lung metastasis in GC patients,it may be po-ssible to construct a good prediction model for both overall survival(OS)and the cumulative incidence prediction(CIP)plot of the tumour.AIM To investigate the predictors of GC with lung metastasis(GCLM)to produce nomograms for OS and generate CIP by using cancer-specific survival(CSS)data.METHODS Data from January 2000 to December 2020 involving 1652 patients with GCLM were obtained from the Surveillance,epidemiology,and end results program database.The major observational endpoint was OS;hence,patients were se-parated into training and validation groups.Correlation analysis determined va-rious connections.Univariate and multivariate Cox analyses validated the independent predictive factors.Nomogram distinction and calibration were performed with the time-dependent area under the curve(AUC)and calibration curves.To evaluate the accuracy and clinical usefulness of the nomograms,decision curve analysis(DCA)was performed.The clinical utility of the novel prognostic model was compared to that of the 7th edition of the American Joint Committee on Cancer(AJCC)staging system by utilizing Net Reclassification Improvement(NRI)and Integrated Discrimination Improvement(IDI).Finally,the OS prognostic model and Cox-AJCC risk stratification model modified for the AJCC system were compared.RESULTS For the purpose of creating the OS nomogram,a CIP plot based on CSS was generated.Cox multivariate regression analysis identified eleven significant prognostic factors(P<0.05)related to liver metastasis,bone metastasis,primary site,surgery,regional surgery,treatment sequence,chemotherapy,radiotherapy,positive lymph node count,N staging,and time from diagnosis to treatment.It was clear from the DCA(net benefit>0),time-de-pendent ROC curve(training/validation set AUC>0.7),and calibration curve(reliability slope closer to 45 degrees)results that the OS nomogram demonstrated a high level of predictive efficiency.The OS prediction model(New Model AUC=0.83)also performed much better than the old Cox-AJCC model(AUC difference between the new model and the old model greater than 0)in terms of risk stratification(P<0.0001)and verification using the IDI and NRI.CONCLUSION The OS nomogram for GCLM successfully predicts 1-and 3-year OS.Moreover,this approach can help to ap-propriately classify patients into high-risk and low-risk groups,thereby guiding treatment.
基金supported by National Science Foundation of China(52201254)Shandong Province(ZR2020MB090,ZR2020QE012)the project of“20 Items of University”of Jinan(202228046)。
文摘The sluggish kinetics of both hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)generate the large overpotential in water electrolysis and thus high-cost hydrogen production.Here,multidimensional nanoporous interpenetrating-phase FeNiZn alloy and FeNi_(3)intermetallic heterostructure is in situ constructed on NiFe foam(FeNiZn/FeNi_(3)@NiFe)by dealloying protocol.Coupling with the eminent synergism among specific constituents and the highly efficient mass transport from integrated porous backbone,FeNiZn/FeNi_(3)@NiFe depicts exceptional bifunctional activities for water splitting with extremely low overpotentials toward OER and HER(η_(1000)=367/245 mV)as well as the robust durability during the 400 h testing in alkaline solution.The as-built water electrolyzer with FeNiZn/FeNi_(3)@NiFe as both anode and cathode exhibits record-high performances for sustainable hydrogen output in terms of much lower cell voltage of 1.759 and 1.919 V to deliver the current density of 500 and 1000 mA cm^(-2)as well long working lives.Density functional theory calculations disclose that the interface interaction between FeNiZn alloy and FeNi_(3)intermetallic generates the modulated electron structure state and optimized intermediate chemisorption,thus diminishing the energy barriers for hydrogen production in water splitting.With the merits of fine performances,scalable fabrication,and low cost,FeNiZn/FeNi_(3)@NiFe holds prospective application potential as the bifunctional electrocatalyst for water splitting.
基金supported by the financial support from Natural Science Foundation of China(Nos.21871065,22209129 and 22071038)High-Level Innovation and Entrepreneurship(QCYRCXM-2022-123)+1 种基金support from the“Young Talent Support Plan”of Xi’an Jiaotong University(HG6J024)“Young Talent Lift Plan”of Xi’an city(095920221352).
文摘Electrocatalytic oxygen evolution reaction(OER)has been recognized as the bottleneck of overall water splitting,which is a promising approach for sustainable production of H_(2).Transition metal(TM)hydroxides are the most conventional and classical non-noble metal-based electrocatalysts for OER,while TM basic salts[M^(2+)(OH)_(2-x)(A_(m^(-))_(x/m),A=CO_(3)^(2−),NO_(3)^(−),F^(−),Cl^(−)]consisting of OH−and another anion have drawn extensive research interest due to its higher catalytic activity in the past decade.In this review,we summarize the recent advances of TM basic salts and their application in OER and further overall water splitting.We categorize TM basic salt-based OER pre-catalysts into four types(CO_(3)^(2−),NO_(3)^(−),F^(−),Cl^(−)according to the anion,which is a key factor for their outstanding performance towards OER.We highlight experimental and theoretical methods for understanding the structure evolution during OER and the effect of anion on catalytic performance.To develop bifunctional TM basic salts as catalyst for the practical electrolysis application,we also review the present strategies for enhancing its hydrogen evolution reaction activity and thereby improving its overall water splitting performance.Finally,we conclude this review with a summary and perspective about the remaining challenges and future opportunities of TM basic salts as catalysts for water electrolysis.
基金Youth Innovation Promotion Association of the Chinese Academy of Sciences,Grant/Award Number:2021174National Natural Science Foundation of China,Grant/Award Number:51902326Natural Science Foundation of Shanxi Province,Grant/Award Numbers:201901D211588,20210302124421。
文摘Transition-metal phosphides(TMPs)with high catalytic activity are widely used in the design of electrodes for water splitting.However,a major challenge is how to achieve the trade-off between activity and stability of TMPs.Herein,a novel method for synthesizing CoP nanoparticles encapsu-lated in a rich-defect carbon shell(CoP/DCS)is developed through the self-assembly of modified polycyclic aromatic molecules.The graft and removal of high-activity C-N bonds of aromatic molecules render the controllable design of crystallite defects of carbon shell.The density functional theory calculation indicates that the carbon defects with unpaired electrons could effectively tailor the band structure of CoP.Benefiting from the improved activity and corrosion resistance,the CoP/DCS delivers outstanding difunctional hydrogen evolution reaction(88 mV)and oxygen evolution reaction(251 mV)performances at 10 mA cm^(−2)current density.Furthermore,the coupled water electrolyzer with CoP/DCS as both the cathode and anode presents ultralow cell voltages of 1.49 V to achieve 10 mA cm^(−2)with long-time stability.This strategy to improve TMPs electrocatalyst with rich-DCS and heterogeneous structure will inspire the design of other transition metal compound electrocatalysts for water splitting.
基金financially supported by the National Natural Science Foundation of China(No.22179014,21603019)program for the Hundred Talents Program of Chongqing University。
文摘The electronic structures and properties of electrocatalysts,which depend on the physicochemical structure and metallic element components,could significantly affect their electrocatalytic performance and their future applications in Zn-air battery(ZAB)and overall water splitting(OWS).Here,by combining vacancies and heterogeneous interfacial engineering,three-dimensional(3D)core-shell NiCoP/NiO heterostructures with dominated oxygen vacancies have been controllably in-situ grown on carbon cloth for using as highly efficient electrocatalysts toward hydrogen and oxygen electrochemical reactions.Theoretical calculation and electrochemical results manifest that the hybridization of NiCoP core with NiO shell produces a strong synergistic electronic coupling effect.The oxygen vacancy can enable the emergence of new electronic states within the band gap,crossing the Fermi levels of the two spin components and optimizing the local electronic structure.Besides,the hierarchical core-shell NiCoP/NiO nanoarrays also endow the catalysts with multiple exposed active sites,faster mass transfer behavior,optimized electronic strutures and improved electrochemical performance during ZAB and OWS applications.
基金the Major Science and Technology Project of Zhejiang Provincial Department of Science and Technology,No.2020C03030the Medical Health Science and Technology Project of Zhejiang Provincial Health Commission,No.2022503200。
文摘BACKGROUND Preoperative anemia is associated with increased postoperative morbidity and mortality and increased perioperative transfusion risk.For surgical patients,this affects physical and cognitive ability and quality of life,but it is an important and modifiable risk factor.AIM To determine the effect of preoperative anemia on the prognosis of gastric cancer(GC)patients and generate a prognostic nomogram to predict the postoperative overall survival(OS)of GC patients with preoperative anemia.METHODS Clinicopathological and follow-up data of GC patients treated at Zhejiang Provincial People's Hospital(China)from 2010 to 2015 were collected.Independent prognostic factors were screened by univariate and multivariate Cox regression analyses.Then,these factors were used to construct a nomogram to predict 1-,3-,and 5-year postoperative OS in preoperative anemic GC patients.The nomogram was assessed by calibration curves,receiver operating characteristic(ROC)curves,and decision curve analysis(DCA).RESULTS Nine hundred and sixty GC patients were divided into two groups(preoper atively anemic and nonanemic),and postoperative survival analysis was performed on both groups,yielding a shorter postoperative survival for preoperatively anemic patients than for nonanemic patients.A total of 347 GC patients with preoperative anemia were included.Age,preoperative alpha-fetoprotein level,monocyte count,lymphocyte count,clinicopathological stage,liver metastasis,and GC type were identified as independent prognostic factors for OS.The area under the ROC curve(AUC)of the nomogram for predicting 1-,3-,and 5-year OS was 0.831,0.845,and 0.840,respectively,for the training cohort,and the corresponding AUC values in the validation cohort were 0.827,0.829,and 0.812,respectively.Calibration curves and DCA indicated good performance of the nomogram.CONCLUSION In all,we have successfully produced and verified a useful nomogram for predicting OS in GC patients with preoperative anemia.This nomogram based on a variety of clinicopathological indices can provide an effective prognostic assessment and help clinicians choose an appropriate treatment strategy for GC patients with preoperative anemia.
基金The authors acknowledge the National Natural Science Foundation of China(NSFC 91834301,21808046 and 21908037)Anhui Provincial Science and Technology Department Foundation(201903a05020021 and 202003a05020046)for funding support.
文摘Improving catalytic activity and durabilty through the structural and compositional development of bifunctional electrocatalysts with low cost,high activity and stability is a challenging issue in electrochemical water splitting.Herein,we report the fabrication of heterostructured P-CoMoO_(4)@NiCoP on a Ni foam substrate through interface engineering,by adjusting its composition and architecture.Benefitting from the tailored electronic structure and exposed active sites,the heterostructured P-CoMoO_(4)@NiCoP/NF arrays can be coordinated to boost the overall water splitting.In addition,the superhydrophilic and superaerophobic properties of P-CoMoO_(4)@NiCoP/NF make it conducive to water dissociation and bubble separation in the electrocatalytic process.The heterostructured PCoMoO_(4)@NiCoP/NF exhibits excellent bifunctional electrocatalysis activity with a low overpotential of 66 mV at 10 mA cm^(-2) for HER and 252 mV at 100 mA cm^(-2) for OER.Only 1.62 V potential is required to deliver 20 mA cm^(-2) in a two-electrode electrolysis system,providing a decent overall water splitting performance.The rational construction of the heterostructure makes it possible to regulate the electronic structures and active sites of the electrocatalysts to promote their catalytic activity.
基金supported by the National Natural Science Foundation of China(12205300 and 12135012)the Natural Science Foundation of Anhui Province(2208085QA28 and 2208085J01)。
文摘Simultaneously realizing improved activity and stability of acidic oxygen evolution reaction(OER) electrocatalysts is highly promising for developing cost-effective sustainable energy in the splitting of water technique.Herein,we report iridium nanocrystals embedded into 3D conductive clothes(Ir-NCT/CC) as a low iridium electrocatalyst realizing ultrahigh acidic OER activity and robust stability.The well-designed Ir-NCT/CC requires a low overpotential of 202 mV to reach the current density of 10 mA cm^(-2)with a high mass activity of 1754 A g^(-1).Importantly,in acidic overall water splitting,Ir-NCT/CC merely delivers a cell voltage of 1.469 V at a typical current density of 10 mA cm^(-2)and also maintains robust durability under continuous operation.We identify that a low working voltage drives the formation of a highly stable amorphous IrOxactive phase over the surface of Ir nanocrystals(surface heterojunction IrOx/Ir-NCT) during operating conditions,which contributes to an effective and durable OER process.
文摘BACKGROUND Fibrinogen-to-albumin ratio(FAR)has been found to be of prognostic significance for several types of malignant tumors.However,less is known about the association between FAR and survival outcomes in hepatocellular carcinoma(HCC)patients.AIM To explore the association between FAR and prognosis and survival in patients with HCC.METHODS A total of 366 histologically confirmed HCC patients diagnosed between 2013 and 2018 in a provincial cancer hospital in southwestern China were retrospectively selected.Relevant data were extracted from the hospital information system.The optimal cutoff for baseline serum FAR measured upon disease diagnosis was established using the receiver operating characteristic(ROC)curve.Univariate and multivariate Cox proportional hazards models were used to determine the crude and adjusted associations between FAR and the overall survival(OS)of the HCC patients while controlling for various covariates.The restricted cubic spline(RCS)was applied to estimate the dose-response trend in the FAR-OS association.RESULTS The optimal cutoff value for baseline FAR determined by the ROC was 0.081.Multivariate Cox proportional hazards model revealed that a lower baseline serum FAR level was associated with an adjusted hazard ratio of 2.43(95%confidence interval:1.87–3.15)in the OS of HCC patients,with identifiable dose-response trend in the RCS.Subgroup analysis showed that this FAR-OS association was more prominent in HCC patients with a lower baseline serum aspartate aminotransferase or carbohydrate antigen 125 level.CONCLUSION Serum FAR is a prominent prognostic indicator for HCC.Intervention measures aimed at reducing FAR might result in survival benefit for HCC patients.
基金funding provided by the National Science Foundation of China(Grant No.41902286)the Open Fund for the State Key Laboratory of Geomechanics and Geotechnical Engineering(Grant No.SKLGME021029)the CRSRI Open Research Program(Grant No.CKWV20221015/KY).
文摘The overall carbonation of MgO-admixed soil provides not only an efficient and environmentally friendly technique for improving soft ground but also a permanently safe solution for CO_(2) sequestration.To evaluate the carbon sequestration potential and promote the carbonation application in soil improvement,a laboratory-scale model investigation is designed under pressurized carbonation considering the influences of MgO dosage and CO_(2) ventilation mode(way).The temperature,dynamic resilience modulus,and dynamic cone penetration(DCP)were tested to assess the carbonation treatment effect.The physical,strength,and microscopic tests were also undertaken to reveal the evolution mechanisms of CO_(2) migration in the MgO-carbonated foundation.The results indicate that the temperature peaks of MgO-treated foundation emerge at w20 h during hydration,but occur at a distance of 0e25 cm from the gas source within 6 h during carbonation.The dynamic resilience moduli of the model foundation increase by more than two times after carbonation and the DCP indices reduce dramatically.As the distance from the gas inlet increases,the bearing capacity,strength,and carbon sequestration decrease,whereas the moisture content increases.Compared to the end ventilation,the middle ventilation produces a higher carbonation degree and a wider carbonation area.The cementation and filling of nesquehonite and dypingite/hydromagnesite are verified to be critical factors for carbonation evolution and enhancing mechanical performances.Finally,the overall carbonation model is described schematically in three stages of CO_(2) migration.The outcomes would help to facilitate the practical application of CO_(2) sequestration in soil treatment.
基金supported by National Natural Science Foundation of China (Grant No. 22279091)。
文摘MXene,the two-dimensional transition metal carbide or nitride material,was first discovered in 2011.They possess superior characteristics such as stability,electric conductivity,and electrochemical properties,that make them attract the attention of the energy engineering field.Overall water splitting which generates hydrogen and oxygen,not only serves as a clean energy supply technology but also demonstrates the capacity for redistribution and integration of renewable energy.MXene based non-noble metal has demonstrated significant potential in terms of cost-effectiveness.Therefore,the current focus is implementing targeted regulation at the micro level to render it effective comparable to the precious metals.In this context,the mechanisms of the hydrogen evolution reaction(HER) and the oxygen evolution reaction(OER) under the influence of MXene can be elucidated in terms of electron and ion transfer processes,hydrogen coverage,and regulation of terminal groups.Certainly,the composition,structure,synthesis,and stability strategies of MXene are the subjects of comprehensive investigation from both theoretical calculations using density functional theory(DFT) and experimental perspectives.In addition,this review provides a comprehensive summary of MXene based non-noble metal and various modification methods.These methods encompass doping,vacancy engineering,hybrid structures,heterojunction formation,multi-scale engineering,surface engineering,and phase engineering.The review also presents suggestions for designing high-performance MXene based on non-noble metals.It offers guidance on employing construction strategies for electrocatalysts.By leveraging the unique properties and tunability of MXene and implementing these modification methods,researchers can enhance the catalytic activity,stability,selectivity,and efficiency of MXene based non-noble metal catalysts.
文摘BACKGROUND Increasingly extranodal marginal B-cell lymphoma of mucosa-associated lymphoid tissue,known as mucosa-associated lymphoid tissue(MALT)lymphoma,is a type of non-Hodgkin’s lymphoma.The prognosis of primary gastric MALT(GML)patients can be affected by many factors.Clinical risk factors,including age,type of therapy,sex,stage and family hematologic malignancy history,also have significant effects on the development of the disease.The available data are mainly focused on epidemiology;in contrast,few studies have investigated the prognostic variables for overall survival(OS)in patients with primary GML.Based on the realities above,we searched a large amount of data on patients diagnosed with primary GML in the Surveillance,Epidemiology and End Results(SEER)database.The aim was to develop and verify a survival nomogram model that can predict the overall survival prognosis of primary GML by com-bining prognostic and determinant variables.AIM To create an effective survival nomogram for patients with primary gastric GML.METHODS All data of patients with primary GML from 2004 to 2015 were collected from the SEER database.The primary endpoint was OS.Based on the LASSO and COX regression,we created and further verified the accuracy and effectiveness of the survival nomogram model by the concordance index(C-index),calibration curve and timedependent receiver operating characteristic(td-ROC)curves.RESULTS A total of 2604 patients diagnosed with primary GML were selected for this study.A total of 1823 and 781 people were randomly distributed into the training and testing sets at a ratio of 7:3.The median follow-up of all patients was 71 mo,and the 3-and 5-year OS rates were 87.2%and 79.8%,respectively.Age,sex,race,Ann Arbor stage and radiation were independent risk factors for OS of primary GML(all P<0.05).The C-index values of the nomogram were 0.751(95%CI:0.729-0.773)and 0.718(95%CI:0.680-0.757)in the training and testing cohorts,respectively,showing the good discrimination ability of the nomogram model.Td-ROC curves and calibration plots also indicated satisfactory predictive power and good agreement of the model.Overall,the nomogram shows favorable performance in discriminating and predicting the OS of patients with primary GML.CONCLUSION A nomogram was developed and validated to have good survival predictive performance based on five clinical independent risk factors for OS for patients with primary GML.Nomograms are a low-cost and convenient clinical tool in assessing individualized prognosis and treatment for patients with primary GML.
基金supported by the National Natural Science Foundation of China (NSFC) (52171206, 51762013)the Key Project of Hebei Natural Science Foundation (E20202201030)+5 种基金the BeijingTianjin-Hebei Collaborative Innovation Community Construction Project (21344301D)The Second Batch of Young Talent of Hebei Province (70280016160250, 70280011808)the Key Fund in Hebei Province Department of Education China (ZD2021014)The Central Government Guide Local Funding Projects for Scientific and Technological Development (216Z4404G, 206Z4402G)the Interdisciplinary Research Program of Natural Science of Hebei University (DXK202107)the China Postdoctoral Science Foundation (No. 2021M701718)。
文摘The development of high-efficiency and cost-effective bifunctional electrocatalysts for overall water splitting remains a formidable challenge.Herein,FeNi-Nd_(2)O_(3) nanoparticles anchored on N-doped carbon nanotubes(FeNi-Nd_(2)O_(3)/NCN) are designed for highly effective overall water splitting via a facile two-step hydrothermal approach.The synthetic FeNi-Nd_(2)O_(3) hetero-trimers(Fe 2p-Ni 2p-Nd 3d orbital coupling)on NCN achieve excellent oxygen evolution reaction(OER) and hydrogen evolution reaction(HER) activities with overpotentials of 270 and 120 mV at 10 mA cm^(-2) in 1 M KOH solution.Moreover,a small voltage of 1.52 V at 10 mA cm^(-2) is achieved when FeNi-Nd_(2)O_(3)/NCN is assessed as bifunctional catalyst for overall water splitting,which is superior to the typically integrated Pt/C and RuO_(2) counterparts(1.54 V at 10 mA cm^(-2)).The related characterizations including X-ray absorption fine structure(XAFS)spectroscopy show that the remarkably improved activity is originated from Nd_(2)O_(3)-induced FeNi bimetallic lattice contraction.Furthermore,density functional theory(DFT) calculations indicate that the lattice contraction reduces binding energies of intermediates by downshifting the position of FeNi bimetallic d-band center relative to the Fermi level to optimize catalytic performance.Therefore,the Nd_(2)O_(3)-induced FeNi bimetallic lattice contraction may provide a new perspective for designing and synthesizing innovative catalytic systems.
基金supported by National Natural Science Foundation of China(22369022)Technology Innovation Leading Program of Shaanxi(2022QFY07-03)。
文摘The efficiency of photocatalytic overall water splitting was mainly limited by the slow reaction kinetics of water oxidation.How to design effective surface active site to overcome the slow water oxidation reaction was a major challenge.Here,we propose a strategy to accelerate surface water oxidation through the fabrication spatially separated double active sites.FeCoPi/Bi_(4)NbO_(8)Cl-OVs photocatalyst with spatially separated double active site was prepared by hydrogen reduction photoanode deposition method.Due to the high matching of the spatial loading positions of FeCoPi and OVs with the photogenerated charge distribution of Bi_(4)NbO_(8)Cl and corresponding reaction mechanisms of substrate,the FeCoPi and OVs on the(001)and(010)crystal planes of Bi_(4)NbO_(8)Cl photocatalyst provided surface active site for water oxidation reaction and electron shuttle reaction(Fe^(3+)/Fe^(2+)),respectively.Under visible light irradiation,the evolution O_(2)rate of FeCoPi/Bi_(4)NbO_(8)Cl OVs was 16.8μmol h^(-1),as 32.9 times as Bi_(4)NbO_(8)Cl.Furthermore,a hydrogen evolution co-catalyst PtRu@Cr_(2)O_(3)was prepared by sequential photodeposition method.Due to the introduction of Ru,the Schottky barrier between PbTiO_(3)and Pt was effectively reduced,which promoted the transfer of photogenerated electrons to PtRu@Cr_(2)O_(3)thermodynamically,the evolution H_(2)rate on PtRu@Cr_(2)O_(3)/PbTiO_(3)increased to 664.8 times.On based of the synchronous enhancement of the water oxidation performance on FeCoPi/Bi_(4)NbO_(8)Cl-OVs and water reduction performance on PtRu@Cr_(2)O_(3)/PbTiO_(3),a novel Z-Scheme photocatalytic overall water splitting system(FeCoPi/Bi_(4)NbO_(8)Cl-OVs)mediated by Fe^(3+)/Fe^(2+)had successfully constructed.Under visible light irradiation,the evolution rates of H_(2)and O_(2)were 2.5 and 1.3μmol h^(-1),respectively.This work can provide some reference for the design of active site and the controllable synthesis of OVs spatial position.On the other hand,the hydrogen evolution co catalyst(PtRu@Cr_(2)O_(3))and the co catalyst FeCoPi for oxygen evolution contributed to the construction of an overall water splitting system.