Effective bulk phase and surface charge separation is critical for charge utilization during the photo-catalytic energy conversion process.In this work,the ternary Ni_(2)P-NiS/twinned Mn_(0.5)Cd_(0.5)S(T-MCS)nanohybri...Effective bulk phase and surface charge separation is critical for charge utilization during the photo-catalytic energy conversion process.In this work,the ternary Ni_(2)P-NiS/twinned Mn_(0.5)Cd_(0.5)S(T-MCS)nanohybrids were successfully constructed via combining Ni_(2)P-NiS with T-MCS solid solution for visible light photocatalytic H_(2)evolution.T-MCS is composed of zinc blende Mn_(0.5)Cd_(0.5)S(ZB-MCS)and wurtzite Mn_(0.5)Cd_(0.5)S(WZ-MCS)and those two alternatively arranged crystal phases endow T-MCS with excellent bulk phase charge separation performance for the slight energy level difference between ZB-MCS and WZ-MCS.S-scheme carriers transfer route between NiS and T-MCS can accelerate the interfacial charge separation and retain the active electrons and holes,meanwhile,co-catalyst Ni_(2)P as electron receiver and proton reduction center can further optimize the H_(2)evolution reaction kinetics based on the surface Schottky barrier effect.The above-formed homo-heterojunctions can establish multiple charge transfer channels in the bulk phase of T-MCS and interface of T-MCS and Ni_(2)P-NiS.Under the synergistic effect of twinned homojunction,S-scheme heterojunction,and Schottky barrier,the ternary Ni_(2)P-NiS/T-MCS com-posite manifested an H_(2)production rate of 122.5 mmol h^(-1)g^(-1),which was 1.33,1.24,and 2.58 times higher than those of the NiS/T-MCS(92.4 mmol h^(-1)g^(-1)),Ni_(2)P/T-MCS(98.4 mmol h^(-1)g^(-1)),and T-MCS(47.5 mmol h^(-1)g^(-1)),respectively.This work demonstrates a promising strategy to develop efficient sul-fides photocatalyst toward targeted solar-driven H_(2)evolution through homo-heterojunction engineering.展开更多
Constructing of heterojunction was identified as a feasible way to improve photocatalytic activity of pho-tocatalyst.In this work,a n-p type Bi_(2)WO_(6)/AgInS_(2)S-scheme heterojunction was successfully prepared for ...Constructing of heterojunction was identified as a feasible way to improve photocatalytic activity of pho-tocatalyst.In this work,a n-p type Bi_(2)WO_(6)/AgInS_(2)S-scheme heterojunction was successfully prepared for organic pollutants degradation.This Bi_(2)WO_(6)/AgInS_(2)S-scheme heterojunction exhibited much higher pho-tocatalytic activity towards Rhodamine B(92.24%,expose to visible light for 60 min),norfloxacin(81.73%,expose to visible light for 90 min)and levofloxacin(87.46%,expose to visible light for 90 min)than pure Bi_(2)WO_(6)and pure AgInS_(2).Toxicity analysis indicated the low environmental toxicity of Rhodamine B degradation intermediates for Rye seeds and Sudangrass seeds germination and growth.Mechanism study displayed that AgInS_(2)and Bi_(2)WO_(6)work as the primary photocatalyst to form·O_(2)−and ·OH,respectively.The improved photocatalytic activity of the Bi_(2)WO_(6)/AgInS_(2)S-scheme heterojunction was due to the im-proved light response range and intensified carrier separation capability.Additionally,a S-scheme charge transfer mechanism including multiple charge transfer channels was proposed.This work could provide an effective strategy for organic pollutants degradation in wastewater.展开更多
Developing machine learning frameworks with predictive power,interpretability,and transferability is crucial,yet it faces challenges in the field of electrocatalysis.To achieve this,we employed rigorous feature engine...Developing machine learning frameworks with predictive power,interpretability,and transferability is crucial,yet it faces challenges in the field of electrocatalysis.To achieve this,we employed rigorous feature engineering to establish a finely tuned gradient boosting regressor(GBR)model,which adeptly captures the physical complexity from feature space to target variables.We demonstrated that environmental electron effects and atomic number significantly govern the success of the mapping process via global and local explanations.The finely tuned GBR model exhibits exceptional robustness in predicting CO adsorption energies(R_(ave)^(2)=0.937,RMSE=0.153 eV).Moreover,the model demonstrated remarkable transfer learning ability,showing excellent predictive power for OH,NO,and N_(2) adsorption.Importantly,the GBR model exhibits exceptional predictive capability across an extensive search space,thereby demonstrating profound adaptability and versatility.Our research framework significantly enhances the interpretability and transferability of machine learning in electrocatalysis,offering vital insights for further advancements.展开更多
The design and construction of heterojunction photocatalysts,which possess a staggered energy band structure and appropriate interfacial contact,is an effective way to achieve outstanding photocatalytic performance.In...The design and construction of heterojunction photocatalysts,which possess a staggered energy band structure and appropriate interfacial contact,is an effective way to achieve outstanding photocatalytic performance.In this study,2D/2D BiOBr/g‐C_(3)N_(4)heterojunctions were successfully obtained by a convenient in situ self‐assembly route.Under simulated sunlight irradiation,99%of RhB(10 mg·L–1,100 mL)was efficiently degraded by 1.5‐BiOBr/g‐C_(3)N_(4)within 30 min,which is better than the performance of both BiOBr and g‐C_(3)N_(4),and it has superior stability.In addition,the composite also exhibits enhanced photocatalytic activity for H2 production.The enhanced activity can be attributed to the intimate interface contact,the larger surface area,and the highly efficient separation of photoinduced electron–hole pairs.Based on the experimental results,a novel S‐scheme model was proposed to illuminate the transfer process of charge carriers.This study presents a simple way to develop novel step‐scheme photocatalysts for environmental and related applications.展开更多
Ag nanoparticles (NPs) were deposited on the surface of g-C3N4 (CN) by an in situ calcination method. NiS was successfully loaded onto the composites by a hydrothermal method. The results showed that the 10 wt%-NiS/1....Ag nanoparticles (NPs) were deposited on the surface of g-C3N4 (CN) by an in situ calcination method. NiS was successfully loaded onto the composites by a hydrothermal method. The results showed that the 10 wt%-NiS/1.0 wt%-Ag/CN composite exhibits excellent photocatalytic H2 generation performance under solar-light irradiation. An H2 production rate of 9.728 mmol·g^-1·h^-1 was achieved, which is 10.82-, 3.45-, and 2.77-times higher than those of pure g-C3N4, 10 wt%-NiS/CN, and 1.0 wt%-Ag/CN composites, respectively. This enhanced photocatalytic H2 generation can be ascribed to the co-decoration of Ag and NiS on the surface of g-C3N4, which efficiently improves light harvesting capacity, photogenerated charge carrier separation, and photocatalytic H2 production kinetics. Thus, this study demonstrates an effective strategy for constructing excellent g-C3N4-related composite photocatalysts for H2 production by using different co-catalysts.展开更多
The demand for the swirl nozzle with enhanced temperature resistance and lightweight properties is in-creasing as the thrust-to-weight ratio of aero-engines rises.The Al_(2)O_(3) ceramic swirl nozzle can maintain high...The demand for the swirl nozzle with enhanced temperature resistance and lightweight properties is in-creasing as the thrust-to-weight ratio of aero-engines rises.The Al_(2)O_(3) ceramic swirl nozzle can maintain high strength in a hostile environment of high temperature and severe corrosion,while also meeting the requirements of aircraft to enhance efficiency and decrease weight.However,Al_(2)O_(3) ceramics are limited in their application for aerospace components due to their poor thermal shock resistance(TSR)stemming from their inherent brittleness.This work reported an innovative design and fabrication strategy based on photopolymerization 3D printing technology to realize the three-dimensional shell structure through element interdiffusion and nanoscale stacking of the reinforced phase.With this strategy,a novel type of the new dual-structure Al_(2)O_(3) ceramic composed of MgAl_(2)O_(4) shell structure and matrix could be con-structed in situ.The nano-sized MgAl_(2)O_(4) caused a crack passivation effect after the thermal shock,which could improve the strength and TSR of 3D-printed Al_(2)O_(3) ceramic.In addition,the effects of MgO content and sintering temperature on sintering behavior,flexural strength,porosity,and TSR of Al_(2)O_(3) ceram-ics manufactured by digital light processing(DLP)processing were systematically studied.The optimum overall performance of Al_(2)O_(3) ceramics was obtained at the sintering temperature of 1550℃and the MgO content of 1.0 wt.%,with a maximum flexural strength of 111.929 MPa and a critical temperature difference of 374.24℃for TSR.Based on the above research,an aero-engine swirl nozzle with high ther-mal shock resistance has been successfully prepared by ceramic 3D printing technology,which enhances high-temperature resistance and promotes lightweight design in aero-engine.展开更多
BACKGROUND Tumor budding(TB)has emerged as a promising independent prognostic biomarker in colorectal cancer(CRC).The prognostic role of TB has been extensively studied and currently affects clinical decision making i...BACKGROUND Tumor budding(TB)has emerged as a promising independent prognostic biomarker in colorectal cancer(CRC).The prognostic role of TB has been extensively studied and currently affects clinical decision making in patients with stage I and II CRC.However,existing prognostic studies on TB in stage III CRC have been confined to small retrospective cohort studies.Consequently,this study investigated the correlation among TB categories,clinicopathological features,and prognosis in stage III-IV CRC to further enhance the precision and individualization of treatment through refined prognostic risk stratification.AIM To analyze the relationship between TB categories and clinicopathological characteristics and assess their prognostic value in stage III-IV CRC to further refine the prognostic risk stratification of stage III-IV CRC.METHODS The clinical data of 547 CRC patients were collected for this retrospective study.Infiltration at the front edge of the tumor buds was counted according to the 2016 International Tumor Budding Consensus Conference guidelines.RESULTS Multivariate Cox proportional hazards regression analysis demonstrated that chemotherapy(P=0.004),clinical stage IV(P<0.001),≥4 regional lymph node metastases(P=0.004),left-sided colonic cancer(P=0.040),and Bd 2-3(P=0.002)were independent prognostic factors in patients with stage III-IV CRC.Moreover,the density of tumor infiltrating lymphocytes was higher in Bd 1 than in Bd 2-3,both in the tumor stroma and its invasive margin.CONCLUSION TB has an independent predictive prognostic value in patients with stage III-IV CRC.It is recommended to complete the TB report of stage III-IV CRC cases in the standardized pathological report to further refine risk stratification.展开更多
Non-flow aqueous zinc-bromine batteries without auxiliary components(e.g.,pumps,pipes,storage tanks)and ion-selective membranes represent a cost-effective and promising technology for large-scale energy storage.Unfort...Non-flow aqueous zinc-bromine batteries without auxiliary components(e.g.,pumps,pipes,storage tanks)and ion-selective membranes represent a cost-effective and promising technology for large-scale energy storage.Unfortunately,they generally suffer from serious diffusion and shuttle of polybromide(Br^(-),Br^(3-))due to the weak physical adsorption between soluble polybromide and host carbon materials,which results in low energy efficiency and poor cycling stability.Here,we develop a novel self-capture organic bromine material(1,10-bis[3-(trimethylammonio)propyl]-4,4'-bipyridinium bromine,NVBr4)to successfully realize reversible solid complexation of bromide components for stable non-flow zinc-bromine battery applications.The quaternary ammonium groups(NV^(4+)ions)can effectively capture the soluble polybromide species based on strong chemical interaction and realize reversible solid complexation confined within the porous electrodes,which transforms the conventional“liquid-liquid”conversion of soluble bromide components into“liquid-solid”model and effectively suppresses the shuttle effect.Thereby,the developed non-flow zinc-bromide battery provides an outstanding voltage platform at 1.7 V with a notable specific capacity of 325 mAh g^(-1)NVBr4(1 A g^(-1)),excellent rate capability(200 mAh g^(-1)NVBr4 at 20 A g^(-1)),outstanding energy density of 469.6 Wh kg^(-1)and super-stable cycle life(20,000 cycles with 100%Coulombic efficiency),which outperforms most of reported zinc-halogen batteries.Further mechanism analysis and DFT calculations demonstrate that the chemical interaction of quaternary ammonium groups and bromide species is the main reason for suppressing the shuttle effect.The developed strategy can be extended to other halogen batteries to obtain stable charge storage.展开更多
BACKGROUND Whether operation is superior to non-operation for humeral shaft fracture remains debatable.We hypothesized that operation could decrease the nonunion and reintervention rates and increase the functional ou...BACKGROUND Whether operation is superior to non-operation for humeral shaft fracture remains debatable.We hypothesized that operation could decrease the nonunion and reintervention rates and increase the functional outcomes.AIM To compare the clinical efficacy between operative and nonoperative approaches for humeral shaft fractures.METHODS We searched the PubMed,Web of Science,ScienceDirect,and Cochrane databases from 1990 to December 2023 for clinical trials and cohort studies comparing the effects of operative and conservative methods on humeral shaft fractures.Two investigators independently extracted data from the eligible studies,and the other two assessed the methodological quality of each study.The quality of the included studies was assessed using the Cochrane risk bias or Newcastle-Ottawa Scale.The nonunion,reintervention and the overall complications and functional scores were pooled and analyzed using Review Manager software(version 5.3).RESULTS A total of four randomized control trials and 13 cohort studies were included,with 1285 and 1346 patients in the operative and nonoperative groups,respectively.Patients in the operative group were treated with a plate or nail,whereas those in the conservative group were managed with splint or functional bracing.Four studies were assessed as having a high risk of bias,and the other 13 were of a low risk of bias according to the Newcastle-Ottawa Scale or Cochrane risk bias tool.The operative group had a significantly decreased rate of nonunion[odds ratio(OR)0.30;95%CI:0.23 to 0.40,reintervention(OR:0.33;95%CI:0.24 to 0.47),and overall complications(OR:0.62;95%CI:0.49 to 0.78)].The pooled effect of the Disabilities of Arm,Shoulder,and Hand score showed a significant difference at 3[mean difference(MD)-8.26;95%CI:-13.60 to-2.92],6(MD:-6.72;95%CI:-11.34 to-2.10),and 12 months(MD:-2.55;95%CI:-4.36 to-0.74).The pooled effect of Visual Analog Scale scores and the Constant-Murley score did not significantly differ between the two groups.CONCLUSION This systematic review and meta-analysis revealed a trend of rapid functional recovery and decreased rates of nonunion and reintervention after operation for humeral shaft fracture compared to conservative treatment.展开更多
Electrocatalytic nitrogen reduction to ammonia has garnered significant attention with the blooming of single-atom catalysts(SACs),showcasing their potential for sustainable and energy-efficient ammonia production.How...Electrocatalytic nitrogen reduction to ammonia has garnered significant attention with the blooming of single-atom catalysts(SACs),showcasing their potential for sustainable and energy-efficient ammonia production.However,cost-effectively designing and screening efficient electrocatalysts remains a challenge.In this study,we have successfully established interpretable machine learning(ML)models to evaluate the catalytic activity of SACs by directly and accurately predicting reaction Gibbs free energy.Our models were trained using non-density functional theory(DFT)calculated features from a dataset comprising 90 graphene-supported SACs.Our results underscore the superior prediction accuracy of the gradient boosting regression(GBR)model for bothΔg(N_(2)→NNH)andΔG(NH_(2)→NH_(3)),boasting coefficient of determination(R^(2))score of 0.972 and 0.984,along with root mean square error(RMSE)of 0.051 and 0.085 eV,respectively.Moreover,feature importance analysis elucidates that the high accuracy of GBR model stems from its adept capture of characteristics pertinent to the active center and coordination environment,unveilling the significance of elementary descriptors,with the colvalent radius playing a dominant role.Additionally,Shapley additive explanations(SHAP)analysis provides global and local interpretation of the working mechanism of the GBR model.Our analysis identifies that a pyrrole-type coordination(flag=0),d-orbitals with a moderate occupation(N_(d)=5),and a moderate difference in covalent radius(r_(TM-ave)near 140 pm)are conducive to achieving high activity.Furthermore,we extend the prediction of activity to more catalysts without additional DFT calculations,validating the reliability of our feature engineering,model training,and design strategy.These findings not only highlight new opportunity for accelerating catalyst design using non-DFT calculated features,but also shed light on the working mechanism of"black box"ML model.Moreover,the model provides valuable guidance for catalytic material design in multiple proton-electron coupling reactions,particularly in driving sustainable CO_(2),O_(2),and N_(2) conversion.展开更多
Lithium-sulfur(Li-S)batteries are regarded as one of the most promising next-generation energy storage systems due to their high theoretical specific energy density and low cost.However,serious shuttle effect and slug...Lithium-sulfur(Li-S)batteries are regarded as one of the most promising next-generation energy storage systems due to their high theoretical specific energy density and low cost.However,serious shuttle effect and sluggish lithium polysulfides(LiPSs)redox kinetics severely impede the practical application of Li-S batteries.Employing polar sulfur hosts is an effective strategy to alleviate the above problems.Herein,the potential of two-dimensional(2D)Ti_(2)B-based sulfur hosts for Li-S batteries was comprehensively explored using first-principles calculations.The results show that functional groups of Ti_(2)B can significantly modulate its structural properties,thus affecting its interaction with sulfurcontaining species.Among S,Se,F,Cl,and Br elements,Ti_(2)B terminated with S and Se atoms possess stronger adsorption capability towards soluble Li_(2)S_(8),Li_(2)S_(6),and Li_(2)S_(4),obviously stronger than organic electrolytes,which indicates that they can completely suppress the shuttle effect.Besides,Ti_(2)BS_(2)and Ti_(2)BSe_(2)can powerfully expedite the electrochemical conversion of LiPSs.Moreover,the decomposition energy barrier of Li_(2)S and diffusion energy barrier of single Li ion on them are also fairly low,manifesting their excellent catalytic performance towards the oxidation of Li_(2)S.Finally,Ti_(2)BS_(2)and Ti_(2)BSe_(2)always keep metallic conductivity during the whole charge/discharge process.Taking all this into account,Ti_(2)BS_(2)and Ti_(2)BSe_(2)are proposed as promising bifunctional sulfur hosts for Li-S batteries.Our results suggest that increasing the proportion of S and Se groups during the synthesis of Ti_(2)B monolayers is greatly helpful for obtaining high-performance Li-S batteries.Besides,our work not only reveals the huge potential of 2D transition metal borides in Li-S batteries,but also provides insightful guidance for the design and screening of new efficient sulfur cathodes.展开更多
Rechargeable metal-air batteries generally require efficient,durable,and safe bifunctional electrocatalysts to simultaneously support oxygen reduction/evolution reactions(ORR/OER).Herein,we employed first-principles c...Rechargeable metal-air batteries generally require efficient,durable,and safe bifunctional electrocatalysts to simultaneously support oxygen reduction/evolution reactions(ORR/OER).Herein,we employed first-principles calculations to explore the structure-activity relationship between the composition control of metal atoms and the catalytic activity of Pt-doped Ti_(2-x) Mn_(x) CO_(2) single-atom catalysts(SACs).The research found a clear linear relationship between the proportion of Mn and bifunctional performance,which can effectively modulate catalytic activity.Additionally,it shows excellent bifunctional catalytic activity at medium concentrations,among which the catalyst of Pt-V_(O)-Ti_(0.89) Mn_(1.11) CO_(2) displays the lowest overpo-tential(η^(ORR/OER)=0.26/0.28 V).Attributed to the modulation of the average magnetism of Mn and the d-band center of Pt by different com ponents,the bonding strength of the active center of Pt to adsorption intermediates is changed,resulting in the enhancement of the catalyst activity.Crucially,the molecular orbital-level bonding between the active site Pt and the adsorbed intermediate OH is clarified,shedding light on the involvement of the partially occupied antibonding state of Pt’s d orbital in the activation process.The research extensively explores the control of catalyst activity through composition,offering strong support for designing and optimizing highly active Janus MXene-supported SACs.展开更多
This study investigated the removal of dissolved organic matter（DOM） from real dyeing bio-treatment effluents（DBEs） with the use of a novel magnetic anion exchange resin（NDMP）.DOMs in two typical DBEs were fract...This study investigated the removal of dissolved organic matter（DOM） from real dyeing bio-treatment effluents（DBEs） with the use of a novel magnetic anion exchange resin（NDMP）.DOMs in two typical DBEs were fractionized using DAX-8/XAD-4 resin and ultrafiltration membranes. The hydrophilic fractions and the low molecular weight（MW）（〈3 kDa） DOM fractions constituted a major portion（〉50%） of DOMs for the two effluents. The hydrophilic and low MW fractions of both effluents were the greatest contributors of specific UV254absorbance（SUVA254）,and the SUVA254 of DOM fractions decreased with hydrophobicity and MW. Two DBEs exhibited acute and chronic biotoxicities. Both acute and chronic toxicities of DOM fractions increased linearly with the increase of SUVA254 value. Kinetics of dissolved organic carbon（DOC） removal via NDMP treatment was performed by comparing it with that of particle active carbon（PAC）. Results indicated that the removal of DOC from DBEs via NDMP was 60%,whereas DOC removals by PAC were lower than 15%. Acidic organics could be significantly removed with the use of NDMP. DOM with large MW in DBE could be removed significantly by using the same means. Removal efficiency of NDMP for DOM decreased with the decrease of MW. Compared with PAC,NDMP could significantly reduce the acute and chronic bio-toxicities of DBEs. NaCl/NaOH mixture regenerants,with selected concentrations of 10% NaCl（m/m）/1%NaOH（m/m）,could improve desorption efficiency.展开更多
Two-dimensional mesoporous ultrathin Cd0.5Zn0.5S nanosheets with a thickness of~1.5 nm were fabricated using a multistep chemical transformation strategy involving inorganic–organic hybrid ZnS-ethylenediamine(denoted...Two-dimensional mesoporous ultrathin Cd0.5Zn0.5S nanosheets with a thickness of~1.5 nm were fabricated using a multistep chemical transformation strategy involving inorganic–organic hybrid ZnS-ethylenediamine(denoted as ZnS(en)0.5)as a hard template.Inorganic–organic hybrid ZnS(en)0.5,Cd0.5Zn0.5S(en)x,and Cd0.5Zn0.5S nanosheets were sequentially fabricated,and their transformation processes were analyzed in detail.The fabricated Cd0.5Zn0.5S nanosheets exhibited high photocatalytic hydrogen evolution reaction activity in the presence of a sacrificial agent.The Cd0.5Zn0.5S nanosheets exhibited remarkably high H2 production activity of~1395μmol∙h^−1∙g^−1 in pure water with no co-catalyst,which is the highest value reported thus far for bare photocatalysts,to the best of our knowledge.The high activity of these nanosheets is attributed to their distinct nanostructure(e.g.,short transfer distance of photoinduced charge carriers,large number of unsaturated surface atoms,and large surface area).Moreover,ternary NiCo2S4 nanoparticles were employed to facilitate the charge separation and enhance the surface kinetics of H2 evolution.The H2 production rate reached~62.2 and~2436μmol∙h^−1∙g^−1 in triethanolamine and pure water,respectively,over the NiCo2S4/Cd0.5Zn0.5S heterojunctions.The result indicated that the Schottky junction was critical to the enhanced activity.The proposed method can be used for fabricating other highly efficient CdZnS-based photocatalysts for solar-energy conversion or other applications.展开更多
In this work,a novel plasmon-assisted UV-vis-NIR-driven W_(18)O_(49)/Cd_(0.5)Zn_(0.5)S heterostructure photocatalyst was obtained by a facile ultrasonic-assisted electrostatic self-assembly strategy.The hybrid exhibit...In this work,a novel plasmon-assisted UV-vis-NIR-driven W_(18)O_(49)/Cd_(0.5)Zn_(0.5)S heterostructure photocatalyst was obtained by a facile ultrasonic-assisted electrostatic self-assembly strategy.The hybrid exhibits extraordinary H2 evolution activity of 147.7 mmol·g^(-1)·h^(-1) at room temperature due to the efficient charge separation and expanded light absorption.Our investigation shows that the unique Step-scheme(S-scheme)charge transfer and the‘hot electron’injection are both responsible for the extraordinary H2 evolution process,depending on the wavelength of the incident light.Moreover,by accelerating the surface reaction kinetics,the activity can be further elevated to 306.1 mmol·g^(-1)·h^(-1),accompanied by a high apparent quantum yield of 45.3% at 365±7.5 nm.This work provides us a potential strategy for the highly efficient conversion of the solar energy by elaborately combining a nonstoichiometric ratio plasmonic material with an appropriate active photocatalyst.展开更多
Optimal use of water and fertilizers can enhance winter wheat yield and increase the efficiencies of water and fertilizer usage in dryland agricultural systems. In order to optimize water and nitrogen （N） management...Optimal use of water and fertilizers can enhance winter wheat yield and increase the efficiencies of water and fertilizer usage in dryland agricultural systems. In order to optimize water and nitrogen （N） management for winter wheat, we conducted field experiments from 2006 to 2008 at the Changwu Agro-ecological Experimental Station of the Chinese Academy of Sciences on the Loess Plateau, China. Regression models of wheat yield and evapotranspiration （ET） were established in this study to evaluate the water and fertilizer coupling effects and to determine the optimal coupling domain. The results showed that there was a positive effect of water and N fertilizer on crop yield, and optimal irrigation and N inputs can significantly increase the yield of winter wheat. In the drought year （2006-2007）, the maximum yield （Yma~） of winter wheat was 9.211 t/hm2 for the treatment with 324 mm irriga- tion and 310 kg/hm2 N input, and the highest water use efficiency （WUE） of 16.335 kg/（hm2.mm） was achieved with 198 mm irrigation and 274 kg/hm2 N input. While in the normal year （2007-2008）, the maximum winter wheat yield of 10.715 t/hm2 was achieved by applying 318 mm irrigation and 291 kg/hm2 N, and the highest WUE was 18.69 kg/（hm2.mm） with 107 mm irrigation and 256 kg/hm2 N input. Crop yield and ET response to irrigation and N inputs followed a quadratic and a line function, respectively. The optimal coupling domain was determined using the elas- ticity index （El） and its expression in the water-N dimensions, and was represented by an ellipse, such that the global maximum WUE （WUErnax） and Ymax values corresponded to the left and right end points of the long axis, respectively. Considering the aim to get the greatest profit in practice, the optimal coupling domain was represented by the lower half of the ellipse, with the Yma~ and WUE^ax on the two end points of the long axis. Overall, we found that the total amount of irrigation for winter wheat should not exceed 324 ram. In addition, our optimal coupling domain visually reflects the optimal range of water and N inputs for the maximum winter wheat yield on the Loess Plateau, and it may also provide a useful reference for identifying appropriate water and N inputs in agricultural applications.展开更多
In large continental orogens, an important research topic is the behavior of deep crustal and upper mantle deformation, and the flow styles of ductile material. The morphology of the eastern margin of the Tibetan plat...In large continental orogens, an important research topic is the behavior of deep crustal and upper mantle deformation, and the flow styles of ductile material. The morphology of the eastern margin of the Tibetan plateau, adjacent to the Sichuan basin, is characterized by very steep relief with high mountain ranges. The crust beneath this region slows the velocities in the middle and lower crust. We have adopted a relatively dense network to inverse the detailed structure of the crust and upper mantle along the eastern margin of the Tibetan plateau and Sichuan basin, using teleseismic data via receiver function analysis. The results are in-line with the hypothesis that viscous crustal material is flowing beneath the eastern margin of the Tibetan plateau and that this process drives overlying crustal material around the strong and rigid Sichuan basin. When the viscous material hits this obstruction, flows are divided into two or more branches with different directions. The upper part of the upwelling viscous flow produces the pressure to intrude the upper crust, thereby driving uplift of mountain ranges and high peaks. In contrast, the lower part of the downwelling viscous flow produces the pressure to intrude the lower crust and upper mantle to deepen the Moho discontinuity, causing observed crustal thickening.展开更多
基金supported by the National Natu-ral Science Foundation of China(Nos.22078261,21676213,and 11974276)Natural Science Basic Research Program of Shaanxi(No.2023-JC-YB-115)+1 种基金Shaanxi Key Science and Technology Innovation Team Project(No.2022TD-33)National College Student Inno-vation and Entrepreneurship Training Program(No.202210697069)for the financial support of this work.
文摘Effective bulk phase and surface charge separation is critical for charge utilization during the photo-catalytic energy conversion process.In this work,the ternary Ni_(2)P-NiS/twinned Mn_(0.5)Cd_(0.5)S(T-MCS)nanohybrids were successfully constructed via combining Ni_(2)P-NiS with T-MCS solid solution for visible light photocatalytic H_(2)evolution.T-MCS is composed of zinc blende Mn_(0.5)Cd_(0.5)S(ZB-MCS)and wurtzite Mn_(0.5)Cd_(0.5)S(WZ-MCS)and those two alternatively arranged crystal phases endow T-MCS with excellent bulk phase charge separation performance for the slight energy level difference between ZB-MCS and WZ-MCS.S-scheme carriers transfer route between NiS and T-MCS can accelerate the interfacial charge separation and retain the active electrons and holes,meanwhile,co-catalyst Ni_(2)P as electron receiver and proton reduction center can further optimize the H_(2)evolution reaction kinetics based on the surface Schottky barrier effect.The above-formed homo-heterojunctions can establish multiple charge transfer channels in the bulk phase of T-MCS and interface of T-MCS and Ni_(2)P-NiS.Under the synergistic effect of twinned homojunction,S-scheme heterojunction,and Schottky barrier,the ternary Ni_(2)P-NiS/T-MCS com-posite manifested an H_(2)production rate of 122.5 mmol h^(-1)g^(-1),which was 1.33,1.24,and 2.58 times higher than those of the NiS/T-MCS(92.4 mmol h^(-1)g^(-1)),Ni_(2)P/T-MCS(98.4 mmol h^(-1)g^(-1)),and T-MCS(47.5 mmol h^(-1)g^(-1)),respectively.This work demonstrates a promising strategy to develop efficient sul-fides photocatalyst toward targeted solar-driven H_(2)evolution through homo-heterojunction engineering.
基金supported by the Specialized Research Fund of Education Department of Shaanxi Province(No.22JY015)the College Students Innovation and Entrepreneurship Plan Training Program(No.S202211396006).
文摘Constructing of heterojunction was identified as a feasible way to improve photocatalytic activity of pho-tocatalyst.In this work,a n-p type Bi_(2)WO_(6)/AgInS_(2)S-scheme heterojunction was successfully prepared for organic pollutants degradation.This Bi_(2)WO_(6)/AgInS_(2)S-scheme heterojunction exhibited much higher pho-tocatalytic activity towards Rhodamine B(92.24%,expose to visible light for 60 min),norfloxacin(81.73%,expose to visible light for 90 min)and levofloxacin(87.46%,expose to visible light for 90 min)than pure Bi_(2)WO_(6)and pure AgInS_(2).Toxicity analysis indicated the low environmental toxicity of Rhodamine B degradation intermediates for Rye seeds and Sudangrass seeds germination and growth.Mechanism study displayed that AgInS_(2)and Bi_(2)WO_(6)work as the primary photocatalyst to form·O_(2)−and ·OH,respectively.The improved photocatalytic activity of the Bi_(2)WO_(6)/AgInS_(2)S-scheme heterojunction was due to the im-proved light response range and intensified carrier separation capability.Additionally,a S-scheme charge transfer mechanism including multiple charge transfer channels was proposed.This work could provide an effective strategy for organic pollutants degradation in wastewater.
基金supported by the Research Grants Council of Hong Kong(CityU 11305919 and 11308620)and NSFC/RGC Joint Research Scheme N_CityU104/19Hong Kong Research Grant Council Collaborative Research Fund:C1002-21G and C1017-22Gsupported by the Hong Kong Research Grant Council Collaborative Research Fund:C6021-19E.
文摘Developing machine learning frameworks with predictive power,interpretability,and transferability is crucial,yet it faces challenges in the field of electrocatalysis.To achieve this,we employed rigorous feature engineering to establish a finely tuned gradient boosting regressor(GBR)model,which adeptly captures the physical complexity from feature space to target variables.We demonstrated that environmental electron effects and atomic number significantly govern the success of the mapping process via global and local explanations.The finely tuned GBR model exhibits exceptional robustness in predicting CO adsorption energies(R_(ave)^(2)=0.937,RMSE=0.153 eV).Moreover,the model demonstrated remarkable transfer learning ability,showing excellent predictive power for OH,NO,and N_(2) adsorption.Importantly,the GBR model exhibits exceptional predictive capability across an extensive search space,thereby demonstrating profound adaptability and versatility.Our research framework significantly enhances the interpretability and transferability of machine learning in electrocatalysis,offering vital insights for further advancements.
文摘The design and construction of heterojunction photocatalysts,which possess a staggered energy band structure and appropriate interfacial contact,is an effective way to achieve outstanding photocatalytic performance.In this study,2D/2D BiOBr/g‐C_(3)N_(4)heterojunctions were successfully obtained by a convenient in situ self‐assembly route.Under simulated sunlight irradiation,99%of RhB(10 mg·L–1,100 mL)was efficiently degraded by 1.5‐BiOBr/g‐C_(3)N_(4)within 30 min,which is better than the performance of both BiOBr and g‐C_(3)N_(4),and it has superior stability.In addition,the composite also exhibits enhanced photocatalytic activity for H2 production.The enhanced activity can be attributed to the intimate interface contact,the larger surface area,and the highly efficient separation of photoinduced electron–hole pairs.Based on the experimental results,a novel S‐scheme model was proposed to illuminate the transfer process of charge carriers.This study presents a simple way to develop novel step‐scheme photocatalysts for environmental and related applications.
基金supported by the National Natural Science Foundation of China(21676213,21476183,51372201)the China Postdoctoral Science Foundation(2016M600809)the Natural Science Basic Research Plan in Shaanxi Province of China(2017JM2026)~~
文摘Ag nanoparticles (NPs) were deposited on the surface of g-C3N4 (CN) by an in situ calcination method. NiS was successfully loaded onto the composites by a hydrothermal method. The results showed that the 10 wt%-NiS/1.0 wt%-Ag/CN composite exhibits excellent photocatalytic H2 generation performance under solar-light irradiation. An H2 production rate of 9.728 mmol·g^-1·h^-1 was achieved, which is 10.82-, 3.45-, and 2.77-times higher than those of pure g-C3N4, 10 wt%-NiS/CN, and 1.0 wt%-Ag/CN composites, respectively. This enhanced photocatalytic H2 generation can be ascribed to the co-decoration of Ag and NiS on the surface of g-C3N4, which efficiently improves light harvesting capacity, photogenerated charge carrier separation, and photocatalytic H2 production kinetics. Thus, this study demonstrates an effective strategy for constructing excellent g-C3N4-related composite photocatalysts for H2 production by using different co-catalysts.
基金National Key Research and Development Program of China(No.2017YFA0700704)National Defense Basic Scientific Research Program of China(Grant No.JCKY2022130C005)+3 种基金National Natural Science Foundation of China(No.U22A20129)National Science and Technology Major Project(No.2017-VI-0002–0072)National Key Research and Development Program of China(No.2018YFB1106600)Students’Innovation and Entrepreneurship Foundation of USTC(Nos.CY2022G10 and CY2022C24)。
文摘The demand for the swirl nozzle with enhanced temperature resistance and lightweight properties is in-creasing as the thrust-to-weight ratio of aero-engines rises.The Al_(2)O_(3) ceramic swirl nozzle can maintain high strength in a hostile environment of high temperature and severe corrosion,while also meeting the requirements of aircraft to enhance efficiency and decrease weight.However,Al_(2)O_(3) ceramics are limited in their application for aerospace components due to their poor thermal shock resistance(TSR)stemming from their inherent brittleness.This work reported an innovative design and fabrication strategy based on photopolymerization 3D printing technology to realize the three-dimensional shell structure through element interdiffusion and nanoscale stacking of the reinforced phase.With this strategy,a novel type of the new dual-structure Al_(2)O_(3) ceramic composed of MgAl_(2)O_(4) shell structure and matrix could be con-structed in situ.The nano-sized MgAl_(2)O_(4) caused a crack passivation effect after the thermal shock,which could improve the strength and TSR of 3D-printed Al_(2)O_(3) ceramic.In addition,the effects of MgO content and sintering temperature on sintering behavior,flexural strength,porosity,and TSR of Al_(2)O_(3) ceram-ics manufactured by digital light processing(DLP)processing were systematically studied.The optimum overall performance of Al_(2)O_(3) ceramics was obtained at the sintering temperature of 1550℃and the MgO content of 1.0 wt.%,with a maximum flexural strength of 111.929 MPa and a critical temperature difference of 374.24℃for TSR.Based on the above research,an aero-engine swirl nozzle with high ther-mal shock resistance has been successfully prepared by ceramic 3D printing technology,which enhances high-temperature resistance and promotes lightweight design in aero-engine.
基金National Key R&D Program of China,No.2022YFF1203300.
文摘BACKGROUND Tumor budding(TB)has emerged as a promising independent prognostic biomarker in colorectal cancer(CRC).The prognostic role of TB has been extensively studied and currently affects clinical decision making in patients with stage I and II CRC.However,existing prognostic studies on TB in stage III CRC have been confined to small retrospective cohort studies.Consequently,this study investigated the correlation among TB categories,clinicopathological features,and prognosis in stage III-IV CRC to further enhance the precision and individualization of treatment through refined prognostic risk stratification.AIM To analyze the relationship between TB categories and clinicopathological characteristics and assess their prognostic value in stage III-IV CRC to further refine the prognostic risk stratification of stage III-IV CRC.METHODS The clinical data of 547 CRC patients were collected for this retrospective study.Infiltration at the front edge of the tumor buds was counted according to the 2016 International Tumor Budding Consensus Conference guidelines.RESULTS Multivariate Cox proportional hazards regression analysis demonstrated that chemotherapy(P=0.004),clinical stage IV(P<0.001),≥4 regional lymph node metastases(P=0.004),left-sided colonic cancer(P=0.040),and Bd 2-3(P=0.002)were independent prognostic factors in patients with stage III-IV CRC.Moreover,the density of tumor infiltrating lymphocytes was higher in Bd 1 than in Bd 2-3,both in the tumor stroma and its invasive margin.CONCLUSION TB has an independent predictive prognostic value in patients with stage III-IV CRC.It is recommended to complete the TB report of stage III-IV CRC cases in the standardized pathological report to further refine risk stratification.
基金the Guangdong Basic and Applied Basic Research Foundation(grant number:2019A1515011819,2021B1515120004)National Natural Science Foundation of China(22005207)Open Research Fund of Songshan Lake Materials Laboratory(2021SLABFN04).
文摘Non-flow aqueous zinc-bromine batteries without auxiliary components(e.g.,pumps,pipes,storage tanks)and ion-selective membranes represent a cost-effective and promising technology for large-scale energy storage.Unfortunately,they generally suffer from serious diffusion and shuttle of polybromide(Br^(-),Br^(3-))due to the weak physical adsorption between soluble polybromide and host carbon materials,which results in low energy efficiency and poor cycling stability.Here,we develop a novel self-capture organic bromine material(1,10-bis[3-(trimethylammonio)propyl]-4,4'-bipyridinium bromine,NVBr4)to successfully realize reversible solid complexation of bromide components for stable non-flow zinc-bromine battery applications.The quaternary ammonium groups(NV^(4+)ions)can effectively capture the soluble polybromide species based on strong chemical interaction and realize reversible solid complexation confined within the porous electrodes,which transforms the conventional“liquid-liquid”conversion of soluble bromide components into“liquid-solid”model and effectively suppresses the shuttle effect.Thereby,the developed non-flow zinc-bromide battery provides an outstanding voltage platform at 1.7 V with a notable specific capacity of 325 mAh g^(-1)NVBr4(1 A g^(-1)),excellent rate capability(200 mAh g^(-1)NVBr4 at 20 A g^(-1)),outstanding energy density of 469.6 Wh kg^(-1)and super-stable cycle life(20,000 cycles with 100%Coulombic efficiency),which outperforms most of reported zinc-halogen batteries.Further mechanism analysis and DFT calculations demonstrate that the chemical interaction of quaternary ammonium groups and bromide species is the main reason for suppressing the shuttle effect.The developed strategy can be extended to other halogen batteries to obtain stable charge storage.
基金Supported by Natural Science Foundation of Chongqing,China,No.CSTB2023NSCQ-MSX1080.
文摘BACKGROUND Whether operation is superior to non-operation for humeral shaft fracture remains debatable.We hypothesized that operation could decrease the nonunion and reintervention rates and increase the functional outcomes.AIM To compare the clinical efficacy between operative and nonoperative approaches for humeral shaft fractures.METHODS We searched the PubMed,Web of Science,ScienceDirect,and Cochrane databases from 1990 to December 2023 for clinical trials and cohort studies comparing the effects of operative and conservative methods on humeral shaft fractures.Two investigators independently extracted data from the eligible studies,and the other two assessed the methodological quality of each study.The quality of the included studies was assessed using the Cochrane risk bias or Newcastle-Ottawa Scale.The nonunion,reintervention and the overall complications and functional scores were pooled and analyzed using Review Manager software(version 5.3).RESULTS A total of four randomized control trials and 13 cohort studies were included,with 1285 and 1346 patients in the operative and nonoperative groups,respectively.Patients in the operative group were treated with a plate or nail,whereas those in the conservative group were managed with splint or functional bracing.Four studies were assessed as having a high risk of bias,and the other 13 were of a low risk of bias according to the Newcastle-Ottawa Scale or Cochrane risk bias tool.The operative group had a significantly decreased rate of nonunion[odds ratio(OR)0.30;95%CI:0.23 to 0.40,reintervention(OR:0.33;95%CI:0.24 to 0.47),and overall complications(OR:0.62;95%CI:0.49 to 0.78)].The pooled effect of the Disabilities of Arm,Shoulder,and Hand score showed a significant difference at 3[mean difference(MD)-8.26;95%CI:-13.60 to-2.92],6(MD:-6.72;95%CI:-11.34 to-2.10),and 12 months(MD:-2.55;95%CI:-4.36 to-0.74).The pooled effect of Visual Analog Scale scores and the Constant-Murley score did not significantly differ between the two groups.CONCLUSION This systematic review and meta-analysis revealed a trend of rapid functional recovery and decreased rates of nonunion and reintervention after operation for humeral shaft fracture compared to conservative treatment.
基金supported by the Research Grants Council of Hong Kong (City U 11305919 and 11308620)the NSFC/RGC Joint Research Scheme N_City U104/19The Hong Kong Research Grant Council Collaborative Research Fund:C1002-21G and C1017-22G。
文摘Electrocatalytic nitrogen reduction to ammonia has garnered significant attention with the blooming of single-atom catalysts(SACs),showcasing their potential for sustainable and energy-efficient ammonia production.However,cost-effectively designing and screening efficient electrocatalysts remains a challenge.In this study,we have successfully established interpretable machine learning(ML)models to evaluate the catalytic activity of SACs by directly and accurately predicting reaction Gibbs free energy.Our models were trained using non-density functional theory(DFT)calculated features from a dataset comprising 90 graphene-supported SACs.Our results underscore the superior prediction accuracy of the gradient boosting regression(GBR)model for bothΔg(N_(2)→NNH)andΔG(NH_(2)→NH_(3)),boasting coefficient of determination(R^(2))score of 0.972 and 0.984,along with root mean square error(RMSE)of 0.051 and 0.085 eV,respectively.Moreover,feature importance analysis elucidates that the high accuracy of GBR model stems from its adept capture of characteristics pertinent to the active center and coordination environment,unveilling the significance of elementary descriptors,with the colvalent radius playing a dominant role.Additionally,Shapley additive explanations(SHAP)analysis provides global and local interpretation of the working mechanism of the GBR model.Our analysis identifies that a pyrrole-type coordination(flag=0),d-orbitals with a moderate occupation(N_(d)=5),and a moderate difference in covalent radius(r_(TM-ave)near 140 pm)are conducive to achieving high activity.Furthermore,we extend the prediction of activity to more catalysts without additional DFT calculations,validating the reliability of our feature engineering,model training,and design strategy.These findings not only highlight new opportunity for accelerating catalyst design using non-DFT calculated features,but also shed light on the working mechanism of"black box"ML model.Moreover,the model provides valuable guidance for catalytic material design in multiple proton-electron coupling reactions,particularly in driving sustainable CO_(2),O_(2),and N_(2) conversion.
基金supported by the Shanxi Province Science Foundation for Youth(202303021212150)1331 Engineering of Shanxi Province,Research Grants Council of Hong Kong(CityU 11306517,11305919,and 11308620)National Natural Science Foundation of ChinaeResearch Grants Council of Hong Kong Joint Research Scheme N_CityU104/19.
文摘Lithium-sulfur(Li-S)batteries are regarded as one of the most promising next-generation energy storage systems due to their high theoretical specific energy density and low cost.However,serious shuttle effect and sluggish lithium polysulfides(LiPSs)redox kinetics severely impede the practical application of Li-S batteries.Employing polar sulfur hosts is an effective strategy to alleviate the above problems.Herein,the potential of two-dimensional(2D)Ti_(2)B-based sulfur hosts for Li-S batteries was comprehensively explored using first-principles calculations.The results show that functional groups of Ti_(2)B can significantly modulate its structural properties,thus affecting its interaction with sulfurcontaining species.Among S,Se,F,Cl,and Br elements,Ti_(2)B terminated with S and Se atoms possess stronger adsorption capability towards soluble Li_(2)S_(8),Li_(2)S_(6),and Li_(2)S_(4),obviously stronger than organic electrolytes,which indicates that they can completely suppress the shuttle effect.Besides,Ti_(2)BS_(2)and Ti_(2)BSe_(2)can powerfully expedite the electrochemical conversion of LiPSs.Moreover,the decomposition energy barrier of Li_(2)S and diffusion energy barrier of single Li ion on them are also fairly low,manifesting their excellent catalytic performance towards the oxidation of Li_(2)S.Finally,Ti_(2)BS_(2)and Ti_(2)BSe_(2)always keep metallic conductivity during the whole charge/discharge process.Taking all this into account,Ti_(2)BS_(2)and Ti_(2)BSe_(2)are proposed as promising bifunctional sulfur hosts for Li-S batteries.Our results suggest that increasing the proportion of S and Se groups during the synthesis of Ti_(2)B monolayers is greatly helpful for obtaining high-performance Li-S batteries.Besides,our work not only reveals the huge potential of 2D transition metal borides in Li-S batteries,but also provides insightful guidance for the design and screening of new efficient sulfur cathodes.
基金supported by the Research Grants Council of Hong Kong(Nos.CityU 11305919 and 11308620)the NSFC/RGC Joint Research Scheme(No.N_CityU104/19)+1 种基金Hong Kong Re-search Grant Council Collaborative Research Fund(Nos.C1002-21 G and C1017-22 G)This research made use of the comput-ing resources of the X-GPU cluster supported by the Hong Kong Research Grant Council Collaborative Research Fund(No.C6021-19EF).
文摘Rechargeable metal-air batteries generally require efficient,durable,and safe bifunctional electrocatalysts to simultaneously support oxygen reduction/evolution reactions(ORR/OER).Herein,we employed first-principles calculations to explore the structure-activity relationship between the composition control of metal atoms and the catalytic activity of Pt-doped Ti_(2-x) Mn_(x) CO_(2) single-atom catalysts(SACs).The research found a clear linear relationship between the proportion of Mn and bifunctional performance,which can effectively modulate catalytic activity.Additionally,it shows excellent bifunctional catalytic activity at medium concentrations,among which the catalyst of Pt-V_(O)-Ti_(0.89) Mn_(1.11) CO_(2) displays the lowest overpo-tential(η^(ORR/OER)=0.26/0.28 V).Attributed to the modulation of the average magnetism of Mn and the d-band center of Pt by different com ponents,the bonding strength of the active center of Pt to adsorption intermediates is changed,resulting in the enhancement of the catalyst activity.Crucially,the molecular orbital-level bonding between the active site Pt and the adsorbed intermediate OH is clarified,shedding light on the involvement of the partially occupied antibonding state of Pt’s d orbital in the activation process.The research extensively explores the control of catalyst activity through composition,offering strong support for designing and optimizing highly active Janus MXene-supported SACs.
基金supported by the Program for Changjiang Scholars and Innovative Research Team in University (Nos.51208249,51290282)Natural Science Foundation of China (Nos.51178215,51308283)+1 种基金the Jiangsu Nature Science Fund,China (Nos.BK2010006,BK2011032)the Joint Innovation Project for Production-Study-Research in Jiangsu Province,China (No.BY2013061)
文摘This study investigated the removal of dissolved organic matter（DOM） from real dyeing bio-treatment effluents（DBEs） with the use of a novel magnetic anion exchange resin（NDMP）.DOMs in two typical DBEs were fractionized using DAX-8/XAD-4 resin and ultrafiltration membranes. The hydrophilic fractions and the low molecular weight（MW）（〈3 kDa） DOM fractions constituted a major portion（〉50%） of DOMs for the two effluents. The hydrophilic and low MW fractions of both effluents were the greatest contributors of specific UV254absorbance（SUVA254）,and the SUVA254 of DOM fractions decreased with hydrophobicity and MW. Two DBEs exhibited acute and chronic biotoxicities. Both acute and chronic toxicities of DOM fractions increased linearly with the increase of SUVA254 value. Kinetics of dissolved organic carbon（DOC） removal via NDMP treatment was performed by comparing it with that of particle active carbon（PAC）. Results indicated that the removal of DOC from DBEs via NDMP was 60%,whereas DOC removals by PAC were lower than 15%. Acidic organics could be significantly removed with the use of NDMP. DOM with large MW in DBE could be removed significantly by using the same means. Removal efficiency of NDMP for DOM decreased with the decrease of MW. Compared with PAC,NDMP could significantly reduce the acute and chronic bio-toxicities of DBEs. NaCl/NaOH mixture regenerants,with selected concentrations of 10% NaCl（m/m）/1%NaOH（m/m）,could improve desorption efficiency.
文摘Two-dimensional mesoporous ultrathin Cd0.5Zn0.5S nanosheets with a thickness of~1.5 nm were fabricated using a multistep chemical transformation strategy involving inorganic–organic hybrid ZnS-ethylenediamine(denoted as ZnS(en)0.5)as a hard template.Inorganic–organic hybrid ZnS(en)0.5,Cd0.5Zn0.5S(en)x,and Cd0.5Zn0.5S nanosheets were sequentially fabricated,and their transformation processes were analyzed in detail.The fabricated Cd0.5Zn0.5S nanosheets exhibited high photocatalytic hydrogen evolution reaction activity in the presence of a sacrificial agent.The Cd0.5Zn0.5S nanosheets exhibited remarkably high H2 production activity of~1395μmol∙h^−1∙g^−1 in pure water with no co-catalyst,which is the highest value reported thus far for bare photocatalysts,to the best of our knowledge.The high activity of these nanosheets is attributed to their distinct nanostructure(e.g.,short transfer distance of photoinduced charge carriers,large number of unsaturated surface atoms,and large surface area).Moreover,ternary NiCo2S4 nanoparticles were employed to facilitate the charge separation and enhance the surface kinetics of H2 evolution.The H2 production rate reached~62.2 and~2436μmol∙h^−1∙g^−1 in triethanolamine and pure water,respectively,over the NiCo2S4/Cd0.5Zn0.5S heterojunctions.The result indicated that the Schottky junction was critical to the enhanced activity.The proposed method can be used for fabricating other highly efficient CdZnS-based photocatalysts for solar-energy conversion or other applications.
文摘In this work,a novel plasmon-assisted UV-vis-NIR-driven W_(18)O_(49)/Cd_(0.5)Zn_(0.5)S heterostructure photocatalyst was obtained by a facile ultrasonic-assisted electrostatic self-assembly strategy.The hybrid exhibits extraordinary H2 evolution activity of 147.7 mmol·g^(-1)·h^(-1) at room temperature due to the efficient charge separation and expanded light absorption.Our investigation shows that the unique Step-scheme(S-scheme)charge transfer and the‘hot electron’injection are both responsible for the extraordinary H2 evolution process,depending on the wavelength of the incident light.Moreover,by accelerating the surface reaction kinetics,the activity can be further elevated to 306.1 mmol·g^(-1)·h^(-1),accompanied by a high apparent quantum yield of 45.3% at 365±7.5 nm.This work provides us a potential strategy for the highly efficient conversion of the solar energy by elaborately combining a nonstoichiometric ratio plasmonic material with an appropriate active photocatalyst.
基金National Natural Science Foundation of China (51239009)National Science and Technology Support Program of China (2011BAD29B05)+1 种基金Key Discipline Foundation of Water Resources and Hydropower Engineering of Xinjiang Province (XJZDXK-2002-10-05)Natural Science Foundation of Shandong Province (ZR2010EM042)
文摘Optimal use of water and fertilizers can enhance winter wheat yield and increase the efficiencies of water and fertilizer usage in dryland agricultural systems. In order to optimize water and nitrogen （N） management for winter wheat, we conducted field experiments from 2006 to 2008 at the Changwu Agro-ecological Experimental Station of the Chinese Academy of Sciences on the Loess Plateau, China. Regression models of wheat yield and evapotranspiration （ET） were established in this study to evaluate the water and fertilizer coupling effects and to determine the optimal coupling domain. The results showed that there was a positive effect of water and N fertilizer on crop yield, and optimal irrigation and N inputs can significantly increase the yield of winter wheat. In the drought year （2006-2007）, the maximum yield （Yma~） of winter wheat was 9.211 t/hm2 for the treatment with 324 mm irriga- tion and 310 kg/hm2 N input, and the highest water use efficiency （WUE） of 16.335 kg/（hm2.mm） was achieved with 198 mm irrigation and 274 kg/hm2 N input. While in the normal year （2007-2008）, the maximum winter wheat yield of 10.715 t/hm2 was achieved by applying 318 mm irrigation and 291 kg/hm2 N, and the highest WUE was 18.69 kg/（hm2.mm） with 107 mm irrigation and 256 kg/hm2 N input. Crop yield and ET response to irrigation and N inputs followed a quadratic and a line function, respectively. The optimal coupling domain was determined using the elas- ticity index （El） and its expression in the water-N dimensions, and was represented by an ellipse, such that the global maximum WUE （WUErnax） and Ymax values corresponded to the left and right end points of the long axis, respectively. Considering the aim to get the greatest profit in practice, the optimal coupling domain was represented by the lower half of the ellipse, with the Yma~ and WUE^ax on the two end points of the long axis. Overall, we found that the total amount of irrigation for winter wheat should not exceed 324 ram. In addition, our optimal coupling domain visually reflects the optimal range of water and N inputs for the maximum winter wheat yield on the Loess Plateau, and it may also provide a useful reference for identifying appropriate water and N inputs in agricultural applications.
基金supported by National Natural Science Foundation of China under grant Nos. 40839909,41074062, and 40674040
文摘In large continental orogens, an important research topic is the behavior of deep crustal and upper mantle deformation, and the flow styles of ductile material. The morphology of the eastern margin of the Tibetan plateau, adjacent to the Sichuan basin, is characterized by very steep relief with high mountain ranges. The crust beneath this region slows the velocities in the middle and lower crust. We have adopted a relatively dense network to inverse the detailed structure of the crust and upper mantle along the eastern margin of the Tibetan plateau and Sichuan basin, using teleseismic data via receiver function analysis. The results are in-line with the hypothesis that viscous crustal material is flowing beneath the eastern margin of the Tibetan plateau and that this process drives overlying crustal material around the strong and rigid Sichuan basin. When the viscous material hits this obstruction, flows are divided into two or more branches with different directions. The upper part of the upwelling viscous flow produces the pressure to intrude the upper crust, thereby driving uplift of mountain ranges and high peaks. In contrast, the lower part of the downwelling viscous flow produces the pressure to intrude the lower crust and upper mantle to deepen the Moho discontinuity, causing observed crustal thickening.
