The integration of redox-active sites into the skeleton of open-framework materials is an efficient strategy toward high-performance organic electrodes for energy storage devices.In this work,stepwise introduction of ...The integration of redox-active sites into the skeleton of open-framework materials is an efficient strategy toward high-performance organic electrodes for energy storage devices.In this work,stepwise introduction of ketone(KT)groups to the skeletons of isostructural two-dimensional(2D)covalent organic frameworks(COFs)was realized by the condensation of 2,4,6-triformylphloroglucinol(Tp,as nodes)with a series of ditopic diamines,which contained none,one,two,and four KT moieties in each linker units,respectively.The precise control of the redox functionalities at the molecular level,combined with regular built-in channels in these KT-Tp COFs endowed them with superior capacitances and excellent rate capabilities for energy storage.In particular,2KT-Tp COF and 4KT-Tp COF electrodes exhibited high capacitances of 256 and 583 F g−1 at a discharge rate of 0.2 A g−1,respectively,which outperformed most reported COF-based electrodes.More importantly,exceptional long-term cyclabilities(>92%capacitance retention)were achieved even after 20,000 cycles at a high current density of 5 A g−1 for these KT-Tp COFs.Our results demonstrated that orthoquinone moieties rendered enhanced performance than the redox COFs with isolated carbonyl groups.展开更多
Both acceleration and pseudo-acceleration response spectra play important roles in structural seismic design.However,only one of them is generally provided in most seismic codes.Therefore,many studies have attempted t...Both acceleration and pseudo-acceleration response spectra play important roles in structural seismic design.However,only one of them is generally provided in most seismic codes.Therefore,many studies have attempted to develop conversion models between the acceleration response spectrum(SA)and the pseudo-acceleration response spectrum(PSA).Our previous studies found that the relationship between SA and PSA is affected by magnitude,distance,and site class.Subsequently,we developed an SA/PSA model incorporating these effects.However,this model is suitable for cases with small and moderate magnitudes and its accuracy is not good enough for cases with large magnitudes.This paper aims to develop an efficient SA/PSA model by considering influences of magnitude,distance,and site class,which can be applied to cases not only with small or moderate magnitudes but also with large ones.For this purpose,regression analyses were conducted using 16,660 horizontal seismic records with a wider range of magnitude.The magnitude of these seismic records varies from 4 to 9 and the distances vary from 10 to 200 km.These ground motions were recorded at 338 stations covering four site classes.By comparing them with existing models,it was found that the proposed model shows better accuracy for cases with any magnitudes,distances,and site classes considered in this study.展开更多
BACKGROUND Surgical site infections(SSIs)are a significant complication in laparoscopic cholecystectomy(LC),affecting patient outcomes and healthcare costs.AIM To identify risk factors associated with SSIs and evaluat...BACKGROUND Surgical site infections(SSIs)are a significant complication in laparoscopic cholecystectomy(LC),affecting patient outcomes and healthcare costs.AIM To identify risk factors associated with SSIs and evaluate the effectiveness of prophylactic antibiotics in reducing these infections.METHODS A comprehensive retrospective evaluation was conducted on 400 patients who underwent LC from January 2022 to January 2024.Patients were divided into infected(n=36)and non-infected(n=364)groups based on the occurrence of SSIs.Data collected included age,diabetes mellitus status,use of prophylactic antibiotics,and specific surgical complications.Statistical analyses using SPSS(Version 27.0)involved univariate and multivariate logistic regression to determine factors influencing the risk of SSIs.RESULTS The use of prophylactic antibiotics significantly reduced the incidence of SSIs(χ²=68.34,P<0.01).Older age(≥60 years)and comorbidities such as diabetes mellitus were identified as significant risk factors.Surgical complications like insufficient cystic duct stump,gallbladder perforation,and empyema also increased SSI risk.Notably,factors such as intraoperative blood loss and operation time did not significantly impact SSI occurrence.CONCLUSION Prophylactic antibiotics are effective in reducing the risk of SSIs in patients undergoing LC.Age,diabetes mellitus,and certain surgical complications significantly contribute to the risk.Effective management of these risk factors is essential to improve surgical outcomes and reduce the incidence of SSIs.展开更多
Background: The redox status of intra-uterine growth retardation(IUGR) piglets post-weaning has been poorly studied.Methods: Newborns from twenty-four sows were weighted, weaned at 21 d and fed a starter diet unti...Background: The redox status of intra-uterine growth retardation(IUGR) piglets post-weaning has been poorly studied.Methods: Newborns from twenty-four sows were weighted, weaned at 21 d and fed a starter diet until sampling.Sampling was done at 14 d post-weaning. A piglet was defined as IUGR when its birth weight was 2 SD below the mean birth weight of the total population. At weaning, eighteen piglets with nearly equal body weight from each category(i.e. IUGR or normal birth weight(NBW) piglets) were selected and then allocated to two treatments,consisted of six replicates with each pen having three piglets.Results: Compared with NBW group, IUGR significantly decreased average daily gain(P 〈 0.001), average daily feed intake(P = 0.003), and feed efficiency(P 〈 0.001) of piglets during the first two weeks post-weaning. IUGR decreased the activities of total antioxidant capacity(P = 0.019), total superoxide dismutase(T-SOD, P = 0.023),and ceruloplasmin(P = 0.044) but increased the levels of malondialdehyde(P = 0.040) and protein carbonyl(P = 0.010) in plasma. Similarly, the decreased activities of T-SOD(P = 0.005), copper- and zinc-containing superoxide dismutase(Cu/Zn-SOD, P = 0.002), and catalase(P = 0.049) was observed in the liver of IUGR piglets than these of NBW piglets. IUGR decreased hepatic Cu/Zn-SOD activity(P = 0.023) per unit of Cu/Zn-SOD protein in piglets when compared with NBW piglets. In addition, IUGR piglets exhibited the decreases in accumulation of copper in both plasma(P = 0.001) and liver(P = 0.014), as well as the concentrations of iron(P = 0.002) and zinc(P = 0.048) in liver. Compared with NBW, IUGR down-regulated m RNA expression of Cu/Zn-SOD(P = 0.021) in the liver of piglets.Conclusions: The results indicated that IUGR impaired antioxidant capacity and resulted in oxidative damage in fully weaned piglets, which might be associated with the decreased levels of redox-active trace minerals. This study highlights the importance of redox status in IUGR offspring and provides a rationale for alleviating oxidative damage by dietary interventions aiming to supplement trace minerals and to restore redox balance in the future.展开更多
The increasing demand of high-performance supercapacitors has aroused great interest in developing specific capacitance and energy density. Active carbon (AC) has attracted much attention as a promising electrode ma...The increasing demand of high-performance supercapacitors has aroused great interest in developing specific capacitance and energy density. Active carbon (AC) has attracted much attention as a promising electrode material for electric double-layer capacitors (EDLCs). Here, a facile strategy has been employed to fabricate high-performance EDLCs using the surface-oxygen functionalized active carbon (FAC) as an electrode and 2 M KOH with K3Fe(CN)6 as an electrolyte. In this system, K3Fe(CN)6 was used as a redox additive to enhance the performance of EDLCs. A 38.5% increase in specific capacitance (207.7 F g-1) was achieved compared with the KOH electrolyte without adding K3Fe(CN)G (152.9 F g-1), due to the synergistic effects between oxygenic functional groups and redox electrolyte. These findings provide an alternative route to improve the performance of EDLCs, which are promising candidates for the broad applications of high-performance supercapacitors.展开更多
Direct growth of redox-active noble metals and rational design of multifunctional electrochemical active materials play crucial roles in developing novel electrode materials for energy storage devices.In this regard,s...Direct growth of redox-active noble metals and rational design of multifunctional electrochemical active materials play crucial roles in developing novel electrode materials for energy storage devices.In this regard,silver(Ag)has attracted great attention in the design of efficient electrodes.Inspired by the house/building process,which means electing the right land,it lays a strong foundation and building essential columns for a complex structure.Herein,we report the construction of multifaceted heterostructure cobalt-iron hydroxide(CFOH)nanowires(NWs)@nickel cobalt manganese hydroxides and/or hydrate(NCMOH)nanosheets(NSs)on the Ag-deposited nickel foam and carbon cloth(i.e.,Ag/NF and Ag/CC)substrates.Moreover,the formation and charge storage mechanism of Ag are described,and these contribute to good conductive and redox chemistry features.The switching architectural integrity of metal and redox materials on metallic frames may significantly boost charge storage and rate performance with noticeable drop in resistance.The as-fabricated Ag@CFOH@NCMOH/NF electrode delivered superior areal capacity value of 2081.9μA h cm^(-2)at 5 mA cm^(-2).Moreover,as-assembled hybrid cell based on NF(HC/NF)device exhibited remarkable areal capacity value of 1.82 mA h cm^(-2)at 5 mA cm^(-2)with excellent rate capability of 74.77%even at 70 mA cm^(-2)Furthermore,HC/NF device achieved maximum energy and power densities of 1.39 mW h cm^(-2)and 42.35 mW cm^(-2),respectively.To verify practical applicability,both devices were also tested to serve as a self-charging station for various portable electronic devices.展开更多
Thermal energy is abundantly available in our daily life and industrial production,and especially,low-grade heat is often regarded as a byproduct.Collecting and utilizing this ignored energy by low-cost and simple tec...Thermal energy is abundantly available in our daily life and industrial production,and especially,low-grade heat is often regarded as a byproduct.Collecting and utilizing this ignored energy by low-cost and simple technologies may become a smart countermeasure to relieve the energy crisis.Here,a unique device has been demonstrated to achieve high value-added conversion of low-grade heat by introducing redox-active organic alizarin(AZ)onto N-doped hollow carbon nanofibers(N–HCNF)surface.As-prepared N–HCNF/AZ can deliver a high specific capacitance of 514.3 F g^(-1)(at 1 A g^(-1))and an outstanding rate capability of 60.3%even at 50 A g^(-1).Meanwhile,the assembled symmetric proton capacitor can deliver a high energy density of 28.0 Wh kg^(-1) at 350.0 W kg^(-1) and a maximum power density of 35.0 kW kg^(-1) at 17.0 Wh kg^(-1).Significantly,the thermally chargeable proton capacitors can attain a surprisingly high Seebeck coefficient of 15.3 mV K^(-1) and a power factor of 6.02µW g^(-1).Taking advantage of such high performance,a satisfying open-circuit voltage of 481.0 mV with a temperature difference of 54 K is achieved.This research provides new insights into construction of high value-added energy systems requiring high electrochemical performances.展开更多
The implementation of pristine covalent organic polymer(CO_(2)P)with well-defined structure as air electrode may spark fresh vitality to rechargeable zinc-air flow batteries(ZAFBs),but it still remains challenges in s...The implementation of pristine covalent organic polymer(CO_(2)P)with well-defined structure as air electrode may spark fresh vitality to rechargeable zinc-air flow batteries(ZAFBs),but it still remains challenges in synergistically regulating their electronic states and structural porosity for the great device performance.Here,we conquer these issues by exploiting N and S co-doped graphene with COP rich in metal-ligand nitrogen to synergistically construct an effective catalyst for oxygen reduction reaction(ORR).Among them,the N and S co-doped sites with high electronegativity properties alter the number of electron occupations in the d orbital of the iron centre and form electron-transfer bridges,thereby boosting the selectivity of the ORR-catalysed four-electron pathway.Meanwhile,the introduction of COP materials aids the formation of pore interstices in the graphene lamellae,which both adequately expose the active sites and facilitate the transport of reactive substances.Benefiting from the synergistic effect,as-prepared catalyst exhibits excellent half-wave potentials(E_(1/2)=912 mV)and stability(merely 8.8%drop after a long-term durability test of 50000 s).Further,ZAFBs assembled with the N/SG@CO_(2)P catalyst demonstrate exceptional power density(163.8 mW cm^(-2))and continuous charge and discharge for approximately 140 h at 10 mA cm^(-2),outperforming the noble-metal benchmarks.展开更多
Three cobalt complexes bearing tunable,redox-active bipyridyl N-heterocyclic carbene(NHC)-based ligands have been studied for electrocatalytic hydrogen evolution from aqueous solutions.The effect of structural modific...Three cobalt complexes bearing tunable,redox-active bipyridyl N-heterocyclic carbene(NHC)-based ligands have been studied for electrocatalytic hydrogen evolution from aqueous solutions.The effect of structural modifications to the ligand framework is investigated across the catalyst series,which includes a non-macrocyclic derivative(1-Co)and 16-(2-Co)and 15-(3-Co)membered macrocycles.A structure-activity relationship is demonstrated,in which the macrocyclic complexes have greater activity compared to their non-macrocyclic counterpart with the most rigid catalyst,supported by the 15-membered macrocycle,performing best overall.Indeed,3-Co catalyzes H2 evolution from aqueous pH 4 acetate buffer with a Faradaic efficiency of 97%at a low overpotential of 330 mV.Mechanistic studies are consistent with formation of a cobalt-hydride species that is subsequently protonated to evolve H2 via a heterolytic pathway.展开更多
We report a novel double-shelled nanoboxes photocatalyst architecture with tailored interfaces that accelerate quantum efficiency for photocatalytic CO_(2) reduction reaction(CO_(2)RR)via Mo–S bridging bonds sites in...We report a novel double-shelled nanoboxes photocatalyst architecture with tailored interfaces that accelerate quantum efficiency for photocatalytic CO_(2) reduction reaction(CO_(2)RR)via Mo–S bridging bonds sites in S_(v)–In_(2)S_(3)@2H–MoTe_(2).The X-ray absorption near-edge structure shows that the formation of S_(v)–In_(2)S_(3)@2H–MoTe_(2) adjusts the coordination environment via interface engineering and forms Mo–S polarized sites at the interface.The interfacial dynamics and catalytic behavior are clearly revealed by ultrafast femtosecond transient absorption,time-resolved,and in situ diffuse reflectance–Infrared Fourier transform spectroscopy.A tunable electronic structure through steric interaction of Mo–S bridging bonds induces a 1.7-fold enhancement in S_(v)–In_(2)S_(3)@2H–MoTe_(2)(5)photogenerated carrier concentration relative to pristine S_(v)–In_(2)S_(3).Benefiting from lower carrier transport activation energy,an internal quantum efficiency of 94.01%at 380 nm was used for photocatalytic CO_(2)RR.This study proposes a new strategy to design photocatalyst through bridging sites to adjust the selectivity of photocatalytic CO_(2)RR.展开更多
The Moon,as the closest celestial body to the Earth,plays a pivotal role in the progression of deep space exploration,and the establishment of research outposts on its surface represents a crucial step in this mission...The Moon,as the closest celestial body to the Earth,plays a pivotal role in the progression of deep space exploration,and the establishment of research outposts on its surface represents a crucial step in this mission.Lunar lava tubes are special underground caves formed by volcanic eruptions and are considered as ideal natural shelters and scientific laboratories for lunar base construction.This paper begins with an in-depth overview of the geological origins,exploration history,and distribution locations of lunar lava tubes.Subsequently,it delves into the presentation of four distinctive advantages and typical concepts for constructing bases within lava tubes,summarizing the ground-based attempts made thus far in lunar lava tube base construction.Field studies conducted on a lava tube in Hainan revealed rock compositions similar to those found during the Apollo missions and clear lava tube structures,making it a promising analog site.Lastly,the challenges and opportunities encountered in the field of geotechnical engineering regarding the establishment of lunar lava tube bases are discussed,encompassing cave exploration technologies,in-situ testing methods,geomechanical properties under lunar extreme environments,base design and structural stability assessment,excavation and reinforcement techniques,and simulated Earth-based lava tube base.展开更多
Zn based electrochemical energy storage systems(EES)have attracted tremendous interests owing to their low cost and high intrinsic safety.Nevertheless,the uncontrolled growth of Zn dendrites and the side reactions of ...Zn based electrochemical energy storage systems(EES)have attracted tremendous interests owing to their low cost and high intrinsic safety.Nevertheless,the uncontrolled growth of Zn dendrites and the side reactions of Zn metal anodes(ZMAs)severely restrict their applications.To address these issues,we design the asymmetric Zn-N_(4) atomic sites embedded hollow fibers(AS-IHF)as the flexible host for stable ZMAs.Through introducing different nitrogen resources in the synthesis,two kinds of coordination,i,e.Zn-N(pyridinic)and Zn-N(pyrrolic),are introduced in the Zn-N_(4) atomic module synchronously.The asymmetric Zn-N_(4) module with regulated micro-environment facilitates the superior zincophilic features and promotes the Zn adsorption.Meanwhile,the highly porous structure of the hollow fiber effectively reduces local current density,homogenize Zn ion flux,and alleviate structure stress.All the advantages endow the high efficiency and good stability for Zn plating/stripping.Both theoretical and experimental results demonstrate the high reversibility,low nucleation overpotential,and dendritefree behavior of the AS-IHF@Zn anode,which afford the high stability in high-rate and long-term cycling.Moreover,the solid-state Zn-ion hybrid capacitor(ZIHC)based on AS-IHF@Zn anode shows the high flexibility,reliability,and superior long-term cycling capability in a wide-range of temperatures(-20-25℃).Therefore,the present work not only gives a new strategy for modulating local environments of single atomic sites,but also propels the development of flexible power sources for diverse electronics.展开更多
Similarities play an important role in the reconstruction of human physical,cultural and technological evolution.The two sites presented in this paper,the Middle Palaeolithic site Lingjing in China Layer 10 and 11 and...Similarities play an important role in the reconstruction of human physical,cultural and technological evolution.The two sites presented in this paper,the Middle Palaeolithic site Lingjing in China Layer 10 and 11 and the Lower Palaeolithic site Schöningen 13Ⅱ-4,the socalled Schöningen Spear Horizon in Germany,show striking similarities.The archaeological record of both sites includes lithic artifacts as well as a very large assemblage of fossil bones.The preservation of the material at both sites is excellent and the faunas encountered at both sites show many similarities.The faunal lists of both sites include a diverse carnivore guild,an elephant species,two different rhinoceros species,two different equids,different cervids and large bovids.Both sites also yielded bone retouchers as well as a unique record of bone hammers that show identical,unusual flaking and percussion damage.These similarities are remarkable if one takes into account the difference in age(ca 200 kaBP)and the geographical distance between the two sites of ca 8000 km.Therefore,we do not assume a close cultural link between the hominin populations active at both sites.The authors assume that the observed similarities show more or less identical,opportunistic hominin behaviour at both sites located in a comparable environment with more or less similar taphonomic conditions.展开更多
Rapid and timely testing is essential to minimize the COVID-19 spread. Decision makers and policy planners need to determine the equal distribution and accessibility of testing sites. This study mainly examines the sp...Rapid and timely testing is essential to minimize the COVID-19 spread. Decision makers and policy planners need to determine the equal distribution and accessibility of testing sites. This study mainly examines the spatial equality of COVID-19 testing sites that maintain a zero COVID policy in Guangzhou City. The study has identified the spatial disparities of COVID testing sites, characteristics of testing locations, and accessibility. The study has obtained information on COVID testing sites in Guangzhou City and population data. Point pattern analyses, Euclidian distance and allocation, and network analyses are the main methods used to achieve the research objectives, and 1183 total COVID testing sites can be recognized in Guangzhou City. Results revealed that spatial disparities could be noticed over the study area. Testing locations of Guangzhou City are highly clustered. The most significant testing sites are located in Haizhu District, which has the third largest population. The highest population density can be identified in Yuexiu District. However, only 94 testing sites are located there. According to all the results, higher disparities can be identified, and a lack of testing sites is located in the north part of the study area. Some people in the northern part have to travel more than 10 km to reach a testing site. Finally, this paper suggests increasing the number of testing sites in the north and south parts of the study area and keeping the same distribution, considering the area, total population, and population density. This kind of research will be helpful to decision-makers in making proper decisions to maintain a zero COVID policy.展开更多
A series of Ni/ZSM-5 containing a small amount of Ni was prepared by an ion exchanged method.The impact of the n(SiO_(2))/n(Al_(2)O_(3))ratio on the catalytic activity was studied using the samples 0.09Ni/ZSM-5(60)and...A series of Ni/ZSM-5 containing a small amount of Ni was prepared by an ion exchanged method.The impact of the n(SiO_(2))/n(Al_(2)O_(3))ratio on the catalytic activity was studied using the samples 0.09Ni/ZSM-5(60)and 0.09Ni/ZSM-5(130).To determine the interaction between the Ni species and acid sites on the surface of the catalyst,the catalysts were characterized by N2 adsorption-desorption,X-ray diffraction(XRD),scanning electron microscopy(SEM),and UV-vis spectroscopy.The performance of the catalysts for the catalytic oligomerization of 1-hexene was investigated in detail.The nickel species were found to be uniformly distributed in all the catalysts.It was discovered that the oligomerization activity of the catalyst can be improved using Ni species;however,the contribution of Brønsted acids in oligomerization reactions is greater than that of Ni sites and Lewis acids.展开更多
The Birimian Baguiomo formations are located in the northern part of the Boromo greenstone belt. In this belt, the volcanic rocks (tholeiitic basalt, calcalkaline basalt, andesite) hosting the gold mineralization are ...The Birimian Baguiomo formations are located in the northern part of the Boromo greenstone belt. In this belt, the volcanic rocks (tholeiitic basalt, calcalkaline basalt, andesite) hosting the gold mineralization are located in the Kwademen-Baguiomo shear zone. This mineralization, located only a few kilometers from the Kwademen gold deposit, is uncharacterized and, together with the latter, could constitute a gold potential capable of being economically exploitable. It is in this sense that this work is carried out with a view to characterizing the gold mineralization of the Baguiomo gold panning site. To carry out this work, we have made direct field measurements, combined with microstructures, and combined all this with data from geochemical rock analysis of the basalts that are the main host formations. Geochemical data show that tholeitic basalts formed from a mantle plume that was emplaced in an oceanic plateau context. Calc-alkaline basalts and andesites are comparable to Paleoproterozoic tholeitic basalts (PTH3), which are slightly enriched in light rare earths. Fertility tests show that these basalts concentrate between 3 and 6 ppb of gold at the time of accretion, which is sufficient for remobilization of this primary gold during the Eburnian orogeny to yield a deposit of around 4 - 5 Moz. Gold mineralization is associated with pyrite crystals when the latter are disseminated in the rock mass, whereas it is associated with hematite in quartz veins concordant with S1 shear deformation. It is mainly the pyrite crystals in the pressure shadows that contain the gold grains, whose development would be synchronous with micro-shear zone reactivation during the first phase of D1<sub>B</sub> deformation. The second phase of D2<sub>B</sub> deformation, which is a crenulation or fracture schistosity, does not significantly affect the shear deformation that controls mineralization.展开更多
Cloud cover plays a pivotal role in assessing observational conditions for astronomical site-testing.Except for the fraction of observing time,its fragmentation also wields a significant influence on the quality of ni...Cloud cover plays a pivotal role in assessing observational conditions for astronomical site-testing.Except for the fraction of observing time,its fragmentation also wields a significant influence on the quality of nighttime sky clarity.In this article,we introduce the functionΓ∈[0,1],designed to comprehensively capture both the fraction of available observing time and its continuity.Leveraging in situ measurement data gathered at the Muztagh-Ata site between 2017 and 2021,we showcase the effectiveness of our approach.The statistical result illustrates that the Muztagh-Ata site affords approximately 122 nights that were absolutely clear and 205 very good nights annually,corresponding toΓ≥0.9 andΓ≥0.36 respectively.展开更多
Polyolefins such as polyethylene(PE)are one of the largest-scale synthetic plastics and play a key role in modern society.However,polyethylene is extremely inert to chemical recycling owing to its lack of chemical fun...Polyolefins such as polyethylene(PE)are one of the largest-scale synthetic plastics and play a key role in modern society.However,polyethylene is extremely inert to chemical recycling owing to its lack of chemical functionality and low polarity,making it one of the most challenging environmental hazards globally.Herein,we developed a phosphorylated CeO_(2)catalyst by an organophosphate precursor and featured efficient photocatalysis of low-density polyethylene(LDPE)without the acid or alkaline pre-treatment.Compared to pristine CeO_(2),the surface phosphorylation allows to introduce Brønsted acid sites,which facilitate to form carbonium ions on LDPE via protonation.In addition,the suitable band structure of the phosphorylated CeO_(2)catalyst enables efficient photoabsorption and generates reactive oxygen species,leading to the C–C bond cleavage of LDPE.As a result,the phosphorylated CeO_(2)catalyst exhibited an outstanding carbon conversion rate of>94%after 48 h of photocatalysis under 50 mW/cm^(2)of simulated sunlight,with a high CO_(2)product selectivity of>99%.Furthermore,the PE microparticles with sizes larger than 10μm released from LDPE plastic wrap were directly and completely degraded by photocatalysis within 12 h,suggesting an attractive and environmentally benign strategy of utilizing solar energy-based photocatalysis for reducing potential hazards of LDPE plastic trashes.展开更多
In high-level nuclear waste(HLW)repositories,concrete and compacted bentonite are designed to be employed as buffer materials,which may raise a problem of interactions between concrete and bentonite.These interactions...In high-level nuclear waste(HLW)repositories,concrete and compacted bentonite are designed to be employed as buffer materials,which may raise a problem of interactions between concrete and bentonite.These interactions would lead to mineralogy transformation and buffer performance decay of bentonite under the near field environment conditions in a repository.A small-scale experimental setup was established to simulate the concrete-bentonite-site water interaction system from a potential nuclear waste repository in China.Three types of mortars were prepared to correspond to the concrete at different degradation states.The results permit the determination of the following:(1)The macroproperties of Gaomiaozi(GMZ)bentonite(e.g.swelling pressure,permeability,the final dry density,and water content of reacted samples);(2)The composition evolution of fluids from the synthetic site water-concrete-bentonite interaction systems;(3)The sample characterization including Fourier transform infrared spectroscopy(FTIR)and X-ray powder diffraction(XRD).Under the infiltration of the synthesis Beishan site water(BSW),the swelling pressure of bentonite decreases slowly with time after reaching its second swelling peak.The flux decreases with time during the infiltrations,and it tends to be stable after more than 120 d.Due to the cation exchange reactions in the BSW-concrete-bentonite systems,the divalent cations(Ca and Mg)were consumed,and the monovalent cations(Na and K)were released.The dissolution of minerals in the bentonite such as albite causes Si increasing in the pore water.It was concluded that the hydro-mechanical property degradation of bentonite takes place when it comes into contact with concrete mortar,even under low-pH groundwater conditions.The soil dispersion,the uneven water content,and the uneven dry density in bentonite samples may partly contribute to the swelling decay of bentonite.Therefore,the direct contact with concrete has an obvious effect on the performance of bentonite.展开更多
基金supported financially by the National Key Research and Development Program of China(2017YFA0207500)National Natural Science Foundation of China(51973153)+1 种基金and Natural Science Foundation of Tianjin City(17JCJQJC44600).C.Peng is grateful for the funding from the National Natural Science Foundation of China(21875141),Shanghai Pujiang Program(18PJ1409000)and the Opening Project of State Key Laboratory of Advanced Chemical Power Sources(SKLACPS-C-23).
文摘The integration of redox-active sites into the skeleton of open-framework materials is an efficient strategy toward high-performance organic electrodes for energy storage devices.In this work,stepwise introduction of ketone(KT)groups to the skeletons of isostructural two-dimensional(2D)covalent organic frameworks(COFs)was realized by the condensation of 2,4,6-triformylphloroglucinol(Tp,as nodes)with a series of ditopic diamines,which contained none,one,two,and four KT moieties in each linker units,respectively.The precise control of the redox functionalities at the molecular level,combined with regular built-in channels in these KT-Tp COFs endowed them with superior capacitances and excellent rate capabilities for energy storage.In particular,2KT-Tp COF and 4KT-Tp COF electrodes exhibited high capacitances of 256 and 583 F g−1 at a discharge rate of 0.2 A g−1,respectively,which outperformed most reported COF-based electrodes.More importantly,exceptional long-term cyclabilities(>92%capacitance retention)were achieved even after 20,000 cycles at a high current density of 5 A g−1 for these KT-Tp COFs.Our results demonstrated that orthoquinone moieties rendered enhanced performance than the redox COFs with isolated carbonyl groups.
基金National Natural Science Foundation of China under Grant No.52278135。
文摘Both acceleration and pseudo-acceleration response spectra play important roles in structural seismic design.However,only one of them is generally provided in most seismic codes.Therefore,many studies have attempted to develop conversion models between the acceleration response spectrum(SA)and the pseudo-acceleration response spectrum(PSA).Our previous studies found that the relationship between SA and PSA is affected by magnitude,distance,and site class.Subsequently,we developed an SA/PSA model incorporating these effects.However,this model is suitable for cases with small and moderate magnitudes and its accuracy is not good enough for cases with large magnitudes.This paper aims to develop an efficient SA/PSA model by considering influences of magnitude,distance,and site class,which can be applied to cases not only with small or moderate magnitudes but also with large ones.For this purpose,regression analyses were conducted using 16,660 horizontal seismic records with a wider range of magnitude.The magnitude of these seismic records varies from 4 to 9 and the distances vary from 10 to 200 km.These ground motions were recorded at 338 stations covering four site classes.By comparing them with existing models,it was found that the proposed model shows better accuracy for cases with any magnitudes,distances,and site classes considered in this study.
文摘BACKGROUND Surgical site infections(SSIs)are a significant complication in laparoscopic cholecystectomy(LC),affecting patient outcomes and healthcare costs.AIM To identify risk factors associated with SSIs and evaluate the effectiveness of prophylactic antibiotics in reducing these infections.METHODS A comprehensive retrospective evaluation was conducted on 400 patients who underwent LC from January 2022 to January 2024.Patients were divided into infected(n=36)and non-infected(n=364)groups based on the occurrence of SSIs.Data collected included age,diabetes mellitus status,use of prophylactic antibiotics,and specific surgical complications.Statistical analyses using SPSS(Version 27.0)involved univariate and multivariate logistic regression to determine factors influencing the risk of SSIs.RESULTS The use of prophylactic antibiotics significantly reduced the incidence of SSIs(χ²=68.34,P<0.01).Older age(≥60 years)and comorbidities such as diabetes mellitus were identified as significant risk factors.Surgical complications like insufficient cystic duct stump,gallbladder perforation,and empyema also increased SSI risk.Notably,factors such as intraoperative blood loss and operation time did not significantly impact SSI occurrence.CONCLUSION Prophylactic antibiotics are effective in reducing the risk of SSIs in patients undergoing LC.Age,diabetes mellitus,and certain surgical complications significantly contribute to the risk.Effective management of these risk factors is essential to improve surgical outcomes and reduce the incidence of SSIs.
基金supported by the National Natural Science Foundation of China (31272454)
文摘Background: The redox status of intra-uterine growth retardation(IUGR) piglets post-weaning has been poorly studied.Methods: Newborns from twenty-four sows were weighted, weaned at 21 d and fed a starter diet until sampling.Sampling was done at 14 d post-weaning. A piglet was defined as IUGR when its birth weight was 2 SD below the mean birth weight of the total population. At weaning, eighteen piglets with nearly equal body weight from each category(i.e. IUGR or normal birth weight(NBW) piglets) were selected and then allocated to two treatments,consisted of six replicates with each pen having three piglets.Results: Compared with NBW group, IUGR significantly decreased average daily gain(P 〈 0.001), average daily feed intake(P = 0.003), and feed efficiency(P 〈 0.001) of piglets during the first two weeks post-weaning. IUGR decreased the activities of total antioxidant capacity(P = 0.019), total superoxide dismutase(T-SOD, P = 0.023),and ceruloplasmin(P = 0.044) but increased the levels of malondialdehyde(P = 0.040) and protein carbonyl(P = 0.010) in plasma. Similarly, the decreased activities of T-SOD(P = 0.005), copper- and zinc-containing superoxide dismutase(Cu/Zn-SOD, P = 0.002), and catalase(P = 0.049) was observed in the liver of IUGR piglets than these of NBW piglets. IUGR decreased hepatic Cu/Zn-SOD activity(P = 0.023) per unit of Cu/Zn-SOD protein in piglets when compared with NBW piglets. In addition, IUGR piglets exhibited the decreases in accumulation of copper in both plasma(P = 0.001) and liver(P = 0.014), as well as the concentrations of iron(P = 0.002) and zinc(P = 0.048) in liver. Compared with NBW, IUGR down-regulated m RNA expression of Cu/Zn-SOD(P = 0.021) in the liver of piglets.Conclusions: The results indicated that IUGR impaired antioxidant capacity and resulted in oxidative damage in fully weaned piglets, which might be associated with the decreased levels of redox-active trace minerals. This study highlights the importance of redox status in IUGR offspring and provides a rationale for alleviating oxidative damage by dietary interventions aiming to supplement trace minerals and to restore redox balance in the future.
基金supported by grants from the National Natural Science Foundation of China(Nos.21606033,21376034,21506086)
文摘The increasing demand of high-performance supercapacitors has aroused great interest in developing specific capacitance and energy density. Active carbon (AC) has attracted much attention as a promising electrode material for electric double-layer capacitors (EDLCs). Here, a facile strategy has been employed to fabricate high-performance EDLCs using the surface-oxygen functionalized active carbon (FAC) as an electrode and 2 M KOH with K3Fe(CN)6 as an electrolyte. In this system, K3Fe(CN)6 was used as a redox additive to enhance the performance of EDLCs. A 38.5% increase in specific capacitance (207.7 F g-1) was achieved compared with the KOH electrolyte without adding K3Fe(CN)G (152.9 F g-1), due to the synergistic effects between oxygenic functional groups and redox electrolyte. These findings provide an alternative route to improve the performance of EDLCs, which are promising candidates for the broad applications of high-performance supercapacitors.
基金supported by the National Research Foundation of Korea (NRF)grant funded by the Korean government (MSIP) (2018R1A6A1A03025708)。
文摘Direct growth of redox-active noble metals and rational design of multifunctional electrochemical active materials play crucial roles in developing novel electrode materials for energy storage devices.In this regard,silver(Ag)has attracted great attention in the design of efficient electrodes.Inspired by the house/building process,which means electing the right land,it lays a strong foundation and building essential columns for a complex structure.Herein,we report the construction of multifaceted heterostructure cobalt-iron hydroxide(CFOH)nanowires(NWs)@nickel cobalt manganese hydroxides and/or hydrate(NCMOH)nanosheets(NSs)on the Ag-deposited nickel foam and carbon cloth(i.e.,Ag/NF and Ag/CC)substrates.Moreover,the formation and charge storage mechanism of Ag are described,and these contribute to good conductive and redox chemistry features.The switching architectural integrity of metal and redox materials on metallic frames may significantly boost charge storage and rate performance with noticeable drop in resistance.The as-fabricated Ag@CFOH@NCMOH/NF electrode delivered superior areal capacity value of 2081.9μA h cm^(-2)at 5 mA cm^(-2).Moreover,as-assembled hybrid cell based on NF(HC/NF)device exhibited remarkable areal capacity value of 1.82 mA h cm^(-2)at 5 mA cm^(-2)with excellent rate capability of 74.77%even at 70 mA cm^(-2)Furthermore,HC/NF device achieved maximum energy and power densities of 1.39 mW h cm^(-2)and 42.35 mW cm^(-2),respectively.To verify practical applicability,both devices were also tested to serve as a self-charging station for various portable electronic devices.
基金This work was supported by the National Natural Science Foundation of China(U1802256,21773118)Leading Edge Technology of Jiangsu Province(BK20202008)+1 种基金Postgraduate Research&Practice Innovation Program of Jiangsu Province(KYCX21_0204)Priority Academic Program Development of Jiangsu Higher Education Institutions(PAPD).
文摘Thermal energy is abundantly available in our daily life and industrial production,and especially,low-grade heat is often regarded as a byproduct.Collecting and utilizing this ignored energy by low-cost and simple technologies may become a smart countermeasure to relieve the energy crisis.Here,a unique device has been demonstrated to achieve high value-added conversion of low-grade heat by introducing redox-active organic alizarin(AZ)onto N-doped hollow carbon nanofibers(N–HCNF)surface.As-prepared N–HCNF/AZ can deliver a high specific capacitance of 514.3 F g^(-1)(at 1 A g^(-1))and an outstanding rate capability of 60.3%even at 50 A g^(-1).Meanwhile,the assembled symmetric proton capacitor can deliver a high energy density of 28.0 Wh kg^(-1) at 350.0 W kg^(-1) and a maximum power density of 35.0 kW kg^(-1) at 17.0 Wh kg^(-1).Significantly,the thermally chargeable proton capacitors can attain a surprisingly high Seebeck coefficient of 15.3 mV K^(-1) and a power factor of 6.02µW g^(-1).Taking advantage of such high performance,a satisfying open-circuit voltage of 481.0 mV with a temperature difference of 54 K is achieved.This research provides new insights into construction of high value-added energy systems requiring high electrochemical performances.
基金supported by the National Key Research and Development Program of China(2022YFB3807500)the Natural Science Foundation of China(22220102003)+3 种基金the Beijing Natural Science Foundation(JL23003)"Double-First-Class"construction projects(XK180301 and XK1804-02)China Postdoctoral Science Foundation 2023TQ0020Dostdoctoral Fellowship Program of CPSF(GZC20230199)。
文摘The implementation of pristine covalent organic polymer(CO_(2)P)with well-defined structure as air electrode may spark fresh vitality to rechargeable zinc-air flow batteries(ZAFBs),but it still remains challenges in synergistically regulating their electronic states and structural porosity for the great device performance.Here,we conquer these issues by exploiting N and S co-doped graphene with COP rich in metal-ligand nitrogen to synergistically construct an effective catalyst for oxygen reduction reaction(ORR).Among them,the N and S co-doped sites with high electronegativity properties alter the number of electron occupations in the d orbital of the iron centre and form electron-transfer bridges,thereby boosting the selectivity of the ORR-catalysed four-electron pathway.Meanwhile,the introduction of COP materials aids the formation of pore interstices in the graphene lamellae,which both adequately expose the active sites and facilitate the transport of reactive substances.Benefiting from the synergistic effect,as-prepared catalyst exhibits excellent half-wave potentials(E_(1/2)=912 mV)and stability(merely 8.8%drop after a long-term durability test of 50000 s).Further,ZAFBs assembled with the N/SG@CO_(2)P catalyst demonstrate exceptional power density(163.8 mW cm^(-2))and continuous charge and discharge for approximately 140 h at 10 mA cm^(-2),outperforming the noble-metal benchmarks.
文摘Three cobalt complexes bearing tunable,redox-active bipyridyl N-heterocyclic carbene(NHC)-based ligands have been studied for electrocatalytic hydrogen evolution from aqueous solutions.The effect of structural modifications to the ligand framework is investigated across the catalyst series,which includes a non-macrocyclic derivative(1-Co)and 16-(2-Co)and 15-(3-Co)membered macrocycles.A structure-activity relationship is demonstrated,in which the macrocyclic complexes have greater activity compared to their non-macrocyclic counterpart with the most rigid catalyst,supported by the 15-membered macrocycle,performing best overall.Indeed,3-Co catalyzes H2 evolution from aqueous pH 4 acetate buffer with a Faradaic efficiency of 97%at a low overpotential of 330 mV.Mechanistic studies are consistent with formation of a cobalt-hydride species that is subsequently protonated to evolve H2 via a heterolytic pathway.
基金the Natural Science Foundation of China(11922415,12274471)Guangdong Basic and Applied Basic Research Foundation(2022A1515011168,2019A1515011718,2019A1515011337)the Key Research and Development Program of Guangdong Province,China(2019B110209003).
文摘We report a novel double-shelled nanoboxes photocatalyst architecture with tailored interfaces that accelerate quantum efficiency for photocatalytic CO_(2) reduction reaction(CO_(2)RR)via Mo–S bridging bonds sites in S_(v)–In_(2)S_(3)@2H–MoTe_(2).The X-ray absorption near-edge structure shows that the formation of S_(v)–In_(2)S_(3)@2H–MoTe_(2) adjusts the coordination environment via interface engineering and forms Mo–S polarized sites at the interface.The interfacial dynamics and catalytic behavior are clearly revealed by ultrafast femtosecond transient absorption,time-resolved,and in situ diffuse reflectance–Infrared Fourier transform spectroscopy.A tunable electronic structure through steric interaction of Mo–S bridging bonds induces a 1.7-fold enhancement in S_(v)–In_(2)S_(3)@2H–MoTe_(2)(5)photogenerated carrier concentration relative to pristine S_(v)–In_(2)S_(3).Benefiting from lower carrier transport activation energy,an internal quantum efficiency of 94.01%at 380 nm was used for photocatalytic CO_(2)RR.This study proposes a new strategy to design photocatalyst through bridging sites to adjust the selectivity of photocatalytic CO_(2)RR.
基金supported by the National Natural Science Foundation of China(Nos.52125903 and 52339001).
文摘The Moon,as the closest celestial body to the Earth,plays a pivotal role in the progression of deep space exploration,and the establishment of research outposts on its surface represents a crucial step in this mission.Lunar lava tubes are special underground caves formed by volcanic eruptions and are considered as ideal natural shelters and scientific laboratories for lunar base construction.This paper begins with an in-depth overview of the geological origins,exploration history,and distribution locations of lunar lava tubes.Subsequently,it delves into the presentation of four distinctive advantages and typical concepts for constructing bases within lava tubes,summarizing the ground-based attempts made thus far in lunar lava tube base construction.Field studies conducted on a lava tube in Hainan revealed rock compositions similar to those found during the Apollo missions and clear lava tube structures,making it a promising analog site.Lastly,the challenges and opportunities encountered in the field of geotechnical engineering regarding the establishment of lunar lava tube bases are discussed,encompassing cave exploration technologies,in-situ testing methods,geomechanical properties under lunar extreme environments,base design and structural stability assessment,excavation and reinforcement techniques,and simulated Earth-based lava tube base.
基金supported by the Innovation Foundation of Graduate Student of Harbin Normal University (No.HSDBSCX2023-3),China。
文摘Zn based electrochemical energy storage systems(EES)have attracted tremendous interests owing to their low cost and high intrinsic safety.Nevertheless,the uncontrolled growth of Zn dendrites and the side reactions of Zn metal anodes(ZMAs)severely restrict their applications.To address these issues,we design the asymmetric Zn-N_(4) atomic sites embedded hollow fibers(AS-IHF)as the flexible host for stable ZMAs.Through introducing different nitrogen resources in the synthesis,two kinds of coordination,i,e.Zn-N(pyridinic)and Zn-N(pyrrolic),are introduced in the Zn-N_(4) atomic module synchronously.The asymmetric Zn-N_(4) module with regulated micro-environment facilitates the superior zincophilic features and promotes the Zn adsorption.Meanwhile,the highly porous structure of the hollow fiber effectively reduces local current density,homogenize Zn ion flux,and alleviate structure stress.All the advantages endow the high efficiency and good stability for Zn plating/stripping.Both theoretical and experimental results demonstrate the high reversibility,low nucleation overpotential,and dendritefree behavior of the AS-IHF@Zn anode,which afford the high stability in high-rate and long-term cycling.Moreover,the solid-state Zn-ion hybrid capacitor(ZIHC)based on AS-IHF@Zn anode shows the high flexibility,reliability,and superior long-term cycling capability in a wide-range of temperatures(-20-25℃).Therefore,the present work not only gives a new strategy for modulating local environments of single atomic sites,but also propels the development of flexible power sources for diverse electronics.
文摘Similarities play an important role in the reconstruction of human physical,cultural and technological evolution.The two sites presented in this paper,the Middle Palaeolithic site Lingjing in China Layer 10 and 11 and the Lower Palaeolithic site Schöningen 13Ⅱ-4,the socalled Schöningen Spear Horizon in Germany,show striking similarities.The archaeological record of both sites includes lithic artifacts as well as a very large assemblage of fossil bones.The preservation of the material at both sites is excellent and the faunas encountered at both sites show many similarities.The faunal lists of both sites include a diverse carnivore guild,an elephant species,two different rhinoceros species,two different equids,different cervids and large bovids.Both sites also yielded bone retouchers as well as a unique record of bone hammers that show identical,unusual flaking and percussion damage.These similarities are remarkable if one takes into account the difference in age(ca 200 kaBP)and the geographical distance between the two sites of ca 8000 km.Therefore,we do not assume a close cultural link between the hominin populations active at both sites.The authors assume that the observed similarities show more or less identical,opportunistic hominin behaviour at both sites located in a comparable environment with more or less similar taphonomic conditions.
文摘Rapid and timely testing is essential to minimize the COVID-19 spread. Decision makers and policy planners need to determine the equal distribution and accessibility of testing sites. This study mainly examines the spatial equality of COVID-19 testing sites that maintain a zero COVID policy in Guangzhou City. The study has identified the spatial disparities of COVID testing sites, characteristics of testing locations, and accessibility. The study has obtained information on COVID testing sites in Guangzhou City and population data. Point pattern analyses, Euclidian distance and allocation, and network analyses are the main methods used to achieve the research objectives, and 1183 total COVID testing sites can be recognized in Guangzhou City. Results revealed that spatial disparities could be noticed over the study area. Testing locations of Guangzhou City are highly clustered. The most significant testing sites are located in Haizhu District, which has the third largest population. The highest population density can be identified in Yuexiu District. However, only 94 testing sites are located there. According to all the results, higher disparities can be identified, and a lack of testing sites is located in the north part of the study area. Some people in the northern part have to travel more than 10 km to reach a testing site. Finally, this paper suggests increasing the number of testing sites in the north and south parts of the study area and keeping the same distribution, considering the area, total population, and population density. This kind of research will be helpful to decision-makers in making proper decisions to maintain a zero COVID policy.
基金Financial support was obtained from the State Key Laboratory of Petroleum Molecular&Process Engineering(24-ZC0607-0099)the Natural Science Foundation of China(21706177 and 22378293).
文摘A series of Ni/ZSM-5 containing a small amount of Ni was prepared by an ion exchanged method.The impact of the n(SiO_(2))/n(Al_(2)O_(3))ratio on the catalytic activity was studied using the samples 0.09Ni/ZSM-5(60)and 0.09Ni/ZSM-5(130).To determine the interaction between the Ni species and acid sites on the surface of the catalyst,the catalysts were characterized by N2 adsorption-desorption,X-ray diffraction(XRD),scanning electron microscopy(SEM),and UV-vis spectroscopy.The performance of the catalysts for the catalytic oligomerization of 1-hexene was investigated in detail.The nickel species were found to be uniformly distributed in all the catalysts.It was discovered that the oligomerization activity of the catalyst can be improved using Ni species;however,the contribution of Brønsted acids in oligomerization reactions is greater than that of Ni sites and Lewis acids.
文摘The Birimian Baguiomo formations are located in the northern part of the Boromo greenstone belt. In this belt, the volcanic rocks (tholeiitic basalt, calcalkaline basalt, andesite) hosting the gold mineralization are located in the Kwademen-Baguiomo shear zone. This mineralization, located only a few kilometers from the Kwademen gold deposit, is uncharacterized and, together with the latter, could constitute a gold potential capable of being economically exploitable. It is in this sense that this work is carried out with a view to characterizing the gold mineralization of the Baguiomo gold panning site. To carry out this work, we have made direct field measurements, combined with microstructures, and combined all this with data from geochemical rock analysis of the basalts that are the main host formations. Geochemical data show that tholeitic basalts formed from a mantle plume that was emplaced in an oceanic plateau context. Calc-alkaline basalts and andesites are comparable to Paleoproterozoic tholeitic basalts (PTH3), which are slightly enriched in light rare earths. Fertility tests show that these basalts concentrate between 3 and 6 ppb of gold at the time of accretion, which is sufficient for remobilization of this primary gold during the Eburnian orogeny to yield a deposit of around 4 - 5 Moz. Gold mineralization is associated with pyrite crystals when the latter are disseminated in the rock mass, whereas it is associated with hematite in quartz veins concordant with S1 shear deformation. It is mainly the pyrite crystals in the pressure shadows that contain the gold grains, whose development would be synchronous with micro-shear zone reactivation during the first phase of D1<sub>B</sub> deformation. The second phase of D2<sub>B</sub> deformation, which is a crenulation or fracture schistosity, does not significantly affect the shear deformation that controls mineralization.
基金supported by the Chinese Academy of Science(CAS)“Light of West China”Program(No.2022_XBQNXZ_014)the Joint Research Fund in Astronomy under a cooperative agreement between the National Natural Science Foundation of China(NSFC),the Chinese Academy of Sciences(CAS)(grant No.U2031209)+1 种基金the Xinjiang Natural Science Foundation(grant No.2022D01A357)the National Natural Science Foundation of China(NSFC,grant No.11873081)。
文摘Cloud cover plays a pivotal role in assessing observational conditions for astronomical site-testing.Except for the fraction of observing time,its fragmentation also wields a significant influence on the quality of nighttime sky clarity.In this article,we introduce the functionΓ∈[0,1],designed to comprehensively capture both the fraction of available observing time and its continuity.Leveraging in situ measurement data gathered at the Muztagh-Ata site between 2017 and 2021,we showcase the effectiveness of our approach.The statistical result illustrates that the Muztagh-Ata site affords approximately 122 nights that were absolutely clear and 205 very good nights annually,corresponding toΓ≥0.9 andΓ≥0.36 respectively.
基金the following funding agencies for supporting this work: the National Natural Science Foundation of China (22025502, U23A20552, 22379026, 22222901, 22175022)the Natural Science Foundation of Shanghai (23ZR1407000)the Science and Technology Commission of Shanghai Municipality (21DZ1206800)
文摘Polyolefins such as polyethylene(PE)are one of the largest-scale synthetic plastics and play a key role in modern society.However,polyethylene is extremely inert to chemical recycling owing to its lack of chemical functionality and low polarity,making it one of the most challenging environmental hazards globally.Herein,we developed a phosphorylated CeO_(2)catalyst by an organophosphate precursor and featured efficient photocatalysis of low-density polyethylene(LDPE)without the acid or alkaline pre-treatment.Compared to pristine CeO_(2),the surface phosphorylation allows to introduce Brønsted acid sites,which facilitate to form carbonium ions on LDPE via protonation.In addition,the suitable band structure of the phosphorylated CeO_(2)catalyst enables efficient photoabsorption and generates reactive oxygen species,leading to the C–C bond cleavage of LDPE.As a result,the phosphorylated CeO_(2)catalyst exhibited an outstanding carbon conversion rate of>94%after 48 h of photocatalysis under 50 mW/cm^(2)of simulated sunlight,with a high CO_(2)product selectivity of>99%.Furthermore,the PE microparticles with sizes larger than 10μm released from LDPE plastic wrap were directly and completely degraded by photocatalysis within 12 h,suggesting an attractive and environmentally benign strategy of utilizing solar energy-based photocatalysis for reducing potential hazards of LDPE plastic trashes.
基金supported by the National Natural Science Foundation of China(Grant No.42125701)the Innovation Program of Shanghai Municipal Education Commission(Grant No.2023ZKZD26)+2 种基金Fund of the Shanghai Science and Technology Commission(Grant No.22DZ2201200)Top Discipline Plan of Shanghai Universities-Class I and the Fundamental Research Funds for the Central UniversitiesFinancial support from the International Post-Doc Fund of The Hong Kong Polytechnic University is greatly appreciated.
文摘In high-level nuclear waste(HLW)repositories,concrete and compacted bentonite are designed to be employed as buffer materials,which may raise a problem of interactions between concrete and bentonite.These interactions would lead to mineralogy transformation and buffer performance decay of bentonite under the near field environment conditions in a repository.A small-scale experimental setup was established to simulate the concrete-bentonite-site water interaction system from a potential nuclear waste repository in China.Three types of mortars were prepared to correspond to the concrete at different degradation states.The results permit the determination of the following:(1)The macroproperties of Gaomiaozi(GMZ)bentonite(e.g.swelling pressure,permeability,the final dry density,and water content of reacted samples);(2)The composition evolution of fluids from the synthetic site water-concrete-bentonite interaction systems;(3)The sample characterization including Fourier transform infrared spectroscopy(FTIR)and X-ray powder diffraction(XRD).Under the infiltration of the synthesis Beishan site water(BSW),the swelling pressure of bentonite decreases slowly with time after reaching its second swelling peak.The flux decreases with time during the infiltrations,and it tends to be stable after more than 120 d.Due to the cation exchange reactions in the BSW-concrete-bentonite systems,the divalent cations(Ca and Mg)were consumed,and the monovalent cations(Na and K)were released.The dissolution of minerals in the bentonite such as albite causes Si increasing in the pore water.It was concluded that the hydro-mechanical property degradation of bentonite takes place when it comes into contact with concrete mortar,even under low-pH groundwater conditions.The soil dispersion,the uneven water content,and the uneven dry density in bentonite samples may partly contribute to the swelling decay of bentonite.Therefore,the direct contact with concrete has an obvious effect on the performance of bentonite.