Coordinating the ratio of Bronsted to Lewis acid sites in zeolite catalyst is crucial for the efficient conversion of dihydroxyacetone(DHA)to methyl lactate(ML)in methanol media due to the different acidic requirement...Coordinating the ratio of Bronsted to Lewis acid sites in zeolite catalyst is crucial for the efficient conversion of dihydroxyacetone(DHA)to methyl lactate(ML)in methanol media due to the different acidic requirements of the four fundamental reactions.Herein,we couple Sn-MFI and TS-1 zeolites with different abilities to induce methanol dissociation to rationally regulate the ratio of Bronsted and Lewis acid sites in methanol,thus facilitating the yield of DHA to ML.It is found that framework Sn sites with low dissociation energy(39.2 kJ/mol)induce methanol to release hydrogen protons,creating Bronsted acid sites to enable DHA dehydration to PA.Ti sites in TS-1 zeolite possess high methanol dissociation energy(73.5 kJ/mol),maintaining Lewis acidity in methanol,which provides sufficient active sites for cooperatively intensifying PA addition to HA and subsequent HA isomerization to ML.The synergistic effect of the two zeolites mitigates the side reaction while achieving high DHA conversion,thus steering the reaction toward ML generation.Consequently,ML yield increases by over 25% compared with that of single Sn-MFI zeolite,which offers a promising pathway to promote the synthesis of DHA to ML under mild conditions.展开更多
Oxygen vacancy(Vo)engineering has been recognized as one of the most effective strategies for enhancing the photocatalytic CO_(2) conversion performance of metal oxides,as it can simultaneously facilitate photogenerat...Oxygen vacancy(Vo)engineering has been recognized as one of the most effective strategies for enhancing the photocatalytic CO_(2) conversion performance of metal oxides,as it can simultaneously facilitate photogenerated charge carrier separation efficiency and provide additional surface reaction sites.However,the wide application of Vo engineering in photocatalysis are limited by its poor stability,owing to the easy recovery of these vacancy defects by atmospheric oxygen.Herein,we develop an indium(In)doping strategy to regulate the coordination environment in CeO_(2) with abundant Vo(CeO_(2-x)),thereby enhance its stability during photocatalytic CO_(2) conversion.Confirmed by positron annihilation lifetime spectroscopy(PALS),In dopants combine with Vo by substituting for part of Ce^(4+),forming In^(3+)-Vo complexes that effectively inhibit the formation of unstable va-cancy clusters.Such In^(3+)-Vo complexes can also reduce the energy required for formation of the CO products.Therefore,the optimized In-doped CeO_(2-x) exhibits excellent photocatalytic CO_(2) conversion performance,with a CO yield of 301.6μmol⋅g^(-1) after 5 h of light irradiation,and maintain high activity after four cycles of experiments.Comprehensive experimental and theoretical studies indicate that the introduction of In doping not only significantly improves the stability of Vo in CeO_(2-x),but also reconstruct the reaction kinetics of the CO_(2) conversion by forming In^(3+)-Vo complexes thus facilitating the overall reaction.展开更多
Rechargeable magnesium batteries(RMBs)possess the merits of greater theoretical capacity,cheaper magnesium metal and not easily producing branched crystals,and greater safety.Therefore,the current researches mainly co...Rechargeable magnesium batteries(RMBs)possess the merits of greater theoretical capacity,cheaper magnesium metal and not easily producing branched crystals,and greater safety.Therefore,the current researches mainly concentrate on the exploration of high-performance RMBs in the initial stage,but still face many gigantic challenges.Herein,petal-shaped nanorods CoS/CuS materials are successfully synthesized as RMBs cathode materials through a two-step metal sulfide template-free solvent-thermal synthesis method,which can effectively improve the reaction kinetics due to the petal-like nano-structure and provide rich electrochemically active sites to decrease the transport barrier of Mg^(2+),thus contributing to the enhancement of the reaction kinetics of magnesium storage in RMBs.The electrochemical performance test illustrates that CoS/CuS composite nanomaterials can considerably improve the charging and discharging specific capacity of the batteries as well as the voltage of the batteries due to the existing synergistic effect between them.The specific capacity of CoS/CuS cathode still can still be maintained as high as 62.8 mAh g^(−1)after 300 cycles at 200 mA g^(−1).And the specific capacity of this electrode material changes from 180.6 mAh g^(−1)to 30 mAh g^(−1)at the current densities from 100 mA g^(−1)to 1000 mA g^(−1),and when the current density is restored to 100 mA g^(−1),the specific capacity gradually recovered to 178.6 mAh g^(−1),which showed better rate performance and ultra-high cycling stability.This work highlights how the introduction of CuS into CoS nanostructures can benefit the reversibility and cyclicity of the magnesium storage reaction and offers an original and practical route for the modification of RMBs electrode materials with good electrochemical properties.展开更多
Epidemiological studies have indicated that branched-chain amino acids(BCAAs)increased and gut microbiota disordered in type 2 diabetes mellitus(T2DM).This study aimed to investigate the mechanism of Lactiplantibacill...Epidemiological studies have indicated that branched-chain amino acids(BCAAs)increased and gut microbiota disordered in type 2 diabetes mellitus(T2DM).This study aimed to investigate the mechanism of Lactiplantibacillus plantarum strain 84-3(Lp84-3)combined with Staphylococcus aureus bacteriophage on ameliorating T2DM.Here we perform a case-control study and identify that Staphylococcus_phage was inversely correlated with fasting blood glucose(FBG).It revealed that Lp84-3 could inhibit the growth of S.aureus,and Lp84-3 contains BCAAs degradation enzymes in its genome.Furthermore,Lp84-3 alone or combined with S.aureus bacteriophage interventions can improve blood glucose,insulin resistance,triglycerides,interleukin-1β,tumor necrosis factor-α(TNF-α),BCAAs,and acetyllactate synthase(ALS)in db/db mice.Lp84-3 and S.aureus bacteriophage decreased S.aureus,Malacoplasma iowae,and Oscillibacter sp.,and increased some beneficial such as L.plantarum and Muribaculaceae bacterium.Transcriptomic analyses revealed that Lp84-3 and S.aureus bacteriophage activated the PI3K/AKT/GLUT4 signaling pathway and upregulated key genes of Il22,Hgf,Col6a1,Gh,Itga10,Fgf23,and Prl involved in glucose metabolism in hypothalamus.Collectively,Lp84-3 and S.aureus bacteriophage alleviate T2DM by modulating gut microbiota and enhancing glucose metabolism in hypothalamus,supporting its potential use as a promising functional compound microecological agent for alleviating T2DM.展开更多
The electrochemical performance of all-solid-state lithium batteries(ASSLBs)can be prominently enhanced by minimizing the detrimental degradation of solid electrolytes through their undesirable side reactions with the...The electrochemical performance of all-solid-state lithium batteries(ASSLBs)can be prominently enhanced by minimizing the detrimental degradation of solid electrolytes through their undesirable side reactions with the conductive carbon additives(CCAs)inside the composite cathodes.Herein,the well-defined Mo_(3)Ni_(3)N nanosheets embedded onto the N-doped porous carbons(NPCs)substrate are successfully synthesized(Mo-Ni@NPCs)as CCAs inside LiCoO_(2)for Li_(6)PSC_5)Cl(LPSCl)-based ASSLBs.This nano-composite not only makes it difficult for hydroxide groups(-OH)to survive on the surface but also allows the in situ surface reconstruction to generate the ultra-stable MoS_(2)-Mo_(3)Ni_(3)N heterostructures after the initial cycling stage.These can effectively prevent the occurrence of OH-induced LPSC decomposition reaction from producing harmful insulating sulfates,as well as simultaneously constructing the highly-efficient electrons/ions dual-migration pathways at the cathode interfaces to facilitate the improvement of both electrons and Li+ions conductivities in ASSLBs.With this approach,fine-tuned Mo-Ni@NPCs can deliver extremely outstanding performance,including an ultra-high first discharge-specific capacity of 148.61 mAh g^(-1)(0.1C),a high Coulombic efficiency(94.01%),and a capacity retention rate after 1000 cycles still attain as high as 90.62%.This work provides a brand-new approach of“conversionprotection”strategy to overcome the drawbacks of composite cathodes interfaces instability and further promotes the commercialization of ASSLBs.展开更多
This work is devoted to the development of a low cost dimensionally stable anode with high oxygen evolution catalytic activity for practical applications.For this purpose,a Ti/SnO_(x)/MnO_(2) anode was fabricated thro...This work is devoted to the development of a low cost dimensionally stable anode with high oxygen evolution catalytic activity for practical applications.For this purpose,a Ti/SnO_(x)/MnO_(2) anode was fabricated through an innovative strategy involving Sn electrodeposition,oxidation,and MnO_(2)-layer preparation.The structure of the anode was characterized,and the oxygen evolution performance was evaluated in a H_(2)SO_(4) solution.The results show that compared with the Ti/SnO_(2)/MnO_(2) anode prepared by the conventional brushing-annealing process,the Ti/SnO_(x)/MnO_(2) anode fabricated through the innovative procedure exhibits a lower oxygen evolution potential and a nearly 40%longer accelerated lifespan.The superior oxygen evolution performance of the Ti/SnO_(x)/MnO_(2) anode is attributed to the distinctive SnO_(x) intermediate layer fabricated through Sn electrodeposition followed by oxidation,which indicates the great potential of the anode as a dimensionally stable anode for metal electrowinning and hydrogen production by electrolysis,etc.展开更多
As one of the three payloads for the Advanced Space-based Solar Observatory(ASO-S)mission,the Lyman-alpha(Lyα)Solar Telescope(LST)is composed of three instruments:a Solar Corona Imager(SCI),a LyαSolar Disk Imager(SD...As one of the three payloads for the Advanced Space-based Solar Observatory(ASO-S)mission,the Lyman-alpha(Lyα)Solar Telescope(LST)is composed of three instruments:a Solar Corona Imager(SCI),a LyαSolar Disk Imager(SDI)and a full-disk White-light Solar Telescope(WST).When working in-orbit,LST will simultaneously perform high-resolution imaging observations of all regions from the solar disk to the inner corona up to 2.5 R⊙(R⊙stands for the mean solar radius)with a spatial resolution of 4.8′′and 1.2′′for coronal and disk observations,respectively,and a temporal resolution of 30–120 s and 1–120 s for coronal and disk observations,respectively.The maximum exposure time can be up to20 s due to precise pointing and image stabilization function.Among the three telescopes of LST,SCI is a dual-waveband coronagraph simultaneously and independently observing the inner corona in the HI Lyα(121.6±10 nm)line and white light(WL)(700±40 nm)wavebands by using a narrowband Lyαbeam splitter and has a field of view(FOV)from 1.1 to 2.5 R⊙.The stray-light suppression level can attain<10^-6 B⊙(B⊙is the mean brightness of the solar disk)at 1.1 R⊙and≤5×10^-8 B⊙at 2.5 R⊙.SDI and WST are solar disk imagers working in the Lyαline and 360.0 nm wavebands,respectively,which adopt an off-axis two-mirror reflective structure with an FOV up to 1.2 R⊙,covering the inner coronal edge area and relating to coronal imaging.We present the up-to-date design for the LST payload.展开更多
Grain size is one of the most important factors affecting rice grain quality and yield,and attracts great attention from molecular biologists and breeders.In this study,we engineered a CRISPR/Cas9 system targeting the...Grain size is one of the most important factors affecting rice grain quality and yield,and attracts great attention from molecular biologists and breeders.In this study,we engineered a CRISPR/Cas9 system targeting the miR396 recognition site of the rice GS2 gene,which encodes growth-regulating factor 4(OsGRF4)and regulates multiple agronomic traits including grain size,grain quality,nitrogen use efficiency,abiotic stress response,and seed shattering.In contrast to most previous genome editing efforts in which indel mutations were chosen to obtain null mutants,a mutant named GS2^(E) carrying an in-frame 6-bp deletion and 1-bp substitution within the miR396-targeted sequence was identified.GS2^(E) plants showed increased expression of GS2 in consistent with impaired repression by miR396.As expected,the gain-of-function GS2^(E) mutant exhibited multiple beneficial traits including increased grain size and yield and bigger grain length/width ratio.Thousand grain weight and grain yield per plant of GS2^(E) plants were increased by 23.5%and 10.4%,respectively.These improved traits were passed to hybrids in a semidominant way,suggesting that the new GS2^(E) allele has great potential in rice improvement.Taken together,we report new GS2 germplasm and describe a novel gene-editing strategy that can be widely employed to improve grain size and yield in rice.This trait-improvement strategy could be applied to other genes containing miRNA target sites,in particular the conserved miR396-GRF/GIF module that governs plant growth,development and environmental response.展开更多
Background:As is widely known,an increasing number of forest areas were managed to preserve and enhance the health of forest ecosystems.However,previous research on forest management has often overlooked the importanc...Background:As is widely known,an increasing number of forest areas were managed to preserve and enhance the health of forest ecosystems.However,previous research on forest management has often overlooked the importance of structure-based.Aims:Our objectives were to define the direction of structure-based forest management.Subsequently,we investigated the relationships between forest structure and the regeneration,growth,and mortality of trees under different thinning treatments.Ultimately,the drivers of forest structural change were explored.Methods:On the basis of 92 sites selected from northeastern China,with different recovery time (from 1 to 15years) and different thinning intensities (0–59.9%) since the last thinning.Principal component analysis (PCA)identified relationships among factors determining forest spatial structure.The structural equation model (SEM)was used to analyze the driving factors behind the changes in forest spatial structure after thinning.Results:Light thinning (0–20%trees removed) promoted forest regeneration,and heavy thinning (over 35% of trees removed) facilitated forest growth.However,only moderate thinning (20%–35%trees removed) created a reasonable spatial structure.While dead trees were clustered,and they were hardly affected by thinning intensity.Additionally,thinning intensity,recovery time,and altitude indirectly improve the spatial structure of the forest by influencing diameter at breast height (DBH) and canopy area.Conclusion:Creating larger DBH and canopy area through thinning will promote the formation of complex forest structures,which cultivates healthy and stable forests.展开更多
Pyrolytic graphite (PG) with highly aligned graphene layers,present anisotropic electrical and thermal transport behavior,which is attractive in electronic,electrocatalyst and energy storage.Such pristine PG could mee...Pyrolytic graphite (PG) with highly aligned graphene layers,present anisotropic electrical and thermal transport behavior,which is attractive in electronic,electrocatalyst and energy storage.Such pristine PG could meeting the limit of electrical conductivity (~2.5×10^(4) S·cm^(−1)),although efforts have been made for achieving high-purity sp^(2) hybridized carbon.For manipulating the electrical conductivity of PG,a facile and efficient electrochemical strategy is demonstrated to enhance electrical transport ability via reversible intercalation/de-intercalation of AlCl_(4)^(-)into the graphitic interlayers.With the stage evolution at different voltages,variable electrical and thermal transport behaviors could be achieved via controlling AlCl_(4)^(-)concentrations in the PG because of substantial variation in the electronic density of states.Such evolution leads to decoupled electrical and thermal transport (opposite variation trend) in the in-plane and out-of-plane directions,and the in-plane electrical conductivity of the pristine PG (1.25×10^(4) S·cm^(−1)) could be massively promoted to 4.09×10^(4) S·cm(AlCl_(4)^(-)intercalated PG),much better than the pristine bulk graphitic papers used for the electrical transport and electromagnetic shielding.The fundamental mechanism of decoupled transport feature and electrochemical strategy here could be extended into other anisotropic conductive bulks for achieving unusual behaviors.展开更多
Although many material designs or strategic methods have been proposed for treating oil spills and oily wastewater,the complex oily state,dealing with the harsh operating conditions of oil–water separation(such as th...Although many material designs or strategic methods have been proposed for treating oil spills and oily wastewater,the complex oily state,dealing with the harsh operating conditions of oil–water separation(such as the recovery of viscous spilled crude oil,bacteria-containing oily wastewater,and removal of spilled oil under fire),and the autorecycling of oil and absorption materials remain a great challenge.This work proposed an ingenious design strategy of“several birds with one stone”to prepare p H/thermoresponsive flame-retardant/photothermal bactericidal P-Fe_(3)O_(4)-polydopamine(PDA)@melamine–formaldehyde(MF)foams.This design makes the foams remarkably effective in the recovery of spilled viscous crude oil as well as in the separation of bacteria-containing oily emulsions,particularly for instant fire extinguishing by magnetically controlled oil absorption as well as for fire alarms.The photothermal effect and p H response induce a change in the surface wettability of the foams,facilitating excellent autoadsorption/desorption of the spilled oil.The photothermal bactericidal activity and fouling resistance of the foam are beneficial to the separation of bacteria-containing oily wastewater.Outstanding flame-retardant properties and maneuverable magnetic control enable the foam to rapidly recover the spilled oil in a large range of fires,extinguish fires instantly,and facilitate early fire warning.The proposed strategy is expected to inspire further research on treating oil spills under complex conditions.展开更多
Binders are of vital importance in stabilizing the cathodes to enhance the cycling stability of lithiumsulfur(Li-S) batteries. However, conventional binders are typically confronted with the drawback of inability for ...Binders are of vital importance in stabilizing the cathodes to enhance the cycling stability of lithiumsulfur(Li-S) batteries. However, conventional binders are typically confronted with the drawback of inability for adsorbing lithium polysulfide(Li PS), thus resulting in severe active material losing and rapid capacity fading. Herein, a novel water-soluble hyperbranched poly(amidoamine)(HPAA) binder with controllable hyperbranched molecular structure and abundant amino end groups for Li-S battery is designed and fabricated, which can improve efficient adsorption for Li PS and stability of the sulfur cathodes. Besides, the strong intermolecular hydrogen bonds in HPAA binder can contribute to the structural stability of S cathode and integration of the conductive paths. Therefore, the Li-S battery with this functional binder exhibits excellent cycle performance with a capacity retention of 91% after 200 cycles at 0.1 C.Even at a high sulfur loading of 5.3 mg cm-2, a specific capacity of 601 mA h g-1 can also be achieved.Density functional theory(DFT) calculation further demonstrates that the enhanced electrochemical stability derives from the high binding energy between amino groups and LiP S and the wide electrochemical window(6.87 e V) of HPAA molecule. Based on the above all, this functional polymer will lighten a new species of binders for eco-friendly sulfur cathodes and significantly promote the practical applications of high-performance Li-S batteries.展开更多
The catalyst innovation that aims at noble-metal-free substitutes is one key aspect for future sustainable hydrogen energy deployment.In this paper,a nickel cobalt sulfoselenide/black phosphorus heterostructure(NiCoSe...The catalyst innovation that aims at noble-metal-free substitutes is one key aspect for future sustainable hydrogen energy deployment.In this paper,a nickel cobalt sulfoselenide/black phosphorus heterostructure(NiCoSe|S/BP)was fabricated to realize the highly active and durable water electrolysis through interface and valence dual-engineering.The NiCoSe|S/BP nanostructure was constructed by in-situ growing NiCo hydroxide nanosheet arrays on few-layer BP and subsequently one-step sulfoselenization by SeS2.Besides the conductive merit of BP substrate,holes in p-type BP are capable of oxidizing the Co^(2+)to high-valence and electron-accepting Co^(3+),benefiting the oxygen evolution reaction(OER).Meanwhile,Ni^(3+)/Ni^(2+)ratio in the heterostructure is reduced to maintain the electrical neutrality,which corresponds to the increased electron-donating character for boosting hydrogen evolution reaction(HER).As for HER and OER,the heterostructured NiCoSe|S/BP electrocatalyst exhibits small overpotentials of 172 and 285 mV at 10 mA cm^(-2)(η_(10))in alkaline media,respectively.And overall water splitting has been achieved at a low cell potential of 1.67 V at η_(10) with high stability.Molecular sensing and density functional theory(DFT)calculations are further proposed for understanding the rate-determine steps and enhanced catalytic mechanism.The investigation presents a deep-seated perception for the electrocatalytic performance enhancement of BP-based heterostructure.展开更多
IgG4-related sclerosing cholangitis(IgG4-SC)is an inflammatory disease that leads to bile duct stricture,characterized by the infiltration of IgG4-positive plasma cells into the bile duct wall,thickening of the bile d...IgG4-related sclerosing cholangitis(IgG4-SC)is an inflammatory disease that leads to bile duct stricture,characterized by the infiltration of IgG4-positive plasma cells into the bile duct wall,thickening of the bile duct wall,and narrowing of the lumen.The differential diagnosis of IgG4-SC mainly includes primary sclerosing cholangitis,cholangiocarcinoma,and pancreatic cancer.IgG4-SC is often associated with autoimmune pancreatitis and can be accurately diagnosed based on clinical diagnostic criteria.However,isolated IgG4-SC is difficult to distinguish from biliary tumors.Given the significant differences in biological behavior,treatment,and prognosis between these diseases,accurately identifying isolated IgG4-SC has very important clinical significance.展开更多
In this paper, a new anionic metal-organic framework, [In(PBPTTBA)][(CH_3)_2 NH_2](BUT-29) has been synthesized through the reaction of tetratopic acid ligand with double Lewis pyridine sites, 4,4',4'',4&#...In this paper, a new anionic metal-organic framework, [In(PBPTTBA)][(CH_3)_2 NH_2](BUT-29) has been synthesized through the reaction of tetratopic acid ligand with double Lewis pyridine sites, 4,4',4'',4'''-(4,4'-(1,4-phenylene)bis(pyridine-6,4,2-triyl)) tetrabenzoic acid(H_4 PBPTTBA) and In(NO_3)_2·5H_2O and fully characterized by single-crystal X-ray diffraction(SXRD), powder X-ray diffraction(PXRD),thermogravimetric analysis(TGA), infrared spectroscopy(IR), and elemental analysis(EA). BUT-29 can be used as an efficient adsorbent for the selective removal of organic cationic dyes in N,N0-dimethylformamide(DMF) solution. The adsorption capacities of BUT-29 toward methylene blue and crystal violet at 298 K can reach 1119 mg/g and 832 mg/g, respectively. Moreover, the adsorbed dyes can be released in the DMF solution of LiNO_3 gradually.展开更多
The process of development and calibration for the first Moon-based ex- treme ultraviolet （EUV） camera to observe Earth＇s plasmasphere is introduced and the design, test and calibration results are presented. The E...The process of development and calibration for the first Moon-based ex- treme ultraviolet （EUV） camera to observe Earth＇s plasmasphere is introduced and the design, test and calibration results are presented. The EUV camera is composed of a multilayer film mirror, a thin film filter, a photon-counting imaging detector, a mech- anism that can adjust the direction in two dimensions, a protective cover, an electronic unit and a thermal control unit. The center wavelength of the EUV camera is 30.2 nm with a bandwidth of 4.6nm. The field of view is 14.7° with an angular resolution of 0.08°, and the sensitivity of the camera is 0.11 count s-1 Rayleigh-1. The geomet- ric calibration, the absolute photometric calibration and the relative photometric cal- ibration are carried out under different temperatures before launch to obtain a matrix that can correct geometric distortion and a matrix for relative photometric correction, which are used for in-orbit correction of the images to ensure their accuracy.展开更多
基金the SINOPEC Project(411058,413025)the National Key R&D Program of China(2017YFB0306800)the National Natural Science Foundation of China(21808244,22278441,and 22478452)for funding this research.
文摘Coordinating the ratio of Bronsted to Lewis acid sites in zeolite catalyst is crucial for the efficient conversion of dihydroxyacetone(DHA)to methyl lactate(ML)in methanol media due to the different acidic requirements of the four fundamental reactions.Herein,we couple Sn-MFI and TS-1 zeolites with different abilities to induce methanol dissociation to rationally regulate the ratio of Bronsted and Lewis acid sites in methanol,thus facilitating the yield of DHA to ML.It is found that framework Sn sites with low dissociation energy(39.2 kJ/mol)induce methanol to release hydrogen protons,creating Bronsted acid sites to enable DHA dehydration to PA.Ti sites in TS-1 zeolite possess high methanol dissociation energy(73.5 kJ/mol),maintaining Lewis acidity in methanol,which provides sufficient active sites for cooperatively intensifying PA addition to HA and subsequent HA isomerization to ML.The synergistic effect of the two zeolites mitigates the side reaction while achieving high DHA conversion,thus steering the reaction toward ML generation.Consequently,ML yield increases by over 25% compared with that of single Sn-MFI zeolite,which offers a promising pathway to promote the synthesis of DHA to ML under mild conditions.
基金supported by the National Natural Science Foundation of China(No.22202152)Tianjin Municipal Science and Technology Bureau(No.24JCQNJC00990)Cangzhou Institute of Tiangong University(No.TGCYY-F-0304).
文摘Oxygen vacancy(Vo)engineering has been recognized as one of the most effective strategies for enhancing the photocatalytic CO_(2) conversion performance of metal oxides,as it can simultaneously facilitate photogenerated charge carrier separation efficiency and provide additional surface reaction sites.However,the wide application of Vo engineering in photocatalysis are limited by its poor stability,owing to the easy recovery of these vacancy defects by atmospheric oxygen.Herein,we develop an indium(In)doping strategy to regulate the coordination environment in CeO_(2) with abundant Vo(CeO_(2-x)),thereby enhance its stability during photocatalytic CO_(2) conversion.Confirmed by positron annihilation lifetime spectroscopy(PALS),In dopants combine with Vo by substituting for part of Ce^(4+),forming In^(3+)-Vo complexes that effectively inhibit the formation of unstable va-cancy clusters.Such In^(3+)-Vo complexes can also reduce the energy required for formation of the CO products.Therefore,the optimized In-doped CeO_(2-x) exhibits excellent photocatalytic CO_(2) conversion performance,with a CO yield of 301.6μmol⋅g^(-1) after 5 h of light irradiation,and maintain high activity after four cycles of experiments.Comprehensive experimental and theoretical studies indicate that the introduction of In doping not only significantly improves the stability of Vo in CeO_(2-x),but also reconstruct the reaction kinetics of the CO_(2) conversion by forming In^(3+)-Vo complexes thus facilitating the overall reaction.
基金financially supported by the National Natural Science Foundation of China(Nos.21804008,52102209)the International Technological Collaboration Project of Shanghai(No.17520710300)+1 种基金Anhui Provincial Natural Science Foundation(No.2108085QE197)Guangdong Basic and Applied Basic Research Foundation(Nos.2022A1515010834,2020A1515110221).
文摘Rechargeable magnesium batteries(RMBs)possess the merits of greater theoretical capacity,cheaper magnesium metal and not easily producing branched crystals,and greater safety.Therefore,the current researches mainly concentrate on the exploration of high-performance RMBs in the initial stage,but still face many gigantic challenges.Herein,petal-shaped nanorods CoS/CuS materials are successfully synthesized as RMBs cathode materials through a two-step metal sulfide template-free solvent-thermal synthesis method,which can effectively improve the reaction kinetics due to the petal-like nano-structure and provide rich electrochemically active sites to decrease the transport barrier of Mg^(2+),thus contributing to the enhancement of the reaction kinetics of magnesium storage in RMBs.The electrochemical performance test illustrates that CoS/CuS composite nanomaterials can considerably improve the charging and discharging specific capacity of the batteries as well as the voltage of the batteries due to the existing synergistic effect between them.The specific capacity of CoS/CuS cathode still can still be maintained as high as 62.8 mAh g^(−1)after 300 cycles at 200 mA g^(−1).And the specific capacity of this electrode material changes from 180.6 mAh g^(−1)to 30 mAh g^(−1)at the current densities from 100 mA g^(−1)to 1000 mA g^(−1),and when the current density is restored to 100 mA g^(−1),the specific capacity gradually recovered to 178.6 mAh g^(−1),which showed better rate performance and ultra-high cycling stability.This work highlights how the introduction of CuS into CoS nanostructures can benefit the reversibility and cyclicity of the magnesium storage reaction and offers an original and practical route for the modification of RMBs electrode materials with good electrochemical properties.
基金supported by research grants from the Guangdong Province Basic and Applied Basic Research Fund Project(2022A1515110447)Open Fund Project of the State Key Laboratory of Applied Microbiology in South China(SKLAM006-2022)+1 种基金74th batch of general funding from the China Postdoctoral Science Foundation(2023M740774)Guangdong Provincial People’s Hospital,Postdoctoral Research Launch Fund(BY012022017)。
文摘Epidemiological studies have indicated that branched-chain amino acids(BCAAs)increased and gut microbiota disordered in type 2 diabetes mellitus(T2DM).This study aimed to investigate the mechanism of Lactiplantibacillus plantarum strain 84-3(Lp84-3)combined with Staphylococcus aureus bacteriophage on ameliorating T2DM.Here we perform a case-control study and identify that Staphylococcus_phage was inversely correlated with fasting blood glucose(FBG).It revealed that Lp84-3 could inhibit the growth of S.aureus,and Lp84-3 contains BCAAs degradation enzymes in its genome.Furthermore,Lp84-3 alone or combined with S.aureus bacteriophage interventions can improve blood glucose,insulin resistance,triglycerides,interleukin-1β,tumor necrosis factor-α(TNF-α),BCAAs,and acetyllactate synthase(ALS)in db/db mice.Lp84-3 and S.aureus bacteriophage decreased S.aureus,Malacoplasma iowae,and Oscillibacter sp.,and increased some beneficial such as L.plantarum and Muribaculaceae bacterium.Transcriptomic analyses revealed that Lp84-3 and S.aureus bacteriophage activated the PI3K/AKT/GLUT4 signaling pathway and upregulated key genes of Il22,Hgf,Col6a1,Gh,Itga10,Fgf23,and Prl involved in glucose metabolism in hypothalamus.Collectively,Lp84-3 and S.aureus bacteriophage alleviate T2DM by modulating gut microbiota and enhancing glucose metabolism in hypothalamus,supporting its potential use as a promising functional compound microecological agent for alleviating T2DM.
基金support provided by the National Natural Science Foundation of China(Grant No.21804008,52102209)the International Technological Collaboration Project of Shanghai(Grant No.17520710300).
文摘The electrochemical performance of all-solid-state lithium batteries(ASSLBs)can be prominently enhanced by minimizing the detrimental degradation of solid electrolytes through their undesirable side reactions with the conductive carbon additives(CCAs)inside the composite cathodes.Herein,the well-defined Mo_(3)Ni_(3)N nanosheets embedded onto the N-doped porous carbons(NPCs)substrate are successfully synthesized(Mo-Ni@NPCs)as CCAs inside LiCoO_(2)for Li_(6)PSC_5)Cl(LPSCl)-based ASSLBs.This nano-composite not only makes it difficult for hydroxide groups(-OH)to survive on the surface but also allows the in situ surface reconstruction to generate the ultra-stable MoS_(2)-Mo_(3)Ni_(3)N heterostructures after the initial cycling stage.These can effectively prevent the occurrence of OH-induced LPSC decomposition reaction from producing harmful insulating sulfates,as well as simultaneously constructing the highly-efficient electrons/ions dual-migration pathways at the cathode interfaces to facilitate the improvement of both electrons and Li+ions conductivities in ASSLBs.With this approach,fine-tuned Mo-Ni@NPCs can deliver extremely outstanding performance,including an ultra-high first discharge-specific capacity of 148.61 mAh g^(-1)(0.1C),a high Coulombic efficiency(94.01%),and a capacity retention rate after 1000 cycles still attain as high as 90.62%.This work provides a brand-new approach of“conversionprotection”strategy to overcome the drawbacks of composite cathodes interfaces instability and further promotes the commercialization of ASSLBs.
文摘This work is devoted to the development of a low cost dimensionally stable anode with high oxygen evolution catalytic activity for practical applications.For this purpose,a Ti/SnO_(x)/MnO_(2) anode was fabricated through an innovative strategy involving Sn electrodeposition,oxidation,and MnO_(2)-layer preparation.The structure of the anode was characterized,and the oxygen evolution performance was evaluated in a H_(2)SO_(4) solution.The results show that compared with the Ti/SnO_(2)/MnO_(2) anode prepared by the conventional brushing-annealing process,the Ti/SnO_(x)/MnO_(2) anode fabricated through the innovative procedure exhibits a lower oxygen evolution potential and a nearly 40%longer accelerated lifespan.The superior oxygen evolution performance of the Ti/SnO_(x)/MnO_(2) anode is attributed to the distinctive SnO_(x) intermediate layer fabricated through Sn electrodeposition followed by oxidation,which indicates the great potential of the anode as a dimensionally stable anode for metal electrowinning and hydrogen production by electrolysis,etc.
基金supported by Chinese Academy of Sciences (CAS)supported by the National Natural Science Foundation of China (Grant Nos. 11427803, U1731241, U1731114 and U1531106)the CAS Strategic Pioneer Program on Space Science (Grant Nos. XDA04076100, XDA15052200, XDA15320103 and XDA15320301)
文摘As one of the three payloads for the Advanced Space-based Solar Observatory(ASO-S)mission,the Lyman-alpha(Lyα)Solar Telescope(LST)is composed of three instruments:a Solar Corona Imager(SCI),a LyαSolar Disk Imager(SDI)and a full-disk White-light Solar Telescope(WST).When working in-orbit,LST will simultaneously perform high-resolution imaging observations of all regions from the solar disk to the inner corona up to 2.5 R⊙(R⊙stands for the mean solar radius)with a spatial resolution of 4.8′′and 1.2′′for coronal and disk observations,respectively,and a temporal resolution of 30–120 s and 1–120 s for coronal and disk observations,respectively.The maximum exposure time can be up to20 s due to precise pointing and image stabilization function.Among the three telescopes of LST,SCI is a dual-waveband coronagraph simultaneously and independently observing the inner corona in the HI Lyα(121.6±10 nm)line and white light(WL)(700±40 nm)wavebands by using a narrowband Lyαbeam splitter and has a field of view(FOV)from 1.1 to 2.5 R⊙.The stray-light suppression level can attain<10^-6 B⊙(B⊙is the mean brightness of the solar disk)at 1.1 R⊙and≤5×10^-8 B⊙at 2.5 R⊙.SDI and WST are solar disk imagers working in the Lyαline and 360.0 nm wavebands,respectively,which adopt an off-axis two-mirror reflective structure with an FOV up to 1.2 R⊙,covering the inner coronal edge area and relating to coronal imaging.We present the up-to-date design for the LST payload.
基金supported by the National Key Research and Development Program of China(2016YFD0102000)“Breeding of Major New Varieties of Main Grain Crops”Program(2020ABA016)from Department of Science and Technology of Hubei Province.
文摘Grain size is one of the most important factors affecting rice grain quality and yield,and attracts great attention from molecular biologists and breeders.In this study,we engineered a CRISPR/Cas9 system targeting the miR396 recognition site of the rice GS2 gene,which encodes growth-regulating factor 4(OsGRF4)and regulates multiple agronomic traits including grain size,grain quality,nitrogen use efficiency,abiotic stress response,and seed shattering.In contrast to most previous genome editing efforts in which indel mutations were chosen to obtain null mutants,a mutant named GS2^(E) carrying an in-frame 6-bp deletion and 1-bp substitution within the miR396-targeted sequence was identified.GS2^(E) plants showed increased expression of GS2 in consistent with impaired repression by miR396.As expected,the gain-of-function GS2^(E) mutant exhibited multiple beneficial traits including increased grain size and yield and bigger grain length/width ratio.Thousand grain weight and grain yield per plant of GS2^(E) plants were increased by 23.5%and 10.4%,respectively.These improved traits were passed to hybrids in a semidominant way,suggesting that the new GS2^(E) allele has great potential in rice improvement.Taken together,we report new GS2 germplasm and describe a novel gene-editing strategy that can be widely employed to improve grain size and yield in rice.This trait-improvement strategy could be applied to other genes containing miRNA target sites,in particular the conserved miR396-GRF/GIF module that governs plant growth,development and environmental response.
基金financially supported by the Innovation Foundation for Doctoral Program of Forestry Engineering of Northeast Forestry University,grant number:LYGC202117the China Scholarship Council(CSC),grant number:202306600046+1 种基金the Research and Development Plan of Applied Technology in Heilongjiang Province of China,grant number:GA19C006Research and Demonstration on Functional Improvement Technology of Forest Ecological Security Barrier in Heilongjiang Province,grant number:GA21C030。
文摘Background:As is widely known,an increasing number of forest areas were managed to preserve and enhance the health of forest ecosystems.However,previous research on forest management has often overlooked the importance of structure-based.Aims:Our objectives were to define the direction of structure-based forest management.Subsequently,we investigated the relationships between forest structure and the regeneration,growth,and mortality of trees under different thinning treatments.Ultimately,the drivers of forest structural change were explored.Methods:On the basis of 92 sites selected from northeastern China,with different recovery time (from 1 to 15years) and different thinning intensities (0–59.9%) since the last thinning.Principal component analysis (PCA)identified relationships among factors determining forest spatial structure.The structural equation model (SEM)was used to analyze the driving factors behind the changes in forest spatial structure after thinning.Results:Light thinning (0–20%trees removed) promoted forest regeneration,and heavy thinning (over 35% of trees removed) facilitated forest growth.However,only moderate thinning (20%–35%trees removed) created a reasonable spatial structure.While dead trees were clustered,and they were hardly affected by thinning intensity.Additionally,thinning intensity,recovery time,and altitude indirectly improve the spatial structure of the forest by influencing diameter at breast height (DBH) and canopy area.Conclusion:Creating larger DBH and canopy area through thinning will promote the formation of complex forest structures,which cultivates healthy and stable forests.
基金supported by Shanghai Xuhui District municipal health commission [grant number XHLHGG201806]Shanghai Shenkang three-year project [grant number SHDC2020CR4017]。
基金financially supported by the National Key R&D Program of China (No. 2018YFB0104400)the National Natural Science Foundation of China (Nos. 52074036, 51725401, and 51874019)Beijing Municipal Science and Technology Commission (No. Z191100002719007)
文摘Pyrolytic graphite (PG) with highly aligned graphene layers,present anisotropic electrical and thermal transport behavior,which is attractive in electronic,electrocatalyst and energy storage.Such pristine PG could meeting the limit of electrical conductivity (~2.5×10^(4) S·cm^(−1)),although efforts have been made for achieving high-purity sp^(2) hybridized carbon.For manipulating the electrical conductivity of PG,a facile and efficient electrochemical strategy is demonstrated to enhance electrical transport ability via reversible intercalation/de-intercalation of AlCl_(4)^(-)into the graphitic interlayers.With the stage evolution at different voltages,variable electrical and thermal transport behaviors could be achieved via controlling AlCl_(4)^(-)concentrations in the PG because of substantial variation in the electronic density of states.Such evolution leads to decoupled electrical and thermal transport (opposite variation trend) in the in-plane and out-of-plane directions,and the in-plane electrical conductivity of the pristine PG (1.25×10^(4) S·cm^(−1)) could be massively promoted to 4.09×10^(4) S·cm(AlCl_(4)^(-)intercalated PG),much better than the pristine bulk graphitic papers used for the electrical transport and electromagnetic shielding.The fundamental mechanism of decoupled transport feature and electrochemical strategy here could be extended into other anisotropic conductive bulks for achieving unusual behaviors.
基金financially supported by the National Natural Science Foundation of China(No.22078077)the National Science Foundation of Guangdong Province(No.2021A1515010078)financial support of Taif University Researchers Supporting Project(No.TURSP-2020/14),Taif University,Taif,Saudi Arabia。
文摘Although many material designs or strategic methods have been proposed for treating oil spills and oily wastewater,the complex oily state,dealing with the harsh operating conditions of oil–water separation(such as the recovery of viscous spilled crude oil,bacteria-containing oily wastewater,and removal of spilled oil under fire),and the autorecycling of oil and absorption materials remain a great challenge.This work proposed an ingenious design strategy of“several birds with one stone”to prepare p H/thermoresponsive flame-retardant/photothermal bactericidal P-Fe_(3)O_(4)-polydopamine(PDA)@melamine–formaldehyde(MF)foams.This design makes the foams remarkably effective in the recovery of spilled viscous crude oil as well as in the separation of bacteria-containing oily emulsions,particularly for instant fire extinguishing by magnetically controlled oil absorption as well as for fire alarms.The photothermal effect and p H response induce a change in the surface wettability of the foams,facilitating excellent autoadsorption/desorption of the spilled oil.The photothermal bactericidal activity and fouling resistance of the foam are beneficial to the separation of bacteria-containing oily wastewater.Outstanding flame-retardant properties and maneuverable magnetic control enable the foam to rapidly recover the spilled oil in a large range of fires,extinguish fires instantly,and facilitate early fire warning.The proposed strategy is expected to inspire further research on treating oil spills under complex conditions.
基金the Startup Research Fund of Dongguan University of Technology(KCYKYQD2017015)Leading Talents of Innovation and Entrepreneurship of the Dongguan City D2017(16)the Australian Research Council(ARC)through the ARC Discovery project(DP160104340)。
文摘Binders are of vital importance in stabilizing the cathodes to enhance the cycling stability of lithiumsulfur(Li-S) batteries. However, conventional binders are typically confronted with the drawback of inability for adsorbing lithium polysulfide(Li PS), thus resulting in severe active material losing and rapid capacity fading. Herein, a novel water-soluble hyperbranched poly(amidoamine)(HPAA) binder with controllable hyperbranched molecular structure and abundant amino end groups for Li-S battery is designed and fabricated, which can improve efficient adsorption for Li PS and stability of the sulfur cathodes. Besides, the strong intermolecular hydrogen bonds in HPAA binder can contribute to the structural stability of S cathode and integration of the conductive paths. Therefore, the Li-S battery with this functional binder exhibits excellent cycle performance with a capacity retention of 91% after 200 cycles at 0.1 C.Even at a high sulfur loading of 5.3 mg cm-2, a specific capacity of 601 mA h g-1 can also be achieved.Density functional theory(DFT) calculation further demonstrates that the enhanced electrochemical stability derives from the high binding energy between amino groups and LiP S and the wide electrochemical window(6.87 e V) of HPAA molecule. Based on the above all, this functional polymer will lighten a new species of binders for eco-friendly sulfur cathodes and significantly promote the practical applications of high-performance Li-S batteries.
基金jointly supported by the National Natural Science Foundation of China(Grant No.51802252)Natural Science Foundation of Shaanxi Province(Nos.2020JM-032,2019TD-020)+3 种基金111 project 2.0(BP0618008)the fund of the State Key Laboratory of Solidification Processing in NPU(Grant No.SKLSP202116)supported by Yunnan Provincial Key Laboratory of Energy Saving in Phosphorus Chemical Engineering and New Phosphorus Materials(LHG-2020-0003)China Postdoctoral Science Foundation(2019M663698)。
文摘The catalyst innovation that aims at noble-metal-free substitutes is one key aspect for future sustainable hydrogen energy deployment.In this paper,a nickel cobalt sulfoselenide/black phosphorus heterostructure(NiCoSe|S/BP)was fabricated to realize the highly active and durable water electrolysis through interface and valence dual-engineering.The NiCoSe|S/BP nanostructure was constructed by in-situ growing NiCo hydroxide nanosheet arrays on few-layer BP and subsequently one-step sulfoselenization by SeS2.Besides the conductive merit of BP substrate,holes in p-type BP are capable of oxidizing the Co^(2+)to high-valence and electron-accepting Co^(3+),benefiting the oxygen evolution reaction(OER).Meanwhile,Ni^(3+)/Ni^(2+)ratio in the heterostructure is reduced to maintain the electrical neutrality,which corresponds to the increased electron-donating character for boosting hydrogen evolution reaction(HER).As for HER and OER,the heterostructured NiCoSe|S/BP electrocatalyst exhibits small overpotentials of 172 and 285 mV at 10 mA cm^(-2)(η_(10))in alkaline media,respectively.And overall water splitting has been achieved at a low cell potential of 1.67 V at η_(10) with high stability.Molecular sensing and density functional theory(DFT)calculations are further proposed for understanding the rate-determine steps and enhanced catalytic mechanism.The investigation presents a deep-seated perception for the electrocatalytic performance enhancement of BP-based heterostructure.
基金Supported by The Science and Technology Research Foundation of Guizhou Province,and Zunyi City,No.QKHJC-ZK(2022)YB642,No.ZSKH·HZ(2022)344,and No.gzwjkj2021-071The WBE Liver Fibrosis Foundation,No.CFHPC2025028The Beijing Gandan Phase Mutual Public Welfare Fund for Artificial Liver Project,No.iGandanF-1082024-Rgg018.
文摘IgG4-related sclerosing cholangitis(IgG4-SC)is an inflammatory disease that leads to bile duct stricture,characterized by the infiltration of IgG4-positive plasma cells into the bile duct wall,thickening of the bile duct wall,and narrowing of the lumen.The differential diagnosis of IgG4-SC mainly includes primary sclerosing cholangitis,cholangiocarcinoma,and pancreatic cancer.IgG4-SC is often associated with autoimmune pancreatitis and can be accurately diagnosed based on clinical diagnostic criteria.However,isolated IgG4-SC is difficult to distinguish from biliary tumors.Given the significant differences in biological behavior,treatment,and prognosis between these diseases,accurately identifying isolated IgG4-SC has very important clinical significance.
基金financially supported by the National Natural Science Foundation of China (NSFC, No. U1407119)
文摘In this paper, a new anionic metal-organic framework, [In(PBPTTBA)][(CH_3)_2 NH_2](BUT-29) has been synthesized through the reaction of tetratopic acid ligand with double Lewis pyridine sites, 4,4',4'',4'''-(4,4'-(1,4-phenylene)bis(pyridine-6,4,2-triyl)) tetrabenzoic acid(H_4 PBPTTBA) and In(NO_3)_2·5H_2O and fully characterized by single-crystal X-ray diffraction(SXRD), powder X-ray diffraction(PXRD),thermogravimetric analysis(TGA), infrared spectroscopy(IR), and elemental analysis(EA). BUT-29 can be used as an efficient adsorbent for the selective removal of organic cationic dyes in N,N0-dimethylformamide(DMF) solution. The adsorption capacities of BUT-29 toward methylene blue and crystal violet at 298 K can reach 1119 mg/g and 832 mg/g, respectively. Moreover, the adsorbed dyes can be released in the DMF solution of LiNO_3 gradually.
文摘The process of development and calibration for the first Moon-based ex- treme ultraviolet （EUV） camera to observe Earth＇s plasmasphere is introduced and the design, test and calibration results are presented. The EUV camera is composed of a multilayer film mirror, a thin film filter, a photon-counting imaging detector, a mech- anism that can adjust the direction in two dimensions, a protective cover, an electronic unit and a thermal control unit. The center wavelength of the EUV camera is 30.2 nm with a bandwidth of 4.6nm. The field of view is 14.7° with an angular resolution of 0.08°, and the sensitivity of the camera is 0.11 count s-1 Rayleigh-1. The geomet- ric calibration, the absolute photometric calibration and the relative photometric cal- ibration are carried out under different temperatures before launch to obtain a matrix that can correct geometric distortion and a matrix for relative photometric correction, which are used for in-orbit correction of the images to ensure their accuracy.
