Plasmonic nonmetal semiconductors with localized surface plasmon resonance(LSPR)effects possess extended light-response ranges and can act as highly efficient H2 generation photocatalysts.Herein,an LSPR-enhanced 0D/2D...Plasmonic nonmetal semiconductors with localized surface plasmon resonance(LSPR)effects possess extended light-response ranges and can act as highly efficient H2 generation photocatalysts.Herein,an LSPR-enhanced 0D/2D CdS/MoO3‒x heterojunction has been synthesized by the growth of 0D CdS nanoparticles on 2D plasmonic MoO3‒x elliptical nanosheets via a simple coprecipitation method.Taking advantage of the LSPR effect of the MoO3‒x elliptical nanosheets,the light absorption of the CdS/MoO3‒x heterojunction was extended from 600 nm to the near-infrared region(1400 nm).Furthermore,the introduction of 2D plasmonic MoO3‒x elliptical nanosheets not only provided a platform for the growth of CdS nanoparticles,but also contributed to the construction of an LSPR-enhanced S-scheme structure due to the interface between the MoO3‒x and CdS,accelerating the separation of light-induced electrons and holes.Therefore,the CdS/MoO3‒x heterojunction exhibited higher photocatalytic H2 generation activity than pristine CdS under visible light irradiation,including under 420,450,550,and 650 nm monochromic light,as well as improved photo-corrosion performance.展开更多
Extended light absorption and dynamic charge separation are vital factors that determine the effectivenessof photocatalysts.In this study,a nonmetallic plasmonic S‐scheme photocatalyst was fabricatedby loading 1D pla...Extended light absorption and dynamic charge separation are vital factors that determine the effectivenessof photocatalysts.In this study,a nonmetallic plasmonic S‐scheme photocatalyst was fabricatedby loading 1D plasmonic W_(18)O_(49)nanowires onto 2D g‐C_(3)N_(4)nanosheets.W_(18)O_(49)nanowiresplay the dual role of a light absorption antenna—that extends light adsorption—and a hot electrondonor—that assists the water reduction reaction in a wider light spectrum range.Moreover,S‐scheme charge transfer resulting from the matching bandgaps of W_(18)O_(49)and g‐C_(3)N_(4)can lead tostrong redox capability and high migration speed of the photoinduced charges.Consequently,in thisstudy,W_(18)O_(49)/g‐C_(3)N_(4)hybrids exhibited higher photocatalytic H2 generation than that of pristineg‐C_(3)N_(4)under light irradiation of 420–550 nm.Furthermore,the H2 production rate of thebest‐performing W_(18)O_(49)/g‐C_(3)N_(4)hybrid was 41.5μmol·g^(−1)·h^(−1)upon exposure to monochromaticlight at 550 nm,whereas pure g‐C_(3)N_(4)showed negligible activity.This study promotes novel andenvironmentally friendly hot‐electron‐assisted S‐scheme photocatalysts for the broad‐spectrumutilization of solar light.展开更多
Durable and inexpensive graphitic carbon nitride(g-C_(3)N_(4))demonstrates great potential for achieving efficient photocatalytic hydrogen evolution reduction(HER).To further improve its activity,g-C_(3)N_(4)was subje...Durable and inexpensive graphitic carbon nitride(g-C_(3)N_(4))demonstrates great potential for achieving efficient photocatalytic hydrogen evolution reduction(HER).To further improve its activity,g-C_(3)N_(4)was subjected to atomic-level structural engineering by doping with transition metals(M=Fe,Co,or Ni),which simultaneously induced the formation of metal-N active sites in the g-C_(3)N_(4)framework and modulated the bandgap of g-C_(3)N_(4).Experiments and density functional theory calculations further verified that the as-formed metal-N bonds in M-doped g-C_(3)N_(4)acted as an"electron transfer bridge",where the migration of photo-generated electrons along the bridge enhanced the efficiency of separation of the photogenerated charges,and the optimized bandgap of g-C_(3)N_(4)afforded stronger reduction ability and wider light absorption.As a result,doping with either Fe,Co,or Ni had a positive effect on the HER activity,where Co-doped g-C_(3)N_(4)exhibited the highest performance.The findings illustrate that this atomic-level structural engineering could efficiently improve the HER activity and inspire the design of powerful photocatalysts.展开更多
Recently,the theoretically predicted lanthanum superhydride,LaH 10±δ,with a clathrate-like structure was successfully synthesized and found to exhibit a record high superconducting transition temperature T c≈25...Recently,the theoretically predicted lanthanum superhydride,LaH 10±δ,with a clathrate-like structure was successfully synthesized and found to exhibit a record high superconducting transition temperature T c≈250 K at∼170 GPa,opening a new route for room-temperature superconductivity.However,since in situ experiments at megabar pressures are very challenging,few groups have reported the∼250 K superconducting transition in LaH 10±δ.Here,we establish a simpler sample-loading procedure that allows a relatively large sample size for synthesis and a standard four-probe configuration for resistance measurements.Following this procedure,we successfully synthesized LaH 10±δwith dimensions up to 10×20μm^2 by laser heating a thin La flake and ammonia borane at∼1700 K in a symmetric diamond anvil cell under the pressure of 165 GPa.The superconducting transition at T c≈250 K was confirmed through resistance measurements under various magnetic fields.Our method will facilitate explorations of near-room-temperature superconductors among metal superhydrides.展开更多
Pigment intensity and patterns are important factors that determine the nutritional and market values of tomato fruits.The acropetal manner of light-dependent anthocyanin accumulation with the highest levels at the st...Pigment intensity and patterns are important factors that determine the nutritional and market values of tomato fruits.The acropetal manner of light-dependent anthocyanin accumulation with the highest levels at the stem end of the fruit makes Pro35S:BrTT8 tomato plants an ideal system for investigating the effects of light intensity on anthocyanin biosynthesis.Extensive transcript analyses indicate that anthocyanin pigmentation in Pro35S:BrTT8 plants under high light might be coordinately regulated by the exogenous protein BrTT8 and endogenous proteins SlAN2 and SlMYBL2.Furthermore,yeast two-hybrid assays showed that BrTT8 could interact efficiently with SlAN2,SlMYBL2,and SlAN11.Moreover,the physical interaction between BrTT8 and SlAN2 was validated by FRET.Simultaneous overexpression of SlAN2 and BrTT8 activated significant anthocyanin biosynthesis in infiltrated tobacco leaves.In addition,the ability of SlMYBL2 to suppress anthocyanin accumulation was also demonstrated in infiltrated tobacco leaves.Altogether,these results prove that tissue-specific assemblage of the heterogeneous MYB-bHLH-WD40 complex consisting of SlAN2,BrTT8 and SlAN11 triggers nonuniform anthocyanin accumulation in tomato fruit under high light.Additionally,it is proposed that a negative-feedback loop fulfilled by SlMYBL2 also participates in the regulation of anthocyanin production.展开更多
Cassava,Manihot esculenta Crantz (Me),is a major dietary source of calories for over 700 million people in tropical regions.The production of cassava is constantly threatened by cassava bacterial blight (CBB),caused b...Cassava,Manihot esculenta Crantz (Me),is a major dietary source of calories for over 700 million people in tropical regions.The production of cassava is constantly threatened by cassava bacterial blight (CBB),caused by Xanthomonas axonopodis pv.manihotis (Xam).The gene resources for CBB-resistant breeding of cassava are limited.In model plant species,ethylene response factors play important roles in response to pathogen infection.In this study,cassava ethylene response factors (MeERFs) were identified and characterized as the first step in studying their potential for CBB-resistant breeding of cassava.In the cassava genome 155 MeERFs were identified,of which 23 were induced by Xam infection.The promoter regions of204 genes harbored GCC-box that had the potential to interact with MeERFs.Using 37 transcriptomes derived from Xam infection treatment,four gene co-expression modules for the MeERFs and GCC-box containing genes were constructed.Six MeERFs were associated with two GCC-box containing genes:transcription initiation factor TFIIE subunit beta (MeTFIIE),and histone-lysine N-methyltransferase ASHR1 (MeASHR1).Dual-luciferase reporter assays showed that MeERF10 and MeERF58 positively regulated Me TFIIE;MeERF137 negatively regulated Me TFIIE;MeERF10 and MeERF137 positively regulated Me ASHR1;and MeERF35 negatively regulated Me ASHR1.The four MeERFs may mediate pathogen response by regulating the expression of the two GCC-box containing genes.展开更多
δ-(Al,Fe)OOH is considered to be one of the most important hydrous phases on Earth,remaining stable under the extreme conditions throughout the mantle.The behavior ofδ-(Al,Fe)OOH at high pressure is essential to und...δ-(Al,Fe)OOH is considered to be one of the most important hydrous phases on Earth,remaining stable under the extreme conditions throughout the mantle.The behavior ofδ-(Al,Fe)OOH at high pressure is essential to understanding the deep water cycle.δ-(Al_(0.956)Fe_(0.044))OOH crystals synthesized at 21 GPa and 1473 K were investigated by high-pressure Brillouin light scattering spectroscopy and synchrotron X-ray diffraction up to 135.4 GPa in diamond anvil cells.The incorporation of 5 mol%FeOOH increases the unit-cell volume ofδ-AlOOH by~1%and decreases the shear-wave velocity(VS)by~5%at 20–135 GPa.In particular,the compressional(V_(P))and shear(VS)wave velocities ofδ-(Al_(0.956)Fe_(0.044))OOH are 7%–16%and 10%–24%greater than all the major minerals in the mantle transition zone including wadsleyite,ringwoodite,and majorite.The distinctly high sound velocities ofδ-(Al_(0.956)Fe_(0.044))OOH at 20–25 GPa may contribute to the seismic anomalies observed at~560–680 km depths in the cold and stagnant slab beneath Izu-Bonin and/or Korea.Furthermore,the VS ofδ-(Al_(0.956)Fe_(0.044))OOH is about 10%and 4%–12%lower than iron-bearing bridgmanite Mg_(0.96)Fe_(0.05)Si_(0.99O3)and ferropericlase(Mg_(0.92)Fe_(0.08))O,respectively,under the lowermost mantle conditions,which might partially contribute to the large low-shear-velocity provinces and ultralow velocity zones at the bottom of the lower mantle.展开更多
In the 18^(th)century,British gardens began to transform from a classical to a natural landscape style.During this period,they were influenced by the economy,local nature,as well as foreign cultures.The 18^(th)century...In the 18^(th)century,British gardens began to transform from a classical to a natural landscape style.During this period,they were influenced by the economy,local nature,as well as foreign cultures.The 18^(th)century was the golden period of cultural exchange between China and the West which gave Britain the opportunity to absorb the cultures of Chinese classical gardens.British gardeners had used various elements of Chinese classical gardens as their point of reference which promoted the development of British natural landscape gardens.展开更多
BACKGROUND: Lead can cause structural changes in the hippocampus, followed by damage to learning and memory functions, but its specific mechanisms are not yet clear. OBJECTIVE: To observe long-term toxicity of high-...BACKGROUND: Lead can cause structural changes in the hippocampus, followed by damage to learning and memory functions, but its specific mechanisms are not yet clear. OBJECTIVE: To observe long-term toxicity of high-dose lead in drinking water on hippocampal tissue in rats, and analyze the potential association of oxidative damage, cell apoptosis, and pathology. DESIGN, TIME AND SETTING: A randomized, controlled animal experiment was performed at the Center for Medical Experiment, Lanzhou General Hospital of Lanzhou Military Area Command of Chinese PLA from May 2007 to October 2008. MATERIALS; Rabbit anti Bcl-2, Bax, and inducible nitric oxide synthase (iNOS) polyclonal antibodies were purchased from Santa Cruz Biotechnology, USA. An streptavidin-peroxidase immunohistochemistry kit and concentrated DAB kit were purchased from Beijing Zhongshan Biotechnology Company Limited, China. Crystal violet was purchased from Sigma, USA. METHODS: A total of 72 Wistar rats, aged 3 months, were randomly divided into control, low-, middle-, and high-dose lead groups, with 18 rats per group. Animal models were established through free drinking water contaminated by Pb2+ for 1, 3, and 6 months, respectively. MAIN OUTCOME MEASURES: The general toxicity of lead was dynamically observed; the levels of Pb2+ in the blood and brain tissue homogenete were detected using atomic absorption method; pathological changes were observed using hematoxylin-eosin staining and tigroid body staining; the protein expression levels of Bcl-2, Bax, and iNOS were dynamically observed using streptavidin-peroxidase immunohistochemistry of the hippocampus. RESULTS: Lead exposure reduced autonomic activities, produced a slumped appearance, slow responses, and lusterless fur, especially in the high-dose group. The amount of ingestion and hydroposia showed a decreasing trend, especially in middle- and high-dose groups. Lead levels in whole blood and brain homogenate were higher than controls (P 〈 0.01). Lead caused degeneration of hippocampal neurons and pyknosis, with fewer tigroid bodies, especially in high-dose lead group. Bcl-2 expression decreased with increasing lead dose (P 〈 0.01), whereas lead dose-dependently increased Bax levels (P 〈 0.01) and iNOS levels (P 〈 0.05). CONCLUSION: High levels of Pb^2+ may disrupt hippocampal structure by passing through the blood brain barrier. Oxidative damage and apoptosis may be a toxicity mechanism of Pb^2+ on the hippocampus.展开更多
It has been recognized that a small amount of propane mixed with methane can change greatly in not only the thermodynamics but also the structural properties of gas hydrate.However,its mechanism is still not well unde...It has been recognized that a small amount of propane mixed with methane can change greatly in not only the thermodynamics but also the structural properties of gas hydrate.However,its mechanism is still not well understood yet.In this research,structure-Ⅱ(sⅡ)hydrate is synthesized using a methanepropane gas mixture with an initial mole ratio of 99:1,and it is found that large(5~(12)6~4)cages are cooccupied by multiple gases based on the rigid structure analysis of neutron diffraction data.The first principles calculation and molecular dynamics simulation are conducted to uncover the molecular mechanism for sⅡmethane-propane hydrate formation,revealing that the presence of propane inhibits the formation of structure-Ⅰ(sⅠ)hydrate but promotes sⅡhydrate formation.The results help to understand the accumulation mechanism of natural gas hydrate and benefit to optimize the condition for gas storage and transportation in hydrate form.展开更多
Chilling-induced accumulation of reactive oxygen species(ROS) is harmful to plants,which usually produce anthocyanins to scavenge ROS as protection from chilling stress.As a tropical crop,cassava is hypersensitive to ...Chilling-induced accumulation of reactive oxygen species(ROS) is harmful to plants,which usually produce anthocyanins to scavenge ROS as protection from chilling stress.As a tropical crop,cassava is hypersensitive to chilling,but the biochemical basis of this hypersensitivity remains unclear.We previously generated Me MYB2-RNAi transgenic cassava with increased chilling tolerance.Here we report that Me MYB2-RNAi transgenic cassava accumulated less ROS but more cyanidin-3-O-glucoside than the wild type under early chilling stress.Under this stress,the anthocyanin biosynthesis pathway was more active in Me MYB2-RNAi lines than in the wild type,and several genes involved in the pathway,including Me TT8,were up-regulated by Me MYB2-RNAi in the transgenic cassava.Me MYB2 bound to the Me TT8 promoter and blocked its expression under both normal and chilling conditions,thereby inhibiting anthocyanin accumulation.Me TT8 was shown to bind to the promoter of Dihydroflavonol 4-reductase(Me DFR-2)and increased Me DFR-2 expression.Me MYB2 appears to act as an inhibitor of chilling-induced anthocyanin accumulation during the rapid response of cassava to chilling stress.展开更多
In recent years,transition metal borides(TMBs)have attracted much attention because they are considered as potential superhard materials and have more abundant crystal structures compared with traditional superhard ma...In recent years,transition metal borides(TMBs)have attracted much attention because they are considered as potential superhard materials and have more abundant crystal structures compared with traditional superhard materials.So far,however,no superhard materials have been found in TMBs.A large number of structures and potential new properties in TMBs are induced by the various hybridization ways of boron atoms and the high valence electrons of transition metals,which provide many possibilities for its application.And most TMBs have layered structures,which make TMBs have the potential to be a two-dimensional(2D)material.The 2D materials have novel properties,but the research on 2D TMBs is still nearly blank.In this paper,the research progress of TMBs is summarized involving structure,mechanical properties,and multifunctional properties.The strong covalent bonds of boron atoms in TMBs can form one-dimensional,twodimensional,and three-dimensional substructures,and the multiple electron transfer between transition metal and boron leads to a variety of chemical bonds in TMBs,which are the keys to obtain high hardness and multifunctional properties of TMBs.Further research on the multifunctional properties of TMBs,such as superconductors,catalysts,and high hardness ferromagnetic materials,is of great significance to the discovery of new multifunctional hard materials.展开更多
In the High-Pressure Synergetic Measurements Station (HP-SymS) of the Synergic Extreme Condition User Facility (SECUF), we will develop ultrahigh-pressure devices based on diamond-anvil cell (DAC) techniques, wi...In the High-Pressure Synergetic Measurements Station (HP-SymS) of the Synergic Extreme Condition User Facility (SECUF), we will develop ultrahigh-pressure devices based on diamond-anvil cell (DAC) techniques, with a target pressure up to 300 GPa. With the use of cryostat and magnet, we will reach 300 GPa4.2 K-9 T and conduct simultaneous measurements of the electrical-transport property and Raman/Brillouin spectrascopy. With resistance heating and laser heating, we will reach temperatures of at least 1000 and 3000 K, respectively, coupled with Raman/Brillouin spectroscopy measurements. Some designs of supporting devices, such as a femtosecond laser gasket-drilling device, electrode-deposition device, and the gas-loading device, are also introduced in this article. Finally, we conclude by providing some perspectives on the applications of the DAC in related research fields.展开更多
Developing efficient adsorbents for radon(Rn)capture from the ambient environment is of paramount importance for public health.However,it poses a great challenge due to the chemical inertness and extremely low molar c...Developing efficient adsorbents for radon(Rn)capture from the ambient environment is of paramount importance for public health.However,it poses a great challenge due to the chemical inertness and extremely low molar concentration of Rn in air.Herein,we report a zeolite imidazolate frameworkderived metallic carbon adsorbent(Zn@NPC)with record high Rn removal performance under ambient conditions.Upon one-step pyrolysis,the prepared Zn@NPC possesses pores with a preference for Rn and atomically dispersed Zn sites,achieving a high Rn removal efficiency that doubles in adsorption coefficient(9.47 L·g^(−1))and triples in adsorption kinetic coefficient(20.25 mL·g^(−1)·min^(−1))over the benchmark Rn adsorbent coconut activated charcoal.Density functional theory calculations elucidate the important role of the metal polarization effect,which cooperates with the pore size confinement effect to boost the overall Rn adsorption performance.This work launches a promising alternative for practical Rn capture.展开更多
The PdPtVO_(x)/CeO_(2)-ZrO_(2)(PdPtVO_(x)/CZO)catalysts were obtained by using different approaches,and their physical and chemical properties were determined by various techniques.Catalytic activities of these materi...The PdPtVO_(x)/CeO_(2)-ZrO_(2)(PdPtVO_(x)/CZO)catalysts were obtained by using different approaches,and their physical and chemical properties were determined by various techniques.Catalytic activities of these materials in the presence of H_(2)O or SO_(2)were evaluated for the oxidation of ethylbenzene(EB).The PdPtVO_(x)/CZO sample exhibited high catalytic activity,good hydrothermal stability,and reversible sulfur dioxide-poisoning performance,over which the specific reaction rate at 160℃,turnover frequency at 160℃(TOF_(Pd or Pt)),and apparent activation energy were 72.6 mmol/(g_(Pt)·sec)or 124.2 mmol/(g_(Pd)·sec),14.2 sec^(-1)(TOF_(Pt))or 13.1 sec^(-1)(TOF_(Pd)),and 58 k J/mol,respectively.The large EB adsorption capacity,good reducibility,and strong acidity contributed to the good catalytic performance of PdPtVO_(x)/CZO.Catalytic activity of PdPtVO_(x)/CZO decreased when 50 ppm SO_(2)or(1.0 vol.%H_(2)O+50 ppm SO_(2))was added to the feedstock,but was gradually restored to its initial level after the SO_(2)was cut off.The good reversible sulfur dioxide-resistant performance of PdPtVO_(x)/CZO was associated with the facts:(i)the introduction of SO_(2)leads to an increase in surface acidity;(ii)V can adsorb and activate SO_(2),thus accelerating formation of the SO_(x)^(2-)(x=3 or 4)species at the V and CZO sites,weakening the adsorption of sulfur species at the PdPt active sites,and hence protecting the PdPt active sites to be not poisoned by SO_(2).EB oxidation over PdPtVO_(x)/CZO might take place via the route of EB→styrene→phenyl methyl ketone→benzaldehyde→benzoic acid→maleic anhydride→CO_(2)and H_(2)O.展开更多
对电极(counter electrode,CE)作为染料敏化太阳能电池(dye-sensitized solar cell,DSSC)的重要组成部分之一,其作用是收集外电路电子和催化还原电解质.硫化镍具有低成本和优异的电催化活性等优点,是Pt的理想替代材料.本文制备的NiS电...对电极(counter electrode,CE)作为染料敏化太阳能电池(dye-sensitized solar cell,DSSC)的重要组成部分之一,其作用是收集外电路电子和催化还原电解质.硫化镍具有低成本和优异的电催化活性等优点,是Pt的理想替代材料.本文制备的NiS电极的透光率可以达到80%以上(600 nm处),从正面(光阳极)照射时,制备的DSSC器件光电转化效率达到7.54%,与Pt对电极的(7.48%)相当.从反面(对电极)照射时,光电转化效率达到3.96%,远高于Pt对电极(0.58%).在硫化镍电极中掺入石墨烯,可以进一步提升DSSC器件的光电转化效率,正面照射达到7.84%,反面照射达到4.59%,是正面照射效率的58.5%.电化学阻抗、循环伏安测试表明NiS对电极具有很小的串联电阻和高的电催化活性,这是其性能优于Pt的主要原因;而高的反面照射光电转化效率主要得益于NiS电极的高透光率.本文提供了一种简单、快捷、低成本的方法来制备透明、高效硫化镍对电极.展开更多
文摘Plasmonic nonmetal semiconductors with localized surface plasmon resonance(LSPR)effects possess extended light-response ranges and can act as highly efficient H2 generation photocatalysts.Herein,an LSPR-enhanced 0D/2D CdS/MoO3‒x heterojunction has been synthesized by the growth of 0D CdS nanoparticles on 2D plasmonic MoO3‒x elliptical nanosheets via a simple coprecipitation method.Taking advantage of the LSPR effect of the MoO3‒x elliptical nanosheets,the light absorption of the CdS/MoO3‒x heterojunction was extended from 600 nm to the near-infrared region(1400 nm).Furthermore,the introduction of 2D plasmonic MoO3‒x elliptical nanosheets not only provided a platform for the growth of CdS nanoparticles,but also contributed to the construction of an LSPR-enhanced S-scheme structure due to the interface between the MoO3‒x and CdS,accelerating the separation of light-induced electrons and holes.Therefore,the CdS/MoO3‒x heterojunction exhibited higher photocatalytic H2 generation activity than pristine CdS under visible light irradiation,including under 420,450,550,and 650 nm monochromic light,as well as improved photo-corrosion performance.
文摘Extended light absorption and dynamic charge separation are vital factors that determine the effectivenessof photocatalysts.In this study,a nonmetallic plasmonic S‐scheme photocatalyst was fabricatedby loading 1D plasmonic W_(18)O_(49)nanowires onto 2D g‐C_(3)N_(4)nanosheets.W_(18)O_(49)nanowiresplay the dual role of a light absorption antenna—that extends light adsorption—and a hot electrondonor—that assists the water reduction reaction in a wider light spectrum range.Moreover,S‐scheme charge transfer resulting from the matching bandgaps of W_(18)O_(49)and g‐C_(3)N_(4)can lead tostrong redox capability and high migration speed of the photoinduced charges.Consequently,in thisstudy,W_(18)O_(49)/g‐C_(3)N_(4)hybrids exhibited higher photocatalytic H2 generation than that of pristineg‐C_(3)N_(4)under light irradiation of 420–550 nm.Furthermore,the H2 production rate of thebest‐performing W_(18)O_(49)/g‐C_(3)N_(4)hybrid was 41.5μmol·g^(−1)·h^(−1)upon exposure to monochromaticlight at 550 nm,whereas pure g‐C_(3)N_(4)showed negligible activity.This study promotes novel andenvironmentally friendly hot‐electron‐assisted S‐scheme photocatalysts for the broad‐spectrumutilization of solar light.
文摘Durable and inexpensive graphitic carbon nitride(g-C_(3)N_(4))demonstrates great potential for achieving efficient photocatalytic hydrogen evolution reduction(HER).To further improve its activity,g-C_(3)N_(4)was subjected to atomic-level structural engineering by doping with transition metals(M=Fe,Co,or Ni),which simultaneously induced the formation of metal-N active sites in the g-C_(3)N_(4)framework and modulated the bandgap of g-C_(3)N_(4).Experiments and density functional theory calculations further verified that the as-formed metal-N bonds in M-doped g-C_(3)N_(4)acted as an"electron transfer bridge",where the migration of photo-generated electrons along the bridge enhanced the efficiency of separation of the photogenerated charges,and the optimized bandgap of g-C_(3)N_(4)afforded stronger reduction ability and wider light absorption.As a result,doping with either Fe,Co,or Ni had a positive effect on the HER activity,where Co-doped g-C_(3)N_(4)exhibited the highest performance.The findings illustrate that this atomic-level structural engineering could efficiently improve the HER activity and inspire the design of powerful photocatalysts.
基金Supported by the Strategic Priority Research Program of the Chinese Academy of Sciences(Grant Nos.XDB33000000 and XDB25000000)the Beijing Natural Science Foundation(Grant No.Z190008)+2 种基金the National Natural Science Foundation of China(Grant Nos.11575288, 11921004, 11888101, 11904391, 11834016 and 11874400)the National Key R&D Program of China(Grant Nos.2016YFA0401503 and 2018YFA0305700)the Youth Innovation Promotion Association,the Key Research Program of Frontier Sciences and the Interdisciplinary Innovation Team of Chinese Academy of Sciences(Grant Nos.2016006, JCTD-2019-01,and QYZDBSSW-SLH013)
文摘Recently,the theoretically predicted lanthanum superhydride,LaH 10±δ,with a clathrate-like structure was successfully synthesized and found to exhibit a record high superconducting transition temperature T c≈250 K at∼170 GPa,opening a new route for room-temperature superconductivity.However,since in situ experiments at megabar pressures are very challenging,few groups have reported the∼250 K superconducting transition in LaH 10±δ.Here,we establish a simpler sample-loading procedure that allows a relatively large sample size for synthesis and a standard four-probe configuration for resistance measurements.Following this procedure,we successfully synthesized LaH 10±δwith dimensions up to 10×20μm^2 by laser heating a thin La flake and ammonia borane at∼1700 K in a symmetric diamond anvil cell under the pressure of 165 GPa.The superconducting transition at T c≈250 K was confirmed through resistance measurements under various magnetic fields.Our method will facilitate explorations of near-room-temperature superconductors among metal superhydrides.
基金supported by the National Natural Science Foundation of China(nos.31601760,31301778)the Industry−University−Research Collaboration Grants of Henan Province(172107000020).
文摘Pigment intensity and patterns are important factors that determine the nutritional and market values of tomato fruits.The acropetal manner of light-dependent anthocyanin accumulation with the highest levels at the stem end of the fruit makes Pro35S:BrTT8 tomato plants an ideal system for investigating the effects of light intensity on anthocyanin biosynthesis.Extensive transcript analyses indicate that anthocyanin pigmentation in Pro35S:BrTT8 plants under high light might be coordinately regulated by the exogenous protein BrTT8 and endogenous proteins SlAN2 and SlMYBL2.Furthermore,yeast two-hybrid assays showed that BrTT8 could interact efficiently with SlAN2,SlMYBL2,and SlAN11.Moreover,the physical interaction between BrTT8 and SlAN2 was validated by FRET.Simultaneous overexpression of SlAN2 and BrTT8 activated significant anthocyanin biosynthesis in infiltrated tobacco leaves.In addition,the ability of SlMYBL2 to suppress anthocyanin accumulation was also demonstrated in infiltrated tobacco leaves.Altogether,these results prove that tissue-specific assemblage of the heterogeneous MYB-bHLH-WD40 complex consisting of SlAN2,BrTT8 and SlAN11 triggers nonuniform anthocyanin accumulation in tomato fruit under high light.Additionally,it is proposed that a negative-feedback loop fulfilled by SlMYBL2 also participates in the regulation of anthocyanin production.
基金supported by the Natural Science Foundation of Hainan Province (2018CXTD330 and 318QN204)Key R&D Program of Hainan Province (ZDYF2019063)+1 种基金China Agriculture Research System (CARS11-hncyh)the National Natural Science Foundation of China (31560497)。
文摘Cassava,Manihot esculenta Crantz (Me),is a major dietary source of calories for over 700 million people in tropical regions.The production of cassava is constantly threatened by cassava bacterial blight (CBB),caused by Xanthomonas axonopodis pv.manihotis (Xam).The gene resources for CBB-resistant breeding of cassava are limited.In model plant species,ethylene response factors play important roles in response to pathogen infection.In this study,cassava ethylene response factors (MeERFs) were identified and characterized as the first step in studying their potential for CBB-resistant breeding of cassava.In the cassava genome 155 MeERFs were identified,of which 23 were induced by Xam infection.The promoter regions of204 genes harbored GCC-box that had the potential to interact with MeERFs.Using 37 transcriptomes derived from Xam infection treatment,four gene co-expression modules for the MeERFs and GCC-box containing genes were constructed.Six MeERFs were associated with two GCC-box containing genes:transcription initiation factor TFIIE subunit beta (MeTFIIE),and histone-lysine N-methyltransferase ASHR1 (MeASHR1).Dual-luciferase reporter assays showed that MeERF10 and MeERF58 positively regulated Me TFIIE;MeERF137 negatively regulated Me TFIIE;MeERF10 and MeERF137 positively regulated Me ASHR1;and MeERF35 negatively regulated Me ASHR1.The four MeERFs may mediate pathogen response by regulating the expression of the two GCC-box containing genes.
基金the National Key Research and Development Program of China(2019YFA0708502)the National Natural Science Foundation of China(Grant No.U1930401)+3 种基金BL14U1 of the Shanghai Synchrotron Radiation Facility for beamtime access based on proposal 2019-SSRF-PT-011035 and Geo-SoilEnviroCARS(Sector 13-BMC and 13-BMD)at the Advanced Photon Source,Argonne National Laboratory,USAthe National Science Foundation Earth Sciences(Grant No.EAR1128799)the Department of Energy-GeoSciences(Grant No.DEFG02-94ER14466)The Advanced Photon Source is a U.S.Department of Energy(DOE)Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract No.DE-AC02-06CH11357.
文摘δ-(Al,Fe)OOH is considered to be one of the most important hydrous phases on Earth,remaining stable under the extreme conditions throughout the mantle.The behavior ofδ-(Al,Fe)OOH at high pressure is essential to understanding the deep water cycle.δ-(Al_(0.956)Fe_(0.044))OOH crystals synthesized at 21 GPa and 1473 K were investigated by high-pressure Brillouin light scattering spectroscopy and synchrotron X-ray diffraction up to 135.4 GPa in diamond anvil cells.The incorporation of 5 mol%FeOOH increases the unit-cell volume ofδ-AlOOH by~1%and decreases the shear-wave velocity(VS)by~5%at 20–135 GPa.In particular,the compressional(V_(P))and shear(VS)wave velocities ofδ-(Al_(0.956)Fe_(0.044))OOH are 7%–16%and 10%–24%greater than all the major minerals in the mantle transition zone including wadsleyite,ringwoodite,and majorite.The distinctly high sound velocities ofδ-(Al_(0.956)Fe_(0.044))OOH at 20–25 GPa may contribute to the seismic anomalies observed at~560–680 km depths in the cold and stagnant slab beneath Izu-Bonin and/or Korea.Furthermore,the VS ofδ-(Al_(0.956)Fe_(0.044))OOH is about 10%and 4%–12%lower than iron-bearing bridgmanite Mg_(0.96)Fe_(0.05)Si_(0.99O3)and ferropericlase(Mg_(0.92)Fe_(0.08))O,respectively,under the lowermost mantle conditions,which might partially contribute to the large low-shear-velocity provinces and ultralow velocity zones at the bottom of the lower mantle.
文摘In the 18^(th)century,British gardens began to transform from a classical to a natural landscape style.During this period,they were influenced by the economy,local nature,as well as foreign cultures.The 18^(th)century was the golden period of cultural exchange between China and the West which gave Britain the opportunity to absorb the cultures of Chinese classical gardens.British gardeners had used various elements of Chinese classical gardens as their point of reference which promoted the development of British natural landscape gardens.
基金a Research Grant for Science From Gansu Provincial Science & Technology Department, No. 090NKCA106
文摘BACKGROUND: Lead can cause structural changes in the hippocampus, followed by damage to learning and memory functions, but its specific mechanisms are not yet clear. OBJECTIVE: To observe long-term toxicity of high-dose lead in drinking water on hippocampal tissue in rats, and analyze the potential association of oxidative damage, cell apoptosis, and pathology. DESIGN, TIME AND SETTING: A randomized, controlled animal experiment was performed at the Center for Medical Experiment, Lanzhou General Hospital of Lanzhou Military Area Command of Chinese PLA from May 2007 to October 2008. MATERIALS; Rabbit anti Bcl-2, Bax, and inducible nitric oxide synthase (iNOS) polyclonal antibodies were purchased from Santa Cruz Biotechnology, USA. An streptavidin-peroxidase immunohistochemistry kit and concentrated DAB kit were purchased from Beijing Zhongshan Biotechnology Company Limited, China. Crystal violet was purchased from Sigma, USA. METHODS: A total of 72 Wistar rats, aged 3 months, were randomly divided into control, low-, middle-, and high-dose lead groups, with 18 rats per group. Animal models were established through free drinking water contaminated by Pb2+ for 1, 3, and 6 months, respectively. MAIN OUTCOME MEASURES: The general toxicity of lead was dynamically observed; the levels of Pb2+ in the blood and brain tissue homogenete were detected using atomic absorption method; pathological changes were observed using hematoxylin-eosin staining and tigroid body staining; the protein expression levels of Bcl-2, Bax, and iNOS were dynamically observed using streptavidin-peroxidase immunohistochemistry of the hippocampus. RESULTS: Lead exposure reduced autonomic activities, produced a slumped appearance, slow responses, and lusterless fur, especially in the high-dose group. The amount of ingestion and hydroposia showed a decreasing trend, especially in middle- and high-dose groups. Lead levels in whole blood and brain homogenate were higher than controls (P 〈 0.01). Lead caused degeneration of hippocampal neurons and pyknosis, with fewer tigroid bodies, especially in high-dose lead group. Bcl-2 expression decreased with increasing lead dose (P 〈 0.01), whereas lead dose-dependently increased Bax levels (P 〈 0.01) and iNOS levels (P 〈 0.05). CONCLUSION: High levels of Pb^2+ may disrupt hippocampal structure by passing through the blood brain barrier. Oxidative damage and apoptosis may be a toxicity mechanism of Pb^2+ on the hippocampus.
基金supported by the National Key Research and Development Program of China(2016YFA0401503 and 2018YFA0305700)the National Natural Science Foundation of China(11575288,91934303,21935001 and 11775011)+4 种基金the Strategic Priority Research ProgramKey Research Program of Frontier Sciences of the Chinese Academy of Sciences(XDB33000000,XDB25000000 and QYZDBSSW-SLH013)the Youth Innovation Promotion Association of the Chinese Academy of Sciences(Y202003)the China Geological Survey(DD20190234)the Scientific Instrument Developing Project(ZDKYYQ20170001)of the Chinese Academy of Sciences。
文摘It has been recognized that a small amount of propane mixed with methane can change greatly in not only the thermodynamics but also the structural properties of gas hydrate.However,its mechanism is still not well understood yet.In this research,structure-Ⅱ(sⅡ)hydrate is synthesized using a methanepropane gas mixture with an initial mole ratio of 99:1,and it is found that large(5~(12)6~4)cages are cooccupied by multiple gases based on the rigid structure analysis of neutron diffraction data.The first principles calculation and molecular dynamics simulation are conducted to uncover the molecular mechanism for sⅡmethane-propane hydrate formation,revealing that the presence of propane inhibits the formation of structure-Ⅰ(sⅠ)hydrate but promotes sⅡhydrate formation.The results help to understand the accumulation mechanism of natural gas hydrate and benefit to optimize the condition for gas storage and transportation in hydrate form.
基金supported by the Hainan Provincial Natural Science Foundation of China (322RC798)the National Key Research and Development Program of China (2018YFD1000501)+1 种基金the Major Science and Technology Plan of Hainan Province (ZDKJ2021012)the China Agriculture Research System (CARS11-HNCX)。
文摘Chilling-induced accumulation of reactive oxygen species(ROS) is harmful to plants,which usually produce anthocyanins to scavenge ROS as protection from chilling stress.As a tropical crop,cassava is hypersensitive to chilling,but the biochemical basis of this hypersensitivity remains unclear.We previously generated Me MYB2-RNAi transgenic cassava with increased chilling tolerance.Here we report that Me MYB2-RNAi transgenic cassava accumulated less ROS but more cyanidin-3-O-glucoside than the wild type under early chilling stress.Under this stress,the anthocyanin biosynthesis pathway was more active in Me MYB2-RNAi lines than in the wild type,and several genes involved in the pathway,including Me TT8,were up-regulated by Me MYB2-RNAi in the transgenic cassava.Me MYB2 bound to the Me TT8 promoter and blocked its expression under both normal and chilling conditions,thereby inhibiting anthocyanin accumulation.Me TT8 was shown to bind to the promoter of Dihydroflavonol 4-reductase(Me DFR-2)and increased Me DFR-2 expression.Me MYB2 appears to act as an inhibitor of chilling-induced anthocyanin accumulation during the rapid response of cassava to chilling stress.
基金supported by the National Key Research and Development Program of China(Grant Nos.2016YFA0401503 and 2018YFA0305700)the National Natural Science Foundation of China(Grant No.11575288)+1 种基金the Strategic Priority Research Program and Key Research Program of Frontier Sciences of the Chinese Academy of Sciences(Grant Nos.XDB33000000,XDB25000000,and QYZDBSSW-SLH013)the Youth Innovation Promotion Association of the Chinese Academy of Sciences(Grant No.Y202003)。
文摘In recent years,transition metal borides(TMBs)have attracted much attention because they are considered as potential superhard materials and have more abundant crystal structures compared with traditional superhard materials.So far,however,no superhard materials have been found in TMBs.A large number of structures and potential new properties in TMBs are induced by the various hybridization ways of boron atoms and the high valence electrons of transition metals,which provide many possibilities for its application.And most TMBs have layered structures,which make TMBs have the potential to be a two-dimensional(2D)material.The 2D materials have novel properties,but the research on 2D TMBs is still nearly blank.In this paper,the research progress of TMBs is summarized involving structure,mechanical properties,and multifunctional properties.The strong covalent bonds of boron atoms in TMBs can form one-dimensional,twodimensional,and three-dimensional substructures,and the multiple electron transfer between transition metal and boron leads to a variety of chemical bonds in TMBs,which are the keys to obtain high hardness and multifunctional properties of TMBs.Further research on the multifunctional properties of TMBs,such as superconductors,catalysts,and high hardness ferromagnetic materials,is of great significance to the discovery of new multifunctional hard materials.
基金Project supported by the National Key R&D Program of China(Grant No.2016YFA0401503)the National Natural Science Foundation of China(Grant Nos.11575288 and 51402350)
文摘In the High-Pressure Synergetic Measurements Station (HP-SymS) of the Synergic Extreme Condition User Facility (SECUF), we will develop ultrahigh-pressure devices based on diamond-anvil cell (DAC) techniques, with a target pressure up to 300 GPa. With the use of cryostat and magnet, we will reach 300 GPa4.2 K-9 T and conduct simultaneous measurements of the electrical-transport property and Raman/Brillouin spectrascopy. With resistance heating and laser heating, we will reach temperatures of at least 1000 and 3000 K, respectively, coupled with Raman/Brillouin spectroscopy measurements. Some designs of supporting devices, such as a femtosecond laser gasket-drilling device, electrode-deposition device, and the gas-loading device, are also introduced in this article. Finally, we conclude by providing some perspectives on the applications of the DAC in related research fields.
基金funding support from the National Key R&D Program of China(grant nos.2021YFB3200400 and 2022YFE0105300)the New Cornerstone Science Foundation through the XPLORER PRIZE,the National Natural Science Foundation of China(grant nos.22276131,21825601,U21A20296,U1967217,12275190,U1932124,and 22206144)+2 种基金the Science Foundation of Jiangsu Province(grant no.BK20220026)the China-Portugal Joint Laboratory of Cultural Heritage Conservation Science(grant no.2021YFE0200100)Soochow University-Western University Centre for Synchrotron Radiation Research.
文摘Developing efficient adsorbents for radon(Rn)capture from the ambient environment is of paramount importance for public health.However,it poses a great challenge due to the chemical inertness and extremely low molar concentration of Rn in air.Herein,we report a zeolite imidazolate frameworkderived metallic carbon adsorbent(Zn@NPC)with record high Rn removal performance under ambient conditions.Upon one-step pyrolysis,the prepared Zn@NPC possesses pores with a preference for Rn and atomically dispersed Zn sites,achieving a high Rn removal efficiency that doubles in adsorption coefficient(9.47 L·g^(−1))and triples in adsorption kinetic coefficient(20.25 mL·g^(−1)·min^(−1))over the benchmark Rn adsorbent coconut activated charcoal.Density functional theory calculations elucidate the important role of the metal polarization effect,which cooperates with the pore size confinement effect to boost the overall Rn adsorption performance.This work launches a promising alternative for practical Rn capture.
基金supported by the National Natural Science Foundation Committee of China-Liaoning Provincial People’s Government Joint Fund(No.U1908204)the National Natural Science Foundation of China(21976009)+2 种基金the National Key R&D Program of China(Nos.2022YFB3506200 and 2022YFB3504100)the Beijing Natural Science Foundation(J210006)the R&D Program of Beijing Municipal Education Commisson(No.KZ202210005011)。
文摘The PdPtVO_(x)/CeO_(2)-ZrO_(2)(PdPtVO_(x)/CZO)catalysts were obtained by using different approaches,and their physical and chemical properties were determined by various techniques.Catalytic activities of these materials in the presence of H_(2)O or SO_(2)were evaluated for the oxidation of ethylbenzene(EB).The PdPtVO_(x)/CZO sample exhibited high catalytic activity,good hydrothermal stability,and reversible sulfur dioxide-poisoning performance,over which the specific reaction rate at 160℃,turnover frequency at 160℃(TOF_(Pd or Pt)),and apparent activation energy were 72.6 mmol/(g_(Pt)·sec)or 124.2 mmol/(g_(Pd)·sec),14.2 sec^(-1)(TOF_(Pt))or 13.1 sec^(-1)(TOF_(Pd)),and 58 k J/mol,respectively.The large EB adsorption capacity,good reducibility,and strong acidity contributed to the good catalytic performance of PdPtVO_(x)/CZO.Catalytic activity of PdPtVO_(x)/CZO decreased when 50 ppm SO_(2)or(1.0 vol.%H_(2)O+50 ppm SO_(2))was added to the feedstock,but was gradually restored to its initial level after the SO_(2)was cut off.The good reversible sulfur dioxide-resistant performance of PdPtVO_(x)/CZO was associated with the facts:(i)the introduction of SO_(2)leads to an increase in surface acidity;(ii)V can adsorb and activate SO_(2),thus accelerating formation of the SO_(x)^(2-)(x=3 or 4)species at the V and CZO sites,weakening the adsorption of sulfur species at the PdPt active sites,and hence protecting the PdPt active sites to be not poisoned by SO_(2).EB oxidation over PdPtVO_(x)/CZO might take place via the route of EB→styrene→phenyl methyl ketone→benzaldehyde→benzoic acid→maleic anhydride→CO_(2)and H_(2)O.
文摘对电极(counter electrode,CE)作为染料敏化太阳能电池(dye-sensitized solar cell,DSSC)的重要组成部分之一,其作用是收集外电路电子和催化还原电解质.硫化镍具有低成本和优异的电催化活性等优点,是Pt的理想替代材料.本文制备的NiS电极的透光率可以达到80%以上(600 nm处),从正面(光阳极)照射时,制备的DSSC器件光电转化效率达到7.54%,与Pt对电极的(7.48%)相当.从反面(对电极)照射时,光电转化效率达到3.96%,远高于Pt对电极(0.58%).在硫化镍电极中掺入石墨烯,可以进一步提升DSSC器件的光电转化效率,正面照射达到7.84%,反面照射达到4.59%,是正面照射效率的58.5%.电化学阻抗、循环伏安测试表明NiS对电极具有很小的串联电阻和高的电催化活性,这是其性能优于Pt的主要原因;而高的反面照射光电转化效率主要得益于NiS电极的高透光率.本文提供了一种简单、快捷、低成本的方法来制备透明、高效硫化镍对电极.