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1.
Deng H Grunder S Cordova KE Valente C Furukawa H Hmadeh M Gándara F Whalley AC Liu Z Asahina S Kazumori H O'Keeffe M Terasaki O Stoddart JF Yaghi OM 《Science (New York, N.Y.)》2012,336(6084):1018-1023
We report a strategy to expand the pore aperture of metal-organic frameworks (MOFs) into a previously unattained size regime (>32 angstroms). Specifically, the systematic expansion of a well-known MOF structure, MOF-74, from its original link of one phenylene ring (I) to two, three, four, five, six, seven, nine, and eleven (II to XI, respectively), afforded an isoreticular series of MOF-74 structures (termed IRMOF-74-I to XI) with pore apertures ranging from 14 to 98 angstroms. All members of this series have noninterpenetrating structures and exhibit robust architectures, as evidenced by their permanent porosity and high thermal stability (up to 300°C). The pore apertures of an oligoethylene glycol-functionalized IRMOF-74-VII and IRMOF-74-IX are large enough for natural proteins to enter the pores. 相似文献
2.
Côté AP Benin AI Ockwig NW O'Keeffe M Matzger AJ Yaghi OM 《Science (New York, N.Y.)》2005,310(5751):1166-1170
Covalent organic frameworks (COFs) have been designed and successfully synthesized by condensation reactions of phenyl diboronic acid {C6H4[B(OH)2]2} and hexahydroxytriphenylene [C18H6(OH)6]. Powder x-ray diffraction studies of the highly crystalline products (C3H2BO)6.(C9H12)1 (COF-1) and C9H4BO2 (COF-5) revealed expanded porous graphitic layers that are either staggered (COF-1, P6(3)/mmc) or eclipsed (COF-5, P6/mmm). Their crystal structures are entirely held by strong bonds between B, C, and O atoms to form rigid porous architectures with pore sizes ranging from 7 to 27 angstroms. COF-1 and COF-5 exhibit high thermal stability (to temperatures up to 500 degrees to 600 degrees C), permanent porosity, and high surface areas (711 and 1590 square meters per gram, respectively). 相似文献
3.
Interpenetration (catenation) has long been considered a major impediment in the achievement of stable and porous crystalline structures. A strategy for the design of highly porous and structurally stable networks makes use of metal-organic building blocks that can be assembled on a triply periodic P-minimal geometric surface to produce structures that are interpenetrating-more accurately considered as interwoven. We used 4,4',4"-benzene-1,3,5-triyl-tribenzoic acid (H(3)BTB), copper(II) nitrate, and N,N'-dimethylformamide (DMF) to prepare Cu(3)(BTB)(2)(H(2)O)(3).(DMF)(9)(H(2)O)(2) (MOF-14), whose structure reveals a pair of interwoven metal-organic frameworks that are mutually reinforced. The structure contains remarkably large pores, 16.4 angstroms in diameter, in which voluminous amounts of gases and organic solvents can be reversibly sorbed. 相似文献
4.
为探求氮素对米槁幼苗叶片CO_2响应特征影响,以1年生米槁幼苗为试验材料,采用砂培法,利用Li-6400光合仪测定4种不同氮浓度胁迫下米槁叶片CO_2响应曲线及气孔导度(Gs)、胞间CO_2浓度(Ci)、蒸腾速率(Tr)等相关光合参数,并运用直角双曲线、非直角双曲线、直角双曲线修正3种模型拟合米槁叶片CO_2响应曲线。结果显示,直角双曲线修正模型拟合米槁叶片CO_2响应曲线,可克服直角双曲线模型未考虑曲线凸度缺陷及无法拟合CO_2过饱和净光合速率(Pn)下降缺点,得到光合参数与实测值相近,直接确定CO_2饱和点(CSP)。在控制外界条件下,各氮处理米槁Ci随叶室内CO_2浓度(Ca)升高呈同步直线上升趋势。同一Ca值下,米槁叶片Ci随氮浓度水平增加而增大。各氮处理下米槁叶片Gs随Ci升高总体呈下降趋势;Tr变化趋势与Gs一致,在同一Ci下,Gs与Tr均随氮浓度增大而增加。米槁叶片Pn随Ci升高逐步升高,但在高Ci阶段Pn略下降,增施氮素可提高米槁叶片CSP、最大净光合速率(Pnmax),降低叶片CO_2补偿点(CCP),表明增施氮素能可强米槁叶片光合作用对CO_2适应幅度,提高CO_2利用效率,促进有机物积累。研究表明,直角双曲线修正模型拟合米槁叶片CO_2响应曲线效果最佳,施氮可有效促进米槁幼苗生长。 相似文献
5.
Photosynthesis and chlorophyll a fluorescence parameters, photochemical efficiency of PS II （Fv/Fm）, photochemical quenching of PS II （qP）, nonphotochemical quenching of PS II （NPQ）, maximum activity of PS II （Fv/Fo） as well as electron transport rate （ETR）, and quantum yield of PS II （ФPS II） were measured on flag leaves of the winter wheat treated by methanol at different concentrations. The results revealed that photosynthesis was greatly improved by methanol, as indicated by higher photosynthetic rates and stomatal conductance. The enhancement effect of methanol on photosynthesis was maintained for 3-4 days. Different methanol concentration treatments also increased intercellular CO2 concentration and transpiration rates. No significant decline was found in Fv/Fm, Fv/Fo, and ФPS II, which revealed no photoinhibition during methanol application in different methanol concentrations. Methanol showing no apparent inhibitory effects indicated higher potential photosynthetic capacity of flag leaves of winter wheat. However, the increase in photosynthesis was not followed by an increase in the photosynthetic activity （Fv/Fm）, and fluorescence parameters did not indicate an improvement in intercellular CO2 concentration and PS II photochemical efficiency compared with the control, thereby encouraging us to propose that lower leaf temperatures caused by applied methanol would reduce both dark respiration and photorespiration （most importantly）, thus, increasing net CO2 uptake and photosynthetic rates. 相似文献
6.
Anaerobic CO dehydrogenases catalyze the reversible oxidation of CO to CO2 at a complex Ni-, Fe-, and S-containing metal center called cluster C. We report crystal structures of CO dehydrogenase II from Carboxydothermus hydrogenoformans in three different states. In a reduced state, exogenous CO2 supplied in solution is bound and reductively activated by cluster C. In the intermediate structure, CO2 acts as a bridging ligand between Ni and the asymmetrically coordinated Fe, where it completes the square-planar coordination of the Ni ion. It replaces a water/hydroxo ligand bound to the Fe ion in the other two states. The structures define the mechanism of CO oxidation and CO2 reduction at the Ni-Fe site of cluster C. 相似文献
7.
Polychalcogenide compounds with open polymeric frameworks are rare, and they represent a class of compounds in which microporosity might be achieved. Microporous frameworks that are not oxide-based are now attracting interest because of the combination of catalytic and electronic properties they may simultaneously possess. Three new compounds that may be forerunners to such materials have been discovered and are reported here. The reaction of gallium (Ga), indium (In), and thallium (TI) metal with (Ph(4)P)(2)Se(5) (Ph, phenyl) and an excess of elemental selenium (Se) in a sealed, evacuated Pyrex tube at 200 degrees C yielded small red crystals of (Ph(4)P)[Ga(Se(6))(2)] (I), (Ph(4)P)[In(Se(6))(2)] (II), and (Ph(4)P)[TI(Se(6))(2)] (III), respectively. The [M(Se(6))(2)](-) (M = Ga, In, TI) ions form a two-dimensional, open framework filled with Ph(4)P(+) ions. The [M(Se(6))(2)](n)(n-) structure consists of tetrahedral M(3+) centers and bridging Se(6)(2-) ligands, leading to an extended structure in two dimensions. These layers stack perfectly one on top of the other giving rise to one-dimensional channels running down the c axis that are filled with Ph(4)P(+) cations. These cations are situated in the layers, as opposed to between the layers, and the whole structure can be viewed as a template. Compound II shows remarkable thermal stability and melts congruently at 242 degrees C. Upon cooling to room temperature it gives a glassy phase that recrystallizes upon subsequent heating to 160 degrees C. 相似文献
8.
高CO2浓度条件下农田土壤有机质的化学稳定性研究 总被引：1，自引：0，他引：1
大气CO2浓度升高显著增加作物生物量,从而使进入土壤的有机碳增加,这势必会影响土壤碳的稳定和积累。采取利用化学方法获得的具有不同化学稳定性的有机物,间接地研究大气CO2浓度升高以后通过直接影响秸秆生物量和化学成分对土壤碳变化的影响。结果显示,相对于对照处理:高CO2浓度处理使土壤经Na2S2O8化学氧化后的抗氧化部分,在LN、NN和HN水平下,分别增加16.4%、21.7%和降低3.8%;使土壤经硫酸水解后的第一组分分别降低2.2%,增加9.5%和7.5%,第二组分分别增加4.7%、17.6%和降低4.9%,第三组分分别增加7.3%,降低4.2%和2.6%。表明土壤有机质的化学稳定性有所增加,可能与高CO2浓度条件下向土壤输入的有机质量及化学组成有关,且受N水平的影响较大。 相似文献
9.
不同的施肥水平对大豆产量及品质影响较大,各肥料组合处理对产量、脂肪和蛋白质的影响都达到显著水平;蛋脂总量相对稳定,不同施肥水平间差异不显著。研究表明,氮肥对蛋白质的影响较大,磷钾肥对脂肪影响较大,但是每种肥料的影响作用都不是单独作用,而是与其它两种肥料的共同作用。此外,每种肥料都有一个最佳施用量。蛋白质含量最高的施肥组合为:尿素80kg 磷酸二铵180kg 氯化钾20kg/hm2;脂肪含量最高的处理为:尿素60kg 磷酸二铵180kg 氯化钾50kg/hm2;蛋脂总量最高的处理为:尿素60kg 磷酸二铵120kg 氯化钾50kg/hm2;产量最高的处理为:尿素60kg 磷酸二铵120kg 氯化钾50kg/hm2。 相似文献
10.
The delta(13)C value of the dissolved inorganic carbon in the surface waters of the Pacific Ocean has decreased by about 0.4 per mil between 1970 and 1990. This decrease has resulted from the uptake of atmospheric CO(2) derived from fossil fuel combustion and deforestation. The net amounts of CO(2) taken up by the oceans and released from the biosphere between 1970 and 1990 have been determined from the changes in three measured values: the concentration of atmospheric CO(2), the delta(13)C of atmospheric CO(2) and the delta(13)C value of dissolved inorganic carbon in the ocean. The calculated average net oceanic CO(2) uptake is 2.1 gigatons of carbon per year. This amount implies that the ocean is the dominant net sink for anthropogenically produced CO(2) and that there has been no significant net CO(2) released from the biosphere during the last 20 years. 相似文献
11.
[目的]对基于CO Ⅱ全基因的差翅亚目昆虫的分子系统学进行研究。[方法]设计蜻蜓目昆虫CO Ⅱ全基因的非特异性引物,获得差翅亚目5科6属8种共8条CO Ⅱ全序列。采用CluxtalX1.8、ContigExpress、MEGA2.1、PHYLIP3.6a以及MrBayes V3.0等生物学软件及简约法和最大似然法对其进行分析并构建分子系统树。[结果]CO Ⅱ的A＋T含量较低（68.6%）,说明蜻蜓目是一比较原始的类群;每条序列均含有2个半胱氨酸,这一点有别于其他类群昆虫;不支持将大蜻亚科上升为科的观点;支持将大蜓科和蜓科归入蜓总科,而将春蜓科上升为总科的观点;差翅亚目5科之间的进化关系由慢到快依次为：春蜓科→大蜓科→蜓科→伪蜻科→蜻科。[结论]为蜻蜓目分子系统学研究提供相关依据。 相似文献
12.
We used strong-field laser pulses that were tailored with closed-loop optimal control to govern specified chemical dissociation and reactivity channels in a series of organic molecules. Selective cleavage and rearrangement of chemical bonds having dissociation energies up to approximately 100 kilocalories per mole (about 4 electron volts) are reported for polyatomic molecules, including (CH3)2CO (acetone), CH3COCF3 (trifluoroacetone), and C6H5COCH3 (acetophenone). Control over the formation of CH(3)CO from (CH3)2CO, CF3 (or CH3) from CH3COCF3, and C6H5CH3 (toluene) from C6H5COCH3 was observed with high selectivity. Strong-field control appears to have generic applicability for manipulating molecular reactivity because the tailored intense laser fields (about 10(13) watts per square centimeter) can dynamically Stark shift many excited states into resonance, and consequently, the method is not confined by resonant spectral restrictions found in the perturbative (weak-field) regime. 相似文献
13.
JB McClain DE Betts DA Canelas ET Samulski JM DeSimone JD Londono HD Cochran GD Wignall D Chillura-Martino R Triolo 《Science (New York, N.Y.)》1996,274(5295):2049-2052
Interfacially active block copolymer amphiphiles have been synthesized and their self-assembly into micelles in supercritical carbon dioxide (CO2) has been demonstrated with small-angle neutron scattering (SANS). These materials establish the design criteria for molecularly engineered surfactants that can stabilize and disperse otherwise insoluble matter into a CO2 continuous phase. Polystyrene-b-poly(1,1-dihydroperfluorooctyl acrylate) copolymers self-assembled into polydisperse core-shell-type micelles as a result of the disparate solubility characteristics of the different block segments in CO2. These nonionic surfactants for CO2 were shown by SANS to be capable of emulsifying up to 20 percent by weight of a CO2-insoluble hydrocarbon into CO2. This result demonstrates the efficacy of surfactant-modified CO2 in reducing the large volumes of organic and halogenated solvent waste streams released into our environment by solvent-intensive manufacturing and process industries. 相似文献
14.
Waite JH Young DT Cravens TE Coates AJ Crary FJ Magee B Westlake J 《Science (New York, N.Y.)》2007,316(5826):870-875
Titan's lower atmosphere has long been known to harbor organic aerosols (tholins) presumed to have been formed from simple molecules, such as methane and nitrogen (CH4 and N2). Up to now, it has been assumed that tholins were formed at altitudes of several hundred kilometers by processes as yet unobserved. Using measurements from a combination of mass/charge and energy/charge spectrometers on the Cassini spacecraft, we have obtained evidence for tholin formation at high altitudes (approximately 1000 kilometers) in Titan's atmosphere. The observed chemical mix strongly implies a series of chemical reactions and physical processes that lead from simple molecules (CH4 and N2) to larger, more complex molecules (80 to 350 daltons) to negatively charged massive molecules (approximately 8000 daltons), which we identify as tholins. That the process involves massive negatively charged molecules and aerosols is completely unexpected. 相似文献
15.
16.
Hu J Zhong C Ding C Chi Q Walz A Mombaerts P Matsunami H Luo M 《Science (New York, N.Y.)》2007,317(5840):953-957
Carbon dioxide (CO2) is an important environmental cue for many organisms but is odorless to humans. It remains unclear whether the mammalian olfactory system can detect CO2 at concentrations around the average atmospheric level (0.038%). We demonstrated the expression of carbonic anhydrase type II (CAII), an enzyme that catabolizes CO2, in a subset of mouse olfactory neurons that express guanylyl cyclase D (GC-D+ neurons) and project axons to necklace glomeruli in the olfactory bulb. Exposure to CO2 activated these GC-D+ neurons, and exposure of a mouse to CO2 activated bulbar neurons associated with necklace glomeruli. Behavioral tests revealed CO2 detection thresholds of approximately 0.066%, and this sensitive CO2 detection required CAII activity. We conclude that mice detect CO2 at near-atmospheric concentrations through the olfactory subsystem of GC-D+ neurons. 相似文献
17.
Fully optimized quantum mechanical calculations indicate that Al2O3 transforms from the corundum structure to the as yet unobserved Rh2O3 (II) structure at about 78 gigapascals, and it further transforms to Pbnm-perovskite structure at 223 gigapascals. The predicted x-ray spectrum of the Rh2O3 (II) structure is similar to that of the corundum structure, suggesting that the Rh2O3 (II) structure could go undetected in high-pressure x-ray measurements. It is therefore possible that the ruby (Cr3+-doped corundum) fluorescence pressure scale is sensitive to the thermal history of the ruby chips in a given experiment. 相似文献
18.
T Rockmann CAM Brenninkmeijer G Saueressig P Bergamaschi JN Crowley H Fischer PJ Crutzen 《Science (New York, N.Y.)》1998,281(5376):544-546
Atmospheric carbon monoxide (CO) exhibits mass-independent fractionation in the oxygen isotopes. An 17O excess up to 7.5 per mil was observed in summer at high northern latitudes. The major source of this puzzling fractionation in this important trace gas is its dominant atmospheric removal reaction, CO + OH --> CO2 + H, in which the surviving CO gains excess 17O. The occurrence of mass-independent fractionation in the reaction of CO with OH raises fundamental questions about kinetic processes. At the same time the effect is a useful marker for the degree to which CO in the atmosphere has been reacting with OH. 相似文献
19.
气温对杂交水稻Ⅱ优718产量优势的影响分析 总被引：2，自引：1，他引：1
本文采用5个品种,6个播期的裂区试验设计,3次重复,研究不同播期和气温对水稻Ⅱ优718与对照Ⅱ优838不同性状及产量杂种优势的影响.结果表明:①Ⅱ优718和Ⅱ优838不同性状的杂种优势强弱均表现不同;②F1代产量高的并不一定是中亲优势强的,这主要取决于亲本的自身表现;③不同的环境对产量优势的表现都具有不同的影响,其影响的大小取决于环境因素是否有利于F1代的生长发育和双亲的遗传基础是否正常表达;④采用逐步回归分析后发现F1代及其父母本不同生育阶段的活动积温和有效积温对Ⅱ优718和Ⅱ优838的产量优势均有不同程度的影响. 相似文献
20.
Little is known about the effects of enriched CO(2) atmospheres, which may exist in the next century, on natural plant-insect herbivore interactions. Larvae of a specialist insect herbivore, Junonia coenia (Lepidoptera: Nymphalidae), were reared on one of its host plants, Plantago lanceolata (Plantaginaceae), grown in either current low (350 parts per million) or high (700 ppm) CO(2) environments. Those larvae raised on high-CO(2) foliage grew more slowly and experienced greater mortality, especially in early instars, than those raised on low-CO(2) foliage. Poor larval performance on high-CO(2) foliage was probably due to the reduced foliar water and nitrogen concentrations of those plants and not to changes in the concentration of the defensive compounds, iridoid glycosides. Adult pupal weight and female fecundity were not affected by the CO(2) environment of the host plant. These results indicate that interactions between plants and herbivorous insects will be modified under the predicted CO(2) conditions of the 21st century. 相似文献