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1.
Blue and red sepals of Hydrangea macrophylla were quantitatively analyzed for aluminium, anthocyanin (delphinidin 3-glucoside) and copigments (caffeoyl- and p-coumaroylquinic acids). All the blue sepals examined contained both Al and copigments (especially 3-caffeoylquinic acid) in considerable amounts. In in vitro experiments using 3- and 5-caffeoylquinic acids, Al and delphinidin 3-glucoside, it was shown that 3-caffeoylquinic acid and Al formed a blue complex with the anthocyanin. Absorption spectra of the blue complex were practically identical with those of the blue solutions obtained from blue hydrangea sepals by extraction with 4 M NACl. In contrast, 5-caffeoylquinic acid (chlorogenic acid) which was also present in hydrangea sepals gave only a red-purple colour with Al and the anthocyanin. Neither 3-caffeoylquinic acid nor Al independently produced blue colour when mixed with the anthocyanin in the mole ratios of 1–30, this being the range that the compounds were found in blue sepals. These results suggest that blue colour of hydrangea sepals is due mainly to the blue complex of delphinidin 3-glucoside-aluminium-3-caffeoylquinic acid. The role of aluminium may be to stabilize an interaction between the quinic ester and the anthocyanin.  相似文献   

2.
Yoshida K  Ito D  Shinkai Y  Kondo T 《Phytochemistry》2008,69(18):3159-3165
The sepal color of a chameleon hydrangea, Hydrangea macrophylla cv. Hovaria™ ‘Homigo’ changes in four stages, from colorless to blue, then to green, and finally to red, during maturation and the senescence periods. To clarify the chemical mechanism of the color change, we analyzed the components of the sepals at each stage. Blue-colored sepals contained 3-O-sambubiosyl- and 3-O-glucosyldelphinidin along with three co-pigments, 5-O-p-coumaroyl-, 5-O-caffeoyl- and 3-O-caffeoylquinic acids. The contents of glycosyldelphinidins decreased toward the green-colored stage, with a coincident increase in the number of chloroplasts. During the last red colored stage, the two species of 3-O-glycosyldelphinidin almost disappeared, and another two anthocyanins, 3-O-sambubiosyl- and 3-O-glucosylcyanidin, increased in amounts. Mixing of 3-O-glycosylcyanidins, co-pigments, and Al3+ in a buffered solution at pH 3.0-3.5 gave not a blue, but a red, colored solution that was the same as that of the sepal color of the 4th stage. Sepals of hydrangea grown in an highland area also turned red in autumn, and contained the same cyanidin glycosides. The red coloration of the hydrangea during senescence was due to a change in anthocyanin biosynthesis.  相似文献   

3.
Red, purple, and blue sepals on selected cultivars of Hydrangea macrophylla were analyzed for their aluminum content. This content was determined to be a function of the sepal color with red sepals possessing 0–10 μg Al/g fresh sepal, purple sepals having 10–40 μg Al/g fresh sepal, and blue sepals containing greater than 40 μg Al/g fresh sepal. Accordingly, the threshold aluminum content needed to change H. macrophylla sepals from red to blue was about 40 μg Al/g fresh sepal. Higher aluminum concentrations were incorporated into the sepals, but this additional aluminum did not affect the intensity or hue of the blue color. These observations agreed with a chemical model proposing that the concentration of the blue Al3+-anthocyanin complex reached a maximum when a sufficient excess of aluminum was present. In addition, the visible absorbance spectra of harvested red, purple, and blue sepals were duplicated by Al3+ and anthocyanin (delphinidin-3-glucoside) mixtures in this model chemical system.  相似文献   

4.
From blue sepals of Hydrangea macrophylla, copigments which show a blueing effect on the hydrangea anthocyanin were isolated and identified as 3-p-coumaroylquinic acid and 3-caffeoylquinic acid. 5-Caffeoylquinic acid (chlorogenic acid) which was also found in the blue sepals, however, did not show such a blueing effect though it acted as a copigment. Likewise, the 4-esters of p-coumaroyl- and caffeoylquinic acids (not found in sepals) produced purple rather than blue colours. The facts suggest that the stereostructures of 3-p-coumaroyl- and 3-caffeoylquinic acids are effective for molecular interaction between the p-coumaroyl or caffeoyl residue in the compounds and the anthocyanin. The anthocyanin in red and blue sepals of hydrangea was confirmed to be delphinidin 3-monoglucoside.  相似文献   

5.
Sepal color of hydrangea varies with the environmental conditions. Although chemical and biological studies on this color variation have a long history, little correct knowledge has been generated about color development. All colored sepals contain the same anthocyanin, delphinidin 3-glucoside. Thus, there must be some other system for developing the wide variety of colors. In hydrangea sepals the cells of the epidermis are colorless and only the second layer of cells contain pigment. We prepared protoplasts without any color change during enzyme treatment of sepals and measured the vacuolar pH of each of the colored cells. We could correlate the color of a single hydrangea cell with its vacuolar pH using a combination of micro-spectrophotometry and a proton-selective microelectrode. Values for the vacuolar pH of blue (lambda vismax: 589 nm) and red cells (lambda vismax: 537 nm) were 4.1 and 3.3, respectively, the vacuolar pH of blue cells being significantly higher.  相似文献   

6.
Previous investigators have disagreed about whether hemalum stains DNA or its associated nucleoproteins. I review here the literature and describe new experiments in an attempt to resolve the controversy. Hemalum solutions, which contain aluminum ions and hematein, are routinely used to stain nuclei. A solution containing 16 Al3+ ions for each hematein molecule, at pH 2.0–2.5, provides selective progressive staining of chromatin without cytoplasmic or extracellular “background color.” Such solutions contain a red cationic dye-metal complex and an excess of Al3+ ions. The red complex is converted to an insoluble blue compound, assumed to be polymeric, but of undetermined composition, when stained sections are blued in water at pH 5.5–8.5. Staining experiments with DNA, histone and DNA + histone mixtures support the theory that DNA, not histone, is progressively colored by hemalum. Extraction of nucleic acids, by either a strong acid or nucleases at near neutral pH, prevented chromatin staining by a simple cationic dye, thionine, pH 4, and by hemalum, with pH adjustments in the range, 2.0–3.5. Staining by hemalum at pH 2.0–3.5 was not inhibited by methylation, which completely prevented staining by thionine at pH 4. Staining by hemalum and other dye-metal complexes at pH ≤ 2 may be due to the high acidity of DNA-phosphodiester (pKa ~ 1). This argument does not explain the requirement for a much higher pH to stain DNA with those dyes and fluorochromes not used as dye-metal complexes. Sequential treatment of sections with Al2(SO4)3 followed by hematein provides nuclear staining that is weaker than that attainable with hemalum. Stronger staining is seen if the pH is raised to 3.0–3.5, but there is also coloration of cytoplasm and other materials. These observations do not support the theory that Al3+ forms bridges between chromatin and hematein. When staining with hematein is followed by an Al2(SO4)3 solution, there is no significant staining. Taken together, the results of my study indicate that the red hemalum cation is electrostatically attracted to the phosphate anion of DNA. The bulky complex cation is too large to intercalate between base pairs of DNA and is unlikely to fit into the minor groove. The short range van der Waals forces that bind planar dye cations to DNA probably do not contribute to the stability of progressive hemalum staining. The red cation is precipitated in situ as a blue compound, insoluble in water, ethanol and water-ethanol mixtures, when a stained preparation is blued at pH > 5.5.  相似文献   

7.
Al3+‐resistant cultivars of wheat (Triticum aestivum L.) release malate through the Al3+‐activated anion transport protein Triticum aestivum aluminum‐activated malate transporter 1 (TaALMT1). Expression of TaALMT1 in Xenopus oocytes and tobacco suspension cells enhances the basal transport activity (inward and outward currents present in the absence of external Al3+), and generates the same Al3+‐activated currents (reflecting the Al3+‐dependent transport function) as observed in wheat cells. We investigated the amino acid residues involved in this Al3+‐dependent transport activity by generating a series of mutations to the TaALMT1 protein. We targeted the acidic residues on the hydrophilic C‐terminal domain of TaALMT1 and changed them to uncharged residues by site‐directed mutagenesis. These mutant proteins were expressed in Xenopus oocytes and their transport activity was measured before and after Al3+ addition. Three mutations (E274Q, D275N and E284Q) abolished the Al3+‐activated transport activity without affecting the basal transport activity. Truncation of the hydrophilic C‐terminal domain abolished both basal and Al3+‐activated transport activities. Al3+‐dependent transport activity was recovered by fusing the N‐terminal region of TaALMT1 with the C‐terminal region of AtALMT1, a homolog from Arabidopsis. These findings demonstrate that the extracellular C‐terminal domain is required for both basal and Al3+‐dependent TaALMT1 activity. Furthermore, we identified three acidic amino acids within this domain that are specifically required for the activation of transport function by external Al3+.  相似文献   

8.
9.
Dy3+‐doped Y3Al5O12 phosphors were prepared at a relatively low temperature using molten salt synthesis. The phase of the prepared Dy3+‐doped Y3Al5O12 phosphors was confirmed using X‐ray powder diffraction. Results indicated that Dy3+ doping did not change the Y3Al5O12 phase. Following excitation at 352 nm, emission spectra of the Dy3+‐doped Y3Al5O12 phosphors consisted of blue, yellow, and red emission bands. The influence of Dy3+ concentration and excitation wavelength on emission was investigated. The ratio of yellow light to blue light varied with change in Dy3+ doping concentration, due to changes in the structure around Dy3+. Emission intensities also changed when the excitation wavelength was changed. This variation is luminescence generated a system for tunable white light for Dy3+‐doped Y3Al5O12 phosphors.  相似文献   

10.
Rose cultivars with blue flower color are among the most attractive breeding targets in floriculture. However, they are difficult to produce due to the low efficiency of transformation systems, interactive effects of hosts and vectors, and lengthy processes. In this study, agroinfiltration-mediated transient expression was investigated as a tool to assess the function of flower color genes and to determine appropriate host cultivars for stable transformation in Rosa hybrida. To induce delphinidin accumulation and consequently to produce blue hue, the petals of 30 rose cultivars were infiltrated with three different expression vectors namely pBIH-35S-CcF3′5′H, pBIH-35S-Del2 and pBIH-35S-Del8, harbouring different sets of flower color genes. The results obtained showed that the ectopic expression of the genes was only detected in three cultivars with dark pink petals (i.e. ‘Purple power’, ‘High & Mora’ and ‘Marina’) after 6–8 days. The high performance liquid chromatography analyses confirmed delphinidin accumulation in the infiltrated petals caused by transient expression of CcF3′5′H gene. Moreover, there were significant differences in the amounts of delphinidin among the three cultivars infiltrated with the three different expression vectors. More specifically, the highest delphinidin content was detected in the cultivar ‘Purple power’ (4.67 µg g?1 FW), infiltrated with the pBIH-35S-Del2 vector. The expression of CcF3′5′H gene in the infiltrated petals was also confirmed by real time PCR. In conclusion and based on the findings of the present study, the agroinfiltration could be regarded as a reliable method to identify suitable rose cultivars in blue rose flower production programs.  相似文献   

11.
For white light-rendering research activities, interpretation by using colored emitting materials is an alternative approach. But there are issues in designing the white color emitting materials. Particularly, differences in thermal and decay properties of discrete red, green, and blue emitting materials led to the quest for the search of a single-phased material, able to emit primary colors for white light generation. The current study is an effort to design a simple, single-phase, and cost-effective material with the tunable emission of primary colors by a series of Mg1−xBaxAl2O4:Mn2+ nanopowders. Doping of manganese ion (Mn2+) in the presence of the larger barium cation (Ba2+) at tetrahedral-sites of the spinel magnesium aluminate (MgAl2O4) structure led to the creation of antisite defects. Doped samples were found to have lower bandgaps compared with MgAl2O4, and hybridization of 3d-orbitals of Mn2+ with O(2p), Mg(2s)/Al(2s3p) was found to be responsible for narrowing the bandgap. The distribution of cations at various sites at random results in a variety of electronic transitions between the valance band and oxygen vacancies as well as electron traps produced the antisite defects. The suggested compositions might be used in white light applications since they have three emission bands with centers at 516 nm (green), 464 nm (blue) and 622 nm (red) at an excitation wavelength of 380 nm. A detailed discussion to analyze the effects of the larger cationic radius of Ba2+ on the lattice strain, unit cell parameters, and cell volumes using X-ray diffraction analysis is presented.  相似文献   

12.
This study is designed to examine the participation of the major red cell membrane protein, band 3 protein, in the chain which transmits information from the cardiac glycoside site on the external face of the cell (Na+ + K+)-ATPase to the megadalton glycolytic enzyme complex within the cell. The experiments show that the anion transport inhibitor, 4,4′-diisothiocyano-2,2′-stilbenedisulfonic acid, affects the resonance of 2,3-diphosphoglycerate, as does the cardiac glycoside cation transport inhibitor, ouabain. Resonance shifts induced by the cardiac glycoside alone are modulated by addition of the anion transport inhibitor which indicates that there is coupling in the red cell between the (Na+ + K+)-ATPase and band 3 protein. Band 3 protein was separated from the membrane and partially purified following the technique of Yu and Steck ((1975) J. Biol. Chem. 250, 9170–9175). When glyceraldehyde-3-phosphate dehydrogenase was added to the separated band 3 protein preparation, addition of cardiac glycosides caused shifts in the 31P resonance of glyceraldehyde 3-phosphate. These experiments indicate that there is coupling between the (Na+ + K+)-ATPase and band 3 protein in the separated preparation and suggest that the anion and cation transport systems may be closely related spatially and functionally in the intact red cell.  相似文献   

13.
Flower colour and cytochromes P450   总被引:8,自引:0,他引:8  
Flavonoids are major constituents of flower colour. Plants accumulate specific flavonoids and thus every species often exhibits a limited flower colour range. Three cytochromes P450 play critical roles in the flavonoid biosynthetic pathway. Flavonoid 3′-hydroxylase (F3′H, CYP75B) and flavonoid 3′,5′-hydroxylase (F3′5′H, CYP75A) catalyze the hydroxylation of the B-ring of flavonoids and are necessary to biosynthesize cyanidin-(red to magenta) and delphinidin-(violet to blue) based anthocyanins, respectively. Pelargonidin-based anthocyanins (orange to red) are synthesized in their absence. Some species such as roses, carnations and chrysanthemums do not have violet/blue flower colour due to deficiency of F3′5′H. Successful expression of heterologous F3′5′H genes in roses and carnations results in delphinidin production, causing a novel blue/violet flower colour. Down-regulation of F3′H and F3′5′H genes has yielded orange petunia and pink torenia colour that accumulate pelargonidin-based anthocyanins. Flavone synthase II (CYP93B) catalyzes the synthesis of flavones that contribute to the bluing of flower colour, and modulation of FNSII gene expression in petunia and tobacco changes their flower colour. Extensive engineering of the anthocyanin pathway is therefore now possible, and can be expected to enhance the range of flower colours.  相似文献   

14.
Tomato plants (Lycopersicon esculentum L. var. Ailsa Craig) were grown in water culture in nutrient solution in a series of 10 increasing levels of nitrate nutrition. Using whole plant data derived from analytical and yield data of individual plant parts, the fate of anion charge arising from increased NO3 assimilation was followed in its distribution between organic anion accumulation in the plant and OH efflux into the nutrient solution as calculated by excess anion over cation uptake. With increasing NO3 nutrition the bulk of the anion charge appeared as organic anion accumulation in the plants. OH efflux at a maximum accounted for only 20% of the anion charge shift. The major organic anion accumulated in response to nitrate assimilation was malate. The increase in organic anion accumulation was paralleled by an increase in cation concentration (K+, Ca2+, Mg2+, Na+). Total inorganic anion levels (NO3, SO42−, H2PO4, Cl) were relatively constant. The effect of increasing NO3 nutrition in stimulating organic anion accumulation was much more pronounced in the tops than in the roots.  相似文献   

15.
该研究以7个品种铁筷子(Helleborus thibetanus Franch.)为试验材料,借助目视测色、RHSCC比色卡、色差仪进行花色表型的测定,采用高效液相色谱法-光电二极管阵列检测方法(HPLC-DAD)及高效液相色谱-电喷雾离子化-质谱联用技术(HPLC-ESI-MS)测定分析铁筷子花瓣中花青素苷成分及含量,以探究不同品种铁筷子的花色与花青素苷成分及含量之间的关系。结果显示:(1)紫色系品种花瓣的a*值最高b*值最低,黄色系品种花瓣的b*值最高a*值最低,不同品种的铁筷子花色越深L*值越低。(2)从5个有花青素苷积累的铁筷子品种中检测出11种花青素苷成分,分别为6种矢车菊素苷,4种飞燕草素苷,1种矮牵牛素苷;供试的铁筷子材料中红色系2个品种的花青素苷含量最高,紫色系品种次之;矢车菊素苷与飞燕草素苷为影响铁筷子花瓣呈色的主要色素物质。(3)不同种类的花青素和修饰基团的差异,导致铁筷子花瓣呈现不同的色彩,含有多种酰基化修饰的飞燕草素苷使铁筷子花色蓝移进而使花色加深。(4)相关分析表明,铁筷子花瓣的L*值与a*值呈显著负相关关系,与b*值呈显著的正相关关系;L*值与总花青素苷含量呈显著负相关关系,且随着花青素苷含量的累积a*值增加,花色红移。研究表明,花青素苷的成分及含量是导致铁筷子花瓣呈现不同颜色的主要原因,矢车菊素苷和飞燕草素苷的互作以及酰基化的修饰使铁筷子呈现不同程度的紫色,花青素苷的不同累积量影响了花瓣颜色的明暗变化,从而使铁筷子花瓣颜色丰富。  相似文献   

16.
为研究金花茶组植物花色与细胞内重要环境因子的关系,该研究以花色不同的8个金花茶组物种的9个居群为材料,测定了其花瓣的颜色、总黄酮含量、含水量、细胞pH、7种金属离子浓度。结果表明:所测金花茶组植物的花色平均明度L~*为80.82、色相a~*为-2.88、色相b~*为53.97、彩度C~*为54.10、色相角h为93.19°,故金花茶花色为明度较亮的黄色,其中色相b~*为描述黄色的主要指标,据此可将所测植物分为金黄、黄、浅黄3类。花瓣总黄酮含量为20.17%,花瓣含水量为88.14%,物种间均达到差异显著,且均与花色呈弱相关,对黄色呈现影响较小。花瓣细胞偏弱酸性,pH平均值为6.19,不同物种间差异显著,细胞pH与花色呈显著正相关,即中偏弱酸性细胞环境有利于金花茶花瓣黄色的呈现。金属离子浓度中,K~+含量最高(12.61 mg·g~(-1)),其他依次为Ca2+(3.91 mg·g~(-1))、Mg~(2+)(1.28 mg·g~(-1))、Al~(3+)(0.98 mg·g~(-1))、Na~+(0.17mg·g~(-1))、Fe~(3+)(0.07 mg·g~(-1)),Cu~(2+)含量最低(0.003 8 mg·g~(-1)),7种金属离子在所测植物间均存在显著差异,其中Al~(3+)、Fe~(3+)和Ca~(2+)对金花茶黄色花的形成具有不同程度的干扰作用,随着这3种金属离子浓度升高,黄度降低,花色变淡。因此,较低浓度的Al~(3+)、Fe~(3+)、Ca~(2+)可能更有利于金花茶黄色花的呈现。  相似文献   

17.
The present communication is strongly focused on the investigation of synthesis, structural and luminescence properties of cerium (Ce3+)- and europium (Eu3+)-activated Zn4Al22O37 phosphors. Ce3+- and Eu3+-doped Zn4Al22O37 novel phosphors were prepared using a solution combustion synthesis route. Structural properties were studied using powder X-ray diffraction and high-resolution transverse electron microscopy. The optical properties were studied using ultraviolet–visible light spectroscopy and Fourier transform infrared spectroscopy; luminescence properties were studied using a photoluminescence (PL) technique. The crystal structure of the prepared Zn4Al22O37 host and Ce3+- and Eu3+-activated Zn4Al22O37 phosphors was investigated and was found to have a hexagonal structure. The measured PL emission spectrum of the Ce3+-doped Zn4Al22O37 phosphor showed an intense and broad emission band centred at 421 nm under a 298 nm excitation wavelength. By contrast, the Eu3+-doped Zn4Al22O37 phosphor exhibited two strong and intense emission bands at approximately 594 nm (orange) and 614 nm (red), which were monitored under 395 nm excitation. The Commission Internationale de l’Eclairage (CIE) colour coordinates of the Ce3+-doped Zn4Al22O37 were investigated and found to be x = 0.1567, y = 0.0637 (blue) at 421 nm and for Eu3+-doped Zn4Al22O37 were x = 0.6018, y = 0.3976 (orange) at 594 nm and x = 0.6779, y = 0.3219 (red) at 614 nm emission. The luminescence behaviour of the synthesized phosphors suggested that these phosphors may be used in lighting applications.  相似文献   

18.
Ca2Al2O5:Eu3+, Ca2Al2O5:Dy3+ and Ca2Al2O5:Tb3+ phosphors were synthesized using a combustion synthesis method. The prepared phosphors were characterized by X‐ray powder diffraction for phase purity, by scanning electron microscopy for morphology, and by photoluminescence for emission and excitation measurements. The Ca2Al2O5:Eu3+ phosphors could be efficiently excited at 396 nm and showed red emission at 594 nm and 616 nm due to 5D0 → 7F1 and 5D0 → 7F2 transitions. Dy3+‐doped phosphors showed blue emission at 482 nm and yellow emission at 573 nm. Ca2Al2O5:Tb3+ phosphors showed emission at 545 nm when excited at 352 nm. Concentration quenching occurred in both Eu3+ and Dy3+phosphors at 0.5 mol%. Photoluminescence results suggested that the aluminate‐based phosphor could be a potential candidate for application in environmentally friendly based lighting technologies.  相似文献   

19.
A series of Ca2Mg0.25Al1.5Si1.25O7:Ce3+/Eu2+/Tb3+ phosphors was been prepared via a conventional high temperature solid‐state reaction and their luminescence properties were studied. The emission spectra of Ca2Mg0.25Al1.5Si1.25O7:Ce3+,Eu2+ and Ca2Mg0.25Al1.5Si1.25O7:Ce3+,Tb3+ phosphors show not only a band due to Ce3+ ions (409 nm) but also as a band due to Eu2+ (520 nm) and Tb3+ (542 nm) ions. More importantly, the effective energy transfer from Ce3+ to Eu2+ and Tb3+ ions was confirmed and investigated by emission/excitation spectra and luminescent decay behaviors. Furthermore, the energy level scheme and energy transfer mechanism were investigated and were demonstrated to be of resonant type via dipole–dipole (Ce3+ to Eu2+) and dipole–quadrupole (Ce3+ to Tb3+) reactions, respectively. Under excitation at 350 nm, the emitting color could be changed from blue to green by adjusting the relative doping concentration of Ce3+ and Eu2+ ions as well as Ce3+ and Tb3+ ions. The above results indicate that Ca2Mg0.25Al1.5Si1.25O7:Ce3+,Eu2+/Tb3+ are promising single‐phase blue‐to‐green phosphors for application in phosphor conversion white‐light‐emitting diodes. Copyright © 2015 John Wiley & Sons, Ltd.  相似文献   

20.
D. Curtin  G. Wen 《Plant and Soil》2004,267(1-2):109-115
Plants that remove an excess of cations over anions may cause soil acidification. The acidification potential of plants has been evaluated using solution culture techniques, but the influence of ionic composition of the medium on the plant cation-anion balance remains unclear. Our objective was to determine how electrolyte concentration and salt type affect the cation- anion balance of two test plants [barley (Hordeum vulgare L.) and kochia (Kochia scoparia L. Schrad.)]. Seedlings were grown in sand culture and irrigated with nutrient solution (Hoagland’s solution), which was adjusted to a range of electrolyte concentrations (target electrical conductivity of 7.5, 17.5 and 27.5 dS m−1) using either chloride or sulphate salts. Increase in electrolyte concentration reduced yield of kochia, a salt-tolerant plant, by up to 38%. Total cation (Ca + Mg + K + Na) equivalents in kochia exceeded those of anions (Cl + S + P + NO3) by 250 to 280 cmolc kg−1 of dry matter. Electrolyte concentration had no effect on the cation-anion balance of kochia, but excess cation values were significantly greater in the sulphate than in the chloride system. Kochia had a large content of water-soluble oxalate (194 to 226 cmolc kg−1), which was linearly related to the excess cation content. Growth of barley was severely restricted at the intermediate and high electrolyte concentrations. Cations exceeded anions by 21 to 59 cmolc kg−1 of barley dry matter. Excess cation content was greater in the sulphate than in the chloride medium, but electrolyte concentration did not have a consistent effect on the cation-anion balance. The small amounts of oxalate found in barley (0.9 to 2.6 cmolc kg−1) were insufficient to balance the cation excess.  相似文献   

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