WO2006057006A1 - Composition utile dans la fabrication de verre en oxyde de phosphore, potassium et souffre exempt d'azote et a liberation lente et procede de fabrication de verre a partir de celle-ci - Google Patents

Composition utile dans la fabrication de verre en oxyde de phosphore, potassium et souffre exempt d'azote et a liberation lente et procede de fabrication de verre a partir de celle-ci Download PDF

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Publication number
WO2006057006A1
WO2006057006A1 PCT/IN2004/000369 IN2004000369W WO2006057006A1 WO 2006057006 A1 WO2006057006 A1 WO 2006057006A1 IN 2004000369 W IN2004000369 W IN 2004000369W WO 2006057006 A1 WO2006057006 A1 WO 2006057006A1
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WIPO (PCT)
Prior art keywords
potassium
composition
glass
phosphorous
sulfur
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PCT/IN2004/000369
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English (en)
Inventor
Nisha Biswas
Gour Krishna Das Mahapatra
Koushik Ghosh
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Council of Scientific and Industrial Research CSIR
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Council of Scientific and Industrial Research CSIR
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Priority to PCT/IN2004/000369 priority Critical patent/WO2006057006A1/fr
Publication of WO2006057006A1 publication Critical patent/WO2006057006A1/fr
Anticipated expiration legal-status Critical
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Classifications

    • C—CHEMISTRY; METALLURGY
    • C03—GLASS; MINERAL OR SLAG WOOL
    • C03C—CHEMICAL COMPOSITION OF GLASSES, GLAZES OR VITREOUS ENAMELS; SURFACE TREATMENT OF GLASS; SURFACE TREATMENT OF FIBRES OR FILAMENTS MADE FROM GLASS, MINERALS OR SLAGS; JOINING GLASS TO GLASS OR OTHER MATERIALS
    • C03C3/00—Glass compositions
    • C03C3/12—Silica-free oxide glass compositions
    • C03C3/16—Silica-free oxide glass compositions containing phosphorus
    • C03C3/17—Silica-free oxide glass compositions containing phosphorus containing aluminium or beryllium
    • C—CHEMISTRY; METALLURGY
    • C03—GLASS; MINERAL OR SLAG WOOL
    • C03C—CHEMICAL COMPOSITION OF GLASSES, GLAZES OR VITREOUS ENAMELS; SURFACE TREATMENT OF GLASS; SURFACE TREATMENT OF FIBRES OR FILAMENTS MADE FROM GLASS, MINERALS OR SLAGS; JOINING GLASS TO GLASS OR OTHER MATERIALS
    • C03C3/00—Glass compositions
    • C03C3/12—Silica-free oxide glass compositions
    • C03C3/16—Silica-free oxide glass compositions containing phosphorus

Definitions

  • the present invention relates to a composition useful for making slow release nitrogen free phosphorous, potassium and sulfur oxide glass and a process of making glass therefrom.
  • the process of the present invention provides high content phosphorous, potassium and sulfur glass capable of slow release of phosphorous, potassium and sulfur which particularly relates to the application of the glass as fertilizer for agricultural applications and for any other plant which requires phosphorous, potassium and sulfur as their elemental combinations.
  • These materials may have applications in such other fields where controlled release of phosphorous, potassium and sulfur is required such as fungicide, weedicide and for purposes other than agriculture.
  • fertilizer elements i.e., the elements that provide the nutrients required for the growth of crops, are divided into three categories; major elements, i.e.; nitrogen (N), Phosphorous(P) and Potassium(K); Secondary elements, i.e.; calcium(Ca), magnesium(Mg) and sulfur(S); and micronutrient elements, i.e., boron(B), cobalt(Co), copper (Cu), iron (Fe) , manganese(Mn), molybdenum(Mo) and Zinc (Zn).
  • major elements i.e.; nitrogen (N), Phosphorous(P) and Potassium(K)
  • Secondary elements i.e.; calcium(Ca), magnesium(Mg) and sulfur(S)
  • micronutrient elements i.e., boron(B), cobalt(Co), copper (Cu), iron (Fe) , manganese(Mn), molybdenum(Mo) and Zinc (Zn).
  • Sulfur is
  • a fertilizer that does not have any provision for obtaining controlled release of nutrients is liable to a number of disadvantages.
  • dry soil the plants are liable to damage by excessive nutrient concentrations, while in wet conditions the nutrients are liable to be wasted as a result of being removed from the region of soil.
  • leaching is liable to produce pollution to adjacent water bodies.
  • the present invention relates to the compositions, which are soluble in water or other polar solvent.
  • the process of present invention provides phosphorous, potassium and sulfur which particularly relates to the application of glass as fertilizer for agricultural applications and for any other plant which requires phosphorous, potassium and sulfur as the constituents of their elemental combination.
  • the material may have applications in such other field where controlled release of phosphorous, potassium and sulfur is required such as fungicide, pesticide, and weedicide and for purpose other than agriculture.
  • the principal object of the present invention is to provide novel glass compositions and more particularly, glass compositions that are adapted to provide major nutrient elements except nitrogen.
  • a glass for this purpose.
  • the solubility of glass in water should be relatively small in order to prevent them from being rendered unfavorable to the plant and soil through chemical reaction in the soil.
  • the solubility cannot be so small that the rate of release of the nutrients from the glass is inadequate for plant growth.
  • the glass must be non-toxic in high concentrations to plants or seeds, so that large amounts of the glass can be applied at one time to furnish an ample supply of the nutrient in the soil over an extended period of time.
  • the present invention is based on a glass composition of phosphorous pent -oxide and sulfur trioxide, which constitute the glass forming oxides.
  • the composition also contains glass-modifying oxides, in particular alkali oxide such as potassium oxide, together with an oxide of one or more metals of group II and group III of periodic table such as calcium oxide or aluminum oxide.
  • Alkali metal oxides have the effect of increasing the water solubility of the glass while the group II and group III oxides reduces the solubility.
  • the solubility rate may be adjusted to a desired value.
  • Phosphorous is a beautiful plant nutrient. It is involved in a wide range of plant process, starting from root development, photosynthesis, genetic transfer, cell division, crop maturity to improvement in plant disease resistance, crop quality and water use efficiency. Phosphorus after its application in soil is either removed by crop or gets converted into various insoluble forms (iron and aluminum phosphate in acid soil and calcium phosphate in alkaline soil) and gets fixed in soil clay or organic matter.
  • Potassium is another very important plant nutrient and is involved in root growth, photosynthesis, enzyme activation, turgor maintenance and reducing water losses and wilting, crop disease resistance, transpiration reduction, increase in protein content and enhancement of translocation of sugar and starch, thus improving grain and fodder quality.
  • Potassium is most abundant plant nutrient in soil, but is more mobile than phosphorous and is susceptible to loss by leaching, run off and erosion. Which along with phosphorous and nitrogen increases eutrophication of water bodies.
  • Murate of potash, sulfate of potash and NPK complexes are commonly used as potassium fertilizer. They are highly soluble and migrate from one place to another along with soil water.
  • Sulfur in soil is gradually reducing and around 50% of soil is found sulfur deficient. Therefore along with nitrogen, phosphorous and potassium, sulfur is considered as the fourth major nutrient required for plant growth, development and yield. Strong metabolic coupling between sulfur and nitrogen assimilation, deficiency of sulfur limits nitrogen utilization efficiency of plant and thus affecting plant growth, development and yield. Sulfur plays a significant role in all stages of plant development. It increases photosynthesis rate, chlorophyll formation, amino-acid and protein synthesis, activates enzymes, helps in vitamin formations, winter hardening etc.
  • Gypsum single- super phosphate and iron pyrites are the conventional sources of sulfur fertilizer of which gypsum is widely used to provide necessary sulfur to the plant but due to its high solubility in stagnant water large part of sulfate radicals derived from it percolates in the underground water damaging its quality. Repeated application of gypsum to the soil enhances calcium load on the soil.
  • a much more successful technique resides in preparing phosphorus - potassium - sulfur containing glass which is added directly to the soil.
  • small amount of phosphate, potassium and sulfate radicals are made available in the immediate vicinity of the seeds and plant roots.
  • solubility of the glass in water should be relatively small in order to prevent a quick release of nutrient elements and also to prevent them from being rendered unsuitable to the plants through chemical reaction in the soil.
  • the solubility should not be so small that the rate of release of nutrients from the glass is inadequate for plant growth.
  • the glass must not contain any such element that is harmful to the plant and its growth.
  • the glass composition soil condition can be altered locally, in particular in an alkaline soil, which is generally regarded as being difficult form to supply essential nutrients, to less alkaline or even acidic micro- environment around the roots of plants or around seeds.
  • Sulfate - phosphate glasses are made of highly correlated regions known as clusters, which are held together by connective tissue material. Two types of clusters - sulphate rich and phosphate rich clusters interconnected by the tissue of average composition exist in these glasses. Sulfate and phosphate rich clusters can also be of two types: clusters rich in potassium or calcium ions. Sulfate rich cluster is made of random close packing of sulfate spheres wherein potassium ion is enclosed in tetrahedral void created by four large sulfate ion spheres in contact with each other, but the spheres are oriented in such a way that the central hole can accommodate a K ion in a virtual dodecahedron of oxygen ions.
  • the calcium rich sulfate cluster because of the high field strength of calcium ions, draw the ions closer and hence oxygen of different sulfate ions make more contacts with each other than to those with K + ions.
  • the spheres of sulfate ions are so drawn by calcium ions that they overlap each other and no sulfate ion can be turned without disturbing the other sulfate ions - a kind of "interlocking" of sulfate ions occurs.
  • the structure of phosphate rich region can be explained by the cross-linking between phosphate tetrahedra where the addition of alkali creates more non-bridging oxygen and the cross-linking is more effectively done by calcium ions than by potassium ions.
  • the novelty of the process of the present invention lies in the fact that phosphorous, potassium and sulfur will be released slowly into the soil in presence of water as and when required at the same time maintaining the acidity of the soil as the alkali metals are not available to the reacting system in the present material. Additionally the glasses do not contain harmful elements to the plants like Na 2 O, Li 2 O and ZnO.
  • the inventive step lies in the incorporation of P 2 O 5 , SO 3 , K 2 O, CaO and Al 2 O 3 in a novel glass composition having high weight percent of P 2 O 5 , K 2 O and SO 3 .
  • the present day method of making glasses for agricultural application is essentially phosphate glasses containing micronutrient elements in oxide form, such as zinc, copper, magnesium, molybdenum or boron oxide or mixtures thereof; phosphate- borate glass; phosphate glass containing potassium, magnesium, calcium along with trace elements such as iron, boron, magnesium, sulfur, vanadium, copper, cobalt, zinc and molybdenum (trace elements not more than 1 wt % in aggregate); nitrogen containing slow release glass fertilizer prepared by co-melting phosphorous oxynitride and phosphorous pentoxide along with an oxide of a element of Group II or III of the periodic table; copper phosphate glass formed from cupric oxide and phosphorous pentoxide glass which also incorporates one or more glass modifying oxide such as alkali metal oxide and alumina to control solubility; alkali metal oxide - phosphorous pentoxide glass along with transition metal oxide; glass matrix comprising P 2 O 5 as partial and / or full replacement of SiO
  • the present day method of making sulfate-phosphate glasses essentially consists of mixtures of K 2 SO 4 , ZnSO 4 and NaPO 3 ; ZnSO 4 , KPO 3 and NaPO 3 ; K 2 SO 4 , Na 2 SO 4 and NaPO 3 ; Na 2 SO 4 , ZnSO 4 and NaPO 3 ; K 2 SO 4 , Li 2 CO 3 , NH 4 H 2 PO 4 .
  • V.L.Mamoshin V.G.Arkhipov, P.I.Bular, L.V.Ivanova and OJ.Pupkova
  • R 2 SO 4 (RHSO 4 ) - ZnSO 4 - NaPO 3 (P 2 O 5 ), R Li, Na, K, Fiz. Khim. Stekla 16,860-866(1990);
  • V. L. Mamoshin " Formation of low melting glasses in ZnSO 4 - KPO 3 - NaPO 3 and Li 2 SO 4 - Na 2 SO 4 - K 2 SO 4 - NaPO 3 system", Glass and Ceramics 53, 166-168 (1996); M. Ganguli & K. J. Rao, " Studies of ternary Li 2 SO 4 - Li 2 O - P 2 O 5 Glasses", J. Non. Cryst. Solids, 243, 251-267(1999).
  • temperature and duration of glass melting is very critical. Slight increase in melting temperature and / or duration enhances sulfur and phosphorous loss by evolution of SO 2 gas which carries with it a significant amount of P 2 O 5 which melts at much lower temperature and melting reactions starts along with localized reaction with other components that form the said glass and thereby reducing the losses in SO 3 and P 2 O 5 .
  • Inventive step in the present invention lies in obtaining the required composition of glass with much ease and not so much critically dependent on melting temperature and duration as in the stated invention. The main drawbacks of the above processes are:
  • the glass contains alkali like Na 2 O, Li 2 O that are harmful to the plants and increases soil alkalinity that hinders absorption of other nutrients by the plants. 3.
  • the glass contains high percentage of ZnO, which is toxic to the plants.
  • the main object of the present invention is to provide a composition useful for making slow release nitrogen free phosphorous, potassium and sulfur oxide glass and a process of glass therefrom, which does not contain alkali like Na 2 O, Li 2 O and ZnO etc that are harmful to plants.
  • Another object of the present invention is to increase phosphate, potassium and sulfur content of the prepared glass.
  • Another object of the present invention is to provide nutrients like phosphorous, potassium and sulfur to the crop in a slow and controlled manner.
  • Still another object of the present invention is to reduce the phosphorous, potassium and sulfur release rate when leached.
  • Another object of the present invention is to reduce calcium oxide content in the glass to reduce calcium load on the soil.
  • Still another object of the present invention is to provide phosphorous, potassium and sulfur releasing glass which minimize pollution to underground water by reducing leaching rate of the constituent elements.
  • Yet another object of the present invention is to maintain acidity of the soil.
  • Still another object of the present invention is to provide essential micronutrients like zinc, boron, cobalt, iron, copper, manganese and molybdenum with low release rate in leached solution.
  • the present invention provides a composition useful for making slow release nitrogen free phosphorous, potassium and sulfur oxide glass which comprises Constituent as oxides Amount of oxide in wt.%
  • the source OfP 2 O 5 in the composition may be provided as chemical compounds such as ortho-phosphoric acid, ammonium di- hydrogen orthophosphate, di-ammonium hydrogen orthophosphate, potassium di- hydrogen phosphate, tri- calcium phosphate, aluminum phosphate or the mixtures thereof.
  • the source of SO 3 in the composition may be provided as chemical compounds such as potassium sulfate, potassium di- sulfate, potassium per-sulfate, potassium bi-sulfate, calcium sulfate, ammonium sulfate, aluminum sulfate or the mixtures thereof.
  • the source of K 2 O in the composition may be provided as chemical compounds such as potassium sulfate, potassium di-sulfate, potassium per-sulfate, potassium bi-sulfate, potassium carbonate or the mixtures thereof.
  • the source of CaO in the composition may be provided as chemical compounds such as tri-calcium phosphate, calcium sulfate, calcium carbonate, gypsum or the mixtures thereof.
  • the source of Al 2 O 3 in the composition may be provided as chemical compounds such as aluminum sulfate, aluminum orthophosphate, alumina or the mixtures thereof.
  • the melting may be effected for a time period in the range of 30 to 70 minutes.
  • composition of the present invention is not a mere admixture but a mixture having properties, which are distinct from the mere aggregation of the properties of the individual constituents.
  • the present invention relates to a composition useful for making slow release nitrogen free phosphorous, potassium and sulfur oxide glass and a process of making glass therefrom which comprises proportioning and thorough mixing of the above composition, melting the composition at a temperature in the range of 800-
  • the glass was made by thoroughly mixing 55.8 g of ammonium dihydrogen orthophosphate, 12.6 g of potassium sulphate, 33.4 g of gypsum , 26.8 g of potassium carbonate and 15.2 g of aluminium sulphate and heating the mixture at 1000 0 C for 30 minutes and then by quenching the melt.
  • the glass so obtained was checked for its solubility rate by treating 1.0 gm of glass powder of size 0.6 to 1.0 mm with 50 ml of distilled water for 24 hrs. The solution is then filtered. The undissolved glass was weighed after drying the residue to the constant weight. Solubility of glass is 5.7 %.
  • Example 1 The glass given in Example 1 is found suitable for food crops. There is 20-30% increase in grain yield in the case of wheat with reduced application of 30-40% K20, 70-80% CaO & 60-70% SO3.
  • Example 2 The glass was prepared by thoroughly mixing 34.8 g potassium sulphate, 34.3 g of gypsum, 18.0 g of aluminium sulfate and 46.0 g ammonium dihydrogen orthophosphate and heating the mixture at 85O 0 C for 40 minutes and then raising the temperature to 95O 0 C and kept for 10 minutes and then quenching the melt.
  • the glass so obtained was checked for its solubility by treating 1.0 gm of glass powder of size 0.6 to 1.0 mm with 50 ml of distilled water for 24 hrs. The solution is then filtered. The undissolved glass was weighed after drying the residue to the constant weight. Solubility of glass is 2.8 %.
  • the glass was made by thoroughly mixing 26.3 g potassium disulphate, 35.6 g gypsum, 24.2 g ammonium dihydrogen orthophosphate, 28.0 g potassium hydrogen phosphate and 11.7 g aluminium sulfate and heating the mixture at 95O 0 C for 20 minutes followed by heating to 1050 0 C for another 15 minutes and then by quenching the melt.
  • the glass so obtained was checked for its solubility by treating 1.0 gm of glass powder of size 0.6 to 1.0 mm with 50 ml of distilled water for 24 hrs. The solution is then filtered. The undissolved glass was weighed after drying the residue to the constant weight. Solubility of glass is 5.0 %.
  • Another way of making the glass was by melting a homogeneous mixture of 18. Ig of calcium carbonate, 55.4g of potassium disulphate, 46.5g of ammonium dihydrogen orthophosphate and 11.6 g of aluminium sulfate at 1000 0 C for 30 minutes and then by quenching the melt. The glass so obtained was checked for its solubility by treating
  • Another way of making the glass was by melting a homogeneous mixture of 31.8g of gypsum, 46.8g of potassium disulphate, 34.2g of ammonium dihydrogen orthophosphate and 10.3 g of aluminium sulfate at 95O 0 C for 30 minutes and then by quenching the melt.
  • the glass so obtained was checked for its solubility rate by treating 1.0 gm of glass powder of size 0.6 to 1.0 mm with 50 ml of distilled water for 24 hrs. The solution is then filtered. The undissolved glass was weighed after drying the residue to the constant weight. Solubility of glass is 53.0 %.
  • Another way of making the glass was by melting a homogeneous mixture of 37.6g of gypsum, 40.7g of potassium sulphate, 48.4g of ammonium dihydrogen orthophosphate and 1.2 g of aluminium phosphate charging at 600 0 C and kept for 30 minutes and then raising the temperature to 95O 0 C and keeping for 10 minutes and then by quenching the melt.
  • the glass so obtained was checked for its solubility rate by treating 1.0 gm of glass powder of size 0.6 to 1.0 mm with 50 ml of distilled water for 24 hrs. The solution is then filtered. The undissolved glass was weighed after drying the residue to the constant weight. Solubility of glass is 9.0%.
  • Example 6 glass is tested for oilseeds like mustard and groundnut.
  • the increase in seed yield is 10-20% in mustard and 5-15% in the case of groundnut.
  • Fertilizer application reduces to 30-40% P2O5, 45-60% CaO & 20-40% SO3 in mustard and 60-70% P2O5, 3-7% K2O, 65-75% Cao & 45-55% SO3 in the case of groundnut.

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  • Chemical & Material Sciences (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • General Chemical & Material Sciences (AREA)
  • Geochemistry & Mineralogy (AREA)
  • Materials Engineering (AREA)
  • Organic Chemistry (AREA)
  • Glass Compositions (AREA)
  • Fertilizers (AREA)

Abstract

Selon l'invention, le phosphore, le potassium et le soufre jouent un rôle important dans la croissance et le développement de plantes et de matière organique du sol en raison de leur implication dans plusieurs voies métaboliques. Une déficience de ces éléments restreint la croissance des plantes et le rendement des cultures. Le phosphate de di-ammonium, le murate de potasse et le gypse sont les engrais classiques à base de phosphore, potassium et souffre respectivement. En raison de leur solubilité élevée et de l'augmentation de la charge calcique sur le sol due à l'application de gypse, ceux-ci endommagent la qualité du sol et polluent les eaux de surface et souterraines. La technique la plus efficace est l'application de verre de phosphore-potassium-soufre pouvant être ajouté directement dans le sol. L'invention concerne principalement une formulation et un procédé de fabrication d'une composition de verre renfermant une concentration élevée de phosphore, potassium et soufre exempte d'alcalin tel que Na20, Li2O et ZnO, qui sont toxiques pour les plantes. De tels verres sont capables libérer lentement du phosphore, du potassium et du soufre nécessaires dans le domaine de l'agriculture, de fongicide, de pesticide et de désherbant etc. L'invention concerne également l'optimisation de contenu nutritif, la réduction de la charge calcique sur le sol, la minimisation de la pollution des eaux de surface et souterraines et de l'entretien d'environnement acide à proximité des racines des plantes dans le sol.
PCT/IN2004/000369 2004-11-29 2004-11-29 Composition utile dans la fabrication de verre en oxyde de phosphore, potassium et souffre exempt d'azote et a liberation lente et procede de fabrication de verre a partir de celle-ci Ceased WO2006057006A1 (fr)

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PCT/IN2004/000369 WO2006057006A1 (fr) 2004-11-29 2004-11-29 Composition utile dans la fabrication de verre en oxyde de phosphore, potassium et souffre exempt d'azote et a liberation lente et procede de fabrication de verre a partir de celle-ci

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PCT/IN2004/000369 WO2006057006A1 (fr) 2004-11-29 2004-11-29 Composition utile dans la fabrication de verre en oxyde de phosphore, potassium et souffre exempt d'azote et a liberation lente et procede de fabrication de verre a partir de celle-ci

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Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN104550226A (zh) * 2014-12-29 2015-04-29 黑龙江盛瑞康生物科技开发有限公司 一种用于促进水稻和泥鳅共生的复合微生物菌剂

Citations (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US4334908A (en) * 1978-09-29 1982-06-15 Bfg Glassgroup Vitreous fertilizer compositions
CH639635A5 (en) * 1978-01-01 1983-11-30 Itt Biologically active composition from which the active substance is released slowly
SU1742276A1 (ru) * 1987-11-04 1992-06-23 Самаркандский сельскохозяйственный институт им.В.В.Куйбышева Стеклообразное гранулированное удобрение пролонгированного действи на основе фосфатного стекла
EP0648713A1 (fr) * 1993-10-18 1995-04-19 Corning Incorporated Verres de sulfophosphate de zinc
EP1088806A1 (fr) * 1999-09-30 2001-04-04 Giuseppe Macchioni Mélange d'engrais à matrice de verre
US6217629B1 (en) * 1999-04-15 2001-04-17 Rutgers, The State University Of New Jersey Phosphate sulfur fertilizer particles and methods for making same

Patent Citations (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CH639635A5 (en) * 1978-01-01 1983-11-30 Itt Biologically active composition from which the active substance is released slowly
US4334908A (en) * 1978-09-29 1982-06-15 Bfg Glassgroup Vitreous fertilizer compositions
SU1742276A1 (ru) * 1987-11-04 1992-06-23 Самаркандский сельскохозяйственный институт им.В.В.Куйбышева Стеклообразное гранулированное удобрение пролонгированного действи на основе фосфатного стекла
EP0648713A1 (fr) * 1993-10-18 1995-04-19 Corning Incorporated Verres de sulfophosphate de zinc
US6217629B1 (en) * 1999-04-15 2001-04-17 Rutgers, The State University Of New Jersey Phosphate sulfur fertilizer particles and methods for making same
EP1088806A1 (fr) * 1999-09-30 2001-04-04 Giuseppe Macchioni Mélange d'engrais à matrice de verre

Non-Patent Citations (1)

* Cited by examiner, † Cited by third party
Title
DATABASE WPI Section Ch Week 199324, Derwent World Patents Index; Class C04, AN 1993-195075, XP002346550 *

Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN104550226A (zh) * 2014-12-29 2015-04-29 黑龙江盛瑞康生物科技开发有限公司 一种用于促进水稻和泥鳅共生的复合微生物菌剂

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