CN105947993A - Method for improving bio-availability of sulfur by means of converting sulfur into polysulfide - Google Patents
Method for improving bio-availability of sulfur by means of converting sulfur into polysulfide Download PDFInfo
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- CN105947993A CN105947993A CN201610377070.8A CN201610377070A CN105947993A CN 105947993 A CN105947993 A CN 105947993A CN 201610377070 A CN201610377070 A CN 201610377070A CN 105947993 A CN105947993 A CN 105947993A
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Abstract
The invention belongs to the field of wastewater treatment, and provides a method for improving bio-availability of sulfur by means of converting the sulfur into polysulfide. The method is characterized in that solid elemental sulfur in an aqueous solution is quickly dissolved and is converted into the polysulfide under normal temperature and normal pressure by means of controlling a pH value and an initial HS<-> concentration, so that the bio-availability of the sulfur is improved. The method disclosed by the invention has the advantages that a synthesis process of dissolved zero-valent sulfur is explained, the biological reduction rate of the elemental sulfur is improved by the dissolved zero-valent sulfur, meanwhile the sulfide production rate is also accelerated, and the synthesis rate of the dissolved zero-valent sulfur is increased with the increasing of the biological reduction rate of the elemental sulfur, therefore a positive feedback reaction among the biological reduction rate of the elemental sulfur, the sulfide production rate and the dissolved zero-valent sulfur is formed under the conditions limited by the method.
Description
Technical field
The invention belongs to field of waste water treatment, particularly relate to a kind of make sulfur turn to polysulfide sulfide with the method improving its bioavailability.
Background technology
Elemental sulfur is the material being widely present in nature, it has the feature of oxidisability, reproducibility concurrently, make it can be used as reducing agent or oxidant at sewage disposal process, the autotrophic denitrification denitrogenation of the leanest nutrient sewage, the biological treatment of heavy metal-containing waste water, drinking water and subsoil water denitrogenation, it might even be possible to realize the municipal sewage treatment of low mud production rate.
Under anaerobic condition, microorganism may utilize Organic substance or H2As electron donor dissimilatory reduction elemental sulfur sulphidisation, (sulfide has S in aqueous phase2-、HS-And H2Tri-kinds of forms of S).Elemental sulfur under naturalness exists with chain and annular form, and most stable of under normal temperature and pressure is rhombic sulfur α-sulfur (orthorhombic α-sulfur) and monoclinic sulphur β-sulfur (monoclinic β-sulfur).The two is the most all circulus, and the extremely low (19 ± 6nmolL of water solublity-1), the bioavailability of elemental sulfur is the highest the most in theory.Elemental sulfur wants by microorganism fast restore, and circulus and the raising autolysis of opening self are important premises.Polysulfide sulfide (or claim polysulfide, polysuldie, it is called for short PS) it is dissolubility zeroth order sulfur transfer vector main in water, by the transfer of PS, water-fast solid elemental sulfur can be utilized by microorganism in split-up to aqueous phase.During the biological reducing of elemental sulfur, solid elemental sulfur changes into dissolubility zeroth order sulfur by PS, its water solubility (19 ± 6nmol 1-1[10]) obtaining great lifting, this is more beneficial for the mass transfer (Mass transfer) of reduction reaction, and PS here serves an effect converting transport.
The fast restore of elemental sulfur, is affected by several aspects:
1) sulfide: HS-It is the raw material of the thio one-tenth of dissolubility zeroth order, simultaneously in sulfur alienation biological reducing, H2The toxicity of S also can produce suppression to microorganism；
2)HS-: elemental sulfur crystal unlinks the catenulate PS of shape, needs HS-Participation, HS-The size of concentration would necessarily affect the synthesis of dissolubility zeroth order sulfur and the alienation biological reducing of elemental sulfur；
3) pH: sulphion (monosulfide) and (HS-) ionization equilibrium receive pH and strongly affect, the synthetic reaction of dissolubility zeroth order sulfur the most just has certain relation with pH.
Summary of the invention
Present invention aim to overcome that the deficiencies in the prior art, a kind of technical method is provided, the method is by control ph and reaction premature cure substrate concentration, the solid elemental sulfur in aqueous phase is made to be rapidly converted into polysulfide sulfide, its bioavailability is improved with this, the method accelerates elemental sulfur rate of reduction, increases the motive force of sulfur reduction process, improves mass transfer effect and the bioavailability of elemental sulfur.
The present invention solves it and technical problem is that and take techniques below scheme to realize:
Sulfur is made to be converted into polysulfide sulfide with the method improving its bioavailability, it is characterised in that: at normal temperatures and pressures, make the solid elemental sulfur in aqueous solution by control ph and initial HS-Concentration, rapid solution is also converted into polysulfide sulfide, with the method improving its bioavailability.
Further, zeroth order sulfur reduction reaction, zeroth order sulfur oxidation reaction or the zeroth order sulfur dismutation reaction under described method can be used for (including but are not limited to) biocatalysis.
Further, described zeroth order sulfur reduction reaction refers under anaerobic, Organic substance or H2As electron donor, making the zeroth order sulfur such as elemental sulfur, polymeric form sulfur be converted into the process of sulphidisation, described electron donor includes that glucose, lactate, acetate or formates, described sulfide have S in aqueous phase2-、HS-And H2Tri-kinds of forms of S；Described zeroth order sulfur oxidation reaction refers under aerobic or anoxia condition, with nitrate, nitrite or oxygen as electron acceptor, makes zeroth order sulfur be converted into the sulfate of high-valence state or sulphite or the process of thiosulfate；Described zeroth order sulfur dismutation reaction refers to generate the process of sulfide and thiosulfate or sulfate the most simultaneously.
Further, described polysulfide sulfide is made up of at least one zeroth order sulphur atom and at least one sulphion, and described sulphion includes S2 2-、S3 2-、S4 2-、S5 2-、S6 2-、S7 2-、S8 2-、S9 2-、S10 2-And S11 2-。
Further, described bioavailability refers in the aqueous solution or moist environment of normal temperature and pressure, and described elemental sulfur is utilized by microorganisms such as sulfur reducing bacteria or ancient bacterium, sulfur-oxidizing bacteria or ancient bacterium to promote growth of microorganism, and the characteristic of decomposition and inversion elemental sulfur.
Further; described elemental sulfur be exist in solid form and valence state be the elementary sulfur of 0; its form existed is drusen or Sublimed Sulfur or colloid sulfur or biological sulfur or polymeric form sulfur, and described elemental sulfur chemical constitution at normal temperatures and pressures is rhombic sulfur α-sulfur or monoclinic sulphur β-sulfur.
Further, described polysulfide sulfide is dissolubility zeroth order sulfur transfer vector in water, by the transfer of polysulfide sulfide, water-fast solid elemental sulfur can split-up to utilizing in aqueous phase and by microorganism, accelerate the speed that elemental sulfur is utilized.
Further, described pH value optimum range is 6.0～9.5, described initial HS-Optimum concentration range is 10～500mg/L, and described room temperature is about 5 DEG C-50 DEG C, and described normal pressure is about 1.01 × 105Pa ± 20%.
The principle of the present invention includes herein below:
Currently known elemental sulfur also original route has two kinds, i.e. directly utilizes and indirect utilization elemental sulfur.
Elemental sulfur directly utilizes with ancient bacterium Acidianusambivalens as representative, and it can use H2Do electron donor and directly utilize solid elemental sulfur, but as it has been described above, be limited to the low solubility of elemental sulfur, be reduced directly inefficient.
Indirect reduction elemental sulfur, refers to that solid sulfur (mainly S8) is first converted into water solublity zeroth order sulfur, is utilized by microorganism.Among these, and polysulfide sulfide (or claim polysulfide, Polysulfide, it is called for short PS) it is topmost dissolubility zeroth order sulfur-donor.Wollinelasuccidogenus can produce PS reductase, directly uses PS to grow as electron acceptor, and aoxidizes H2.PS can be formed, the most visual indirect reduction for elemental sulfur owing to elemental sulfur is combined with HS-.
Except PS, colloid sulfur and polythionate (polythionate) are also the existing forms of possible dissolubility zeroth order sulfur.But colloid sulfur, polythionate only occur in sulfur aoxidizes.If Acidithiobacillusthiooxidans and Acidithiobacillusferroxidans oxidation S0 is sulphuric acidDuring, polythionate can be generated.Polythionate is unstable under conditions of with the presence of sulfide.Therefore, in the sulfur reduction process of lower oxidation reduction potential, PS is electron acceptor only possible in elemental sulfur indirect utilization approach.
The invention has the beneficial effects as follows:
The present invention explains the building-up process of dissolubility zeroth order sulfur, it is found that dissolubility zeroth order sulfur improves elemental sulfur biological reducing speed, this accelerates again the speed that sulfide generates simultaneously, it is found that the raising of elemental sulfur biological reducing speed adds dissolubility zeroth order sulfur synthesis rate subsequently, it was found that in this patent qualifications, between speed and dissolubility zeroth order sulfur three that elemental sulfur biological reducing speed, sulfide generate, form a positive feedback reaction.
Accompanying drawing explanation
Below in conjunction with accompanying drawing, the present invention is further described:
Fig. 1 is the synthetic effect schematic diagram of dissolubility zeroth order sulfur in the present invention；
Fig. 2 is the dissolubility zeroth order sulfur impact (little figure: averagely advancing the speed of front 3h sulfide concentration) on sulfur rate of reduction in the present invention；
Fig. 3 is the concentration change schematic diagram of dissolubility zeroth order sulfur in the present invention；
Fig. 4 is at the sulfide concentration result of variations schematic diagram controlled and under the conditions of non-controlling in the present invention.
Detailed description of the invention
Below in conjunction with detailed description of the invention, the present invention is further described:
With reference to Fig. 1～4, the present invention disclose and a kind of makes sulfur be converted into polysulfide sulfide with the method improving its bioavailability, it is characterised in that: at normal temperatures and pressures, make the solid elemental sulfur in aqueous solution pass through control ph and initial HS-Concentration, rapid solution is also converted into polysulfide sulfide, with the method improving its bioavailability, described method can be used for the zeroth order sulfur reduction reaction under (including but are not limited to) biocatalysis, zeroth order sulfur oxidation reaction or zeroth order sulfur dismutation reaction.
Sulfur is made to be converted into polysulfide sulfide to improve in the method for its bioavailability above-mentioned, it should be pointed out that described zeroth order sulfur reduction reaction refers under anaerobic, Organic substance or H2As electron donor, making the zeroth order sulfur such as elemental sulfur, polymeric form sulfur be converted into the process of sulphidisation, described electron donor includes that glucose, lactate, acetate or formates, described sulfide have S in aqueous phase2-、HS-And H2Tri-kinds of forms of S；Described zeroth order sulfur oxidation reaction refers under aerobic or anoxia condition, with nitrate, nitrite or oxygen as electron acceptor, makes zeroth order sulfur be converted into the sulfate of high-valence state or sulphite or the process of thiosulfate；Described zeroth order sulfur dismutation reaction refers to generate the process of sulfide and thiosulfate or sulfate the most simultaneously.
Sulfur is made to be converted into polysulfide sulfide to improve in the method for its bioavailability above-mentioned, it should be pointed out that described polysulfide sulfide is made up of at least one zeroth order sulphur atom and at least one sulphion, and described sulphion includes S2 2-、S3 2-、S4 2-、S5 2-、S6 2-、S7 2-、S8 2-、S9 2-、S10 2-And S11 2-。
Sulfur is made to be converted into polysulfide sulfide to improve in the method for its bioavailability above-mentioned, it is to be noted, described bioavailability refers in the aqueous solution or moist environment of normal temperature and pressure, described elemental sulfur is by sulfur reducing bacteria or ancient bacterium, the microorganisms such as sulfur-oxidizing bacteria or ancient bacterium utilize to promote growth of microorganism, and the characteristic of decomposition and inversion elemental sulfur, described elemental sulfur be exist in solid form and valence state be the elementary sulfur of 0, its form existed is drusen or Sublimed Sulfur or colloid sulfur or biological sulfur or polymeric form sulfur, described elemental sulfur chemical constitution at normal temperatures and pressures is rhombic sulfur α-sulfur or monoclinic sulphur β-sulfur.
Sulfur is made to be converted into polysulfide sulfide to improve in the method for its bioavailability above-mentioned, it is to be noted, described polysulfide sulfide is dissolubility zeroth order sulfur transfer vector in water, transfer by polysulfide sulfide, water-fast solid elemental sulfur can split-up to utilizing in aqueous phase and by microorganism, accelerate the speed that elemental sulfur is utilized.
Sulfur is made to be converted into polysulfide sulfide to improve in the method for its bioavailability above-mentioned, it should be pointed out that described pH value optimum range is 6.0～9.5, described initial HS-Optimum concentration range is 10～500mg/L, and described room temperature is about 5 DEG C-50 DEG C, and described normal pressure is about 1.01 × 105Pa ± 20%.
The synthesis of embodiment 1 dissolubility zeroth order sulfur
In the present embodiment, by arranging 6 200ml conical flasks, pH is respectively under the scope of 6～8.5, exploratory response equilibration time and the equilibrium concentration of dissolubility zeroth order sulfur.The synthesis of dissolubility zeroth order sulfur, is independent of the existence of microorganism, say, that simply by the presence of S0And HS-, PS under suitable pH, can be formed.
It is proportionate with sulfide concentration, pH with reference to Fig. 1, PS concentration.When pH is 8.5, needing 2.5h reaction to can be only achieved balance, now dissolubility zeroth order sulfur balance concentration is 135.00mg/L.But when pH is down to 6, reacting balance time is extremely short, dissolubility zeroth order sulfur is only 0.38mg/L, it is virtually impossible to synthesis.In figure, dissolubility zeroth order sulfur balance concentration and the relation of pH, be consistent with the theoretical calculation model of Wilfred E.Kleinian, under this explanation neutrality and slight alkali environment, and S0Easily and HS-In conjunction with, generate the PS being dissolved in water.
The impact that sulfur is reduced by embodiment 2 dissolubility zeroth order sulfur
In the present embodiment, by arranging 6 conical flasks (2.4L), premature cure substrate concentration 0～200mg/L, using glucose as carbon source, sludge concentration is 0.68gVSS/L, and elemental sulfur dosage is 5g/L, and initial pH utilizes HCL or NaOH regulation pH to optimum range 7.5.
In Fig. 2 and Fig. 3, reflect dissolubility zeroth order sulfur to the impact of sulfur rate of reduction and the concentration change of dissolubility zeroth order sulfur.
1). premature cure substrate concentration increases to 200mg/L from 0mg/L, and Initial Solubility zeroth order sulphur concentration is risen to 206.34mg/L by an extremely low value, which increases the motive force of sulfur reduction process.In front 3h, the sulfur reduction Mean Speed under different premature cure substrate concentrations presents increasing with a near-linear, and elemental sulfur biological reducing speed obtains the biggest lifting.At front 2h, dissolubility zeroth order sulfur is quickly consumed, and is always maintained at a stationary value afterwards, and this explanation PS consumption now has reached a dynamic equilibrium with synthesis, and its synthesis rate limits wear rate.It is to say, when design elemental sulfur biological reducing sewage treatment process or other related process, improve the synthesis rate of PS, the most just improve mass transfer effect and the bioavailability of elemental sulfur.
2). it is limited by the limited total amount of organic carbon (40mg/L) and H2The S inhibitory action to microorganism, adds variable concentrations sulfide during primary response, sulfur rate of reduction presents different situations, as described below.The sulfur rate of reduction of 200mg/L is in a high level all the time, but is but being gradually reduced.Along with the propelling of sulfur reduction, the sulfur rate of reduction of 0mg/L is from 4.24mg L-1h-1Rise to 34.36mg L-1h-1.The accumulation of sulfide increases the rate of reduction of elemental sulfur, this is because newly-generated HS-Attack S further0, this results in a positive feedback, constantly promote PS synthesis, the formation of dissolubility zeroth order sulfur and S0Dissimilatory reduction.
3). when premature cure substrate concentration is relatively low, along with S0Reduction process advances, and sulfide concentration gets a promotion, and this not only promotes the synthesis of PS, and accelerates the most again sulfur rate of reduction.Abundant, the H at neutral pH, electron donor2S concentration is the highest be not enough to embody toxicity under conditions of, above-mentioned response path is the process that a positive feedback is constantly accelerated.Under high concentration dosage, although sulfur rate of reduction the most constantly declines.By contrast, under low dosage, sulfide promotes sulfur reduction reaction in the early stage, but occurs in that decline the most respectively after 5h and 7h.
The control of embodiment 3 dissolubility zeroth order sulfur
With reference to Fig. 4, in the present embodiment, by arranging 3 conical flasks (2.4L), premature cure substrate concentration is all 0mg/L.Using glucose as carbon source (TOC=40mg/L), sludge concentration is 0.66gVSS/L, S0Dosage is 5g/L.First initial pH of conical flask utilizes HCL or NaOH to regulate to 7.5 (NC), second 12.48mMFe to be added2+(C1), the 3rd conical flask utilizes HCL to regulate pH to 6, and remains its pH constant (C2) in an experiment.
After precipitation falls PS and sulfide, microorganism will and S0Directly contact.S during 9h0Percent reduction, C1 is only the 2.5% of NC, and C2 does not has obvious sulfide to accumulate.After experiment terminates, the TOC of C1 and C2 does not has significant change, and during reaction, the dissolubility zeroth order sulfur of the two is also without being detected.And under the conditions of non-controlling, TOC clearance is 65.70%, dissolubility zeroth order sulfur mean concentration is 7.07mg/L.By PS as transport agent, solid S0Being converted into dissolubility zeroth order sulfur, sulfur rate of reduction is 40 times under control condition.It is reduction mechanism main in sulfur reduction that PS converts transport sulfur source as intermediate.
The present invention has been described in detail by above example, but described content is only presently preferred embodiments of the present invention, it is impossible to be considered the practical range for limiting the present invention.All impartial changes made according to the present patent application scope and improvement etc., within all should still belonging to the patent covering scope of the present invention.
Claims (10)
1. make sulfur be converted into polysulfide sulfide with the method improving its bioavailability, it is characterised in that: at normal temperatures and pressures,
Make the solid elemental sulfur in aqueous solution by control ph and initial HS-Concentration, rapid solution is also converted into polysulfide sulfide, with
The method improving its bioavailability.
The most according to claim 1 making sulfur be converted into polysulfide sulfide with the method improving its bioavailability, it is special
Levy and be: zeroth order sulfur reduction reaction that described method can be used under (including but are not limited to) biocatalysis, zeroth order sulfur oxygen
Change reaction or zeroth order sulfur dismutation reaction.
The most according to claim 2 making sulfur be converted into polysulfide sulfide with the method improving its bioavailability, it is special
Levy and be: described zeroth order sulfur reduction reaction refers under anaerobic, Organic substance or H2As electron donor, make elemental sulfur, gather
Closing the zeroth order sulfur such as state sulfur and be converted into the process of sulphidisation, described electron donor includes glucose, lactate, acetate or formic acid
Salt, described sulfide has S in aqueous phase2-、HS-And H2Tri-kinds of forms of S.
The most according to claim 2 making sulfur be converted into polysulfide sulfide with the method improving its bioavailability, it is special
Levy and be: described zeroth order sulfur oxidation reaction refers to, under aerobic or anoxia condition, be subject to for electronics with nitrate, nitrite or oxygen
Body, makes zeroth order sulfur be converted into the sulfate of high-valence state or sulphite or the process of thiosulfate.
The most according to claim 2 making sulfur be converted into polysulfide sulfide with the method improving its bioavailability, it is special
Levy and be: described zeroth order sulfur dismutation reaction refers to generate the mistake of sulfide and thiosulfate or sulfate the most simultaneously
Journey.
The most according to claim 1 making sulfur be converted into polysulfide sulfide with the method improving its bioavailability, it is special
Levy and be: described polysulfide sulfide is made up of at least one zeroth order sulphur atom and at least one sulphion, and described sulphion includes S2 2-、
S3 2-、S4 2-、S5 2-、S6 2-、S7 2-、S8 2-、S9 2-、S10 2-And S11 2-。
The most according to claim 1 making sulfur be converted into polysulfide sulfide with the method improving its bioavailability, it is special
Levying and be: described bioavailability refers in the aqueous solution or moist environment of normal temperature and pressure, described elemental sulfur is thin by sulfur reduction
The microorganisms such as bacterium or ancient bacterium, sulfur-oxidizing bacteria or ancient bacterium utilize to promote growth of microorganism, and the characteristic of decomposition and inversion elemental sulfur.
The most according to claim 1 making sulfur be converted into polysulfide sulfide with the method improving its bioavailability, it is special
Levy and be: described elemental sulfur be exist in solid form and valence state be the elementary sulfur of 0, its exist form be drusen or
Sublimed Sulfur or colloid sulfur or biological sulfur or polymeric form sulfur, described elemental sulfur chemical constitution at normal temperatures and pressures is rhombic sulfur α-sulfur
Or monoclinic sulphur β-sulfur.
The most according to claim 1 making sulfur be converted into polysulfide sulfide with the method improving its bioavailability, it is special
Levy and be: described polysulfide sulfide is dissolubility zeroth order sulfur transfer vector in water, by the transfer of polysulfide sulfide, water insoluble
Solid elemental sulfur can split-up to utilizing in aqueous phase and by microorganism, accelerate the speed that elemental sulfur is utilized.
The most according to claim 1 sulfur is made to be converted into polysulfide sulfide with the method improving its bioavailability, its
It is characterised by: described pH value optimum range is 6.0～9.5, described initial HS-Optimum concentration range is 10～500mg/L, described
Room temperature is about 5 DEG C-50 DEG C, and described normal pressure is about 1.01 × 105Pa ± 20%.
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Cited By (3)
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| CN109052641A (en) * | 2018-09-05 | 2018-12-21 | 南京大学 | A kind of coupling filler autotrophic denitrification biofilter and application |
| CN114369625A (en) * | 2022-01-19 | 2022-04-19 | 中山大学 | Method for producing sulfur by artificially enhancing elemental sulfur biological disproportionation and method for biologically removing heavy metal in wastewater by using same |
| CN114409096A (en) * | 2022-01-19 | 2022-04-29 | 中山大学 | Method for realizing efficient deep denitrification of sewage by coupling elemental sulfur disproportionation and sulfur autotrophic denitrification |
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| CN109052641A (en) * | 2018-09-05 | 2018-12-21 | 南京大学 | A kind of coupling filler autotrophic denitrification biofilter and application |
| CN114369625A (en) * | 2022-01-19 | 2022-04-19 | 中山大学 | Method for producing sulfur by artificially enhancing elemental sulfur biological disproportionation and method for biologically removing heavy metal in wastewater by using same |
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