CN103406105B - A kind of modified abandoned tealeaf residue adsorbent, preparation method and application - Google Patents
A kind of modified abandoned tealeaf residue adsorbent, preparation method and application Download PDFInfo
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- CN103406105B CN103406105B CN201310320360.5A CN201310320360A CN103406105B CN 103406105 B CN103406105 B CN 103406105B CN 201310320360 A CN201310320360 A CN 201310320360A CN 103406105 B CN103406105 B CN 103406105B
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Abstract
A kind of modified abandoned tealeaf residue adsorbent, preparation method and application, belong to technical field of absorbent.Adsorbent of the present invention is the discarded tealeaf residue adsorbent of hydrochloric Acid Modification process, its preparation method is: select the discarded green tea slag after finishing tea, get a certain amount of discarded tealeaf residue distilled water flushing for several times, then tealeaf residue is soaked 12 ~ 24h in hydrochloric acid solution, isolated by filtration, filter residue distilled water cleans to pH in neutral, dry.The discarded tealeaf residue adsorbent of hydrochloric Acid Modification is for removing the Reactive Brilliant Blue KN-R in waste water.The present invention is simple to operate, and cost is low, environmentally friendly, opens the new way of discarded tealeaf residue recycling.
Description
Technical field
The invention belongs to technical field of absorbent, relate to a kind of method utilizing adsorbent to remove Reactive Brilliant Blue KN-R in waste water, particularly relate to a kind of method utilizing modified abandoned tealeaf residue adsorbent to remove Reactive Brilliant Blue KN-R in waste water.
Background technology
In recent years, synthetic dyestuffs are widely used in the industries such as weaving, process hides, plastics, papermaking, about produce 7 × 10 in annual worldwide
5~ 1 × 10
6ton synthetic dyestuffs, wherein the dyestuff of 10 ~ 20% is discharged in environment in production and use procedure.Due to characteristics such as dyestuff chemistry Stability Analysis of Structures and difficult degradations, bring serious harm to ecological environment.In recent years, pollutant emission standard increasingly stringent, waste water from dyestuff can need discharge after suitable process, not only needs the COD of high-load in removal waste water, ammonia nitrogen and suspended particulate substance etc., also needs the color of sloughing waste water from dyestuff.But a small amount of dyestuff can produce obvious color, decoloring dye waste water is made to become a difficult problem for extensive concern.
Biosorption process is a kind of emerging wastewater processing technology, in process is containing the waste water of dyestuff, heavy metal ion and other pollutants, have the irreplaceable advantage of other method, as advantages such as cheap, efficient, abundance, non-secondary pollutions.And conventional method is as higher in ion-exchange, membrane separation process and active carbon adsorption cost, and the precipitation method, oxidation-reduction method and ferrite process are because excessive to the consumption of chemical reagent and energy, also may cause secondary pollution, limit their extensive use.
As everyone knows, tea is the drink of Chinese tradition, and there is long tea-drinking culture in China.China is Tea planting big country, Chinese tea output 191.5 ten thousand tons in 2012, but the tealeaf residue produced after drinking tea seldom utilizes, and be directly abandon mostly, the waste not only causing resource also pollutes environment.In fact, it is very large and be rich in oxygen, nitrogen, p and s isoreactivity group that tealeaves has network structure, porous, surface area, is a kind of sorbing material with development potentiality.Discarded tealeaf residue is utilized to prepare Reactive Brilliant Blue KN-R in sorbent treatment waste water, not only achieve resource and the economic worth of discarded tealeaf residue, and the pollution that discarded tealeaf residue causes can be alleviated, effectively can remove the dyestuff in waste water simultaneously, reach the effect of turn waste into wealth, control with useless (discarded tealeaf residue) useless (waste water from dyestuff).
Summary of the invention
The object of patent of the present invention is to provide the application of a kind of modified abandoned tealeaf residue adsorbent of efficient, low cost, preparation method and adsorption activity brilliant blue KN-R dyestuff.
To achieve these goals, modified abandoned tealeaf residue adsorbent proposed by the invention is the discarded tealeaf residue adsorbent of hydrochloric Acid Modification, and its preparation method, comprises the following steps:
(soak for 6 ~ 10 times) after green tea being soaked in boiling water 2h, take out tealeaf residue distilled water flushing for several times, then tealeaf residue is soaked 12 ~ 24h in hydrochloric acid solution, isolated by filtration, filter residue distilled water cleans to pH in neutral, dry, namely obtains modified abandoned tealeaf residue adsorbent.
The concentration preferably 0.10 ~ 0.50mol/L of above-mentioned hydrochloric acid solution, the consumption of discarded tealeaf residue and hydrochloric acid solution is preferably discarded tealeaf residue weight (g): hydrochloric acid solution volume (mL) is: 1:20 ~ 1:100, the temperature of modification preferably 20 ~ 50 DEG C.Discarded green tea slag is preferably and soaks 6 ~ 10 times in boiling water, and soak time is the discarded green tea slag of 2h.
Modified abandoned tealeaf residue adsorbent of the present invention is used for the Adsorption of Reactive Brilliant Blue KN-R in solution.
The Adsorption optimum condition that above-mentioned modified abandoned tealeaf residue adsorbent is used for Reactive Brilliant Blue KN-R in solution is: regulate pH to be that 1 ~ 11(is preferably 1 ~ 3 the solution containing Reactive Brilliant Blue KN-R), add modified abandoned tealeaf residue adsorbent, modified abandoned tealeaf residue absorbent concentration is made to be 4 ~ 20g/L, after absorption 6 ~ 24h, isolated by filtration, filtrate is adjusted to neutrality, discharge.
The invention has the beneficial effects as follows: adopt modified abandoned tealeaf residue adsorbent of the present invention for containing solution or the wastewater treatment of Reactive Brilliant Blue KN-R, compared with ion-exchange, membrane separation process, the precipitation method, active carbon adsorption etc., cost is low, consumption of chemical agent is few, non-secondary pollution.Modified abandoned tealeaf residue adsorbent of the present invention, to the adsorption capacity of the solution containing Reactive Brilliant Blue KN-R large (20 DEG C, maximum mono layer adsorption amount Q
0149.25mg/g), removal effect is significantly (the highest clearance can reach 96.79%, and minimum clearance is 94.16%).Adsorbent abundance of the present invention, preparation is simple, and cost is low, and the waste water not only making receptor 1 activity brilliant blue KN-R pollute is purified, and alleviates because tealeaf residue deals with the pollution caused improperly.
Accompanying drawing explanation
Fig. 1 is that discarded tealeaf residue adsorbent and the adsorption effect of modified abandoned tealeaf residue adsorbent of the present invention to Reactive Brilliant Blue KN-R compare.
Fig. 2 is that different initial pH is on the impact of modified abandoned tealeaf residue adsorbent Reactive Brilliant Blue KN-R of the present invention.
Fig. 3 is the adsorption effect of Reactive Brilliant Blue KN-R and the relation curve of modified abandoned tealeaf residue adsorbent amount of the present invention.
Fig. 4 is adsorption effect and the relation curve of Reactive Brilliant Blue KN-R initial mass concentration and time of Reactive Brilliant Blue KN-R.
Fig. 5 is the Langmuir adsorption isotherm of modified abandoned tealeaf residue adsorbent Reactive Brilliant Blue KN-R of the present invention.
Fig. 6 is the Temkin adsorption isotherm of modified abandoned tealeaf residue adsorbent Reactive Brilliant Blue KN-R of the present invention.
Fig. 7 is the infrared spectrogram of modified abandoned tealeaf residue adsorbent of the present invention before and after adsorption activity brilliant blue KN-R.
Detailed description of the invention
In order to have better understanding to technical characteristic of the present invention, object and beneficial effect, further illustrate the present invention below in conjunction with specific embodiment, but the present invention is not restricted to embodiment.
Embodiment 1
(soak for 6 times) after the green tea of certain mass is soaked 2h in boiling water, take out tealeaf residue distilled water flushing for several times, then by this discarded tealeaf residue and hydrochloric acid solution according to discarded tealeaf residue weight (g): the ratio that hydrochloric acid solution volume (mL) is 1:100 is soaked in conical flask, wherein the concentration of hydrochloric acid solution is 0.10mol/L, in 20 DEG C of water bath with thermostatic control shaking tables after vibration (150 revs/min) 24h, isolated by filtration, filter residue distilled water cleans to pH in neutral, dry (drying or freeze drying), namely obtains modified abandoned tealeaf residue adsorbent.
Comparative example 1
(soak for 6 times) after the green tea of certain mass is soaked 2h in boiling water, take out tealeaf residue distilled water flushing for several times, dry (drying or freeze drying), namely obtains discarded tealeaf residue adsorbent.
Absorption test case 1
It is in the 50mg/L Reactive Brilliant Blue KN-R solution of 1.3 that the adsorbent 1.5g that respectively prepared by Example 1 and comparative example 1 adds 50mL, pH respectively, vibrate after (150 revs/min) 24h in water bath with thermostatic control shaking table at 20 DEG C, isolated by filtration, measures the concentration of residual activity brilliant blue KN-R in filtrate.
Discarded tealeaf residue adsorbent and modified abandoned tealeaf residue adsorbent are to the adsorption effect contrast of Reactive Brilliant Blue KN-R as shown in Figure 1.The result of Fig. 1 shows, the Reactive Brilliant Blue KN-R clearance clearance of discarded tealeaf residue adsorbent is 73.42%, and modified abandoned tealeaf residue adsorbent is 98.22%.Compared with discarded tealeaf residue adsorbent, modified abandoned tealeaf residue adsorbent of the present invention considerably improves the clearance (improve 24.80%) of Reactive Brilliant Blue KN-R.
Embodiment 2
(soak for 7 times) after the green tea of certain mass is soaked 2h in boiling water, take out tealeaf residue distilled water flushing for several times, then by this discarded tealeaf residue and hydrochloric acid solution according to discarded tealeaf residue weight (g): the ratio that hydrochloric acid solution volume (mL) is 1:60 is soaked in conical flask, wherein the concentration of hydrochloric acid solution is 0.15mol/L, in 25 DEG C of water bath with thermostatic control shaking tables after vibration (120 revs/min) 24h, isolated by filtration, filter residue distilled water cleans to pH in neutral, dry (drying or freeze drying), namely obtains modified abandoned tealeaf residue adsorbent.
Getting modified abandoned tealeaf residue adsorbent 1g, to add solution ph be respectively 1.0,2.0,3.0,5.0,7.0,9.0,11.0, in the Reactive Brilliant Blue KN-R solution of 50mL55mg/L, vibrate after (150 revs/min) 24h in water bath with thermostatic control shaking table at 20 DEG C, isolated by filtration, measures the concentration of residual activity brilliant blue KN-R in filtrate.
According to following formulae discovery adsorption capacity:
Wherein: q
efor adsorption capacity, mg/g; C
0for Reactive Brilliant Blue KN-R initial concentration, C
efor Reactive Brilliant Blue KN-R concentration during adsorption equilibrium, mg/L; V is liquor capacity, mL; M is adsorbent mass, g.
Different initial pH on the impact of modified abandoned tealeaf residue adsorbent Reactive Brilliant Blue KN-R as shown in Figure 2.Along with pH is increased to 3.0 by 1.0, adsorption capacity drops to 5.18mg/g by 5.38mg/g, but change is little; PH continues to raise, and adsorption capacity declines gradually, and when pH is 11.0, adsorption capacity is 3.81mg/g, and test proves that modified abandoned tealeaf residue adsorbent Reactive Brilliant Blue KN-R has good adsorption effect when pH is 1.0 ~ 3.0.
Embodiment 3
(soak for 8 times) after the green tea of certain mass is soaked 2h in boiling water, take out tealeaf residue distilled water flushing for several times, then by this discarded tealeaf residue and hydrochloric acid solution according to discarded tealeaf residue weight (g): the ratio that hydrochloric acid solution volume (mL) is 1:40 is soaked in conical flask, wherein the concentration of hydrochloric acid solution is 0.25mol/L, in 30 DEG C of water bath with thermostatic control shaking tables after vibration (150 revs/min) 20h, isolated by filtration, filter residue distilled water cleans to pH in neutral, dry (drying or freeze drying), namely obtains modified abandoned tealeaf residue adsorbent.
Get modified abandoned tealeaf residue adsorbent 0.20 respectively, 0.40,0.60,0.80,1.00, add that 50mL, pH are 1.0 respectively, in the Reactive Brilliant Blue KN-R solution of 50mg/L, after (150 revs/min) 24h that vibrates in water bath with thermostatic control shaking table at 20 DEG C, isolated by filtration, measures the concentration of residual activity brilliant blue KN-R in filtrate.
The relation curve of Reactive Brilliant Blue KN-R adsorption effect and modified abandoned tealeaf residue adsorbent amount of the present invention as shown in Figure 3.As seen from Figure 3, along with modified abandoned tealeaf residue adsorbent amount is elevated to 20.0g/L by 4.0g/L, the equilibrium adsorption capacity of Reactive Brilliant Blue KN-R drops to 2.34mg/g by 12.08mg/g, and clearance is increased to 98.32% by 94.95%.Modified abandoned tealeaf residue adsorbent mass concentration is 8.0g/L(and consumption is 0.40g) time, both ensure that adsorbent amount was less, in turn ensure that relatively high Reactive Brilliant Blue KN-R clearance.
Embodiment 4
(soak for 9 times) after the green tea of certain mass is soaked 2h in boiling water, take out tealeaf residue distilled water flushing for several times, then by this discarded tealeaf residue and hydrochloric acid solution according to discarded tealeaf residue weight (g): the ratio that hydrochloric acid solution volume (mL) is 1:40 is soaked in conical flask, wherein the concentration of hydrochloric acid solution is 0.30mol/L, in 35 DEG C of water bath with thermostatic control shaking tables after vibration (120 revs/min) 16h, isolated by filtration, filter residue distilled water cleans to pH in neutral, dry (drying or freeze drying), namely obtains modified abandoned tealeaf residue adsorbent.
Get modified abandoned tealeaf residue adsorbent 0.40g and add that 50mL, pH are 1.0, Reactive Brilliant Blue KN-R concentration is respectively in 40,80,120,160 and 200mg/L Reactive Brilliant Blue KN-R solution respectively, vibrate after (150 revs/min) 6h in water bath with thermostatic control shaking table at 20 DEG C, isolated by filtration, measures the concentration of residual activity brilliant blue KN-R in filtrate.
The adsorption effect of Reactive Brilliant Blue KN-R and the relation curve of Reactive Brilliant Blue KN-R initial mass concentration are as shown in Figure 4.As seen from Figure 4, most Reactive Brilliant Blue KN-Rs is removed in front 2h.Under the driving of mass concentration gradient, along with Reactive Brilliant Blue KN-R initial mass concentration is increased to 200mg/L by 40mg/L, adsorption capacity rises to 22.59mg/g by 4.65mg/g, and clearance only drops to 94.16% by 96.79%, this shows that modified abandoned tealeaf residue adsorbent of the present invention has good adsorption effect within the scope of wider Reactive Brilliant Blue KN-R mass concentration.
Embodiment 5
(soak for 10 times) after the green tea of certain mass is soaked 2h in boiling water, take out tealeaf residue distilled water flushing for several times, then by this discarded tealeaf residue and hydrochloric acid solution according to discarded tealeaf residue weight (g): the ratio that hydrochloric acid solution volume (mL) is 1:30 is soaked in conical flask, wherein the concentration of hydrochloric acid solution is 0.40mol/L, in 50 DEG C of water bath with thermostatic control shaking tables after vibration (150 revs/min) 12h, isolated by filtration, filter residue distilled water cleans to pH in neutral, dry (drying or freeze drying), namely obtains modified abandoned tealeaf residue adsorbent.
Get modified abandoned tealeaf residue adsorbent 0.40g and join that 50mL, pH are 1.0, Reactive Brilliant Blue KN-R concentration is respectively in 40,80,120,160 and 200mg/L Reactive Brilliant Blue KN-R solution respectively, respectively at 20 DEG C, 35 DEG C, vibrate after (150 revs/min) 6h in water bath with thermostatic control shaking table at 50 DEG C, isolated by filtration, measures the concentration of residual activity brilliant blue KN-R in filtrate.
Absorption result Langmuir and the matching of Temkin adsorption isotherm, as shown in Figure 5,6, fitting result is as shown in table 1 for the adsorption isotherm under different temperatures.
As can be seen from Fig. 5,6 and table 1, from fitting coefficient and other parameters, compared to Temkin model, Langmuir model is better to the fitting effect of the isothermal adsorption test data of Reactive Brilliant Blue KN-R to modified abandoned tealeaf residue adsorbent, and therefore Langmuir model can describe the isothermal adsorption test data of modified abandoned tealeaf residue adsorbent to Reactive Brilliant Blue KN-R better.As can be seen from Table 1, Q
0all raise along with the rising of temperature with b, this shows that the surface-active of modified abandoned tealeaf residue adsorbent increases along with the rising of temperature, and has higher compatibility under the high temperature conditions with Reactive Brilliant Blue KN-R is intermolecular.
When 20 DEG C, the maximum mono layer adsorption amount Q of the modified abandoned tealeaf residue adsorbent Reactive Brilliant Blue KN-R calculated with Langmuir thermoisopleth
0149.25mg/g.The adsorption capacity of different adsorbents to reactive dye is more as shown in table 2, compared with the adsorption capacity of other high efficiency low cost adsorbents in table, modified abandoned tealeaf residue of the present invention can as the adsorbent of process containing a kind of high efficiency, low cost of Reactive Brilliant Blue KN-R waste water.
Table 1 adsorption isotherm parameter
The adsorption capacity of the different adsorbent of table 2 to reactive dye compares
| Adsorbent | Reactive dye | Maximum mono layer adsorption amount Q 0(mg/g) |
| Powdered Activated Carbon | Reactive Brilliant Blue KN-R | 371.75 |
| Modified abandoned tealeaf residue (the present invention) | Reactive Brilliant Blue KN-R | 149.25 |
| Oyster shell loading chitosan | Active red 152 | 135.14 |
| CMC immobilization deactivation aspergillus fumigatus bead | Reactive Brilliant Blue KN-R | 66.7 |
| Chemical plant excess sludge | Reactive Red 4 | 31.13 |
The thermodynamic analysis of modified abandoned tealeaf residue adsorbent Reactive Brilliant Blue KN-R shows, modified abandoned tealeaf residue at Gibbs free energy (Δ G °) the Fen other Wei – 6.73kJ/mol, – 7.34kJ/mol of adsorption activity brilliant blue KN-R at 20 DEG C, 35 DEG C and 50 DEG C with – 8.01kJ/mol, be negative value, show that the process of modified abandoned tealeaf residue adsorbent Reactive Brilliant Blue KN-R all can spontaneously occur under three test temperatures.Temperature rises to 50 DEG C from 20 DEG C, Gibbs free energy (Δ G °) Jiang Dao – 8.01kJ/mol Cong – 6.73kJ/mol thereupon, illustrates that high temperature promotes the generation of adsorption reaction.The numerical value of enthalpy change (Δ H °) is 13.70kJ/mol, and the numerical value of Entropy Changes (Δ S °) is 69.74J/molK, both be on the occasion of, illustrate that modified abandoned tealeaf residue adsorbent Reactive Brilliant Blue KN-R is the endothermic reaction, and the randomness of solid liquid interface increases to some extent.The above results shows, technological process of the present invention to operating condition and equipment requirement low, be a kind of economy, economize energy containing Reactive Brilliant Blue KN-R method of wastewater treatment, be suitable for propagation and employment.
Embodiment 6
(soak for 6 times) after the green tea of certain mass is soaked 2h in boiling water, take out tealeaf residue distilled water flushing for several times, then by this discarded tealeaf residue and hydrochloric acid solution according to discarded tealeaf residue powder weight (g): the ratio that hydrochloric acid solution volume (mL) is 1:20 is soaked in conical flask, wherein the concentration of hydrochloric acid solution is 0.50mol/L, in 20 DEG C of water bath with thermostatic control shaking tables after vibration (120 revs/min) 24h, isolated by filtration, filter residue distilled water cleans to pH in neutral, dry (drying or freeze drying), namely obtains modified abandoned tealeaf residue adsorbent.
Getting modified abandoned tealeaf residue adsorbent 0.40g adds in 50mL, pH=1.0,50mg/L Reactive Brilliant Blue KN-R solution, vibrate after (150 revs/min) 24h in water bath with thermostatic control shaking table at 20 DEG C, isolated by filtration, will adsorb the modified abandoned tealeaf residue adsorbent freeze drying of Reactive Brilliant Blue KN-R.
Modified abandoned tealeaf residue adsorbent before and after adsorbing in the present embodiment is characterized.
Infrared spectrum analysis
In the present embodiment, modified abandoned tealeaf residue adsorbent infrared spectrogram such as Fig. 7 before and after adsorption activity brilliant blue KN-R shows, can find out that the spectrogram of modified abandoned tealeaf residue adsorbent before and after adsorption activity brilliant blue KN-R has obvious similitude, illustrate that this sorbent structure is stablized.At 3432cm
-1the absworption peak at place represents the overlap of the stretching vibration of O – H and N – H, at 2925cm
-1with 2855cm
-1the absworption peak at place is the vibration of C-H in aliphatic compound, at 1637cm
-1the absworption peak at place be in carbonyl and protein C – O in conjunction with C – N(I type amido) stretching vibration, 1535cm
-1the absworption peak at place is the deformation vibration of (acid amides combination) N-H on the stretching vibration of C-N and protein, 1450cm
-1that the absworption peak located may represent is CH
2deformation vibration and CH
3antisymmetric vibration, 1365cm
-1the absworption peak at place is the deformation vibration of O-H, 1123cm
-1the absworption peak at place is the superposition of the stretching vibration of C-O-C in P-O-C and polysaccharose substance in phosphonyl group, 616cm
-1the absworption peak at place may cause due to C-N stretching vibration, and the absworption peak of its all band (in figure near finger print) is the vibration of phosphate group or sulphur group.The above results shows, modified abandoned tealeaf residue adsorbent surface is rich in oxygen, nitrogen, p and s isoreactivity group.After modified abandoned tealeaf residue adsorbent Reactive Brilliant Blue KN-R, 3432cm
-1, 2925cm
-1,2855cm
-1, 1637cm
-1, 1535cm
-1, 1450cm
-1, l365cm
-1, 1123cm
-1, 616cm
-1the absworption peak at place all reduces, and shows that hydroxyl, amido, phosphonyl group, phosphate group and sulphur group take part in the absorption of Reactive Brilliant Blue KN-R jointly.
Above-described embodiment shows, modified abandoned tealeaf residue adsorbent cost of the present invention is low, wide material sources, and preparation is simple, and adsorption operations condition is easy to realize, and can be widely used in the process containing Reactive Brilliant Blue KN-R waste water.
Claims (1)
1. the discarded tealeaf residue adsorbent of hydrochloric Acid Modification is used for the removal of Reactive Brilliant Blue KN-R in waste water, it is characterized in that, after the green tea of certain mass is soaked 2h 10 times in boiling water, take out tealeaf residue distilled water flushing for several times, then tealeaf residue and hydrochloric acid solution will be discarded according to discarded tealeaf residue weight g: hydrochloric acid solution volume mL is that the ratio of 1:30 is soaked in conical flask, wherein the concentration of hydrochloric acid solution is 0.40mol/L, in 50 DEG C of water bath with thermostatic control shaking tables after 150 revs/min of vibration 12h, isolated by filtration, filter residue distilled water cleans to pH in neutral, dry, namely modified abandoned tealeaf residue adsorbent is obtained,
Get modified abandoned tealeaf residue adsorbent 0.40g and join that 50mL, pH are 1.0, Reactive Brilliant Blue KN-R concentration is respectively in 40,80,120,160 and 200mg/L Reactive Brilliant Blue KN-R solution respectively, after 150 revs/min of vibration 6h in water bath with thermostatic control shaking table at 50 DEG C, isolated by filtration.
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| CN104549168B (en) * | 2014-12-04 | 2016-07-06 | 安徽农业大学 | Modified tea grounds biology defluorinating agent and its preparation method and application is participated in by surfactant |
| CN104785213A (en) * | 2015-02-10 | 2015-07-22 | 广州市顺泽美汽车用品有限公司 | Formaldehyde absorption tea stalk filling material preparation method and automobile cushion |
| CN105080500A (en) * | 2015-05-18 | 2015-11-25 | 江苏大学 | Natural dye wastewater adsorbent and preparation and application method thereof |
| CN105170109B (en) * | 2015-10-21 | 2018-01-26 | 南阳师范学院 | A kind of biological adsorption agent for handling waste water from dyestuff, preparation method and applications |
| CN106268648B (en) * | 2016-06-03 | 2019-04-16 | 浙江工商大学 | A kind of Modified Green Tea and the method for going water removal neutral and alkali blackish green with Modified Green Tea |
| CN108275838A (en) * | 2018-02-02 | 2018-07-13 | 回音必集团安徽制药有限公司 | A kind of pharmacy sewage treatment process |
| CN108314258A (en) * | 2018-02-02 | 2018-07-24 | 回音必集团安徽制药有限公司 | A kind for the treatment of process of pharmacy sewage |
| CN108275839A (en) * | 2018-02-02 | 2018-07-13 | 回音必集团安徽制药有限公司 | A kind of novel pharmacy sewage processing method |
| CN108249705A (en) * | 2018-02-02 | 2018-07-06 | 回音必集团安徽制药有限公司 | A kind of new and effective pharmacy sewage processing method |
| CN111346613A (en) * | 2018-12-21 | 2020-06-30 | 中国石油化工股份有限公司 | Dye wastewater adsorbent and preparation method thereof |
| CN109967045A (en) * | 2019-04-12 | 2019-07-05 | 阳江职业技术学院 | Biomass adsorbent, preparation method and the usage |
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