CN106944117A - The preparation method and application of cobalt sulfide tin/mesoporous carbon nitride catalyst - Google Patents
The preparation method and application of cobalt sulfide tin/mesoporous carbon nitride catalyst Download PDFInfo
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- 239000003054 catalyst Substances 0.000 title claims abstract description 36
- 238000002360 preparation method Methods 0.000 title claims abstract description 25
- VPRQBUKXDDOQKQ-UHFFFAOYSA-N [Sn].[Co]=S Chemical compound [Sn].[Co]=S VPRQBUKXDDOQKQ-UHFFFAOYSA-N 0.000 title claims abstract description 8
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 title description 2
- 239000002131 composite material Substances 0.000 claims abstract description 24
- 238000006243 chemical reaction Methods 0.000 claims abstract description 7
- UCKMPCXJQFINFW-UHFFFAOYSA-N Sulphide Chemical compound [S-2] UCKMPCXJQFINFW-UHFFFAOYSA-N 0.000 claims description 18
- ZMXDDKWLCZADIW-UHFFFAOYSA-N N,N-Dimethylformamide Chemical compound CN(C)C=O ZMXDDKWLCZADIW-UHFFFAOYSA-N 0.000 claims description 16
- 239000000243 solution Substances 0.000 claims description 15
- 238000003756 stirring Methods 0.000 claims description 15
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 13
- RBTBFTRPCNLSDE-UHFFFAOYSA-N 3,7-bis(dimethylamino)phenothiazin-5-ium Chemical compound C1=CC(N(C)C)=CC2=[S+]C3=CC(N(C)C)=CC=C3N=C21 RBTBFTRPCNLSDE-UHFFFAOYSA-N 0.000 claims description 11
- 229960000907 methylthioninium chloride Drugs 0.000 claims description 11
- 239000007787 solid Substances 0.000 claims description 11
- 239000012153 distilled water Substances 0.000 claims description 10
- 238000005406 washing Methods 0.000 claims description 8
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 claims description 6
- BOTDANWDWHJENH-UHFFFAOYSA-N Tetraethyl orthosilicate Chemical compound CCO[Si](OCC)(OCC)OCC BOTDANWDWHJENH-UHFFFAOYSA-N 0.000 claims description 6
- 238000001816 cooling Methods 0.000 claims description 5
- QGBSISYHAICWAH-UHFFFAOYSA-N dicyandiamide Chemical compound NC(N)=NC#N QGBSISYHAICWAH-UHFFFAOYSA-N 0.000 claims description 5
- 238000001035 drying Methods 0.000 claims description 5
- 238000001354 calcination Methods 0.000 claims description 4
- 239000000919 ceramic Substances 0.000 claims description 4
- 229910017665 NH4HF2 Inorganic materials 0.000 claims description 3
- 241000238370 Sepia Species 0.000 claims description 3
- 238000000034 method Methods 0.000 claims description 3
- 239000011259 mixed solution Substances 0.000 claims description 3
- 229920000428 triblock copolymer Polymers 0.000 claims description 3
- 238000002604 ultrasonography Methods 0.000 claims description 3
- 238000001291 vacuum drying Methods 0.000 claims description 3
- 238000005119 centrifugation Methods 0.000 claims description 2
- 238000004821 distillation Methods 0.000 claims description 2
- 230000001699 photocatalysis Effects 0.000 abstract description 8
- 238000007146 photocatalysis Methods 0.000 abstract description 8
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 abstract description 3
- 229910052799 carbon Inorganic materials 0.000 abstract description 2
- 230000009286 beneficial effect Effects 0.000 abstract 1
- 239000011941 photocatalyst Substances 0.000 abstract 1
- 238000013033 photocatalytic degradation reaction Methods 0.000 description 4
- 230000003197 catalytic effect Effects 0.000 description 3
- 238000006555 catalytic reaction Methods 0.000 description 3
- 238000006731 degradation reaction Methods 0.000 description 3
- 230000015572 biosynthetic process Effects 0.000 description 2
- 230000015556 catabolic process Effects 0.000 description 2
- 239000000356 contaminant Substances 0.000 description 2
- 238000005516 engineering process Methods 0.000 description 2
- 238000010438 heat treatment Methods 0.000 description 2
- 238000005286 illumination Methods 0.000 description 2
- 229910052573 porcelain Inorganic materials 0.000 description 2
- 230000035484 reaction time Effects 0.000 description 2
- 238000000967 suction filtration Methods 0.000 description 2
- 238000003786 synthesis reaction Methods 0.000 description 2
- 229910052724 xenon Inorganic materials 0.000 description 2
- FHNFHKCVQCLJFQ-UHFFFAOYSA-N xenon atom Chemical compound [Xe] FHNFHKCVQCLJFQ-UHFFFAOYSA-N 0.000 description 2
- 238000002835 absorbance Methods 0.000 description 1
- 239000012298 atmosphere Substances 0.000 description 1
- 238000004140 cleaning Methods 0.000 description 1
- 150000001875 compounds Chemical class 0.000 description 1
- 239000013078 crystal Substances 0.000 description 1
- 230000007547 defect Effects 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 238000003912 environmental pollution Methods 0.000 description 1
- 229910002804 graphite Inorganic materials 0.000 description 1
- 239000010439 graphite Substances 0.000 description 1
- 238000000703 high-speed centrifugation Methods 0.000 description 1
- 238000011065 in-situ storage Methods 0.000 description 1
- 239000000463 material Substances 0.000 description 1
- 230000013011 mating Effects 0.000 description 1
- 239000003863 metallic catalyst Substances 0.000 description 1
- 125000000325 methylidene group Chemical group [H]C([H])=* 0.000 description 1
- 239000012299 nitrogen atmosphere Substances 0.000 description 1
- 231100000252 nontoxic Toxicity 0.000 description 1
- 230000003000 nontoxic effect Effects 0.000 description 1
- 230000003287 optical effect Effects 0.000 description 1
- JMANVNJQNLATNU-UHFFFAOYSA-N oxalonitrile Chemical compound N#CC#N JMANVNJQNLATNU-UHFFFAOYSA-N 0.000 description 1
- 239000002994 raw material Substances 0.000 description 1
- 238000001228 spectrum Methods 0.000 description 1
- 239000006228 supernatant Substances 0.000 description 1
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J27/00—Catalysts comprising the elements or compounds of halogens, sulfur, selenium, tellurium, phosphorus or nitrogen; Catalysts comprising carbon compounds
- B01J27/24—Nitrogen compounds
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J35/00—Catalysts, in general, characterised by their form or physical properties
- B01J35/30—Catalysts, in general, characterised by their form or physical properties characterised by their physical properties
- B01J35/39—Photocatalytic properties
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- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F1/00—Treatment of water, waste water, or sewage
- C02F1/30—Treatment of water, waste water, or sewage by irradiation
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- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2101/00—Nature of the contaminant
- C02F2101/30—Organic compounds
- C02F2101/308—Dyes; Colorants; Fluorescent agents
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- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2101/00—Nature of the contaminant
- C02F2101/30—Organic compounds
- C02F2101/40—Organic compounds containing sulfur
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Abstract
The present invention relates to a kind of preparation of cobalt sulfide tin/mesoporous nitridation carbon composite photocatalyst, including step：The preparation of preparation, the preparation of cobalt sulfide tin (SnCoS4) and the cobalt sulfide tin of mesoporous carbonitride (MCN)/mesoporous carbonitride (SnCoS4/MCN) composite catalyst.The beneficial effects of the invention are as follows：The preparation method is relatively simple, and preparation condition is easily controlled, and prepared cobalt sulfide tin/mesoporous carbonitride (SnCoS4/MCN) composite catalyst course of reaction is simple, it is easily controlled, with non-secondary pollution, the advantages of photocatalysis efficiency is high, with certain application value.
Description
Technical field
Present invention relates particularly to a kind of preparation method and application of cobalt sulfide tin/mesoporous carbonitride composite catalyst, belong to
Photocatalysis degradation organic contaminant field.
Background technology
In recent years, energy shortage and problem of environmental pollution are increasingly severe, it has also become it is two big important that the mankind must face
Challenge.Photocatalysis technology using abundant, cleaning solar energy as power, with it is easy to operate, energy-efficient, clean it is nontoxic etc. excellent
Point, as the study hotspot for solving this two large problems.
It is used as a kind of non-metallic catalyst, graphite phase carbon nitride (g-C3N4) because with unique band structure, good change
Learn stability, it is cheap and easy to get the features such as, be widely used in photocatalysis field.But traditional g-C3N4Specific surface area is smaller, right
It can be seen that light utilization efficiency is relatively low etc., defect limits its application in terms of photocatalysis.By controlling pattern to g-C3N4It is modified
It is to improve one of these not enough methods.Mesoporous carbonitride (MCN) has larger specific surface area, and in general specific surface area is got over
Greatly, light-catalyzed reaction avtive spot is more, is more conducive to the progress of light-catalyzed reaction, therefore as numerous researchers research
One of focus.
Sulfide is a kind of conventional catalyst during light-catalyzed reaction.But conventional binary sulfide band-gap energy compared with
Greatly, less stable, easily occur photoetch.And ternary sulfide has good stability, band-gap energy small, visible light-responded etc. spy
Point, has attracted the attention of researchers.
The present invention is prepared for SnS2、CoS2、SnCoS4Sulfide, and be supported on MCN and obtain composite catalyst, will
It is applied on photocatalysis degradation organic contaminant methylene blue (MB).
The content of the invention
The purpose of the present invention be prepare a kind of effective catalyst there is provided sulfide/mesoporous carbonitride composite catalyst and
Its preparation method.The composite catalyst catalytic efficiency prepared is higher and whole preparation method is simple.
The concrete scheme that the present invention is used is：
Sulfide/mesoporous carbonitride composite catalyst is prepared from by situ synthesis, have studied binary sulfide and
The photocatalysis performance of ternary sulfide composite, and probed into influence of the catalyst to catalytic activity of different proportion.Wherein
Described SnCoS4/ MCN (0.5) composite catalysts have highest catalytic activity to MB.
The preparation method of sulfide of the present invention/mesoporous carbonitride composite catalyst, is carried out in accordance with the following steps：
(1) preparation of mesoporous carbonitride (MCN)
The preparation of SBA-15 templates：Weigh triblock copolymer P123 and HCl solution is dissolved under 30 DEG C of stirring conditions, afterwards
Add tetraethyl orthosilicate (TEOS) and 24h is stirred at 40 DEG C, solution is then poured into 130 DEG C of reaction 24h of autoclave, cooling
Suction filtration and with distillation water washing, is put into ceramic crucible, 550 DEG C of calcining 4h are to remove P123 after 60 DEG C of drying afterwards.
It is prepared by MCN：Weigh to be dissolved in dimethylformamide (DMF) under dicyandiamide stirring condition and be added dropwise to and be placed with SBA-
In 15 beaker.Placing into ultrasonic cleaner after stirring 6h, (frequency is 50KHz, power density 0.24W/cm2) ultrasound 2h, it
Beaker is put into dried overnight in 90 DEG C of oil bath pans afterwards.Obtained solid is polished to be put into ceramic crucible, 550 DEG C of calcinings
4h, heating rate is 3 DEG C/min, is cooled to room temperature, grinds obtained sepia solid and is placed in NH4HF2Soaked two days in solution,
Centrifuged afterwards and with distilled water and absolute ethanol washing.Obtained yellow-brown solid is MCN in 100 DEG C of vacuum drying.
Dicyandiamide and SBA-15 mass ratio are 10 wherein in step (1):1.
(2) preparation of sulfide/mesoporous carbonitride
Cys, SnCl are weighed respectively4·5H2O、CoCl4·5H2O, which is dissolved under distilled water stirring condition, to be added dropwise
Into MCN solution, persistently stir and mixed solution is transferred to 180 DEG C of reaction 24h of autoclave after 2h.Centrifuged after cooling
And with distilled water, absolute ethanol washing, 80 DEG C of drying.
In this way, it is respectively synthesized SnS2/MCN、CoS2/MCN、SnCoS4/MCN(0.3)、SnCoS4/MCN(0.5)、
SnCoS4/ MCN (1.0) composite catalyst, and synthesized SnS2、CoS2、SnCoS4Single catalyst.
Cys, SnCl wherein in step (2)4·5H2O、CoCl4·5H2O mol ratio is 10:1:1.
Wherein SnS in step (2)2/MCN、CoS2/ MCN mass ratioes are 0.5:1, SnCoS4/MCN mass ratio is respectively 0.3,
0.5、1.0。
The application of sulfide/mesoporous carbonitride composite catalyst, for photocatalytic degradation methylene blue (MB) solution, according to
Following step is carried out：
Weigh 20mg catalyst to be put into test tube, 50ml 25mg/L MB solution is added, with 420nm optical filters
500W xenon lamps carry out photocatalytic degradation reaction as light source.Dark reaction time is 30min, after illumination, and time sample is taken per 20min, is entered
Row centrifugation, and then survey its absorbance.
The present invention is prepared for a variety of sulfide/mesoporous nitridation carbon composite using in situ synthesis, passes through regulation
SnCoS4Different proportion composite catalyst is prepared with MCN ratios, so as to obtain the compound with different catalytically active.Its
Advantage is as follows：
(1) catalyst SnCoS is prepared4/ MCN raw material is easy to get, and technique is simple.
(2) SnCoS prepared4/ MCN catalyst photocatalysis performances are excellent.
Brief description of the drawings
The present invention is further described below in conjunction with the accompanying drawings.
Fig. 1 is the XRD of the different catalysts of embodiment 1~2.
Fig. 2 is embodiment 1~2 different catalysts TEM and SnCoS4/ MCN (0.5) EDS figures, (a:MCN,b:CoS2,c:
SnS2,d:SnCoS4,e:CoS2/MCN,f:SnS2/MCN,g:SnCoS4/MCN(0.5),h:SnCoS4/ MCN (0.5) EDS).
Fig. 3 is 20mg SnCoS in embodiment 34The uv atlas of/MCN (0.5) degraded 25mg/L methylene blues.
Embodiment
In order to preferably explain the present invention, present disclosure is expanded on further with reference to embodiment, but the present invention
Content is not limited solely to following embodiment.
Embodiment 1
(1) preparation of mesoporous carbonitride (MCN)
The preparation of SBA-15 templates：Weigh 4.0g triblock copolymer P123s and be added to 150mL 1.6mol/LHCl solution,
It is completely dissolved in 30 DEG C of stirred in water bath to P123.Add 8.8g tetraethyl orthosilicates (TEOS) and 24h is stirred at 40 DEG C, then will
Solution pours into 130 DEG C of autoclave reaction 24h, suction filtration and is repeatedly washed with distilled water after cooling, pottery is put into after 60 DEG C of drying
In porcelain crucible, calcine 4h to remove P123 for 550 DEG C in air atmosphere.
It is prepared by MCN：Weigh and 35mL dimethylformamides (DMF) are dissolved under 10g dicyandiamide stirring conditions and are slowly added dropwise
Enter to being placed with 1.0g SBA-15 beaker.Placing into ultrasonic cleaner after stirring 6h, (frequency is 50KHz, power density
0.24W/cm2) ultrasound 2h, beaker is put into dried overnight in 90 DEG C of oil bath pans afterwards.Obtained solid is polished to be put into pottery
In porcelain crucible, in nitrogen atmosphere, rise to 550 DEG C with 3 DEG C/min heating rate and keep 4h.Room temperature is naturally cooled to, is ground
Obtained sepia solid is placed in 100mL 4mol/L NH4HF2Soaked two days in solution, centrifuged afterwards and use distilled water
And absolute ethanol washing.Obtained yellow-brown solid is MCN in 100 DEG C of vacuum drying.MCN XRD spectrum is understood in Fig. 1 a,
The g-C corresponding to (100) and (002) crystal face is occurred in that at 13.1 ° and 27.4 °3N4Diffractive features peak.
(2) preparation of sulfide/mesoporous carbonitride
1.875mmol Cys, 0.1875mmol SnCl are weighed respectively4·5H2O、0.1875mmolCoCl4·
5H2O, which is dissolved under 20mL distilled water, stirring condition, to be added dropwise in 20mL MCN solution.Persistently by mixed solution after stirring 2h
It is transferred to 180 DEG C of reaction 24h of 100mL autoclaves.Naturally cool to after room temperature and centrifuged and with distilled water, absolute ethyl alcohol
Repeatedly washing, obtained black solid is dried at 80 DEG C as SnCoS4/MCN(0.3)。
In this way, it is respectively synthesized SnS2/MCN、CoS2/MCN、SnCoS4/MCN(0.3)、SnCoS4/MCN(0.5)、
SnCoS4/ MCN (1.0) composite catalyst, and synthesized SnS2、CoS2、SnCoS4Single catalyst.
The XRD for the catalyst prepared is as shown in Fig. 1 a, b, SnS2、CoS2、SnCoS4Occur in that respective diffractive features
Peak, after being combined with MCN, occurs in that the characteristic peak of sulfide and MCN two kinds of materials, indicates sulfide in composite catalyst
Load on MCN, this can also have TEM figures and EDS figures in Fig. 2 to further demonstrate that.
(3) photocatalytic degradation methylene blue (MB)
20mg different catalysts are weighed respectively to be put into test tube, are added 50ml 25mg/L MB solution, are filtered with 420nm
The 500W xenon lamps of mating plate carry out photocatalytic degradation reaction as light source.Dark reaction time is 30min, after illumination, every
20min takes time sample, and the high speed centrifugation under the conditions of 5000rpm, takes supernatant liquor to survey its concentration with ultraviolet-uisible spectrophotometer
Change.Fig. 3 is 20mg SnCoS4Degradation rate in/MCN (0.5) degraded 25mg/L MB activity figure, 160min reaches
87.84%.
Claims (6)
1. cobalt sulfide tin/mesoporous carbonitride (SnCoS4/ MCN) composite catalyst is a kind of new composite catalyst, passes through original position
Growth method is prepared from.
2. the preparation method of sulfide/mesoporous carbonitride composite catalyst, it is characterised in that carry out as steps described below：
(1) preparation of mesoporous carbonitride (MCN)
The preparation of SBA-15 templates：Weigh triblock copolymer P123 and HCl solution is dissolved under 30 DEG C of stirring conditions, add afterwards
Tetraethyl orthosilicate (TEOS) stirs 24h at 40 DEG C, and solution then is poured into 130 DEG C of reaction 24h of autoclave, taken out after cooling
Filter and use solid obtained by distillation water washing, be put into after 60 DEG C of drying in ceramic crucible, 550 DEG C of calcining 4h remove P123.
It is prepared by MCN：Weigh to be dissolved in dimethylformamide (DMF) under dicyandiamide stirring condition and be added dropwise to and be placed with SBA-15's
In beaker.Placing into ultrasonic cleaner after stirring 6h, (frequency is 50KHz, power density 0.24W/cm2) ultrasound 2h, afterwards will
Beaker is put into dried overnight in 90 DEG C of oil bath pans.Obtained solid is polished to be put into ceramic crucible, 550 DEG C of calcining 4h, is risen
Warm speed is 3 DEG C/min, is cooled to room temperature, grinds obtained sepia solid and is placed in NH4HF2In solution soak two days, it is laggard
Row centrifugation and with distilled water and absolute ethanol washing.Obtained yellow-brown solid obtains MCN in 100 DEG C of vacuum drying.
(2) preparation of sulfide/mesoporous carbonitride
Cys, SnCl are weighed respectively4·5H2O、CoCl4·5H2O, which is dissolved under distilled water, stirring condition, to be added dropwise to
In MCN solution, persistently stir and mixed solution is transferred to 180 DEG C of reaction 24h of autoclave after 2h.Centrifuged simultaneously after cooling
With distilled water, absolute ethanol washing, 80 DEG C of drying.
In this way, it is respectively synthesized SnS2/MCN、CoS2/MCN、SnCoS4/MCN(0.3)、SnCoS4/MCN(0.5)、
SnCoS4/ MCN (1.0) composite catalyst, and synthesized SnS2、CoS2、SnCoS4Single catalyst.
3. the preparation method of mesoporous carbonitride according to claim 2, it is characterised in that wherein in step (1) dicyandiamide with
SBA-15 mass ratio is 10:1.
4. the preparation method of sulfide according to claim 2/mesoporous carbonitride composite catalyst, it is characterised in that wherein
Cys, SnCl in step (2)4·5H2O、CoCl4·5H2O mol ratio is 10:1:1.
5. the preparation method of sulfide according to claim 2/mesoporous carbonitride composite catalyst, it is characterised in that wherein
SnS in step (2)2/MCN、CoS2/ MCN mass ratioes are 0.5:1, SnCoS4/ MCN mass ratioes are respectively 0.3,0.5,1.0.
6. the SnCoS described in claim 14/ MCN (0.5) composite catalyst reaches in 160min to the clearance of methylene blue
87.84%.
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Cited By (4)
| Publication number | Priority date | Publication date | Assignee | Title |
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| CN107469854A (en) * | 2017-09-06 | 2017-12-15 | 淮北师范大学 | A kind of synthetic method of composite photo-catalyst |
| CN107930671A (en) * | 2017-12-06 | 2018-04-20 | 福州大学 | A kind of ternary metal sulfide/graphite phase carbon nitride composite photocatalyst material and its preparation method and application |
| CN108043439A (en) * | 2017-11-23 | 2018-05-18 | 江南大学 | A kind of preparation method of cobalt sulfide/class graphene carbon nitrogen compound composite catalyst |
| CN112279306A (en) * | 2020-10-21 | 2021-01-29 | 南京晓庄学院 | Optimization method of sulfide nanocrystal, Sn-S-Co nanocrystal and optimized product thereof |
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Cited By (6)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN107469854A (en) * | 2017-09-06 | 2017-12-15 | 淮北师范大学 | A kind of synthetic method of composite photo-catalyst |
| CN107469854B (en) * | 2017-09-06 | 2020-05-15 | 淮北师范大学 | Synthetic method of composite photocatalyst |
| CN108043439A (en) * | 2017-11-23 | 2018-05-18 | 江南大学 | A kind of preparation method of cobalt sulfide/class graphene carbon nitrogen compound composite catalyst |
| CN107930671A (en) * | 2017-12-06 | 2018-04-20 | 福州大学 | A kind of ternary metal sulfide/graphite phase carbon nitride composite photocatalyst material and its preparation method and application |
| CN112279306A (en) * | 2020-10-21 | 2021-01-29 | 南京晓庄学院 | Optimization method of sulfide nanocrystal, Sn-S-Co nanocrystal and optimized product thereof |
| CN112279306B (en) * | 2020-10-21 | 2021-07-06 | 南京晓庄学院 | Optimization method of sulfide nanocrystal, Sn-S-Co nanocrystal and optimized product thereof |
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