CN109225135A - A kind of modification biological charcoal adsorbent material and preparation method thereof with to Pb in water body2+Removal application - Google Patents
A kind of modification biological charcoal adsorbent material and preparation method thereof with to Pb in water body2+Removal application Download PDFInfo
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- CN109225135A CN109225135A CN201811234065.7A CN201811234065A CN109225135A CN 109225135 A CN109225135 A CN 109225135A CN 201811234065 A CN201811234065 A CN 201811234065A CN 109225135 A CN109225135 A CN 109225135A
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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
- B01J20/00—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof
- B01J20/02—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising inorganic material
- B01J20/20—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising inorganic material comprising free carbon; comprising carbon obtained by carbonising processes
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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
- C02F1/28—Treatment of water, waste water, or sewage by sorption
- C02F1/281—Treatment of water, waste water, or sewage by sorption using inorganic sorbents
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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
- C02F1/48—Treatment of water, waste water, or sewage with magnetic or electric fields
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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
- C02F2101/10—Inorganic compounds
- C02F2101/20—Heavy metals or heavy metal compounds
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Abstract
The present invention relates to a kind of modification biological charcoal adsorbent material and preparation method thereof with to Pb in water body2+Removal in application, which assigns magnetic, limit oxygen pyrolysis using agricultural solid waste as raw material, by dipping, and surface covers chitosan, and obtained after being chemically modified to chitosan, and the adsorbent material is to the Pb in water body2+Removal ability with higher.This method had not only realized the resource utilization to agricultural solid residue, but also had achieved the purpose that with pollution treatment of giving up, while being difficult to recycle the difficulty of removal after overcoming the application of conventional absorbtion material again.Material source of the invention is abundant, preparation process simple possible, to the Pb in water body2+Removal effect is significant, and without secondary pollution, and cost is relatively low for preparation and absorption, has preferable application value.
Description
Technical field
The present invention relates to the resource utilizations of agricultural solid residue to prepare water process adsorbent material field, and in particular to one
Plant modification biological charcoal adsorbent material and preparation method thereof and to Pb in water body2+Minimizing technology.
Background technique
A large amount of agricultural solid residue is generated with the rapid development of China's intensive agriculture as large agricultural country.According to
Incomplete statistics, being often only various agricultural crop straws just has more than 7.5 hundred million tons.Due to the pattern of farming in present rural area, energy resource structure
It being varied widely, burning disposal is thrown aside everywhere or carried out to a large amount of agricultural wastes, the waste of resource is caused in this way,
The pollution of environment is resulted in again.
The continuous propulsion of process of industrialization, the discharge amount of China's industrial wastewater are also increasing year by year, some heavy metal ion
It can enter in water system with the discharge of industrial wastewater.The amount of Heavy Metals in Waters ion be more than certain threshold value after, can be to people
Class health generates serious threat.How to eliminate the harm of heavy metal and effectively recycle the heavy metal in waste water, and is current
Water body environment protects problem to be solved.
The method for handling Heavy Metals in Waters pollution, has there is many research.Wherein, absorption method has at low cost
It is honest and clean, it is easy to operate, many advantages, such as can be recycled, in processing heavy metal water body pollution the most commonly used effective ways it
One.However that there are adsorption capacities is low for these common common adsorbent materials, adsorbent material is difficult to reclaiming after absorption, causes to locate
Manage increase and the waste of time of cost.
Therefore, a kind of suitable technique is found, prepares novel absorption material using agricultural solid residue, and be applied to weight
The improvement of metallic pollution water body realizes that resource utilization reaches mitigation environmental pressure to the innoxious of agricultural solid residue,
Purpose of improving the ecological environment seems particularly significant.
There are many patent documents to report about magnetic adsorptive material is prepared also using agricultural solid residue, such as: China
Patent document CN103316636A discloses a kind of preparation method of biomass-based magnetic active carbon, and this method uses and first prepares work
Property charcoal again with the method for magnetic powder mixing and absorption by magnetisable material load on activated carbon.But what this charcoal was mixed with magnetic powder
Fill process causes magnetic medium to be easy to fall off, and material structure is unstable, and adsorption capacity reduces.Chinese patent document
CN10156467B discloses a kind of synthetic method of superparamagnetism porous carbon absorption material, uses the 600- in nitrogen atmosphere
The method of 900 DEG C of roastings prepares magnetic adsorptive material.But the temperature that this method uses is higher, and energy consumption is larger.Chinese patent document
CN104028214A discloses a kind of preparation method of carbon-based magnetic adsorptive material of agricultural biomass.This method is from plant
The agricultural biomass of object organism be raw material, the load process for using ferric ion to be blended with biomass ultrasound, alkali precipitation with
And magnetic technique is assigned in low-temperature hydrothermal carbonization, obtains and has magnetic biological carbon adsorbing material.This method preparation process is relatively complicated, makes
The equipment such as Ultrasound Instrument and autoclave are used, amplification production is unfavorable for.In addition, though the research of related adsorbent material preparation compared with
It is more, but rarely have and the adsorbent material of preparation is applied to Pb in water body2+Removal research.
Summary of the invention
In view of the deficiencies of the prior art, the present invention provide a kind of modified magnetic charcoal adsorbent material, preparation method and its
The Pb in water body2+Removal application.Resource utilization agricultural solid residue, cost of investment is low, Pb in water body2+Removal
Significant effect.
Technical scheme is as follows:
A kind of preparation method of modification biological charcoal adsorbent material, comprises the following steps that
(1) biological material is crushed, is placed in FeCl3In solution, stir evenly, after filtering, aging；
(2) biological material after aging is pyrolyzed in nitrogen atmosphere in 200-600 DEG C, after natural cooling, grinding obtains magnetic
Property charcoal；
(3) magnetic biological carbon is added in the aqueous acetic acid of chitosan, is stirred evenly, strong base solution reaction is added dropwise,
Filtering, solid is washed to neutrality, dry, and grinding obtains chitosan magnetic biological carbon；
(4) chitosan magnetic biological carbon and ethylenediamine tetra-acetic acid (EDTA) are added to the water, heat temperature raising stirring, cooling
Strong base solution and 1- ethyl -3- (3- DimethylAminopropyl) carbodiimide hydrochloride (EDAC) reaction are added afterwards, reaction is completed
After filter, it is dry after solid washing, grind to get modification biological charcoal adsorbent material.
, according to the invention it is preferred to, biological material described in step (1) is reed straw, corn stover, corn
Core, cotton stalk, rice husk, peanut shell etc.；
Preferably, biological material is crushed to 1-3mm；
Preferably, FeCl3The concentration of solution is 1-3mol/L；
Preferably, biological material and FeCl3Mass ratio be 1:1；
Preferably, the temperature of aging is 70-90 DEG C, ageing time 1-3h.
According to the present invention, the effect of step (1) is that iron ion enters in biomass, is the beginning that charcoal assigns magnetic.
, according to the invention it is preferred to, the atmosphere being pyrolyzed in step (2) is nitrogen, and pyrolysis temperature is 450-550 DEG C
Preferably, the heating rate in pyrolytic process is 3-10 DEG C/min, further preferred 5 DEG C/min；
Preferably, pyrolysis time 1-5h, further preferred 2h.
According to the present invention, the effect of step (2) is that the biomass limit oxygen high temperature pyrolysis after molysite dipping prepares magnetic bio
Charcoal is conducive to collection of the adsorbent material under externally-applied magnetic field.
, according to the invention it is preferred to, in step (3) in the aqueous acetic acid of chitosan, the mass fraction of chitosan is
1%-3%；
Preferably, the mass ratio of magnetic bio charcoal and chitosan reaction is 5:(1-5), further preferred 5:3；
Preferably, the highly basic is sodium hydroxide or potassium hydroxide；
Preferably, pH is adjusted as 8-11 after strong base solution is added dropwise, and further preferred pH is 10.
According to the present invention, the effect of step (3) is the magnetic bio charcoal for preparing surface and being covered with chitosan, considerably increases suction
Characteristic group's quantity on enclosure material surface, enhances adsorption capacity.
, according to the invention it is preferred to, the mass ratio of chitosan magnetism charcoal and EDTA are (2-8) in step (4): 4, into
The preferred 5:4 of one step；
Preferably, it is heated to 50-70 DEG C, further preferred 60 DEG C；After be cooled to 35-45 DEG C, further preferred 40
℃；
Preferably, the mole ratio of the EDAC and EDTA of addition are (1-3): 1, further preferred 2:1；
Preferably, the highly basic is sodium hydroxide or potassium hydroxide；EDAC and highly basic mole ratio are (0.5-1.5):
1, further preferred 1:1；
Preferably, NaOH solution, HCl solution, deionization washing, until pH value is neutrality are used in washing process respectively；Then
75 DEG C of drying, grind and sieve with 100 mesh sieve, obtain modification of chitosan magnetic bio charcoal, modification biological carbon adsorption material as of the present invention
Material.
According to the present invention, the effect of step (4) is to prepare modification of chitosan magnetic bio charcoal adsorbent material.Pass through amidation
EDTA is connected to chitosan magnetism charcoal surface by reaction, enhances adsorption energy while having added adsorbent material chemical stability
Power.
According to the present invention, the modification biological charcoal adsorbent material that the above method is prepared, the Pb in removal waste water2+In answer
With.
Application according to the present invention, it is preferred that removal Pb2+The step of it is as follows:
Modification biological charcoal adsorbent material is taken, addition contains Pb2+Waste water in, rotation concussion absorption, it is additional after the completion of absorption
Magnetic field separates adsorbent material.
Application according to the present invention, it is preferred that the quality of modification biological charcoal adsorbent material and the volume ratio of waste water are 0.5-
1.5g/L.Preferably, adjust wastewater pH be 5-6 removal effect more preferably.
According to the present invention, the adsorbent material has adsorbed Pb2+Afterwards, it is recycled outside plus under magnetic field condition, it is molten in the HCl of 1M
Stirring desorption repeatedly, does not measure Pb until examining in solution in liquid2+.Solution filtering, is washed with deionized and is in filtrate for several times
Property, it can be recycled after filter cake drying.
The present invention assigns magnetic by dipping, and limit oxygen is pyrolyzed to obtain the magnetic bio charcoal for being easy to collect；Pass through chitosan and magnetism
Charcoal reaction covers chitosan in magnetic bio carbon surface, can increase the adsorption capacity to heavy metal ion；By to shell
The chemical modification of glycan magnetic bio carbon surface, greatly strengthens while increasing adsorbent material chemical stability to heavy metal
The adsorption capacity of ion.
The beneficial effects of the present invention are:
1, modification of chitosan magnetic bio charcoal adsorbent material of the invention be using agricultural solid residue as raw material, save at
This while, can effectively reduce its arbitrarily accumulation and burning bring problem of environmental pollution, realize the resource of agricultural solid residue
Change and utilizes.
2, modification of chitosan magnetic bio charcoal adsorbent material of the invention, to Pb in water body2+Adsorbance height it is reachable
158.6mg/g, externally-applied magnetic field is i.e. recyclable, can be recycled after desorption.Material therefor is easy to degrade, without secondary pollution, environment
Compatibility is good.
3, modification of chitosan magnetic bio charcoal adsorbent material preparation process of the invention is relatively easy, with short production cycle, easily
Industrialized production is realized in popularizing.
Detailed description of the invention
Fig. 1 is the surface sweeping electron microscope of modification of chitosan magnetic bio charcoal adsorbent material of the invention.
Fig. 2 is modification of chitosan magnetic bio charcoal adsorbent material of the invention in the separating effect outside plus under magnetic field condition
Figure.
Specific embodiment
The present invention is described in further detail below, but the claimed scope of the invention is not limited to embodiment
The range of expression.
Embodiment 1.
The FeCl of 100ml 2M is added in the reed straw that 30g is pulverized and sieved3Solution stirs 2h at room temperature.80 after filtering
Aging 2h at DEG C.
It is then placed in crucible, 5 DEG C/min in nitrogen atmosphere stove, rises to 500 DEG C, constant temperature keeps 2h.It grinds and sieves with 100 mesh sieve
Magnetic bio charcoal is obtained, MC is labeled as.
Taking 1g to be added dissolved with adjusting pH after in the 100ml2% acetum of 0.6 chitosan, stirring 1h afterwards is 10, and room temperature is stirred
16h is mixed, crushes and sieves with 100 mesh sieve after being filtered, washed, drying, is labeled as CMC.
It takes 1.0g and 0.8g EDTA to be cooled to 40 DEG C after 60 DEG C of stirring 4h in 50ml deionized water again, is separately added into
The sodium hydroxide solution and 0.96g EDAC of 5ml1M, continue stir 1h, the static 16h of room temperature, be filtered, washed, dry after crushed
100 meshes obtain modification of chitosan magnetic bio charcoal, are labeled as CCMC.
The Pb that the pH of 25ml 200mg/L is 6 is added in the modification of chitosan magnetic bio charcoal for taking 25mg to prepare2+The cone of solution
In shape bottle, in 25 DEG C of revolving speeds be vibrated in 110 revs/min of constant-temperature table for 24 hours, externally-applied magnetic field by adsorbent material from solution
Separation.With Pb in atomic absorption detecting solution2+Concentration, calculate adsorbance.
Embodiment 2.
As described in Example 1, unlike: using corncob for raw material, final modification of chitosan magnetic bio charcoal
Labeled as CCMC-1.
Embodiment 3.
As described in Example 1, unlike: using cotton stalk for raw material, final modification of chitosan magnetic bio
Charcoal is labeled as CCMC-2.
Embodiment 4:
As described in Example 1, unlike:
When preparing MC, temperature rises to 300 DEG C, and constant temperature keeps 2h, and final modification of chitosan magnetic bio charcoal is labeled as
CCMC-3。
Embodiment 5:
As described in Example 1, unlike:
When preparing CMC, the quality of chitosan and MC are the final modification of chitosan magnetic bio charcoal of 1g labeled as CCMC-
4。
Embodiment 6:
As described in Example 1, unlike:
When preparing CCMC, 0.5gEDTA is added, final modification of chitosan magnetic bio charcoal is labeled as CCMC-5.
Embodiment 7:
As described in Example 1, unlike:
When preparing CCMC, it is separately added into the sodium hydroxide solution and 0.38g EDAC of 2ml1M, final modification of chitosan magnetic
Property charcoal be labeled as CCMC-6.
Embodiment 8:
As described in Example 1, unlike: when being adsorbed with CCMC, Pb2+The pH of solution is 2.
Comparative example 1:
As described in Example 1, unlike: being added without chitosan-modified and the later period modifying and decorating.
Comparative example 2:
As described in Example 1, unlike: the not no EDTA modifying and decorating in later period after chitosan-modified.
Test example
By embodiment 1-8 and comparative example 1-2, different modification of chitosan magnetic bio charcoals is tested to Pb2+Adsorbance is such as
Shown in table 1, the same embodiment is under condition of different pH to Pb2+Adsorbance is as shown in table 2.
The different modification of chitosan magnetic bio charcoal of table 1. is to Pb2+Adsorbance
| Label | Modification of chitosan magnetic bio charcoal | Pb2+Adsorbance (mg/g) |
| Embodiment 1 | CCMC | 158.6 |
| Embodiment 2 | CCMC-1 | 149.3 |
| Embodiment 3 | CCMC-2 | 151.9 |
| Embodiment 4 | CCMC-3 | 126.8 |
| Embodiment 5 | CCMC-4 | 143.8 |
| Embodiment 6 | CCMC-5 | 130.5 |
| Embodiment 7 | CCMC-6 | 113.4 |
| Comparative example 1 | CM | 3.3 |
| Comparative example 2 | CMC | 16.6 |
Table 2.CCMC is under condition of different pH to Pb2+Adsorbance
| Label | pH | Pb2+Absorption |
| Embodiment 8 | 2 | 142.5 |
| Embodiment 1 | 6 | 158.6 |
By table 1,2 it is found that different raw material, temperature and throwing amount compare last Pb2+Adsorbance have certain shadow
It rings；Chitosan-modified and the later period modification is to Pb2+Adsorbance have a significant impact, change by modified of the invention
Property chitosan magnetism charcoal is to Pb2+Adsorbance significantly improves.Under acid condition, the change Pb of pH2+Adsorbance also have shadow
It rings, but influences little.
The technical means disclosed in the embodiments of the present invention further includes technical side consisting of any combination of the above technical features
Case.For those skilled in the art, without departing from the principle of the present invention, several improvement can also be made and repaired
Decorations, these improvement and modification are also considered as protection scope of the present invention.
Claims (10)
1. a kind of preparation method of modification biological charcoal adsorbent material, comprises the following steps that
(1) biological material is crushed, is placed in FeCl3In solution, stir evenly, after filtering, aging；
(2) biological material after aging is pyrolyzed in nitrogen atmosphere in 200-600 DEG C, after natural cooling, grinding obtains magnetic green
Object charcoal；
(3) magnetic biological carbon is added in the aqueous acetic acid of chitosan, is stirred evenly, strong base solution reaction is added dropwise, filters,
Solid is washed to neutrality, dry, and grinding obtains chitosan magnetic biological carbon；
(4) chitosan magnetic biological carbon and ethylenediamine tetra-acetic acid (EDTA) are added to the water, heat temperature raising stirring adds after cooling
Enter strong base solution and 1- ethyl -3- (3- DimethylAminopropyl) carbodiimide hydrochloride (EDAC) reaction, after the reaction was completed mistake
Filter, it is dry after solid washing, it grinds to get modification biological charcoal adsorbent material.
2. the preparation method of modification biological charcoal adsorbent material according to claim 1, which is characterized in that institute in step (1)
The biological material stated is reed straw, corn stover, corncob, cotton stalk, rice husk or peanut shell；
Preferably, biological material is crushed to 1-3mm；
Preferably, FeCl3The concentration of solution is 1-3mol/L；
Preferably, biological material and FeCl3Mass ratio be 1:1.
3. the preparation method of modification biological charcoal adsorbent material according to claim 1, which is characterized in that old in step (1)
The temperature of change is 70-90 DEG C, ageing time 1-3h.
4. the preparation method of modification biological charcoal adsorbent material according to claim 1, which is characterized in that hot in step (2)
Solving temperature is 450-550 DEG C.
5. the preparation method of modification biological charcoal adsorbent material according to claim 1, which is characterized in that step (2) pyrolysis
Heating rate in the process is 3-10 DEG C/min, pyrolysis time 1-5h.
6. the preparation method of modification biological charcoal adsorbent material according to claim 1, which is characterized in that shell in step (3)
In the aqueous acetic acid of glycan, the mass fraction of chitosan is 1%-3%；
Preferably, the mass ratio of magnetic bio charcoal and chitosan reaction is 5:(1-5).
7. the preparation method of modification biological charcoal adsorbent material according to claim 1, which is characterized in that institute in step (3)
The highly basic stated is sodium hydroxide or potassium hydroxide；
Preferably, pH is adjusted after strong base solution is added dropwise as 8-11.
8. the preparation method of modification biological charcoal adsorbent material according to claim 1, which is characterized in that shell in step (4)
The mass ratio of glycan magnetic bio charcoal and EDTA are (2-8): 4；
Preferably, it is heated to 50-70 DEG C；After be cooled to 35-45 DEG C；
Preferably, the mole ratio of the EDAC and EDTA of addition are (1-3): 1；
Preferably, the highly basic is sodium hydroxide or potassium hydroxide；EDAC and highly basic mole ratio are (0.5-1.5): 1；
Preferably, NaOH solution, HCl solution, deionization washing, until pH value is neutrality are used in washing process respectively；Then 75 DEG C
Drying, grinds and sieves with 100 mesh sieve, obtain modification of chitosan magnetic bio charcoal to get modification biological carbon adsorbing material.
9. modification biological charcoal adsorbent material made from a kind of any one of claim 1-8 preparation method.
10. modification biological charcoal adsorbent material as claimed in claim 9, the Pb in removal waste water2+In application；
Preferably, Pb is removed2+The step of it is as follows:
Modification biological charcoal adsorbent material is taken, addition contains Pb2+Waste water in, rotation concussion absorption, externally-applied magnetic field after the completion of absorption
Magnetic Isolation adsorbent material.
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Cited By (8)
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| CN110117038A (en) * | 2019-06-05 | 2019-08-13 | 清华大学深圳研究生院 | A kind of selective absorption and the method for recycling heavy metal in sewage |
| CN110124639A (en) * | 2019-06-05 | 2019-08-16 | 清华大学深圳研究生院 | The chitosan of carboxyl grafting and biological carbon composite and its preparation method and application |
| CN110124638A (en) * | 2019-06-05 | 2019-08-16 | 清华大学深圳研究生院 | The chitosan of grafted by quaternary ammonium group and biological carbon composite and its preparation method and application |
| CN111111612A (en) * | 2019-12-19 | 2020-05-08 | 燕山大学 | Preparation and use method of magnetic porous biochar for removing chromium in water |
| CN112516965A (en) * | 2020-12-16 | 2021-03-19 | 河南省科学院生物研究所有限责任公司 | Preparation method and application of adsorbent for heavy metals of lead and chromium |
| CN112934831A (en) * | 2021-02-09 | 2021-06-11 | 北京理工大学 | Treatment method for plant straw material, prepared filter material and application |
| CN115465851A (en) * | 2022-06-01 | 2022-12-13 | 北京化工大学 | Synergistic application method for conditioning red soil by modified biomass carbon/humus/chemical fertilizer |
| CN117339566A (en) * | 2023-09-08 | 2024-01-05 | 东北大学 | Potassium dihydrogen phosphate modified co-pyrolysis biochar-chitosan, preparation method and application |
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Cited By (10)
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|---|---|---|---|---|
| CN110117038A (en) * | 2019-06-05 | 2019-08-13 | 清华大学深圳研究生院 | A kind of selective absorption and the method for recycling heavy metal in sewage |
| CN110124639A (en) * | 2019-06-05 | 2019-08-16 | 清华大学深圳研究生院 | The chitosan of carboxyl grafting and biological carbon composite and its preparation method and application |
| CN110124638A (en) * | 2019-06-05 | 2019-08-16 | 清华大学深圳研究生院 | The chitosan of grafted by quaternary ammonium group and biological carbon composite and its preparation method and application |
| CN110117038B (en) * | 2019-06-05 | 2021-08-27 | 清华大学深圳研究生院 | Method for selectively adsorbing and recovering heavy metals in sewage |
| CN111111612A (en) * | 2019-12-19 | 2020-05-08 | 燕山大学 | Preparation and use method of magnetic porous biochar for removing chromium in water |
| CN112516965A (en) * | 2020-12-16 | 2021-03-19 | 河南省科学院生物研究所有限责任公司 | Preparation method and application of adsorbent for heavy metals of lead and chromium |
| CN112934831A (en) * | 2021-02-09 | 2021-06-11 | 北京理工大学 | Treatment method for plant straw material, prepared filter material and application |
| CN115465851A (en) * | 2022-06-01 | 2022-12-13 | 北京化工大学 | Synergistic application method for conditioning red soil by modified biomass carbon/humus/chemical fertilizer |
| CN115465851B (en) * | 2022-06-01 | 2023-12-19 | 北京化工大学 | Synergistic application method of modified biomass carbon/humus/fertilizer conditioned red soil |
| CN117339566A (en) * | 2023-09-08 | 2024-01-05 | 东北大学 | Potassium dihydrogen phosphate modified co-pyrolysis biochar-chitosan, preparation method and application |
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Application publication date: 20190118 |