CN101413241A - Ecological environment protection type pavement tile and producing process thereof - Google Patents
Ecological environment protection type pavement tile and producing process thereof Download PDFInfo
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- CN101413241A CN101413241A CNA2007101574751A CN200710157475A CN101413241A CN 101413241 A CN101413241 A CN 101413241A CN A2007101574751 A CNA2007101574751 A CN A2007101574751A CN 200710157475 A CN200710157475 A CN 200710157475A CN 101413241 A CN101413241 A CN 101413241A
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02A—TECHNOLOGIES FOR ADAPTATION TO CLIMATE CHANGE
- Y02A30/00—Adapting or protecting infrastructure or their operation
- Y02A30/60—Planning or developing urban green infrastructure
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02W—CLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO WASTEWATER TREATMENT OR WASTE MANAGEMENT
- Y02W30/00—Technologies for solid waste management
- Y02W30/50—Reuse, recycling or recovery technologies
- Y02W30/91—Use of waste materials as fillers for mortars or concrete
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Abstract
The invention belongs to the field of environment-friendly energy-saving building materials, and in particular relates to an ecological environment-friendly footway brick and a production process thereof. The brick comprises a brick body (1), and is characterized in that the upper surface of the brick body (1) is provided with a groove (3); the position of the groove (3) of the brick body (1) is provided with a through hole (2) in the longitudinal direction; the brick body adopts materials (1) comprising a cementitious material, aggregate and activator; the cementitious material contains slag micro-powder, red mud, C-type fly ash and kieselguhr; the aggregate adopts waste residue particles; and the activator contains polycarboxylic acid water reducing agent, power plant desulphurization gypsum, aluminum sulfate slag and fly ash. The production process comprises two parts of: 1) preparing raw materials according to the requirements, and 2) physically molding, which is to install a column-type body on a brick press mold, have the through hole (2) when the brick is physically molded and extrude the groove (3) on the surface of the brick body. The footway brick has the advantages of simple structure and high water seepage efficiency, and can effectively reduce urban heat island effect.
Description
Technical field
The invention belongs to the environment-friendly and energy-efficient building materials field, relate in particular to a kind of ecological environment protection type pavement tile.
Background technology
At present, domestic and international permeable type pavement brick can roughly be divided into following several types:
1) from maintenance method: 1. fire type; 2. steam and press (supporting) type; 3. non-evaporating pressure (supporting) type.
2) material from adopting: 1. cementitious material adopts cement based; 2. bonding adhesive coheres type.3. aggregate adopts high-quality natural sand.
3) on function of use: exist characteristics such as function singleness mostly, as adopt clearance-type infiltration mode, it can seep water, but slow evaporation, though this brick body infiltration, the brick surface does not have hole, and summer, brick surface temperature was through shining upon, temperature is up to more than 40 ℃, to reducing the urban heat land effect DeGrain; Though the brick body that also has is porose, its design is unreasonable, and the efficient that seeps water is low and be unfavorable for walking and environmental protection.
Comprehensive above-mentioned all kinds of pavement bricks, its major defect is:
(1), the cost height, ceramic water-permeable brick will be set up curing kilns and fire, and expends a large amount of fuel;
(2), be that non-evaporating foster type pavement brick expends cement, and later strength is bad, causes durability to descend;
(3), when facing than heavy rainfall, its permeable speed is slow;
(4), adopt cement-based material, by aggregate hole infiltration type pavement brick, its resistance to freezing and thawing is poor, corrosion-vulnerable;
(5), adopt the pavement brick of bonding adhesive, strict to aggregate, cost height, and complex process are not easy to popularize.
(6), because brick laying structure design is unreasonable, its infiltration efficient is low and be unfavorable for walking and environmental protection.
Summary of the invention
The present invention is intended to overcome the deficiencies in the prior art part and provides a kind of simple in structure, and infiltration efficient height can effectively reduce the ecological environment protection type pavement tile and the production technology thereof of urban heat land effect.
For achieving the above object, the present invention can realize according to following mode:
Ecological environment protection type pavement tile comprises the brick body; Its main feature is to be furnished with groove at the upper surface of described brick body; On described brick body groove location, vertically be provided with through hole.
As a kind of preferred version, through hole of the present invention can be frustum cone structure; Described groove can be designed to the closed endless groove in three roads.Through hole of the present invention can be 12~24.
As the third preferred version, the material that brick body of the present invention adopts comprises cementitious material, aggregate and activator; Described cementitious material contains slag micropowder, red mud, C class flyash and kieselguhr; Described aggregate adopts the waste residue particulate; Described activator contains polycarboxylate water-reducer, power plant desulfurization gypsum, aluminium sulfate slag and flyash.
As the 4th kind of preferred version, slag micropowder, red mud, C class flyash and diatomaceous weight ratio are followed successively by 60~90:5~9:7~15:1~5 in the cementitious material of the present invention; Particle diameter 5mm<d<the 8mm of described waste residue particulate; The weight ratio of polycarboxylate water-reducer, power plant desulfurization gypsum, aluminium sulfate slag and flyash is followed successively by 2~8:10~40:10~20:30~60 in the described activator.
As the 5th kind of preferred version, the weight ratio of cementitious material of the present invention and aggregate is 0.5~3:2~8; The weight ratio of activator and cementitious material is 0.5~5:80~120.
The production technology of above-mentioned ecological environment protection type pavement tile comprises the steps:
A) carrying out raw material prepares:
(1), cementitious material contains slag micropowder, red mud, C class flyash and kieselguhr; Slag micropowder, red mud, C class flyash and diatomaceous weight ratio are followed successively by 60~90:5~9:7~15:1~5 in the described cementitious material;
(2), aggregate adopts the waste residue particulate; Particle diameter 5mm<d<the 8mm of described waste residue particulate;
(3), activator contains polycarboxylate water-reducer, power plant desulfurization gypsum, aluminium sulfate slag and flyash; The weight ratio of polycarboxylate water-reducer, power plant desulfurization gypsum, aluminium sulfate slag and flyash is followed successively by 2~8:10~40:10~20:30~60 in the described activator; The weight ratio of cementitious material and water is 80~120:20~35 in the above-mentioned raw materials;
B) physics moulding:
The column type body is installed on the brick machine mould, when making the moulding of brick physics, is stayed through hole; Extrude groove in the brick surface.
The present invention is owing to be furnished with 12~24 circular platform type entire body holes on the brick body, the rainy day seepage velocity is fast, can guarantee phreatic timely recurrence, keeps groundwater table, is beneficial to soil respiration simultaneously again, regulates air quality.In addition, when implementing the porous design, can suitably add the diameter of macropore being beneficial under the condition of walking, this increases the anion concentration of urban air for the evaporation efficiency that improves underground water steam, promotes that winter, snow-broth returned underground certain positive effect that all has.
Compared with prior art, the present invention has following characteristics:
(1), adopts easy manufacture craft, with low cost, do cementitious material and the aggregate cost is low with full waste residue and waste residue micro mist, and (hydration reaction of waste residue will slowly carry out for a long time to make pavement brick good endurance with the silicate-base cementitious material, particularly under moist and environment that humidity is bigger, be beneficial to the later stage growth of its compressive strength, need not fire, fuel saving, free from environmental pollution.
The cost of 1 brick: 0.1 yuan (0.185 yuan/piece of solid brick); 1M
2The cost of brick: 2.5 yuan; 1M
3The cost of brick: 57.84 yuan.Produce 50000 M per year
3Full waste residue porous, permeablely, ventilative, little ooze, the cost of ecological, environmental protective brick: 2,900,000 yuan.The economic benefit of comparing: save 2,250,000 yuan with use solid brick, burned brick and river sand brick; Utilize various waste residues 〉=45,000 ton.
(2), adopt new structure design, brick body to have 12~24 not to wait down greatly upward little many entire bodies hole, the rainy day seepage velocity is fast, the maintenance groundwater table is beneficial to soil respiration.
(3), be convenient to produce and popularize.
(4), air-borne dust gets back to ground with rainwater and moisture, enters micropore, purify air.Studies show that: adopt full waste residue porous, permeablely, ventilative, little ooze, ecological, environmental protective brick pavement road and square, the area of cement floor will be reduced, (the asphalt floor temperature can reach 58 ℃ summer can to reduce city temperature in summer, the cement floor will reach 45 ℃, and just about 30 ℃ on soil property ground), compare with 100% atresia cement based pavement brick, can reduce urban heat land effect 21~42%.
(5), adopt this design can save material 20~40%, the brick body weight is reasonable, the anti-degree that rolls does not descend.
(6), brick body of the present invention also has little function of oozing, because of aggregate adopt approximate simple grain level waste particle (5~8mm), connect the graded aggregate that do not have between the aggregate, cementitious material just, like this, brick laying structure presents open structure, can make the water infiltration of brick surface.If use blast-furnace cinder micro-powder, waste residue micro mist etc., this little oozing is convenient to the further aquation of brick body, forms silicate aquation product, strengthened the intensity of brick, adds the entire body hole, can guarantee not influence its infiltration and evaporation.
(7), use blast-furnace cinder micro-powder to do cementitious material, may worry to influence its time of setting, just in view of this consideration, the designer just uses activator to excite its early strength, facts have proved, the index of this cementitious material and PO cement or PS cement is approaching, application development situation according to product, can suitably add water glass or other rapid hardening, excite component, make its early hydration, and take into account the later strength growth.
Ecological brick and solid brick factory formula (C30) and material cost contrast
Performance indications
Description of drawings
The invention will be further described below in conjunction with the drawings and specific embodiments.Protection scope of the present invention will not only be confined to the statement of following content.
Fig. 1 is overall structure figure of the present invention;
Fig. 2 is through hole overall structure figure of the present invention.
The specific embodiment
Embodiment 1
As shown in Figure 1, ecological environment protection type pavement tile comprises brick body 1; Is furnished with groove 3 at the upper surface of described brick body 1; On described brick body 1 groove 3 positions, vertically be provided with through hole 2.As shown in Figure 2, through hole 2 of the present invention is a frustum cone structure.Described groove 3 is the closed endless grooves of twice.Described through hole 2 is 20.
The material that brick body 1 of the present invention adopts comprises cementitious material, aggregate and activator; Described cementitious material contains slag micropowder, red mud, C class flyash and kieselguhr; Described aggregate adopts the waste residue particulate; Described activator contains polycarboxylate water-reducer, power plant desulfurization gypsum, aluminium sulfate slag and flyash.Slag micropowder, red mud, C class flyash and diatomaceous weight ratio are followed successively by 60kg:5kg:7kg:1kg in the described cementitious material; The particle diameter d of described waste residue particulate is 6mm; The weight ratio of polycarboxylate water-reducer, power plant desulfurization gypsum, aluminium sulfate slag and flyash is followed successively by 2kg:10kg:10kg:30kg in the described activator.The weight ratio of described cementitious material and aggregate is 0.5kg:2kg; The weight ratio of activator and cementitious material is 0.5kg:80kg.
The production technology of above-mentioned ecological environment protection type pavement tile is characterized in that, comprises the steps:
A) carrying out raw material prepares:
(1), cementitious material contains slag micropowder, red mud, C class flyash and kieselguhr; Slag micropowder, red mud, C class flyash and diatomaceous weight ratio are followed successively by 60kg:5kg:7kg:1kg in the described cementitious material;
(2), aggregate adopts the waste residue particulate; The particle diameter d of described waste residue particulate is 6mm;
(3), activator contains polycarboxylate water-reducer, power plant desulfurization gypsum, aluminium sulfate slag and flyash; The weight ratio of polycarboxylate water-reducer, power plant desulfurization gypsum, aluminium sulfate slag and flyash is followed successively by 2kg:10kg:10kg:30kg in the described activator;
The weight ratio of cementitious material and water is 80kg:20kg in the above-mentioned raw materials;
B) physics moulding:
The column type body is installed on the brick machine mould, when making the moulding of brick physics, is stayed through hole 2; Extrude groove 3 in the brick surface.
As shown in Figure 1, ecological environment protection type pavement tile comprises brick body 1; Is furnished with groove 3 at the upper surface of described brick body 1; On described brick body 1 groove 3 positions, vertically be provided with through hole 2.Described through hole 2 is a frustum cone structure.Described groove 3 is the closed endless grooves in three roads.Described through hole 2 is 24.
The material that brick body 1 of the present invention adopts comprises cementitious material, aggregate and activator; Described cementitious material contains slag micropowder, red mud, C class flyash and kieselguhr; Described aggregate adopts the waste residue particulate; Described activator contains polycarboxylate water-reducer, power plant desulfurization gypsum, aluminium sulfate slag and flyash.Slag micropowder, red mud, C class flyash and diatomaceous weight ratio are followed successively by 90kg:9kg:15kg:5kg in the described cementitious material; The particle diameter d of described waste residue particulate is 7mm; The weight ratio of polycarboxylate water-reducer, power plant desulfurization gypsum, aluminium sulfate slag and flyash is followed successively by 8kg:40kg:20kg:60kg in the described activator.The weight ratio of described cementitious material and aggregate is 3kg:8kg; The weight ratio of activator and cementitious material is 5kg:120kg.
The production technology of above-mentioned ecological environment protection type pavement tile comprises the steps:
A) carrying out raw material prepares:
(1), cementitious material contains slag micropowder, red mud, C class flyash and kieselguhr; Slag micropowder, red mud, C class flyash and diatomaceous weight ratio are followed successively by 90kg:9kg:15kg:5kg in the described cementitious material;
(2), aggregate adopts the waste residue particulate; The particle diameter d of described waste residue particulate is 7mm;
(3), activator contains polycarboxylate water-reducer, power plant desulfurization gypsum, aluminium sulfate slag and flyash; The weight ratio of polycarboxylate water-reducer, power plant desulfurization gypsum, aluminium sulfate slag and flyash is followed successively by 8kg:40kg:20kg:60kg in the described activator;
The weight ratio of cementitious material and water is 120kg:35kg in the above-mentioned raw materials;
B) physics moulding:
The column type body is installed on the brick machine mould, when making the moulding of brick physics, is stayed through hole 2; Extrude groove 3 in the brick surface, other are with common brickmaking technology.
Embodiment 3
Ecological environment protection type pavement tile comprises brick body 1; Is furnished with groove 3 at the upper surface of described brick body 1; On described brick body 1 groove 3 positions, vertically be provided with through hole 2.Described through hole 2 is a frustum cone structure.Described groove 3 is the closed endless grooves in three roads.Described through hole 2 is 18.
The material that brick body 1 of the present invention adopts comprises cementitious material, aggregate and activator; Described cementitious material contains slag micropowder, red mud, C class flyash and kieselguhr; Described aggregate adopts the waste residue particulate; Described activator contains polycarboxylate water-reducer, power plant desulfurization gypsum, aluminium sulfate slag and flyash.
Slag micropowder, red mud, C class flyash and diatomaceous weight ratio are followed successively by 80kg:7kg:10kg:3kg in the cementitious material of the present invention; The particle diameter d of described waste residue particulate is 7mm; The weight ratio of polycarboxylate water-reducer, power plant desulfurization gypsum, aluminium sulfate slag and flyash is followed successively by 6kg:20kg:15kg:40kg in the described activator.The weight ratio of described cementitious material and aggregate is 2kg:6kg; The weight ratio of activator and cementitious material is 3kg:90kg.
The production technology of above-mentioned ecological environment protection type pavement tile is characterized in that, comprises the steps:
A) carrying out raw material prepares:
(1), cementitious material contains slag micropowder, red mud, C class flyash and kieselguhr; Slag micropowder, red mud, C class flyash and diatomaceous weight ratio are followed successively by 80kg:7kg:10kg:3kg in the described cementitious material;
(2), aggregate adopts the waste residue particulate; The particle diameter d of described waste residue particulate is 7mm;
(3), activator contains polycarboxylate water-reducer, power plant desulfurization gypsum, aluminium sulfate slag and flyash; The weight ratio of polycarboxylate water-reducer, power plant desulfurization gypsum, aluminium sulfate slag and flyash is followed successively by 6kg:20kg:15kg:40kg in the described activator;
The weight ratio of cementitious material and water is 100:25 in the above-mentioned raw materials;
B) physics moulding:
12~24 column type bodies are installed on the brick machine mould, when making the moulding of brick physics, are stayed 12~24 through holes 2 (20mm on the diameter, following 30mm); Extrude 3 road annular recess 3 (5mm is wide, 5mm is dark) in the brick surface, be beneficial to infiltration, play anti-skidding effect again, other are with common brickmaking technology.
During tile work, at the thick rubble of the bottom on road surface shop 10cm or pulverize dry slag, thick river sand or the machine-processed broken slag of middle level shop 5cm, shop, upper strata calcium carbide ground-slag is an amount of or according to engine request, uses an amount of mortar.
Ecological environment protection type pavement tile can be by natural curing, also can adopt solar energy and artificial heat supply to squirt maintenance bin or the fly ash building block maintenance bin is carried out hydrothermal curing.
Claims (8)
1, ecological environment protection type pavement tile comprises brick body (1); It is characterized in that: be furnished with groove (3) at the upper surface of described brick body (1); On described brick body (1) groove (3) position, vertically be provided with through hole (2).
2, ecological environment protection type pavement tile according to claim 1 is characterized in that: described through hole (2) is a frustum cone structure.
3, ecological environment protection type pavement tile according to claim 1 and 2 is characterized in that: described groove (3) is the closed endless grooves in three roads.
4, ecological environment protection type pavement tile according to claim 3 is characterized in that: described through hole (2) is 12~24.
5, ecological environment protection type pavement tile according to claim 1 and 2 is characterized in that: the material that described brick body (1) adopts comprises cementitious material, aggregate and activator; Described cementitious material contains slag micropowder, red mud, C class flyash and kieselguhr; Described aggregate adopts the waste residue particulate; Described activator contains polycarboxylate water-reducer, power plant desulfurization gypsum, aluminium sulfate slag and flyash.
6, ecological environment protection type pavement tile according to claim 5 is characterized in that: slag micropowder, red mud, C class flyash and diatomaceous weight ratio are followed successively by 60~90:5~9:7~15:1~5 in the described cementitious material; Particle diameter 5mm<d<the 8mm of described waste residue particulate; The weight ratio of polycarboxylate water-reducer, power plant desulfurization gypsum, aluminium sulfate slag and flyash is followed successively by 2~8:10~40:10~20:30~60 in the described activator.
7, ecological environment protection type pavement tile according to claim 6 is characterized in that: the weight ratio of described cementitious material and aggregate is 0.5~3:2~8; The weight ratio of activator and cementitious material is 0.5~5:80~120.
8, the production technology of ecological environment protection type pavement tile according to claim 7 is characterized in that, comprises the steps:
A) carrying out raw material prepares:
(1), cementitious material contains slag micropowder, red mud, C class flyash and kieselguhr; Slag micropowder, red mud, C class flyash and diatomaceous weight ratio are followed successively by 60~90:5~9:7~15:1~5 in the described cementitious material;
(2), aggregate adopts the waste residue particulate; Particle diameter 5mm<d<the 8mm of described waste residue particulate;
(3), activator contains polycarboxylate water-reducer, power plant desulfurization gypsum, aluminium sulfate slag and flyash; The weight ratio of polycarboxylate water-reducer, power plant desulfurization gypsum, aluminium sulfate slag and flyash is followed successively by 2~8:10~40:10~20:30~60 in the described activator;
The weight ratio of cementitious material and water is 80~120:20~35 in the above-mentioned raw materials;
B) physics moulding:
The column type body is installed on the brick machine mould, when making the moulding of brick physics, is stayed through hole (2); Extrude groove (3) in the brick surface.
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CN2007101574751A CN101413241B (en) | 2007-10-16 | 2007-10-16 | Ecological environment protection type pavement tile and producing process thereof |
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CN2007101574751A CN101413241B (en) | 2007-10-16 | 2007-10-16 | Ecological environment protection type pavement tile and producing process thereof |
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CN101413241B CN101413241B (en) | 2010-07-21 |
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Cited By (6)
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CN102276219A (en) * | 2011-05-26 | 2011-12-14 | 四川方大新型建材科技开发有限责任公司 | Autoclaved red mud brick and preparation method thereof |
CN102381856A (en) * | 2010-09-03 | 2012-03-21 | 贵州省建筑材料科学研究设计院 | Red-mud non-fired non-steamed paving brick and preparation method thereof |
CN105218043A (en) * | 2014-06-26 | 2016-01-06 | 北科绿能有限公司 | Brick-shaped structural product and manufacturing method thereof and manufacturing method of flow channel structure contained in brick-shaped structural product |
CN108824115A (en) * | 2018-09-03 | 2018-11-16 | 佛山科学技术学院 | One kind is from breathing pattern ground brick paving brick |
CN109629389A (en) * | 2019-01-31 | 2019-04-16 | 招商局重庆交通科研设计院有限公司 | A kind of accurate curing system in road surface and its method |
CN111978096A (en) * | 2020-08-17 | 2020-11-24 | 浙江天地环保科技股份有限公司 | Fly ash-based ceramic water permeable brick sintered by two-step method and preparation method thereof |
Family Cites Families (7)
Publication number | Priority date | Publication date | Assignee | Title |
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GB395437A (en) * | 1932-02-12 | 1933-07-20 | Charles Alfred Lawson | Improvements in or relating to paving for roads |
CN2410321Y (en) * | 2000-01-24 | 2000-12-13 | 逯若愚 | Pavement brick |
CN2429551Y (en) * | 2000-06-02 | 2001-05-09 | 樊震波 | Environment protecting quick penetratable pavement |
CN2435422Y (en) * | 2000-08-10 | 2001-06-20 | 华南理工大学 | Floor brick capable of lowering temp. |
CN1232468C (en) * | 2003-11-28 | 2005-12-21 | 北京科技大学 | Preparation and using method of steel slag colorful pavement brick with water penetrating function |
CN100417767C (en) * | 2004-01-12 | 2008-09-10 | 谷曰能 | Permeable environmental protection ground tile used for outdoor service |
CN200971462Y (en) * | 2006-08-28 | 2007-11-07 | 罗举茂 | Surface porous typhlosole floor tile |
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- 2007-10-16 CN CN2007101574751A patent/CN101413241B/en not_active Expired - Fee Related
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CN102381856A (en) * | 2010-09-03 | 2012-03-21 | 贵州省建筑材料科学研究设计院 | Red-mud non-fired non-steamed paving brick and preparation method thereof |
CN102381856B (en) * | 2010-09-03 | 2013-09-04 | 贵州省建筑材料科学研究设计院 | Red-mud non-fired non-steamed paving brick and preparation method thereof |
CN102276219A (en) * | 2011-05-26 | 2011-12-14 | 四川方大新型建材科技开发有限责任公司 | Autoclaved red mud brick and preparation method thereof |
CN102276219B (en) * | 2011-05-26 | 2013-12-11 | 四川方大新型建材科技开发有限责任公司 | Autoclaved red mud brick and preparation method thereof |
CN105218043A (en) * | 2014-06-26 | 2016-01-06 | 北科绿能有限公司 | Brick-shaped structural product and manufacturing method thereof and manufacturing method of flow channel structure contained in brick-shaped structural product |
CN108824115A (en) * | 2018-09-03 | 2018-11-16 | 佛山科学技术学院 | One kind is from breathing pattern ground brick paving brick |
CN109629389A (en) * | 2019-01-31 | 2019-04-16 | 招商局重庆交通科研设计院有限公司 | A kind of accurate curing system in road surface and its method |
CN111978096A (en) * | 2020-08-17 | 2020-11-24 | 浙江天地环保科技股份有限公司 | Fly ash-based ceramic water permeable brick sintered by two-step method and preparation method thereof |
CN111978096B (en) * | 2020-08-17 | 2022-05-31 | 浙江天地环保科技股份有限公司 | Fly ash-based ceramic water permeable brick sintered by two-step method and preparation method thereof |
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