CN102872871A - Catalytic agent for catalytic oxidation of elemental mercury in coal-fired flue gas and preparation method thereof - Google Patents
Catalytic agent for catalytic oxidation of elemental mercury in coal-fired flue gas and preparation method thereof Download PDFInfo
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- CN102872871A CN102872871A CN2012103497322A CN201210349732A CN102872871A CN 102872871 A CN102872871 A CN 102872871A CN 2012103497322 A CN2012103497322 A CN 2012103497322A CN 201210349732 A CN201210349732 A CN 201210349732A CN 102872871 A CN102872871 A CN 102872871A
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Abstract
The invention discloses a catalytic agent for the catalytic oxidation of elemental mercury in a coal-fired flue gas, which adopts Ti-PILC as a carrier, and a CoO and Fe2O3 compound oxide as a main active component. The invention also discloses a catalytic agent preparation technology. The catalytic agent has specific excellent performances on the oxidization of the elemental mercury, such as high activity, less dose, low cost, high thermal stability and favorable sulfur resistance, can effectively convert the elemental mercury which is difficult to remove in the flue gas into a bivalent mercury which can be captured by a dust remover and a desulfuration device under a lower HC1 concentration, and is suitable for the desorption field of the mercury and the chemical compound thereof in the coal-fired flue gas.
Description
Technical field
The present invention relates to a kind of catalyst, be specifically related to a kind of catalyst for the elemental mercury from coal-fired flue gas catalytic oxidation, the invention still further relates to the preparation method of this catalyst.
Background technology
It is the Important Problems that environmental protection for electric power faces that the atmosphere pollution of coal-fired power plant is controlled always; after the emission control of the dust in coal-fired flue-gas, oxysulfide (SOx), nitrogen oxide (NOx), the mercury in flue gas is subject to extensive concern gradually.Mercury is a kind of poisonous traces of heavy metals element, has the characteristics such as deposition and hysteresis length in hypertoxicity, high volatile volatile, organism, and the mercury that enters ecological environment can produce long-term harm, to human health and ecological environment, causes very big harm.Mercury content in China's coal is high, and the consumption of coal amount is large, and the mercury pollution problem becomes increasingly conspicuous, and it is imperative that the coal-fired flue-gas mercury pollution is controlled.The up-to-date fossil-fuel power plant atmospheric pollutant emission standard (GB 13223-2011) that China formulates is using mercury as new discharge index, and the emission limit of regulation mercury and mercuric compounds is 0.03mg/m
3.
Mercury in coal-fired plant flue gas is mainly with particle mercury, oxidation state mercury (Hg
2+, Hg
+) and elemental mercury (Hg
0) etc. three kinds of forms exist.General particle mercury is easy to be collected by deduster; Hg
2+soluble in water, can be removed by wet desulphurization device; And Hg
0because volatility is higher, water-soluble lower, be insoluble to acid, be difficult to be removed by the existing environmental protection facility of thermal power plant.The Main Morphology of China's Mercury In Coal Combustion Flue Gas is Hg
0, therefore to Hg
0control become the Important Problems of flue gas demercuration.
At present, various countries show the research of coal-fired unit mercury pollution control technology, and the charcoal absorption demercuration is a kind of effectively mercury pollution control technology, but due to it, to remove cost higher, is difficult to apply in engineering reality.If can take some measures Hg
0be oxidized to Hg
2+, then by deduster and wet desulphurization device, to be removed be more feasible flue gas demercuration mode, and wherein the mode of applications catalyst catalytic oxidation Elemental Mercury is comparatively economical, and the exploitation of corresponding catalyst also becomes current research emphasis.
But at present mainly to take aluminium oxide, titanium dioxide, zirconium dioxide, silica etc. be carrier to the flue gas demercuration catalyst of research, cost of manufacture is high, and catalyst amount is large, is not suitable for applying on a large scale.
Summary of the invention
First purpose of the present invention is to provide a kind of catalyst for the elemental mercury from coal-fired flue gas catalytic oxidation, to Elemental Mercury, oxidation has special excellent properties to this catalyst, activity is high, consumption is few, cost is low, and the heat endurance of catalyst is high, there is good anti-sulphur property, just can effectively the Elemental Mercury that is difficult in flue gas removing be converted into to the divalence mercury that can be trapped by deduster and desulfurizer under low HCl concentration, be applicable to Mercury In Coal Combustion Flue Gas and compound removes field.
Second purpose of the present invention is to provide the preparation method of the above-mentioned catalyst for the elemental mercury from coal-fired flue gas catalytic oxidation.
First purpose of the present invention is achieved through the following technical solutions: a kind of catalyst for the elemental mercury from coal-fired flue gas catalytic oxidation, using titanium layer post clay as carrier, CoO and Fe
2o
3composite oxides are main active component.
The total load capacity of main active component of the present invention is 5～10%(mass percent), described CoO and Fe
2o
3mass ratio be 0.25～4.
The present invention can do following improvement: described catalyst also comprises active component auxiliary agent CeO
2, its load capacity in catalyst is 0.5～2%(mass percent).
Catalyst provided by the invention is cellular or board-like.
Also can do following improvement in the present invention: in described titanium layer post clay, the Ti/clay ratio is 10 ~ 20mmol/g, and wherein clay refers to clay.
Main active component of the present invention adopts the ion-exchange mode of loading to be carried on titanium layer post clay, and active component auxiliary agent CeO
2infusion process is carried on titanium layer post clay.
The present invention can make further improvements: described titanium layer post clay is adopt following methods to prepare and obtain:
(1) will be through the NaCl solution sodium for imvite of purifying, the ratio of sodium ion and imvite is 2～10mmol/g, static 1h after 65 ℃ of stirring 2h, so repeatedly operate 3～5 times after standing over night; Suction filtration, the gained decorating film uses the distilled water cyclic washing extremely without Cl
?till, 110 ℃ of dry 2h, grind, and makes the sodium imvite;
(2) drip titanium tetrachloride solution and constantly stir in hydrochloric acid solution, the mol ratio of titanium tetrachloride and hydrochloric acid is 1 ~ 5, and the concentration of hydrochloric acid solution is 1 ~ 6mol/L, after dropping finishes, in room temperature, continues to stir 3h, ageing 12h, make aging good as clear as crystal titanium crosslinkers;
(3) under room temperature and strong agitation, aging good titanium crosslinkers slowly is added drop-wise in the sodium montmorillonite suspension liquid, the Ti/clay ratio is 10 ~ 20mmol/g, stirring reaction 12h, standing 12h, suction filtration, the gained decorating film with the distilled water cyclic washing to without Cl
?till, 110 ℃ of drying 12 h, grind, and at Muffle furnace Program intensification roasting 3 ~ 6h, naturally cools to normal temperature, makes titanium layer post clay.
Temperature-programmed calcination in described step (3) is divided into two stages: first the speed with 1～10 ℃/min is warming up to 300 ℃ of roasting 1～3h, and then the speed with 1～10 ℃/min is warming up to 400 ℃ of roasting 2～3h.
Second goal of the invention of the present invention is achieved through the following technical solutions: a kind of preparation method of the catalyst for the elemental mercury from coal-fired flue gas catalytic oxidation comprises the following steps:
(1) will be through the NaCl solution sodium for imvite of purifying, the ratio of sodium ion and imvite is 2～10mmol/g, static 1h after 65 ℃ of stirring 2h, so repeatedly operate 3～5 times after standing over night; Suction filtration, the gained decorating film uses the distilled water cyclic washing extremely without Cl
?till, 110 ℃ of dry 2h, grind, and makes the sodium imvite;
(2) drip titanium tetrachloride solution and constantly stir in hydrochloric acid solution, the mol ratio of titanium tetrachloride and hydrochloric acid is 1 ~ 5, and the concentration of hydrochloric acid solution is 1 ~ 6mol/L, after dropping finishes, in room temperature, continues to stir 3h, ageing 12h, make aging good as clear as crystal titanium crosslinkers;
(3) under room temperature and strong agitation, aging good titanium crosslinkers slowly is added drop-wise in the sodium montmorillonite suspension liquid, the Ti/clay ratio is 10 ~ 20mmol/g, stirring reaction 12h, standing 12h, suction filtration, the gained decorating film with the distilled water cyclic washing to without Cl
?till, 110 ℃ of drying 12 h, grind, and at Muffle furnace Program intensification roasting 3 ~ 6h, naturally cools to normal temperature, makes titanium layer post clay;
(4) at 60 ℃, active component nitrate solution and titanium layer post clay are carried out to ion-exchange reactions 6 h, 110 ℃ of drying 12 h, at Muffle furnace Program intensification roasting 3 ~ 5h, naturally cool to normal temperature, make the catalyst for the elemental mercury from coal-fired flue gas catalytic oxidation.
The present invention can do following improvement, also comprise step (5): the catalyst soakage that step (4) is made is in cerium nitrate solution, and 110 ℃ of drying 12 h after dipping 2h under room temperature, at Muffle furnace Program intensification roasting 3 ~ 5h, naturally cool to normal temperature, CeO in catalyst
2load capacity is finally 0.5 ~ 2%.
The quality of cerium nitrate solution of the present invention minute concentration is 0.5 ~ 10%.
Temperature-programmed calcination in described step (3), (4) and (5) is divided into two stages: first the speed with 1～10 ℃/min is warming up to 300 ℃ of roasting 1～3h, and then the speed with 1～10 ℃/min is warming up to 400 ℃ of roasting 2～3h.
The clay loaded cobalt of the titanium layer post that the present invention makes-iron compound oxide catalyst material has higher heat endurance and mechanical strength, therefore, the present invention also comprises step (6), the described catalyst for the elemental mercury from coal-fired flue gas catalytic oxidation is prepared to cellular or plate type integrated demercuration catalyst through extrusion molding, to be suitable for actual applying.
compared with prior art, the present invention has following beneficial effect:
(1) to Elemental Mercury, oxidation has special excellent properties in the present invention, activity is high, consumption is few, cost is low, and the heat endurance of catalyst is high, there is good anti-sulphur property, just can effectively the Elemental Mercury that is difficult in flue gas removing be converted into to the divalence mercury that can be trapped by deduster and desulfurizer under low HCl concentration, be applicable to Mercury In Coal Combustion Flue Gas and compound removes field.In laboratory simulation smoke test result, show, in the temperature range of 300 ~ 400 ℃, this catalyst to the oxygenation efficiency of Elemental Mercury more than 85%.
(2) to adopt titanium layer post clay be carrier in the present invention, to Hg
0excellent absorption property is arranged.
Take the titanium layer post clay of layer column structure for the catalyst of catalytic oxidation Elemental Mercury in the present invention is carrier.Described titanium layer post clay is a kind of material of molecular sieve analog structure, has high-specific surface area, large aperture, high micropore amount, heat endurance and the higher good characteristics such as surface acidity preferably, especially has excellent especially performance aspect the Elemental Mercury catalytic oxidation.Titanium layer post clay is made by montmorillonite and titanium based cross-linker post.Can obtain abundant column duct in the post process, existing a large amount of micropore, also have a lot of mesopores or macropore, thereby greatly improved specific area.On the one hand, abundant duct is conducive to the distribution of active component in catalyst, makes active component cobalt-ferriferous oxide not only be distributed in catalyst surface, also extensively is distributed in duct, thereby has greatly increased Hg
0the active site position of catalytic oxidation.On the other hand, more importantly, Hg
0oxidation at catalyst surface is controlled by adsorption process often, and through the laminated clay column that forms after the titanium crosslink there is special complex surface characteristic, even, Hg large in exhaust gas volumn
0under the actual flue gas condition of the low and smoke components complexity of content, titanium layer post clay itself is also to Hg
0show excellent absorption property, under the synergy of metal oxide active component, the catalyst integral body that the titanium layer post clay of take is carrier is to Hg
0there is very high catalytic oxidation activity.Therefore, with respect to other catalyst carrier, titanium layer post clay is more suitable for preparing Hg
0oxidation catalyst.
(3) in catalyst of the present invention, itself has higher activity to the Elemental Mercury catalytic oxidation active component Co and Fe, and both are in conjunction with mutually promoting, and strengthen the redox ability of whole catalyst.The auxiliary agent Ce further added not only can strengthen the anti-SO of catalyst effectively
2ability, and CeO
2lattice there is the ability that stores oxygen, in the catalytic oxidation process, can provide oxygen to main active component Co-Fe composite oxides, thereby further improve the activity of catalyst.Because this catalyst activity is very high, therefore can greatly reduce the consumption in actual use procedure, and catalyst carrier take imvite as main, also can reduce TiO
2deng consumption, demonstrate good economy.
(4) catalyst provided by the invention is cellular or board-like, is very suitable for actual applying.
The specific embodiment
embodiment 1
1. Ti-PILCs is synthetic
The sodium of imvite: take 50g through pretreated imvites such as 200 mesh sieves of purifying, ground, add lmol/L NaCl solution 200ml, standing 1h after 65 ℃ of stirring 2h; Add again lmol/L NaCl solution 100ml, standing 1h after 65 ℃ of stirring 2h; Add again l mol/L NaCl solution 50ml, standing over night after 65 ℃ of stirring 2h.Suction filtration, decorating film use the distilled water cyclic washing extremely without Cl
?till, 110 ℃ of dry 2h, grinding, can obtain the sodium imvite.
The preparation of titanium crosslinkers: under room temperature and vigorous stirring, by 50ml TiCl
4solution slowly is added drop-wise in the hydrochloric acid solution of 2.5 mol/L of 100ml, drips after finishing and continues to stir 3h in room temperature, and ageing 12 h, obtain as clear as crystal titanium crosslinkers standby.
The preparation of titanium layer post clay: take the imvite of 50g sodium and be made into 1000ml soil liquid, respectively by Ti/clay than being 10,15, during 20mmol/g slowly is added drop-wise to montmorillonite suspension liquid by aging good titanium crosslinkers under room temperature and strong agitation, stirring reaction 12 h, standing 12 h.Suction filtration, decorating film use the distilled water cyclic washing extremely without Cl
?till, 110 ℃ of drying 12 h, grind, and 400 ℃ of lower roasting 3 h, make titanium layer post clay.
2.Ti-PILCs load active component Co-Fe composite oxides, preparation Co (4%)-Fe (1%)-Ti-PILCs catalyst:
Take 9.7g Ti-PILCs, at 60 ℃, to contain a certain amount of cobalt nitrate, ferric nitrate is water-soluble, again nitrate solution and titanium layer post clay are carried out to ion-exchange reactions 6 h, the bead that to make diameter after reaction be 6～8mm is in 110 ℃ of drying 12 h, and after temperature programming to 400 ℃, roasting 5 h obtain 4%CoO-1%Fe
2o
3catalyst, be designated as Co (4%)-Fe (1%)-Ti-PILCs.
Get above catalyst 5mL and pack in tubular fixed-bed quartz reactor (φ 9mm), pass into simulated flue gas, concrete composition is NO 300ppm, NH
3300ppm, O
2be 5%, Hg
0for 0.3mg/m
3, HCl is 5ppm, SO
2for 500ppm, all the other are N
2, temperature is 350 ℃, the control gas space velocity is 40000h
-1investigate catalyst under condition to Hg
0oxidation activity.The results are shown in Table 1.
embodiment 2
1. Ti-PILCs is synthetic, and Ti/clay is than being the titanium layer post clay of 15mmol/g in preparation, and all the other are with embodiment 1.
2. Ti-PILCs load active component Co-Fe composite oxides obtain the Co-Fe-Ti-PILCs catalyst:
According to embodiment 1, adopt ion-exchange to prepare the catalyst that the 10g active component is the Co-Fe composite oxides, wherein the two accounts for catalyst gross mass ratio and is respectively 8%CoO-2% Fe
2o
3, 2%CoO-8% Fe
2o
3, 4%CoO-1% Fe
2o
3, 4%CoO-4% Fe
2o
3, be designated as Co-Fe-Ti-PILCs.
Catalyst 5mL is packed in tubular fixed-bed quartz reactor (φ 9mm), pass into simulated flue gas, concrete composition is NO 300ppm, NH
3300ppm, O
2be 5%, Hg
0for 0.3mg/m
3, HCl is 5ppm, SO
2for 500ppm, all the other are N
2, temperature is 350 ℃, the control gas space velocity is 40000h
-1investigate catalyst under condition to Hg
0oxidation activity.The results are shown in Table 2.
embodiment 3
Preparing active component by existing infusion process is 8%CoO-2% Fe
2o
3, carrier is respectively TiO
2, SiO
2, Al
2o
3catalyst.Get the 8%CoO-2% Fe in embodiment 2
2o
3catalyst and above-mentioned catalyst contrasted.
Each catalyst 5mL gets respectively in the tubular fixed-bed quartz reactor of packing into (φ 9mm), passes into simulated flue gas, and concrete composition is NO 300ppm, NH
3300ppm, O
2be 5%, Hg
0for 0.3mg/m
3, HCl is 5ppm, SO
2for 500ppm, all the other are N
2, temperature is 350 ℃, the control gas space velocity is 40000h
-1investigate catalyst under condition to Hg
0oxidation activity.The results are shown in Table 3.
embodiment 4
Get the 8%CoO-2% Fe in embodiment 2
2o
3catalyst, adopt infusion process to prepare the Ce/Co-Fe-Ti-PILCs catalyst:
1. take 9.95gCo-Fe-Ti-PILCs, in the cerium nitrate solution that to be impregnated in the 9.5g mass concentration be 1%, 110 ℃ of dry 12h after dipping 2h under room temperature, after temperature programming to 400 ℃, roasting 5h obtains CeO
2the Ce/Co-Fe-Ti-PILCs catalyst that content is 0.5wt%, standby;
2. take 9.90gCo-Fe-Ti-PILCs, in the cerium nitrate solution that to be impregnated in the 19g mass concentration be 1%, 110 ℃ of dry 12h after dipping 2h under room temperature, after temperature programming to 400 ℃, roasting 5h obtains CeO
2the Ce/Co-Fe-Ti-PILCs catalyst that content is 1wt%, standby;
3. take 9.85gCo-Fe-Ti-PILCs, in the cerium nitrate solution that to be impregnated in the 28.5g mass concentration be 1%, 110 ℃ of dry 12h after dipping 2h under room temperature, after temperature programming to 400 ℃, roasting 5h obtains CeO
2the Ce/Co-Fe-Ti-PILCs catalyst that content is 1.5wt%, standby;
4. take 9.80gCo-Fe-Ti-PILCs, in the cerium nitrate solution that to be impregnated in the 38g mass concentration be 1%, 110 ℃ of dry 12h after dipping 2h under room temperature, after temperature programming to 400 ℃, roasting 5h obtains CeO
2the Ce/Co-Fe-Ti-PILCs catalyst that content is 2wt%, standby;
Below 1. catalyst ~ is 4. got respectively 5mL and is packed in tubular fixed-bed quartz reactor (φ 9mm), passes into simulated flue gas, and concrete composition is NO 300ppm, NH
3300ppm, O
2be 5%, Hg
0for 0.3mg/m
3, HCl is 5ppm, SO
2for 500ppm, all the other are N
2, temperature is 350 ℃, the control gas space velocity is 40000h
-1investigate catalyst under condition to Hg
0oxidation activity.The results are shown in Table 4.
The present invention can summarize with other the concrete form without prejudice to spirit of the present invention or principal character.Above-mentioned embodiment of the present invention all can only be thought explanation of the present invention rather than restriction, therefore every foundation essence technology of the present invention is done above embodiment any trickle modification, equivalent variations and modification, all belong in the scope of technical solution of the present invention.
Claims (10)
1. the catalyst for the elemental mercury from coal-fired flue gas catalytic oxidation, is characterized in that, usings titanium layer post clay as carrier, CoO and Fe
2o
3composite oxides are main active component.
2. the catalyst for the elemental mercury from coal-fired flue gas catalytic oxidation according to claim 1, is characterized in that, the total load capacity of described main active component is 5～10%, described CoO and Fe
2o
3mass ratio be 0.25～4.
3. the catalyst for the elemental mercury from coal-fired flue gas catalytic oxidation according to claim 1 and 2, is characterized in that, described catalyst also comprises active component auxiliary agent CeO
2, its load capacity in catalyst is 0.5～2%.
4. the catalyst for the elemental mercury from coal-fired flue gas catalytic oxidation according to claim 3, is characterized in that, in described titanium layer post clay, the Ti/clay ratio is 10 ~ 20mmol/g.
5. the catalyst for the elemental mercury from coal-fired flue gas catalytic oxidation according to claim 1 and 2, is characterized in that, described titanium layer post clay is adopt following methods to prepare and obtain:
(1) will be through the NaCl solution sodium for imvite of purifying, the ratio of sodium ion and imvite is 2～10mmol/g, static 1h after 65 ℃ of stirring 2h, so repeatedly operate 3～5 times after standing over night; Suction filtration, the gained decorating film uses the distilled water cyclic washing extremely without Cl
?till, 110 ℃ of dry 2h, grind, and makes the sodium imvite;
(2) drip titanium tetrachloride solution and constantly stir in hydrochloric acid solution, the mol ratio of titanium tetrachloride and hydrochloric acid is 1 ~ 5, and the concentration of hydrochloric acid solution is 1 ~ 6mol/L, after dropping finishes, in room temperature, continues to stir 3h, ageing 12h, make aging good as clear as crystal titanium crosslinkers;
(3) under room temperature and strong agitation, aging good titanium crosslinkers slowly is added drop-wise in the sodium montmorillonite suspension liquid, the Ti/clay ratio is 10 ~ 20mmol/g, stirring reaction 12h, standing 12h, suction filtration, the gained decorating film with the distilled water cyclic washing to without Cl
?till, 110 ℃ of drying 12 h, grind, and at Muffle furnace Program intensification roasting 3 ~ 6h, naturally cools to normal temperature, makes titanium layer post clay.
6. the catalyst for the elemental mercury from coal-fired flue gas catalytic oxidation according to claim 1, it is characterized in that, temperature-programmed calcination in described step (3) is divided into two stages: first the speed with 1～10 ℃/min is warming up to 300 ℃ of roasting 1～3h, and then the speed with 1～10 ℃/min is warming up to 400 ℃ of roasting 2～3h.
7. the preparation method for the catalyst of elemental mercury from coal-fired flue gas catalytic oxidation, is characterized in that, comprises the following steps:
(1) will be through the NaCl solution sodium for imvite of purifying, the ratio of sodium ion and imvite is 2～10mmol/g, static 1h after 65 ℃ of stirring 2h, so repeatedly operate 3～5 times after standing over night; Suction filtration, the gained decorating film uses the distilled water cyclic washing extremely without Cl
?till, 110 ℃ of dry 2h, grind, and makes the sodium imvite;
(2) drip titanium tetrachloride solution and constantly stir in hydrochloric acid solution, the mol ratio of titanium tetrachloride and hydrochloric acid is 1 ~ 5, and the concentration of hydrochloric acid solution is 1 ~ 6mol/L, after dropping finishes, in room temperature, continues to stir 3h, ageing 12h, make aging good as clear as crystal titanium crosslinkers;
(3) under room temperature and strong agitation, aging good titanium crosslinkers slowly is added drop-wise in the sodium montmorillonite suspension liquid, the Ti/clay ratio is 10 ~ 20mmol/g, stirring reaction 12h, standing 12h, suction filtration, the gained decorating film with the distilled water cyclic washing to without Cl
?till, 110 ℃ of drying 12 h, grind, and at Muffle furnace Program intensification roasting 3 ~ 6h, naturally cools to normal temperature, makes titanium layer post clay;
(4) described main active component adopts the ion-exchange mode of loading to be carried on titanium layer post clay, makes the catalyst for the elemental mercury from coal-fired flue gas catalytic oxidation.
8. the preparation method of the catalyst for the elemental mercury from coal-fired flue gas catalytic oxidation according to claim 8, is characterized in that, also comprises step (5), by active component auxiliary agent CeO
2adopt infusion process to be carried on the titanium layer post clay of the catalyst that step (4) makes.
9. the preparation method of according to Claim 8 or 9 or the 10 or 11 described catalyst for the elemental mercury from coal-fired flue gas catalytic oxidation, it is characterized in that, described temperature-programmed calcination is divided into two stages: first the speed with 1～10 ℃/min is warming up to 300 ℃ of roasting 1～3h, and then the speed with 1～10 ℃/min is warming up to 400 ℃ of roasting 2～3h.
10. the preparation method of the catalyst for the elemental mercury from coal-fired flue gas catalytic oxidation according to claim 8, it is characterized in that, also comprise step (6), the described catalyst for the elemental mercury from coal-fired flue gas catalytic oxidation is prepared to cellular or plate type integrated demercuration catalyst through extrusion molding.
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| CN110694474A (en) * | 2019-11-25 | 2020-01-17 | 徐书敏 | Green and low-cost flue gas demercuration method |
| CN110833830A (en) * | 2019-11-25 | 2020-02-25 | 徐书敏 | Method for preparing demercuration catalyst by using natural ore soil and waste residues |
| CN112973667A (en) * | 2021-03-05 | 2021-06-18 | 河南康宁特环保科技股份有限公司 | Novel titanium dioxide doped modified layer columnar clay denitration catalyst and preparation method thereof |
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