WO2019009216A1 - Ｖｏｃ処理用触媒 - Google Patents

Ｖｏｃ処理用触媒 Download PDF

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Publication number
WO2019009216A1
WO2019009216A1 PCT/JP2018/024929 JP2018024929W WO2019009216A1 WO 2019009216 A1 WO2019009216 A1 WO 2019009216A1 JP 2018024929 W JP2018024929 W JP 2018024929W WO 2019009216 A1 WO2019009216 A1 WO 2019009216A1
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Prior art keywords
catalyst
cobalt
platinum
voc
composite oxide
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PCT/JP2018/024929
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English (en)
French (fr)
Japanese (ja)
Inventor
研一郎 井上
正一 染川
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地方独立行政法人東京都立産業技術研究センター
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Priority to CN201880029094.1A priority Critical patent/CN110621399A/zh
Publication of WO2019009216A1 publication Critical patent/WO2019009216A1/ja

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    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
    • B01D53/34—Chemical or biological purification of waste gases
    • B01D53/74—General processes for purification of waste gases; Apparatus or devices specially adapted therefor
    • B01D53/86—Catalytic processes
    • 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
    • B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
    • B01J23/70—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper
    • B01J23/89—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper combined with noble metals
    • 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
    • B01J37/00—Processes, in general, for preparing catalysts; Processes, in general, for activation of catalysts
    • 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
    • B01J37/00—Processes, in general, for preparing catalysts; Processes, in general, for activation of catalysts
    • B01J37/08—Heat treatment
    • 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
    • Y02A50/00—TECHNOLOGIES FOR ADAPTATION TO CLIMATE CHANGE in human health protection, e.g. against extreme weather
    • Y02A50/20—Air quality improvement or preservation, e.g. vehicle emission control or emission reduction by using catalytic converters

Definitions

  • the present invention relates to a platinum directly supported cobalt-cerium composite oxide catalyst for volatile organic compound (VOC) processing.
  • VOC Volatile Organic Compounds
  • various methods such as direct combustion method, catalytic combustion method, physicochemical adsorption method, biological treatment method, plasma method, etc. have been proposed.
  • catalytic combustion method has equipment and maintenance management It is widely used because it is relatively easy.
  • the inventors of the present invention have proposed that a cobalt-cerium composite oxide catalyst is effective for VOC treatment and a new catalyst loading method in Patent Documents 1 to 3 shown below. As a result, low cost and performance equal to or higher than that of a platinum catalyst can be ensured.
  • an aromatic compound such as toluene is about 200 to 250 ° C. Although it can be processed at relatively low temperature, ethyl acetate and the like not containing an aromatic ring need to be processed at a high temperature of about 300 to 350.degree.
  • VOCs containing no aromatic ring can be treated at a relatively low temperature of about 200 to 250 ° C., but they are aromatic
  • the treatment of the compound needs to be carried out at a high temperature of about 300.degree.
  • new catalysts have been developed for new applications for simultaneously treating both VOCs in a temperature range lower than 300 ° C. Challenges have arisen.
  • the inventors of the present invention who carried out earnest studies to solve the above problems directly support a cobalt-cerium composite oxide catalyst, more preferably support a predetermined amount of platinum by a method of using a colloidal solution as a raw material. It has been found that the low temperature activity of the cobalt-cerium composite oxide catalyst is further enhanced by the combination. The details will be described below. It should be noted that, regardless of the category of the invention, definitions of terms etc., which are performed when describing the invention according to any claim, are also included in the invention according to the other claims within the scope permitted by nature regardless of the description order etc. It shall apply.
  • the present invention is intended to solve these problems, and is an invention relating to a catalyst for VOC treatment in which high activity at low temperature regardless of containing an aromatic ring is sustainable.
  • the catalyst for treating VOCs proposed in the present invention By using the catalyst for treating VOCs proposed in the present invention, performance can be secured at a lower temperature as compared with commercially available platinum alumina catalysts and cobalt / cerium composite oxide catalysts. This makes it possible to reduce the cost of electricity and fuel by lowering the processing temperature in a factory or the like, and to put into practical use a compact catalyst processing apparatus for homes and offices. Furthermore, by expanding the application to the processing technology field of the low temperature specification catalyst, which could not be dealt with by the existing catalyst, it can contribute to the improvement of the air environment and the indoor environment. Further, according to the production method proposed in the present invention, the above-mentioned catalyst for treating VOC can be produced.
  • the invention according to claim 1 is most characterized in that it relates to a VOC treatment catalyst in which platinum is directly supported on a cobalt-cerium composite oxide, for gas combustion treatment containing VOC.
  • the mass ratio of the cobalt-cerium composite oxide in the mass of the entire catalyst is 80% or more, and the content of platinum in the mass of the cobalt-cerium composite oxide is a (unit: mass%).
  • the range of 0 ⁇ a ⁇ 20 is preferable. That is, conventionally, platinum was supported on a carrier such as aluminum oxide, but the catalyst for treating VOC according to the present invention is a novel combination in which the catalyst is directly supported on a cobalt-cerium-based oxide. is there.
  • the VOC treatment catalyst includes both of those which are not supported by the inert carrier, and the mass thereof when supported is the mass of the inert carrier.
  • the invention according to claim 2 is characterized in that, as a preferable embodiment of the invention according to claim 1, the platinum relates to a catalyst for treating VOC which uses a solution of platinum colloid protected with a dispersant as a raw material. is there.
  • a dispersing agent polyvinyl pyrrolidone (Polyvinylpyrrolidone, PVP) can be used suitably, for example.
  • the catalyst is molded with a binder component, or stainless steel, steel, copper alloy, aluminum alloy, and ceramics having a desired shape.
  • the carrier is characterized in that it is supported by any one carrier of the material.
  • the invention according to claim 4 is the method for producing a catalyst for treating VOC according to any one of claims 1 to 3, wherein the cobalt-cerium composite oxide is a carbonate of cobalt and cerium as a precursor.
  • the compound is characterized by being calcined at 300 to 500 ° C. in air and then pulverized.
  • the invention according to claim 5 is a method for treating VOC using the catalyst for treating VOC according to any one of claims 1 to 3, wherein the operating temperature is 100 to 300 ° C.
  • the catalyst for treating VOC according to any one of claims 1 to 3 it is possible to treat in the low temperature region.
  • the catalyst for treating VOC according to the present invention is a catalyst in which platinum is directly supported on a cobalt-cerium composite oxide, for gas combustion treatment containing VOC.
  • the mass ratio of the cobalt-cerium composite oxide occupying in the mass of the entire catalyst is 80% or more, and the content of platinum in the mass of the cobalt-cerium composite oxide is a (unit: mass%)
  • the range of 0 ⁇ a ⁇ 20 is preferable. If it is outside the above range, platinum aggregation tends to occur, which is not desirable.
  • the VOC treatment catalyst includes both of those which are not supported on an inert carrier (including a binder, hereinafter the same), and the mass when supported is the mass of the inert carrier described later. Not included.
  • the cobalt-cerium composite oxide can be produced by calcining a compound having a carbonate of cobalt and cerium as a precursor at 300 to 500 ° C. in air, and then grinding. Pulverization process collapses pores, especially micropores, on the cobalt-cerium composite oxide, thereby improving the diffusivity of the platinum colloid protected by the dispersant described later and causticizing the platinum uniformly on the surface. It is believed that the amount will decrease. Micropores refer to pores having a pore diameter of 2 nm or less, but the amount of coking can be more efficiently reduced by collapsing the pores. The reduction of the amount of coking makes high activity sustainable at low temperatures.
  • the platinum is preferably made of a solution of platinum colloid protected with a dispersant.
  • the reason for using a platinum colloid solution as a raw material is considered to be advantageous in terms of enhancing the dispersibility of platinum particles to be supported.
  • a protective agent of platinum colloid polyvinyl poloridone is suitable, but it does not prevent using polymers other than polyvinyl poloridone, a ligand, a micelle, etc. besides it, for example.
  • the catalyst is formed by molding with a binder component, or supported on an inert carrier of stainless steel, steel, copper alloy, aluminum alloy, or ceramic material of a desired shape. You may In the former case, when the powder or powder molded catalyst is loaded into the catalyst packed bed, clogging of the packed bed due to the reduction of voids can be avoided.
  • the operating temperature of the VOC treatment using the VOC treatment catalyst having the above-described structure is preferably in the range of 100 to 300.degree. This is because if the above-mentioned catalyst for VOC treatment is used, VOC treatment can be performed without exceeding 300 ° C. If this state is maintained, electricity costs and fuel costs can be reduced as compared with the conventional processing method. In other words, operating above 300 ° C. is not preferable unless there is a special circumstance, since it dilutes the characteristics that the above-mentioned VOC treatment catalyst can be treated even at low temperatures. Operating temperatures below 100 ° C. should be avoided as they are prone to coking buildup.
  • the catalyst performance was evaluated in the following manner for both Example 1 and Comparative Examples 1 to 3.
  • a catalyst-filled tube installed in a tubular electric furnace equipped with a heater as shown in FIG. 1 was filled with a VOC treatment catalyst, and a VOC-containing gas was allowed to flow continuously through this packed bed.
  • the composition of the VOC-containing gas was such that dry air contained a vapor of toluene or ethyl acetate, and the concentrations of toluene and ethyl acetate were 400 ppm and 900 ppm, respectively, and the dry air flow rate was 100 mL ⁇ min ⁇ 1 .
  • the prepared catalyst powder was pelletized, crushed to a suitable size, and packed so as not to clog the packing tube.
  • the temperature of the catalyst packed bed was adjusted by adjusting the heater temperature of the tubular electric furnace. The temperature was raised to 300 ° C. in toluene combustion and to 400 ° C. in ethyl acetate combustion, and the temperature was maintained for 1 hour, and then the temperature was lowered by 1 ° C. in 1 minute to 30 ° C. When the temperature was lowered, the concentration of carbon dioxide in the gas and the concentration of toluene or ethyl acetate were measured using a gas chromatograph equipped with a thermal conductivity detector.
  • the coking formation evaluation of the catalyst was performed as follows in both Example 1 and Comparative Example 4. Similarly, a catalyst filled tube installed in a tubular electric furnace shown in FIG. 1 was filled with a catalyst, and dry air (VOC-containing gas) containing a vapor of toluene was continuously circulated in the packed bed. The concentration of toluene was 400 ppm, and the flow rate of dry air was 100 mL ⁇ min ⁇ 1 . The prepared catalyst powder was pelletized, crushed to a suitable size, and packed so as not to clog the packing tube. The temperature of the catalyst layer was adjusted using a tubular electric furnace. After raising the temperature to 150 ° C.
  • the temperature was maintained for 24 hours, dry air containing toluene vapor was continuously circulated, and combustion of toluene was continued. Thereafter, the temperature is lowered to 30 ° C. by flowing only dry air, and the temperature is raised by 1 ° C. per minute to 300 ° C. while flowing only the dry air, and the generation of carbon dioxide accompanying combustion of coking accumulated on the catalyst surface is It measured by the gas chromatograph with a conductivity detector.
  • the catalyst processing temperature (combustion temperature) is largely different between the aromatic VOC and the VOC containing no aromatic ring.
  • the test was conducted by selecting toluene as a typical VOC of aromatics and ethyl acetate as a typical VOC containing no aromatic ring. Focusing on the combustion temperature at which the generation rate of CO 2 reaches 90 to 100%, the temperature at which the catalyst can be processed was organized.
  • the temperature at which the CO 2 generation rate of ethyl acetate reaches 90 to 100% is about 200 to 250 ° C.
  • Cerium carbonate was calcined in air at 300 ° C. for 1 hour to prepare cerium oxide, and pulverized using a wet crusher (planet type ball mill Classic Line P-7 manufactured by Fritsch Japan Ltd.).
  • the median diameter before grinding is 23.3 ⁇ m
  • the median diameter after grinding is 0.415 ⁇ m It was m.
  • the pore distribution before and after grinding was measured using BELSORP-max manufactured by Microtrac Bell Inc.
  • the sample after grinding was immersed in an aqueous solution of platinum colloid (manufactured by Tanaka Kikinzoku Kogyo Co., Ltd.) protected by polyvinyl pyrrolidone, and the solution was evaporated and dried while being stirred and heated.
  • the dried sample and cobalt oxide were mixed, the temperature was gradually raised by 0.9 ° C. in 1 minute in air, and the final catalyst was calcined at 300 ° C. for 1 hour to obtain a target catalyst.
  • the platinum loading was 2% by weight relative to the cobalt-cerium composite oxide.

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  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Materials Engineering (AREA)
  • Organic Chemistry (AREA)
  • Environmental & Geological Engineering (AREA)
  • Thermal Sciences (AREA)
  • Physics & Mathematics (AREA)
  • Health & Medical Sciences (AREA)
  • Biomedical Technology (AREA)
  • Analytical Chemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Oil, Petroleum & Natural Gas (AREA)
  • Catalysts (AREA)
  • Exhaust Gas Treatment By Means Of Catalyst (AREA)
PCT/JP2018/024929 2017-07-05 2018-06-29 Ｖｏｃ処理用触媒 WO2019009216A1 (ja)

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JP2017131884A JP7119256B2 (ja) 2017-07-05 2017-07-05 Ｖｏｃ処理用触媒の製造方法、ｖｏｃ処理方法及びｖｏｃ処理用触媒

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CN114269473A (zh) * 2019-08-14 2022-04-01 地方独立行政法人东京都立产业技术研究中心 Voc处理用催化剂的制造方法

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CN114797463B (zh) * 2022-05-30 2023-12-26 中国科学院过程工程研究所 一种烧结烟气co催化换热串联中低温scr脱硝的装置系统及方法

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Publication number Priority date Publication date Assignee Title
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