WO1996025229A1 - Catalyseur pour l'epuration des effluents gazeux industriels et des gaz d'echappement de vehicules automobiles - Google Patents

Catalyseur pour l'epuration des effluents gazeux industriels et des gaz d'echappement de vehicules automobiles Download PDF

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Publication number
WO1996025229A1
WO1996025229A1 PCT/CN1996/000016 CN9600016W WO9625229A1 WO 1996025229 A1 WO1996025229 A1 WO 1996025229A1 CN 9600016 W CN9600016 W CN 9600016W WO 9625229 A1 WO9625229 A1 WO 9625229A1
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Prior art keywords
catalyst
neodymium
halide
weight
tritium
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PCT/CN1996/000016
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English (en)
French (fr)
Inventor
Zhongshan Duan
Fengying Duan
Yongnian Lu
Fuxun Duan
Junwei Duan
Original Assignee
Zhongshan Duan
Fengying Duan
Yongnian Lu
Fuxun Duan
Junwei Duan
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Application filed by Zhongshan Duan, Fengying Duan, Yongnian Lu, Fuxun Duan, Junwei Duan filed Critical Zhongshan Duan
Priority to JP8524555A priority Critical patent/JPH11501863A/ja
Priority to DE59609190T priority patent/DE59609190D1/de
Priority to US08/894,264 priority patent/US6046129A/en
Priority to EP96902215A priority patent/EP0815938B1/de
Priority to AU46625/96A priority patent/AU4662596A/en
Publication of WO1996025229A1 publication Critical patent/WO1996025229A1/zh

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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
    • B01D53/92—Chemical or biological purification of waste gases of engine exhaust gases
    • B01D53/94—Chemical or biological purification of waste gases of engine exhaust gases by catalytic processes
    • B01D53/9445—Simultaneously removing carbon monoxide, hydrocarbons or nitrogen oxides making use of three-way catalysts [TWC] or four-way-catalysts [FWC]
    • B01D53/945—Simultaneously removing carbon monoxide, hydrocarbons or nitrogen oxides making use of three-way catalysts [TWC] or four-way-catalysts [FWC] characterised by a specific catalyst
    • 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
    • B01J23/76—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper combined with metals, oxides or hydroxides provided for in groups B01J23/02 - B01J23/36
    • B01J23/84—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper combined with metals, oxides or hydroxides provided for in groups B01J23/02 - B01J23/36 with arsenic, antimony, bismuth, vanadium, niobium, tantalum, polonium, chromium, molybdenum, tungsten, manganese, technetium or rhenium
    • B01J23/889—Manganese, technetium or rhenium
    • B01J23/8892—Manganese
    • 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
    • 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
    • Y02T—CLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO TRANSPORTATION
    • Y02T10/00—Road transport of goods or passengers
    • Y02T10/10—Internal combustion engine [ICE] based vehicles
    • Y02T10/12—Improving ICE efficiencies

Definitions

  • the invention relates to a tritium agent, and in particular, the present invention relates to a catalyst for purifying industrial exhaust gas and automobile exhaust.
  • Catalysts are still urgently needed. This is because, on the one hand, the conversion of CO and HC is a tritiated reaction, and the reaction of the conversion of NO x into emotional gases (N 2 ) is a reduction reaction. Therefore, the catalyst capable of converting these three types of substances must be capable of catalyzing tritium. Catalyst for reduction and reduction reactions.
  • Catalysts using non-noble metal elements have also been reported in the literature, but conversion at low temperatures There are still deficiencies in terms of efficiency, rapid conversion efficiency and longevity.
  • Some purification catalysts for automobile exhaust gas must be equipped with sensing devices and heating devices. And the composition and quantity ratio of its active components are greatly different from the catalyst of the present invention.
  • Non-precious metal honeycomb combustion catalyst which includes a dual carrier and a halide of copper, vanadium, manganese, cobalt, nickel, or a mixed gaseous composition of the above elements, and contains rare earth elements.
  • Plutonium compounds such as praseodymium, cerium, praseodymium, praseodymium, neodymium, yttrium, or mixtures thereof are used as active components.
  • 8 similar automobile exhaust purification catalyst includes a composite support of a honeycomb ceramic material and a hafnium coating, a mixture of one or more of the non-precious metal elements hafnium, cobalt, nickel, manganese, copper, and chromium, and a halide of a rare earth element.
  • the active component but in its preparation method, the active gaseous substance is reduced with tritium, monogasified carbon, and hydrocarbon compounds. In this way, it can be considered that some metal-free active gases are likely to be converted into metal elements.
  • this patent application a method of preparing the catalyst in the 700- 110 (TC of the firing process is undesirable because Y- A1 2 0 3 is in the amorphous 200- 600'C ⁇ - A1 2 0 3, which activity
  • ⁇ -A1 2 0 3 is the fixed ⁇ -A1 2 0 3 , which has poor activity and stability.
  • Ya-A1 2 0 3 is converted into inactive cx—Al 2 0 3 , which can easily fall off the support.
  • EP0393517A2 discloses catalytic trituration and reduction conversion for the conversion of exhaust gas from internal combustion engine engines, which can completely burn unburned hydrocarbons and monogasified carbon and reduce gaseous gases to elemental helium and tritium.
  • the converter uses Cr, Mn,
  • the catalyst contains one or more kinds of hafnium iron, cobalt hafnium, copper halide, chromium halide, manganese dihalide and nickel halide as active components.
  • a catalyst using at most three of the above-mentioned metal element halides as an active ingredient is disclosed.
  • the catalyst is prepared by impregnating the support with an aqueous solution of these metal salts (such as nitrate), and then drying and calcining to decompose the salt into the corresponding halide.
  • Another object of the present invention is to provide a catalyst for purifying industrial exhaust gas such as sulfide.
  • a third object of the present invention is to provide a method for preparing a catalyst for purifying industrial exhaust gas and automobile exhaust gas.
  • the present invention provides a catalyst for purifying automobile exhaust.
  • the catalyst includes a suitable support, which is characterized in that the catalyst includes copper (Cu), nickel (Ni), cobalt (Co), zinc (Zn), and chromium. (Cr), yttrium (Mn) and neodymium (Nd) halides and the composite halides formed by two or more of the above metal elements are active components, wherein the active components are based on the weight of the carrier with each metal element
  • the weight percentage of the compound meter is as follows:
  • the catalyst is characterized in that, based on the weight of the support, the weight percentage of the active component based on each metal element halide is as follows:
  • NiO Nickel
  • CoO Cobalt gasification
  • the catalyst of the present invention further includes ⁇ -A1 2 0 3 , which has a weight percentage of 2-12% based on the weight of the support.
  • the catalyst includes a suitable support, which is characterized in that the catalyst includes copper, zinc, nickel, cobalt, chromium, iron, manganese and The neodymium halide and two or more of the above-mentioned metal elements form a composite gaseous material as an active component, wherein the percentage of the active component based on the weight of the carrier is as follows:
  • the catalyst for purifying industrial exhaust gas according to the present invention is characterized in that the weight percentages of the active components based on the weight of the support in terms of each metal element halide are as follows:
  • CoO Cobalt gasification
  • the invention provides a method for preparing a catalyst for purifying automobile exhaust.
  • the catalyst includes a convenient carrier and copper (Cu) and nickel as active components.
  • weight active components of the support based on the halide of each metal element, are as follows:
  • the method includes impregnating a suitable carrier with an aqueous solution of a salt of copper, nickel, cobalt, zinc, manganese, and neodymium, and then taking out the soaked carrier, drying it at 70-120'C in air, and — Calcined at 600'C to prepare catalyst.
  • the catalyst prepared as described above is impregnated with an aqueous solution of ⁇ -Al 2 0 3 , and the leached catalyst is dried and calcined at 70-800'C to obtain a catalyst.
  • the metal salt may be any inorganic or organic salt that can form the corresponding metal halide or composite halide when calcined, preferably nitric acid, sulfuric acid, and phosphorus salt, and most preferably nitrate salt.
  • the total concentration of the aqueous solution of the salts of copper, nickel, cobalt, zinc, chromium, manganese and neodymium and the corresponding amounts of various metal salts should make the metal non-plutonium compounds formed by the decomposition of these salts and two or more of these metals Based on the weight of the support, the compound halide falls within the above range based on the individual metal element vapors.
  • the total concentration of the aqueous solution of the metal salt is 5-50% by weight based on the entire aqueous solution, 2-30% by weight of the copper salt, 1-15% by weight of the nickel salt, and 0% of the cobalt salt. 5— 8% (weight), Yu salt is 0.1-1%, zinc salt is 0.1 —20% by weight, chromium salt 0.05—1% by weight, and the rest are neodymium salts.
  • catalysts for purifying halide can be prepared.
  • the catalyst for purifying automobile exhaust gas and industrial exhaust gas prepared as described above is further impregnated with alkaline animal or vegetable oil or soap water, and then dried to obtain a household agent having the ability to remove lead.
  • Aqueous sodium stearate is used.
  • the support used as the catalyst of the present invention may be any suitable support in the art. It is preferred to use a ceramic support, more preferably a ceramic support having a dungite content of 92% and a water absorption of 35-
  • Example 1 A catalyst for purifying automobile exhaust was prepared.
  • Example 2 In a container, 100 ml of the standby solution prepared in Example 1 was added, 2 g of Fe (N0 3 ) 3 ⁇ 9H 2 0 and 20 g of Z ⁇ ( ⁇ 3) 2 were dissolved and stirred uniformly. 50g of ceramic carrier (Shanghai No. 2 Refractory Plant; pore size 300-400 mesh, specific surface area> 3m 2 / g) was immersed in the above solution for about 1 hour. The residual liquid was filtered off, and the soaked support was dried at 70-120'C, and then calcined in air at 120-600'C to obtain catalyst C.
  • ceramic carrier Sandhai No. 2 Refractory Plant; pore size 300-400 mesh, specific surface area> 3m 2 / g
  • the catalysts A, B, (::: Soap (Guben soap produced by Shanghai Fertility Soap)) were impregnated with the catalysts A, B, and 3 prepared in Examples 1, 2 and 3, respectively, and the corresponding catalysts D, E, and
  • the catalyst (support + active component) used weighed approximately 390 grams.
  • the catalyst is housed in a suitably modified car muffler.
  • the obtained catalyst A was tested by Beijing Ji Automobile Co., Ltd.
  • test was carried out in accordance with the US EPA-75 standard using Cherokee CX-1. Test conditions
  • the Japanese ONO SKKI chassis test machine accuracy is 2%.
  • FC-A-3 type dust sampler produced by Shanghai Hongwei Instrument Factory.
  • thermocouple temperature measuring instrument 4. Shanghai Chuansha Weifeng Thermal Engineering Co., Ltd. XMX-101 type thermocouple temperature measuring instrument.
  • the product was tested by the Shanghai Transportation Bureau's testing line, which was commissioned by the Shanghai Public Security Bureau's Transportation Corporation, when it traveled 35,000 and 36 thousand kilometers. From the test results, it was found that it was traveling 3.5
  • the CO and HC efficiencies of 10,000 kilometers and 98,000 kilometers were 99.6 and 99.8%, respectively, and 96.9% and 93.05 at 86,000 kilometers.
  • the product has been tested repeatedly for different kilometers, and it shows that it has good purification effect and long life.
  • the prepared catalyst F was used as a purifier and tested by Shanghai Environmental Monitoring Center.
  • CO and HC were measured by Foshan analyzer ⁇ Factory assembled Japanese HORIBA company MEMS 324F non-infrared infrared car exhaust gas detector, NOx, S0 2 were enriched with U-shaped glass absorption bottle, theophylamine hydrochloride colorimetry and hydrochloric acid were used Analytical colorimetric analysis of rosaniline is used.
  • the analytical instrument uses a Shimadzu UV-240 spectrophotometer. Pb is enriched with a glass fiber filter.
  • the atomic absorption method is used for analysis of Nissan Hitachi (HITACHI 180-70) atomic absorption spectrophotometer. .
  • Table 1 The data in Table 1 is converted into grams per mile and listed in Table 5 compared with the US-California FTP-75 emission standard and the Canadian emission standard.
  • the catalyst of the present invention can simultaneously purify tritiated carbon, carbon ammonium compound (HC) and nitrogen halide (NQx), and can purify sulfide and have the ability to remove lead. It can be started at low temperature and has one-way conversion. High rate, no need to install tritium sensors and heating radiators in the car exhaust pipe.

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  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Health & Medical Sciences (AREA)
  • Organic Chemistry (AREA)
  • Combustion & Propulsion (AREA)
  • Materials Engineering (AREA)
  • Biomedical Technology (AREA)
  • Environmental & Geological Engineering (AREA)
  • Analytical Chemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Oil, Petroleum & Natural Gas (AREA)
  • Catalysts (AREA)
  • Exhaust Gas Treatment By Means Of Catalyst (AREA)

Description

用于净化工业废气和汽车尾气的催化剂
技术领域
^明涉及伥化剂，具体地说，本发明涉及用于净化工业废气 和汽车尾气的催化剂。
背景技术
近年来，随着对环境的重视，许多国家通过立法制定各种废气 的排放标准， 因而促使人们研究转化各种废气的催化剂。随着工业 化的进程汽车成倍地增长，汽车废气已成为污染环境的一个主要 来源。据估计在美囯空气污染 60%来自各种汽车， 17%来自工业污 染。 汽车排出的废气主要是一氡化碳（CO)，未燃烧的碳氬化合物 (HC)和氣氡化物 (NQx)。 氮氣化物主要是 NO和 N02。 氮氡化物是 众所周知的破坏大气臭氡（ o3)层的物质，而臭氡层是太阳紫外线 过滤器。臭氡层的破坏会导致地球接受更多的紫外线。据信皮肤癌 与过多的接收紫外线辐照有关。
现在有许多催化剂针对净化汽车废气中的一氡化碳（CO)和碳 氳化合物（HC)，但对能同时净化一氡化碳（CO)，碳氳化合物（HC) 和氦氡化物 (NOx)的催化剂仍是迫切需要的。 这是因为一方面 CO 和 HC的转化是一个氡化反应，而 NOx的转化成情性气体（N2)的反 应是一个还原反应， 因而能转化这三类物质的催化剂必须是能催 化氡化和还原反应的催化剂。 另一方面，对于能同时转化这三种气 体的催化剂，对汽车发动机提出了很苛刻的操作条件（如燃气比应 保持严格的化学计量）。此外，对于使用有锫汽油的国家（如我囯）， 铅会使催化剂中毒。如果废气中存在硫化物，它们也会使催化剂中 毒。 所以西方一些国家（如美国）通过立法，要求使用无锫汽油。
使用贵金属（如铂、铑、钯）和稀土金属作为活性组分净化汽车 尾气的催化剂， 已有大量文献作了报道。但使用贵金属和稀土元素 作为活性組分的催化剂无疑使其成本上升。
使用非贵金属元素的催化剂也有文献报道，但在低温下的转化 效率，快速转化效率和寿命方面仍有缺陷，有些净化汽车废气催化 剂必须装置氡传感^和加熱装置。且其活性组分组成和量的比例都 与本发明催化剂有较大区别。
中囯专利申请 85109694. 8公开了非贵金属蜂窝状燃烧催化 剂， 它包括使用双载体和铜、钒、锰、钴、镍的氡化物或上述元素中 的几种組成的混合氣化物， 同时含稀土元素如锎、铈、镨、钐、钕、钇 的氡化物或其混合物作为活性組分。
中国专利申请 98105063. 9也公开了 与中囯专利申请
85109694. 8相近的汽车废气净化催化剂。 它包括蜂窝状陶瓷质材 料和氡化铝涂层的复合载体， 非贵金属元素锫、钴、镍、錳、铜、铬的 氣化物中的一种或几种的混合物及稀土元素的氡化物的活性組分， 但其制备方法中，对活性氣化物用氳、一氣化碳、烃类化合物进行了 还原处理。 这样可以认为一些金属无素活性氣化物很可能转化为 金属元素。 另外，该专利申请制备催化剂的方法在 700— 110(TC下 焙烧工艺也是不可取的。 因为 Y— A1203在 200— 600'C下是不定形 的 γ— A1203，其活性和分散性最好。 当温度达 865'C时， γ— A1203便 为定形 γ— A1203，其活性和稳定性较差。 当温度达到 1100'C，丫一 A1203便转化成无活性的 cx—Al203 ,其很容易从载体上脱落下来。
EP0393517A2公开 了用于转化内燃机发动机废气的催化氡化 和还原转化^， 它能^未燃烧的烃和一氣化碳完全燃燒并将氣氣 化物还原成无素氦和氡。作为催化剂，所述转化器使用逸自 Cr，Mn，
Fe ,Co，Ni，Cu， Zn ,Sn,Ba,La和 Ce的金属氡化物，说明书仅给出了 一个化学组成（重 为： Cu26%，Cr21 % ; BaO= l l %的催化剂。 但该转化^装在汽车消音^出口处时，必须使用加热器，以便使该 转化^在 200— 400'C下使欲转化的废气进行反应。
Alkhazov等人在美国专利 4， 519 , 992中公开了一种净化 化 氳的方法，该方法包括使用有下列組分的催化剂： 二氡化钛 10— 30% (重量），氣化铁 20—30% (重量），氡化锌 20— 25% (重量），氡 化铬 20—50% (重量），用空气氣化硫化氨。该催化剂是通过将这些 金属的盐（如盐酸盐）水溶液用氮水转化成其氳氡化物， 然后混合 均匀，干燥，煅烧得相应的氣化物制得。 GB2059934A公开了净化 N20的催化剂，该催化剂含有一种或 多种氡化铁，氡化钴、氡化铜、氡化铬、二氡化锰和氡化镍作为活性 組分，在说明书中，公开了至多使用三种上述金属元素氡化物作为 活性成分的催化剂。该催化剂是使用这些金属盐（如硝酸盐）水溶液 浸渍载体，然后千燥、煅烧使其盐分解成相应的氡化物而制得的。
因此，能用来净化工业废气（如硤化物）和汽车尾气的催化剂， 它应具有低温启动、高效和长寿命的催化剂仍是迫切需要的。
发明内容
因此本发明的一个目的是提供一种用于净化汽车尾气的催化 剂。
本发明的另一个目的是提供一种用于净化工业废气（如硫化 物）的催化剂。
本发明的第三个目的是提供制备用于净化工业废气和汽车尾 气的催化剂的方法。
本发明的最佳实施方式
本发明提供一种用于净化汽车尾气的催化剂， 所述催化剂包 括一种适宜的载体，其特征在于该催化剂包括铜（Cu)、镍（Ni)、钴 (Co)、锌（ Zn) ,铬 (Cr)，钰（Mn)和钕（Nd)的氡化物及上述金属元素 中的两个或多个形成的复合氡化物为活性組分，其中基于载体的 重量活性組分以各个金属元素氡化物计的重量百分数如下：
氡化铜（CuO)2—20%
氡化镍 (NiO)0. 5—8%
氣化钴（CoO)O.
氡化铬 (Cr203) l— 7%
氡化锌（ZnO)0. 5— 10%
氣化锰（MnO)0. 05—6%
氣化钕 (Nd2O3)0. 1—
在一优逸的实施方案中， 所述催化剂特征在于基于载体重量 活性组分以各个金属元素氡化物计的重量百分数如下：
氡化铜（CuO)4—16%
氣化镍 (NiO) l— 6% 氣化钴 (CoO)0.4— 3%
氣化铬 (Cr203)2—5%
氡化锌 (ZnO)l—8%
氡化錳（MnO)0.1-5%
氣化钕 (Nd2O3)0.3—0.9%
在另一个优选的实施方案中，本发明的催化剂还包括 γ— Α1203,其基于载体重量的重量百分数为 2— 12%。
本发明的另一个目的在于提供一种用于净化工业废气的儐化 剂，所述催化剂包括一种适宜的载体，其特征在于该催化剂包括 铜、锌、镍、钴、铬、铁、锰和钕的氡化物及上述金属元素中的两个或 多个形成的复合氣化物作为活性組分，其中活性組分基于载体重 量的百分数如下：
氡化铜 (CuO)2— 20%
氡化镍 (NiO)0.5—8%
氡化钴（CoO)O.l— 4%
氣化铬 (Cr203)l—7%
氡化锌（ZnO)2—16%
I化铁 (Fe2O3)0.2—1.5%
氡化核 (MnO)0.05-6%
氡化钕 (Nd2O3)0.1— l%
在一优逸的实施方案中， 本发明用于净化工业废气的催化剂 的特征在于，基于载体重量活性組分以各个金属元素氡化物计的 重量百分数如下：
氣化铜（CuO)4— 16%
氡化镍 (NiO)2— 6%
氣化钴 (CoO)0.4—3%
氡化铬 (Cr203)2—5%
氡化锌（ZnO)6—12%
氡化铁（Fe2O3)0.4—l%
氡化 ϋ(ΜηΟ)0.1— 5%
氣化钕 (Nd2O3)0.3—0.9% 本发明提供一种制备用于净化汽车尾气的催化剂的方法， 所 述催化剂包括一种遠宜的载体和作为活性組分的铜（ Cu) 、 鎳
(Ni)、钴（Co) 、锌（Zn)，铬（Cr)、锰（Mn)和钕（Nd)的氡化物及上述 金属元素中的两个或多个形成的复合氡化物， 其中基于载体的重 量活性組分以各个金属元素氡化物计的重量百分数如下：
氡化铜（CuO)2— 20%
氣化镍 (NiO)0. 5—8%
氡化钴 (CoO)0. 1— 4%
氡化铬 (Cr203)l— 7%
氡化锌（ZnO)0. 5—10%
氡化锰（ΜηΟ)0· 05-6
氡化钕 (Nd2O3)0. 1 - 1 %
该方法包括用铜、镍、钴、锌、锰和钕的盐的水溶液浸漬一种适宜的 载体，然出取出浸过的载体，在空气中于 70— 120'C下千燥，并于 120— 600'C下煅蛲，从而制得催化剂。
在一优逸的实施方案中，将上述制得的催化剂用 γ—Α1203水 溶液浸渍 ， ^浸清后的催化剂在 70—800'C下千燥和煅燒以制得 催化剂。
从上述的制备可看出，在这些金属盐分解时，可能形成两种或 多种金属的复合氣化物， 为方便起见， 活性成分以各个金属元素 氣化物计算，也就是说，对于可能存在的复合金属氡化物，都折算 成相应金属元素的氡化物。
所述的金属盐可以是在煅蛲时能形成相应金属氡化物或复合 氡化物的任何无机或有机駿的盐，优选硝酸、硫酸和磷駿盐，最好 是硝駿盐。
铜、镍、钴、锌、铬、锰和钕的盐的水溶液的总浓度及相应各种金 属盐的量应使这些盐分解后形成的金属无素氡化物及这些金属中 两个或多个的复合氡化物， 基于载体重量以各个金属元素氣化物 计落在上述范围内。具体地说，所述金属盐的水溶液总浓度以整个 水溶液为基在 5— 50% (重量），铜盐为 2— 30% (重量），镍盐 1— 15% (重量），钴盐 0. 5— 8% (重量），钰盐为 0. 1— 1 %，锌盐为 0. 1 —20% (重量），铬盐 0.05— 1% (重量），其余为钕盐。
类似地可制备用于净化砥化物的催化剂。
在一优逸的实施方案中将上述制得的用于净化汽车废气和工 业尾气的催化剂，再用碱性动植物油或肥皂水溶浸渍，并干燥制得 具有除铅能力的傢化剂，其中优逸使用硬脂酸钠水溶液。
用作本发明催化剂的载体可以是本领域任何适宜的载体， 优 异使用陶瓷载体,更优选陶瓷载体董青石含量 92%,吸水率 35—
40%,比表面积>31112/8。
下面用非限制性实施例进一步描述本发明。
实施例 1 制备用于净化汽车尾气的催化剂。
在一个 5升带搅拌容器中， 加入 200ml水， 361gCu(N03)2 · 3H2O,180g Ni( N03)2 · 6H2O，70g Co(N03)2 · 6H20,搅拌均匀。 在 另一个 200亳升的容 中，加入 20ml 20%的硝酸水溶液，加入 6gNd203和 50ml水形成溶液。 将该溶液加到上述 5升容器中，用硝 酸或水调节溶液的其 PH值在 4一7。 加入 7g硝駿錳， 52g硝駿铬和 35g硝酸锌，加水到 1000ml备用。
^ 50g陶瓷载体（上海第二耐火材料厂生产，孔径 300— 400 目，比表面积 >3m2/g)在 100ml于实施例 1中制备的备用溶液中浸 清 1小时左右。滤掉残液，将浸过的载体在 70— 120'C下干燥，于 120— 600'C下于空气中煅烧，制得催化剂 A。该催化剂基于载体活 性成份的重量百分数 CuO=ll.9%,NiO=4.6%,CoO=l.8%, MnO-0.29%,Cr203=3.3%,ZnO=l.5%和 Nd2O3 = 0.6%。
实施例 2
将 50g陶瓷载体（上海第二耐火材料厂；孔径 300— 400目，比 表面积〉3m2/g)在 100ml于实施例 1中制备的备用溶液中浸渍 1 小时左右。 滤掉滤液，在 70—600'C下千燥和煅烧，冷却后，再浸入 事先配好的 100ιη17%γ— A1203水溶液中 1小时。滤掉残液，在 70 一 800'C下于空气中千燥和煅烧制得催化剂 B。该催化剂基于载体 活性成分重量百分数如下：
CuO=11.9%, NiO=4.6 ,CoO=l.8%,MnO=0.29%,Cr203 =3.3%,ZnO=l.5%和 Nd2O3 = 0.6% 实施例 3 制备用于净化硫化物的催化剂。
在一容 ^中，加入 100ml实施例 1 中制备的备用溶液， 2gFe (Ν03)3 · 9H20和 20g Ζη(Νθ3)2溶解并搅拌均匀。 50g陶瓷载体 (上海第二耐火材料厂；孔径 300—400目，比表面积〉 3m2/g)在上 述溶液中浸潢 1小时左右。滤掉残液， 浸过的载体在 70— 120'C 下千燥，在 120— 600'C下于空气中煅烧，制得催化剂 C。其基于载体 活性成分重量百分数为 CuO=ll.9%, ZnO=9.6%，NiO=4.6%, Cr203 = 3.3^,CoO=l.8¾,MnO=0.29%,Fe2O3 = 0.8%和 Nd203 = 0.6%。
实施例 4
分别将实施例 1，2和 3制得的催化剂 A、B、(：用肥皂（上海肥 皂广生产的古本肥皂）水溶液浸渍，千燥制得相应的催化剂 D、E和
F。
实施例 5
在一个 5升带攬拌的容器中，加入 200ml水， 210g Cu(N03)2 · 3H20,105g Ni(N03)2 · 6H20,35g Co(N03)2 · 6H20。在另一个 200毫 升的容 中，加入 20ml 20%的 δϋί鲛水溶液，加入 6g Nd203和 50ml 水形溶液。 该溶液加到上述的 5升容器中，用硝酸或水调节溶液 的 PH值在 4一 7。加入 91g硝酸锰，63g硝酸铬和 182g硝駿锌，加水 到 1000ml备用。
将 50g陶瓷载体（上海第二耐火材料厂生产，孔径 300— 400 目， 比表面积〉3m2/g)在 100ml上述制备用溶液中浸渍 1小时左 右。滤掉残液，将浸过的载体在 70— 12(TC下千燥， 于 120— 600'C 下于空气中煅烧，制得催化剂 G。 其基于载体的活性成分的重量百 分数：
CuO=6.9%, NiO=2.7%,CoO=0.9%,MnO=3.6%,Cr203 = 4 %， ZnO= 7.8 %和 Nd203 = 0.6 %。
在下面的测试中， 除非特别说明，所用催化剂（载体 +活性组 分）重量约为 390克。 催化剂装在经适当改造后的汽车消音器中。
将制得的催化剂 A，经北京吉汽车有限公司进行了试验。
试验是按美国 EPA— 75标准，用切诺基 CX— 1型进行的。 试验条件
1.试验设备
HORIBA MEXA- 9400排放分析仪及数据处理系统，精度士
Figure imgf000010_0001
HORIBA MEXA— 9300CFV定容取样糸统，精度士 2%
曰本 ONO SKKI底盘测劝机，精度士 2%。
2.道路费负荷
车速 km/h 10 20 30 40 50 60 70 80 90 100 负 # Ps 0. 94 2. 06 3. 46 5. 40 7. 70 10. 4 14. 1 18. 4 24. 8 27. 9 试验结果
排放物
Figure imgf000010_0002
克 /公里 克 /公里 克 /公里 克 /公里 原车 1. 42 16. 01 2. 19 328. 28 加装本发明催化剂 0. 51 5. 76 0. 21 351. 49 将制得的催化剂 D,经上海市环境监測中心进行測试。
一、測试仪器
1.广 东佛山分析仪器厂組装日本 HORIBA公司的 MEXA— 324F便携式汽车尾车測试仪。
2.日本 MECS抹式会杜生产的便携式大气采样仪。
3.上海宏伟仪表厂生产的 FC— A— 3型粉尘采样仪。
4.上海川沙伟丰热工仗表广 XMX— 101型热电偶温度測定 仪。
二、测试方法和依据：
測试时将该型净化 · 分别置于汽油车排气管后， 汽油车分別 測装上后和装上行驶 11. 2万公里后净化效果測试方法按 GB3845 -83及《环境监測技术規范》要求进行。
三、測试结果: 表 2
牌号：上海 HC(ppm) NO,(mg/m3) Pb(mg/m3) 度气温度（ 縻车 （EQ O) 7. 75 4700 6. 510 1. 93 168 装本发明催化剂后 0. 01 12. 5 0. 526 0. 141 350 净化效牟（％) 99. 9 99. 7 91. 9 92. 7 表二 行驶 11万公里后净化效果
表 3
脾号：上海 01/03440 Co( % ) HC(ppm) NO,(mg/ms) Pb(mg/m3) 度气 S度（TQ ) 原车（SH142) 4. 0 1500 8. 654 5. 88 198 装本发明催化剩后 0. 775 210 1. 103 2. 81 500 净化故牟（％) 80. 6 86. 0 87. 2 52. 2 从表 1中数据来看装上后即測该净化器效果尤为明显，各项指标均 达到 91 %以上，且催化剂起燃速度快，装上净化器后短时间内其排 气温度很快达到表 2中所列温度水平。 表 3数据为行驶 11. 2万公 里后的測试数据，从测试数据来看，该净化 ^除锫外仍有 80%以上 的净化效果，但催化剂活性有下降现象，反映在催化起燃速度緩慢， 加热至表 3所例温度是在长时间地加大怠速油门，提高热废气排量 情况下达到的。
另外， 该产品在行驶 3. 5万和 3. 6万公里时由受上海市公安 局交通总队委托的单位上海市交通运输局检測线測试，从測试结果 来看，在行驶 3. 5万公里公里 CO、 HC效率分別达到 99. 6%和 99. 8%，8. 6万公里时达到 96. 9%和 93. 05。 综上所述，该产品经行驶 不同公里数多次測试， 明有良好的净化效果和长寿命。
^制得的催化剂 F作为净化器，经上海市环境监測中心測试。
1.測试方法
CO, HC按 GB3845— 83汽油车怠速污染物测 量方法要求进 行; NOx，S02和 Pb按环境监測技术規范要求进行。
2.測试条件：
測试时汽车水温达 80'C， 净化^前排汽温度达 146'C，净化^ 后废气温度达 48'C，被測车辆为东风牌汽油卡车，其车号为： WJ— 08— N04140 3.測试和分析所用仪
CO, HC用佛山分析仪 · 厂組装日本 HORIBA公司 ΜΕΧΑ— 324F型非分光红外线汽车尾气测定仪測定， NOx，S02用 U型玻璃 吸收瓶富集，分别采用盐酸茶 胺比色法和盐酸付玫瑰苯胺比色法 分析，分析仪器采用日本岛津公司的 UV— 240分光光度计， Pb用 玻璃纤维滤筒富集，以原子吸收法分析用日产日立（HITACHI180— 70)原子吸收分光光度计。
4.測试数据： 表 4
項目 ∞% HC(ppm) S02(mg/ms) NO,(mg/m3) Pb(mg/mj) 儐化净化前 4. 8 3880 2. 005 7. 74 3. 80
催化净化后 1. 2 650 0. 019 3. 07 0. 081
净化致牟（％) 75. 0 83. 2 99. 0 60. 3 97. 9 以上測试均同时在净化器前和净化器进行，从上表的数据看， 该净化器对各污染物均有明显的净化效果。在排出净化器废气温度
48 'C和管道无泄潙情况下，对 S02和 Pb的净化能力特别强，分别达 99. 0%和 97. 9%。对 CO和 HC ^L分別达 75. 0%和 83. 2%。净化效 率最低的 NOx 达 60· 3%。 这可能是由于废气温度较低的缘故。
将表 1数据换算成克 /英里列在表 5中与美囪加州 FTP— 75 排放标准，及加拿大排放标准比较。
表 5
切诺基 CX—1型 CO g/mile HC g/mile NOx g/mile 美国加州 FTP— 75 7 0. 41 1 加拿大 7 0. 41 1 原车 10. 01 0. 888 1. 37 装本发明催化剂后 3. 6 0. 318 0. 13 从表 5可以看出，装本发明催化剂后，排出废气均低于美国加州 HP -75及加拿大排放标准。
工业应用性
~ ~~本发明的催化剂能同时净化一氡化碳，碳氨化合物 (HC)和氮 氡化物（ NQx) ， 并能净化硫化物及具有除铅能力， 它可在低温下 启动，具有单程转化率高， 无须在汽车排气管中加装氡传感器和 加热蓉。

Claims

权 利 要 求
1. 一种用于净化汽车尾气的儐化剂， 所述催化剂包括一种适 宜的载体，其特征在于该催化剂包括铜（ Cu) 、镍（Ni)、钴（Co)、锌 (Zn)，铬 (Cr)、锰（Mn)和钕 (Nd)的氡化物及上述金属元素中的两个 或多个形成的复合氡化物作为活性組分，其中基于载体的重量活 性組分以各个金属元素氣化物计的重量百分数如下：
氡化铜（CuO)2— 20%
氡化镍 (NiO)0. 5— 8%
氡化钴（CoO)O. l— 4%
氡化铬（Cr203)l— 7%
氡化锌（ZnO)0. 5—10%
氣化錳（MnO)0. 05-6%
氣化钕（Nd2O3) 0. 1— l %
2. 按照权利要求 1的儐化剂，其特征在于基于载体重量活性组 分以各个金属元素氣化物计的重量百分数如下- 氡化铜（CuO)4— 16%
氣化镍 (NiO)2— 6%
氡化钴 (CoO)0. 4— 3%
氣化铬（Cr203)2— 5%
氡化锌（ZnO) l—8%
氡化锰（MnO)0. 1-5%
氣化钕（Nd2O3)0. 3—9%
3. 按照权利要求 1或 2的催化剂，其特征在于催化剂还包括丫 — A1203，其基于载体重量的重量百分数为 2— 12%。
4. 一种用于净化工业废气的催化剂，所述傕化剂包括一种 ϋ 宜的载体，其特征在于该催化剂包括铜、锌、镍、钴、铬、铁、錳和钕 的氡化物及上述金属元素中的两个或多个形成的复合氡化物作为 活性组分，其中活性組分基于载体重量的百分数如下：
氡化铜（CuO)2— 20%
氣化锌（ZnO)2—16% 氡化镍 (NiO)0.5—8%
氡化钴（CoO)O.1-4%
氡化铬 (Cr203)l— 7%
氡化铁 (Fe2O3)0.2— 1.5%
氡化锰（Mno)O.05-6%
氡化钕 (Nd2O3)0.1— 1%
5. 按照权利要求 4的催化剂，其特征在于基于载体重量活性組 分以各个金属元素氡化物计的重量百分数如下：
氡化铜（CuO)4— 16%
氡化锌（ZnO)6—12%
氡化镍 (NiO)2— 6%
氣化钴（CoO)0.4—3%
氡化铬 (Cr203)2— 5%
氡化铁（Fe2O3)0.4— 1%
氡化锰（MnO)0.1— 5%
氡化钕（Nd2O3)0.3—0.9%
6. 按照权利要求 1或 4的催化剂，所述的载体为陶瓷载体。
7. 按照权利要求 6的催化剂，所述陶瓷载体董青石含量 92%,吸水率 35—40%,比表面积>31112/8。
8. 按照权利要求 1或 4的催化剂， 所述催化剂是经碱性动植 物油水溶液或肥皂水溶液浸渍、千燥过的。
9. 按照权利要求 8的催化剂，其中肥皂水溶液为硬脂駿钠水溶
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CN106607085B (zh) * 2015-10-21 2020-04-17 中国石油化工股份有限公司 一氧化碳催化脱除氮氧化物的催化剂
CN106607087B (zh) * 2015-10-21 2020-02-07 中国石油化工股份有限公司 一氧化碳催化转化含氮化合物的催化剂
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EP0815938A1 (de) 1998-01-07
EP0815938A4 (en) 1998-04-29
CN1051025C (zh) 2000-04-05
AU4662596A (en) 1996-09-04
JPH11501863A (ja) 1999-02-16
CN1129146A (zh) 1996-08-21
EP0815938B1 (de) 2002-05-08
US6046129A (en) 2000-04-04
DE59609190D1 (de) 2002-06-13

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