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Highly dispersed metal-supported oxides as NH3-SCR catalysts and synthesis processes

A catalyst and compound technology, applied in the direction of metal/metal oxide/metal hydroxide catalyst, chemical/physical process, organic compound/hydride/coordination complex catalyst, etc.

Pending Publication Date: 2022-04-12
TOYOTA MOTOR EUROPE NV SA +3
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

[0012] In order to solve the problem with the selective catalytic reduction of ammonia (NH 3 - Problems related to prior art products and processes in the field of SCR) catalysts, the process and products of the present invention were developed

Method used

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  • Highly dispersed metal-supported oxides as NH3-SCR catalysts and synthesis processes
  • Highly dispersed metal-supported oxides as NH3-SCR catalysts and synthesis processes
  • Highly dispersed metal-supported oxides as NH3-SCR catalysts and synthesis processes

Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1a

[0094] Example 1a - Using [Nb(OEt) 5 ] 2 Preparation of NbOx / CeO as precursor 2

[0095] Step 1: Pretreatment of the support material, ceria (CeO 2 )

[0096] Ceria Actalys HAS-5 Actalys 922 from Solvay (Rare Earth La Rochelle), CeO 2-(200) (The specific surface area is 210±11m 2 g -1 ceria) was calcined for 16 hours and evacuated under vacuum at high temperature. After moisture rehydration under an inert atmosphere, at 200°C and high vacuum (10 -5 Under Torr) the cerium oxide was partially dehydroxylated for 15 hours to obtain a specific surface area of ​​200 ± 9m 2 .g -1 of yellow solid.

[0097] The supported ceria was characterized by DRIFT, BET, NMR and XRD.

[0098] Characterization of Ceria by DRIFT

[0099] The DRIFT study described in Fig. 3 shows that after calcination and hydration, at 200 °C under vacuum (10 -5 mbar) resulted in the removal of physisorbed water and mainly revealed bridging OH groups. The spectrum of ceria dehydroxylated at 200 °C plot...

Embodiment 1b

[0142] Example 1b: By using [Nb(OAR) 5 Preparation of [NbOx] / CeO as a precursor 2-200 , where Ar is 2,6-diisopropyl-phenyl

[0143] Step 1: Support Material CeO 2 preprocessing

[0144] Pretreatment of the support material was carried out in the same manner as the pretreatment of the support in step 1 of Example 1a above.

[0145] Step 2: On CeO 2-(200) Overgrafted [Nb(OAR) 5 ] precursor

[0146] Stir [Nb(Oar) at 25°C 5 ] (1.225mg, 1.75mmol) and CeO 2-(200) (2.5 g) in toluene (20 mL) for 12 hours. After filtration, the solid was washed with toluene [Nb(Oar) 5 ] / CeO 2-200 3 times. under vacuum (10 -5 Torr) to dry the resulting yellow powder. 1 HMAS NMR (ppm, 500MHz): δ6.4 (Oar aromatic proton), 1.8 (methyl ArMe proton) 13 C CP MAS NMR (ppm, 200MHz): δ158.7 (aryl ipso Oar C-ipso), 118.5-126.8 (Oar aromatic carbon), 16.7 (ArCH 3 methyl). Elemental analysis %Nb=0.99% by weight %C=5.19% by weight C / Nb=40.6 (th 32).

[0147] Step 3: Calcination

[0148] The material...

Embodiment 2a

[0149] Example 2a: By using [W=O(Oet 4 ] 2 ) as a precursor to prepare Wox / CeO 2

[0150] Stir at 25°C [W=O(Oet 4 ] 2 (0.625g, 1mmol) and 6g CeO 2-(200) The mixture in toluene (30 mL) for 12 hours. After filtration, the obtained solid was washed with toluene [W=O(Oet) 4 ] 2 / CeO 2 3 times to extract the unreacted complex, then remove the toluene with pentane. In vacuum (10 -5 Torr) to dry the resulting yellow powder.

[0151] 1 H MAS NMR(ppm,500MHz):δ4.8(OCH 2 CH 3 ), 1.3 (OCH 2 CH 3 ) 13 C CP MAS NMR (ppm, 200MHz): δ68.5 (terminal OCH 2 CH 3 ), 64.6 (bridge OCH 2 CH 3 ), 18.3 (terminal OCH 2 CH 3 ), 16.5 (bridge OCH 2 CH 3 ). Elemental analysis %W = 4.1% by weight C = 1.2% by weight C / W = 4.5 (th 6). DRIFT analysis shows that Ce-OH is at a higher wave number (ν(OH)=3400-3700cm -1 ) at the band, corresponding to the selective reaction with the tungsten complex. In addition, it was also found that at 2850-3050 and 1110-1470cm -1 The band characteri...

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Abstract

The present invention relates to a method for preparing a catalyst material, comprising the steps of: (a) providing a support material having surface hydroxyl (OH) groups, where the support material is two or more of ceria (CeO2), zirconia (ZrO2), or a combination thereof, and where the support material comprises at least 0.3 mmol and at most 2.0 mmol OH groups per gram of support material, (a) providing a support material having surface hydroxyl (OH) groups, where the support material is two or more of ceria (CeO2), zirconia (ZrO2), or a combination thereof, and where the support material comprises at least 0.3 mmol and at most 2.0 mmol OH groups per gram of support material; (b) reacting the support material having a surface hydroxyl (OH) group of step (a) with at least one of the following species: (bl) a compound containing at least one alkoxy or phenoxy group bonded via its oxygen atom to a metal element of Group 5 (V, Nb, Ta) or Group 6 (Cr, Mo, W); (b2) a compound containing at least one hydrocarbon group bonded via a carbon atom to a metal element from Group 5 (V, Nb, Ta) or Group 6 (Cr, Mo, W); (b3) a compound containing at least one hydrocarbon group bonded to the metallic element copper (Cu) through a carbon atom; (c) calcining the product obtained in step (b) to provide a catalyst material, wherein a metal element from Group 5 or Group 6 or Cu is present as an oxide on the support material. The invention further relates to a catalyst material obtainable by the above process and to the use of the catalyst material as an ammonia selective catalytic reduction (NH3-SCR) catalyst for the reduction of nitrogen oxides (NOx).

Description

technical field [0001] The present invention relates to selective catalytic reduction of ammonia (NH 3 -SCR) catalyst synthesis. Background technique [0002] Toxic NOx gases (NO, NO 2 , N 2 O) needs to be converted to N before being released into the environment 2 . This is usually achieved by using different types of NOx reduction catalysts such as three-way catalysts (TWC), NOx storage reduction (NSR) or using ammonia as an external reductant (NH 3 -SCR) by selective catalytic reduction (SCR). [0003] Known metal oxides such as V 2 o 5 is good NH 3 -SCR catalyst. It has been suggested that catalytic activity is achieved through the complementary characteristics of acidic and reductive properties of surface species. In short, NH 3 adsorbed on Acid sites (V 5+ -OH), and then through the redox cycle (V 5+ =O / V 4+ -OH) is activated by the adjacent V=O surface group N-H. The resulting surface complex reacts with gaseous or weakly adsorbed NO to form NH via th...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): B01J37/02B01J37/08B01J35/00B01J21/06B01J23/10B01J23/20B01J23/22B01J23/28B01J23/30B01J23/72B01D53/86B01D53/94B01J31/22
CPCB01J2531/56B01J2231/62B01J23/28B01J21/066B01J31/2226B01J37/0207B01J2531/58B01J23/30B01J23/20B01J2531/66B01J2531/64B01J23/72B01J37/086B01J31/1625B01J23/10B01J2531/57B01J23/22B01J37/0209B01J2531/16B01J37/0203B01J31/2295B01J31/2265B01J31/0214B01J31/0212B01D53/9418B01D2255/2065B01D2255/20776B01D2255/207B01D2255/20769B01D2255/407B01D2251/2062B01D2255/20715B01J35/397B01D2255/20723B01D2255/20761
Inventor P·H·阮N·梅尔M-O·查尔林K·C·司徒M·陶菲克
Owner TOYOTA MOTOR EUROPE NV SA