# US 2014/0194642 A1 · Silica-supported catalyst

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- Number: US 2014/0194642 A1
- Document ID: US20140194642A1
- Status: Published application
- Kind: A1
- Application number: 14/112,269
- Filed: 2012-04-09
- Published: 2014-07-10
- Earliest claimed: 2011-04-21
- Assignees: Asahi Kasei Chemicals Corporation
- Inventors: Satoshi Endo; Takaaki Kato
- Web page: https://patentgrep.com/patent/US20140194642A1

## CPC

- C07C 253/24: by ammoxidation of hydrocarbons or substituted hydrocarbons
- B01J 21/08: Silica
- B01J 23/002: {Mixed oxides other than spinels, e.g. perovskite}
- B01J 23/22: Vanadium
- B01J 23/28: Molybdenum
- B01J 23/30: Tungsten
- B01J 23/31: combined with bismuth
- B01J 23/34: Manganese
- B01J 27/0576: {Tellurium; Compounds thereof}
- B01J 35/612: {less than 10 m2/g}
- B01J 35/613: {10-100 m2/g}
- B01J 35/633: {less than 0.5 ml/g}
- B01J 2523/00: Constitutive chemical elements of heterogeneous catalysts
- Y02P 20/52: using catalysts, e.g. selective catalysts
- C07C: ACYCLIC OR CARBOCYCLIC COMPOUNDS
- B01J: CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- Y02P: CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS

## Abstract

A silica-supported catalyst used when producing a corresponding unsaturated nitrile in a vapor-phase catalytic ammoxidation reaction of propane or isobutane, the catalyst including a metal oxide represented by the following formula (1), MoVaNbbXcTdZeOn (1) (wherein X represents at least one or more elements selected from Sb and Te; T represents at least one or more elements selected from Ti, W, Mn, and Bi; Z represents at least one or more elements selected from La, Ce, Yb, and Y; and a, b, c, d, e, and n are in the range of 0.05≦a≦0.5, 0.01≦b≦0.5, 0.001≦c≦0.5, 0≦d≦1, and 0≦e≦1, respectively, and n denotes a value that satisfies an atomic valence) wherein the silica-supported catalyst has an average pore size of 60 to 120 nm, a total pore volume of 0.15 cm3/g or more, a specific surface area of 5 to 25 m2/g, and a crystallite size of 40 to 250 nm as determined from half width of a (001) peak by X-ray diffraction.

## Claims

### Claim 1

A silica-supported catalyst used when producing a corresponding unsaturated nitrile in a vapor-phase catalytic ammoxidation reaction of propane or isobutane, the catalyst comprising a metal oxide represented by the following formula (I),
MoVaNbbXcTdZeOn (1)
(wherein X represents at least one or more elements selected from Sb and Te; T represents at least one or more elements selected from Ti, W, Mn, and Bi; Z represents at least one or more elements selected from La, Ce, Yb, and Y; and a, b, c, d, and e are in a range of 0.05≦a≦0.5, 0.01≦b≦0.5, 0.001≦c≦0.5, 0≦d≦1, and 0≦e≦1, respectively, and n represents a value that satisfies an atomic valence)
wherein the silica-supported catalyst has an average pore size of 60 to 120 nm, a total pore volume of 0.15 cm3/g or more, a specific surface area of 5 to 25 m2/g, and a crystallite size of 40 to 250 nm as determined from half width of a (001) peak by X-ray diffraction.

### Claim 2 (depends on 1)

The silica-supported catalyst according to claim 1, wherein a pore volume of pores having a pore size of less than 60 nm based on total pore volume is less than 30%, and a pore volume of pores having a pore size exceeding 120 nm based on total pore volume is less than 30%.

### Claim 3 (depends on 1, 2)

The silica-supported catalyst according to claim 1 or 2, wherein a support amount of the silica is 20 to 70% by mass based on total mass of the catalyst composed of the metal oxide and the silica.

### Claim 4

A method for producing a silica-supported catalyst, comprising the steps of:
(I) preparing a raw material-prepared solution containing Mo, V, Nb, X, T, and Z, wherein an atomic ratio a of V to one Mo atom is 0.05≦a≦0.5, an atomic ratio b of Nb to one Mo atom is 0.01≦b≦0.5, an atomic ratio c of X to one Mo atom is 0.001≦c≦0.5, an atomic ratio d of T to one Mo atom is 0≦d≦1, and an atomic ratio e of Z to one Mo atom is 0≦e≦1;
(II) drying the raw material-prepared solution to obtain a dry powder;
(III) pre-stage calcining the dry powder at 200 to 400° C. to obtain a pre-stage calcined body; and
(IV) main-calcining the pre-stage calcined body at 600 to 750° C. to obtain a calcined body,
wherein the raw material-prepared solution comprises 0 to 30% by mass based on total mass of silica raw materials of (i) a silica sol having an average primary particle size of 3 nm or more and less than 20 nm, 30 to 70% by mass based on total mass of the silica raw materials of (ii) a silica sol having an average primary particle size of 20 nm or more and 100 nm or less, and 30 to 70% by mass based on total mass of the silica raw materials of a silica powder having an average primary particle size of 50 nm or less, and wherein a total of the silica sol (i), the silica sol (ii), and the silica powder is 100% by mass based on silica.

### Claim 5 (depends on 1, 2)

A method for producing a corresponding unsaturated nitrile by performing a vapor-phase catalytic ammoxidation reaction of propane or isobutane using the silica-supported catalyst according to claim 1 or 2.