Method of oxidative conversion

Claim 3

A method in accordance with claim 1 wherein the solid contact material is selected from the group consisting of: (1) a solid contact material comprising: (A) at least one metal selected from the group consisting of Group IA metals, Group IIA metals and mixtures thereof, (B) oxygen and, (C) at least one material selected from the group consisting of halogen ions and compounds containing halogen ions; (2) a solid contact material comprising: (A) at least one metal selected from the group consisting of Group IA metals, (B) at least one metal selected from the group consisting of lanthanum Series metals, (C) oxygen, (D) at least one material selected from the group consisting of halogen ions and compounds containing halogen ions and, optionally, (E) at least one metal selected from the group consisting of Group IIA metals; (3) a solid contact material comprising: (A) at least one metal selected from the group consisting of Group IA metals, (B) zinc, (C) oxygen, (D) at least one material selected from the group consisting of halogen ions and compounds containing halogen ions and, optionally, (E) at least one metal selected from the group consisting of Group IIA metals; (4) a solid contact material comprising: (A) at least one metal selected from the group consisting of Group IA metals, (B) at least one metal selected from the group consisting of titanium and zirconium; (C) oxygen, (D) at least one material selected from the group consisting of halogen ions and compounds containing halogen ions and, optionally, (E) at least one metal selected from the group consisting of Group IIA metals; (5) a solid contact material comprising: (A) at least one metal selected from the group consisting of Group IA metals, Group IIA metals and mixtures thereof, (B) at least one material selected from the group consisting of phosphate radicals and compounds containing phosphate radicals and, (C) at least one material selected from the group consisting of halogen ions and materials containing halogen ions; and (6) a solid contact material comprising: (A) cobalt, (B) at least one metal selected from the group consisting of zirconium, zinc, niobium, indium, lead and. bismuth, (C) phosphorous, (D) oxygen, (E) at least one material selected from the group consisting of halogen ions and compounds containing halogen ions and, optionally, (F) at least one material selected from the group consisting of Group IA metals, sulfur, compounds containing sulfur and mixtures thereof, under oxidative conversion conditions sufficient to convert said feed organic compounds to said product organic compounds and said solid contact material is at least intervally contacted with the material containing at least one halogen, when said contact material is selected from the group consisting of contact materials (1), (2), (3), (4) and (5), and with at least one of the material containing at least one halogen and the material containing at least one reducing agent, when said contact material is contact material (6).

Claim 4

A method in accordance with claim 1 wherein an ineffective amount of halogen is initially present in the contact material and said amount of halogen is increased to at least an effective amount by contacting said contact material with the material containing at least one halogen prior to contacting the feed organic material and the free oxygen containing gas with said contact material.

Claim 5

A method in accordance with claim 3 wherein the contact material is thus contacted with the material containing at least one halogen, prior to contacting the feed organic material and the free oxygen containing gas with said contact material, in a reaction zone in which the oxidative conversion is carried out.

Claim 6

A method is accordance with claim 3 wherein the contact material is also intervally contacted with the material containing at least one halogen during the conduct of the oxidative conversion.

Claim 7

A method in accordance with claim 3 wherein the contact material is also contacted with the material containing at least one halogen by continuously adding said material containing at least one halogen to the feed organic compound and the free oxygen containing gas during the conduct of the oxidative conversion.

Claim 8

A method in accordance with claim 1 wherein an effective amount of halogen is initially present in the contact material and the contact material is intervally contacted with the material containing at least one halogen during the conduct of the oxidative conversion.

Claim 9

A method in accordance with claim 1 wherein an effective amount of halogen is initially present in the contact material and the contact material is continuously contacted with the material containing at least one halogen during the conduct of the oxidative conversion.

Claim 10

A method in accordance with claim 1 wherein the selected contact material is contact material (6) and the introduction of the free oxygen containing gas is intervally discontinued and the material containing at least one reducing agent is substituted therefor.

Claim 11

A method in accordance with claim 9 wherein the feed organic compound comprises methane and the material containing at least one reducing agent thus substituted for the free oxygen containing gas is said methane.

Claim 12

A method in accordance with claim 9 wherein the feed organic compound comprises ethane and the material containing at least one reducing agent thus substituted for the free oxygen containing gas is said ethane.

Claim 13

A method in accordance with claim 1 wherein the selected contact material is contact material (6), the introduction of the feed organic compound and the free oxygen containing gas is intervally discontinued and the material containing at least one reducing agent is substituted for said free oxygen containing gas.

Claim 14

A method in accordance with claim 12 wherein the material containing at least one halogen is intervally contacted with the contact material simultaneously with the material containing at least one reducing agent.

Claim 15

A method in accordance with claim 12 wherein the material containing at least one halogen is intervally contacted with the contact material prior to thus substituting the material containing at least one reducing agent for the free oxygen containing gas.

Claim 16

A method in accordance with claim 14 wherein the feed organic compound comprises methane, the introduction of said methane is resumed after thus contacting the contact material with the material containing at least one halogen and the material containing at least one reducing agent thus substituted for the free oxygen containing gas is said methane.

Claim 17

A method in accordance with claim 14 wherein the feed organic material comprises ethane, the introduction of said ethane is resumed after thus contacting the contact material with the material containing at least one halogen and the material containing at least one reducing agent thus substituted for the free oxygen containing gas is said ethane.

Claim 18

In a method for the oxidative conversion of feed organic compounds to product organic compounds, in which said feed organic compounds and a free oxygen containing gas are contacted with a reaction-promoting solid contact material containing at least one metal, oxygen and at least one halogen under oxidative conversion conditions sufficient to convert said feed organic compounds to said product organic compounds, the improved method of reactivating said solid contact material, when its reaction-promoting effect has deteriorated, comprising: at least intervally contacting said solid contact material with at least one of a material containing at least one halogen and a material containing at least one reducing agent.

Claim 19

In a method for the oxidative conversion of feed organic compounds to product organic compounds, in which said feed organic compounds and a free oxygen containing gas are contacted with a reaction-promoting solid contact material containing at least one metal, oxygen and at least one halogen under oxidative conversion conditions sufficient to convert said feed organic compounds to said product organic compounds, the improved method of reactivating said solid contact material, when its reaction-promoting effect has deteriorated, comprising: at least intervally contacting said solid contact material with at least one of a material containing at least one halogen and a material containing at least one reducing agent.

Claim 20

A method in accordance with claim 17 wherein the solid contact material is selected from the group consisting of: (1) a solid contact material comprising: (A) at least one metal selected from the group consisting of Group IA metals, Group IIA metals and mixtures thereof, (B) oxygen and (C) at least one material selected from the group consisting of halogen ions and compounds containing halogen ions; (2) a solid contact material comprising: (A) at least one metal selected from the group consisting of Group IA metals, (B) at least one metal selected from the group consisting of lanthanum Series metals, (C) oxygen, (D) at least one material selected from the group consisting of halogen ions, and compounds containing halogen ions and, optionally, (E) at least one metal selected from the group consisting of Group IIA metals; (3) a solid contact material comprising: (A) at least one metal selected from the group consisting of Group IA metals, (B) zinc, (C) oxygen, (D) at least one material selected from the group consisting of halogen ions and compounds containing halogen ions and, optionally, (E) at least one metal selected from the group consisting of Group IIA metals; (4) a solid contact material comprising: (A) at least one metal selected from the group consisting of Group IA metals, (B) at least one metal selected from the group consisting of titanium and zirconium; (C) oxygen, (D) at least one material selected from the group consisting of halogen ions and compounds containing halogen ions, and, optionally, (E) at least one metal selected from the group consisting of Group IIA metals; (5) a solid contact material comprising: (A) at least one metal selected from the group consisting of Group IA metals, Group IIA metals and mixtures thereof, (B) at least one material selected from the group consisting of phosphate radicals and compounds containing phosphate radicals and, (C) at least one material selected from the group consisting of halogen ions and compounds containing halogen ions; and (6) a solid contact material comprising: (A) cobalt, (B) at least one metal selected from the group consisting of zirconium, zinc, niobium, indium, lead and bismuth, (C) phosphorous, (D) oxygen, (E) at least one material selected from the group consisting of halogen ions, and compounds containing halogen ions and, optionally, (F) at least one material selected from tht group consisting of Group IA metals, sulfur, compounds containing sulfur and mixtures thereof and said solid contact material is at least intervally contacted with the with the material containing at least one halogen, when said solid contact material is selected from the group consisting of contact materials (1), (2), (3), (4) and (5), and with at least one of the material containing at least one halogen and the material containing at least one reducing agent, when said contact material is contact material (6).

Claim 21

A method in accordance with claim 17 wherein the contact material is intervally contacted with the material containing at least one halogen.

Claim 22

A method in accordance with claim 17 wherein the contact material is continuously contacted with the material containing at least one halogen.

Claim 23

A method in accordance with claim 17 wherein the selected contact material is contact material (6) and the introduction of the free oxygen containing gas is intervally discontinued and the material containing at least one reducing agent is substituted therefor.

Claim 24

A method in accordance with claim 17 wherein the feed organic compound comprises methane and the material containing at least one reducing agent thus substituted for the free oxygen containing gas is said methane.

Claim 25

A method in accordance with claim 17 wherein the feed organic compound comprises ethane and the material containing at least one reducing agent thus substituted for the free oxygen containing gas is said ethane.

Claim 26

A method in accordance with claim 18 wherein the selected contact material is contact material (6) and the introduction of the feed organic compound and the free oxygen containing gas is intervally discontinued and the material containing at least one reducing agent is substituted for said free oxygen containing gas.

Claim 27

A method in accordance with claim 24 wherein the material containing at least one halogen is intervally contacted with the contact material simultaneously with the material containing at least one reducing agent.

Claim 28

A method in accordance with claim 24 wherein the material containing at least one halogen is intervally contacted with the contact material prior to thus substituting the material containing at least one reducing agent for the feed organic compound and the free oxygen containing gas.

Claim 29

A method in accordance with claim 24 wherein the feed organic compound comprises methane, the introduction of said methane is resumed after thus contacting the contact material with the material containing at least one halogen and the material containing at least one reducing agent thus substituted for the free oxygen containing gas is said methane.

Claim 30

A method in accordance with claim 24 wherein the feed organic material comprises ethane, the introduction of said ethane is resumed after thus contacting the contact material with the material containing at least one halogen and the material containing at least one reducing agent thus substituted for the free oxygen containing gas is said ethane.

Claim 33

A method in accordance with claim 29 wherein the solid contact material is selected from the group consisting of: (1) a solid contact material comprising: (A) at least one metal selected from the group consisting of Group IA metals, Group IIA metals and mixtures thereof; (B) oxygen and (C) at least one material selected from the group consisting of halogen ions and compounds containing halogen ions; (2) a solid contact material comprising: (A) at least one metal selected from the group consisting of Group IA metals, (B) at least one metal selected from the group consisting of lanthanum Series metals, (C) oxygen, (D) at least one material selected from the group consisting of halogen ions and compounds containing halogen ions and, optionally, (E) at least one metal selected from the group consisting of Group IIA metals; (3) a solid contact material comprising: (A) at least one metal selected from the group consisting of Group IA metals, (B) zinc, (C) oxygen, (D) at least one material selected from the group consisting of halogen ions and compounds containing halogen ions; and, optionally, (E) at least one metal selected from the group consisting of Group IIA metals; (4) a solid contact material comprising: (A) at least one metal selected from the group consisting of Group IA metals, (B) at least one metal selected from the group consisting of titanium and zirconium, (C) oxygen, (D) at least one material selected from the group consisting of halogen ions and compounds containint halogen ions and, optionally, (E) at least one metal selected from the group consisting of Group IIA metals; (5) a solid contact material comprising: (A) at least one metal selected from the group consisting of Group IA metals, Group IIA metals and mixtures thereof, (B) at least one material selected from the group consisting of phosphate radicals and compounds containing phosphate radicals and (C) at least one material selected from the group consisting of halogen ions and compounds containing halogen ions; and (6) a solid contact material comprising: (A) cobalt, (B) at least one metal selected from the group consisting of zirconium, zinc, niobium, indium, lead and bismuth, (C) phosphorous, (D) oxygen, (E) at least one material selected from the group consisting of halogen ions and compounds containing halogen ions and, optionally, (F) at least one material selected from the group consisting of Group IA metals, sulfur, compounds containing sulfur and mixtures thereof and the thus calcined combined compounds are contacted with the material containing at least one halogen, when said contact material is selected from the group consisting of contact materials (1), (2), (3), (4) and (5), and with at least one of the material containing at least one halogen and the material containing at least one reducing agent, when said contact material is contact material (6).

Claim 34

A method in accordance with claim 30 wherein the calcined combined compounds are thus contacted with a material containing at least one halogen, when said contact material is selected from the group consisting of contact materials (1), (2), (3), (4) and (5), and with at least one of the material containing at least one halogen, and with the material containing at least one reducing agent, when said contact material is contact material (6), in a reaction zone in which the feed organic compounds are to be converted to the product organic compounds.

Claim 35

A method in accordance with claim 30 wherein the selected contact material is contact material (6) and said contact material is thus contacted with the material containing at least one reducing agent.

Claim 36

A method in accordance with claim 30 wherein the selected contact material is contact material (6) and said contact material is thus contacted with the material containing at least one halogen and the material containing at least one reducing agent.

Claim 39

A method in accordance with claim 1 wherein an ineffective amount of halogen is initially present in the contact material and said amount of halogen is increased to at least an effective amount by contacting said contact material with the material containing at least one halogen prior to contacting the feed organic material and the free oxygen containing gas with said contact material.

Claim 40

A method in accordance with claim 2 wherein the contact material is thus contacted with the material containing at least one halogen, prior to contacting the feed organic material and the free oxygen containing gas with said contact material, in a reaction zone in which the oxidative conversion is carried out.

Claim 41

A method is accordance with claim 3 wherein the contact material is also intervally contacted with the material containing at least one halogen during the conduct of the oxidative conversion.

Claim 42

A method in accordance with claim 3 wherein the contact material is also contacted with the material containing at least one halogen by continuously adding said material containing at least one halogen to the feed organic compound and the free oxygen containing gas during the conduct of the oxidative conversion.

Claim 44

A method in accordance with claim 1 wherein the selected contact material is contact material (6) and the introduction of the free oxygen containing gas is intervally discontinued and the material containing at least one reducing agent is substituted therefor.

Claim 45

A method in accordance with claim 7 wherein the feed organic compound comprises methane or ethane and the material containing at least one reducing agent thus substituted for the free oxygen containing gas is said methane or said ethane respectively.

Claim 46

A method in accordance with claim 1 wherein the selected contact material is contact material (6), the introduction of the feed organic compound and the free oxygen containing gas is intervally discontinued and the material containing at least one reducing agent is substituted for said free oxygen containing gas.

Claim 47

A method in accordance with claim 9 wherein the material containing at least one halogen is intervally contacted with the contact material simultaneously with the material containing at least one reducing agent.

Claim 48

A method in accordance with claim 9 wherein the material containing at least one halogen is intervally contacted with the contact material prior to thus substituting the material containing at least one reducing agent for the free oxygen containing gas.

Claim 49

A method in accordance with claim 11 wherein the feed organic compound comprises methane or ethane, the introduction of said methane or ethane is resumed after thus contacting the contact material with the material containing at least one halogen and the material containing at least one reducing agent thus substituted for the free oxygen containing gas is said methane or ethane respectively.

Claim 53

A method in accordance with claim 13 or 14 wherein the contact material is intervally contacted with the material containing at least one halogen.

Claim 54

A method in accordance with claim 13 or 14 wherein the contact material is continuously contacted with the material containing at least one halogen.

Claim 55

A method in accordance with claim 13 or 14 wherein the selected contact material is contact material (6) and the introduction of the free oxygen containing gas is intervally discontinued and the material containing at least one reducing agent is substituted therefor.

Claim 56

A method in accordance with claim 13 or 14 wherein the feed organic compound comprises methane or ethane and the material containing at least one reducing agent thus substituted for the free oxygen containing gas is said methane or ethane respectively.

Claim 57

A method in accordance with claim 14 wherein the selected contact material is contact material (6) and the introduction of the feed organic compound and the free oxygen containing gas is intervally discontinued and the material containing at least one reducing agent is substituted for said free oxygen containing gas.

Claim 58

A method in accordance with claim 19 wherein the material containing at least one halogen is intervally contacted with the contact material simultaneously with the material containing at least one reducing agent.

Claim 59

A method in accordance with claim 19 wherein the material containing at least one halogen is intervally contacted with the contact material prior to thus substituting the material containing at least one reducing agent for the feed organic compound and the free oxygen containing gas.

Claim 60

A method in accordance with claim 19 wherein the feed organic compound comprises methane or ethane, the introduction of said methane or ethane is resumed after thus contacting the contact material with the material containing at least one halogen and the material containing at least one reducing agent thus substituted for the free oxygen containing gas is said methane or ethane respectively.

Claim 63

A method in accordance with claim 23 wherein the solid contact material is selected from the group consisting of: (1) a solid contact material comprising: (A) at least one metal selected from the group consisting of Group IA metals, Group IIA metals and mixtures thereof; (B) oxygen and (C) at least one material selected from the group consisting of halogen ions and compounds containing halogen ions; (2) a solid contact material comprising: (A) at least one metal selected from the group consisting of Group IA metals, (B) at least one metal selected from the group consisting of lanthanum Series metals, (C) oxygen, (D) at least one material seletted from the group consisting of halogen ions and compounds containing halogen ions and, optionally, (E) at least one metal selected from the group consisting of Group IIA metals; (3) a solid contact material comprising: (A) at least one metal selected from the group consisting of Group IA metals, (B) zinc, (C) oxygen, (D) at least one material selected from the group consisting of halogen ions and compounds containing halogen ions; and, cptionally, (E) at least one metal selected from the group consisting of Group IIA metals; (4) a solid contact material comprising: (A) at least one metal selected from the group consisting of Group IA metals, (B) at least one metal selected from the group consisting of titanium and zirconium, (C) oxygen, (D) at least one material selected from the group consisting of halogen ions and compounds containint halogen ions and, optionally, (E) at least one metal selected from the group consisting of Group IIA metals; (5) a solid contact material comprising: (A) at least one metal selected from the group consisting of Group IA metals, Group IIA metals and mixtures thereof, (B) at least one material selected from the group consisting of phosphate radicals and compounds containing phosphate radicals and (C) at least one material selected from the group consisting of halogen ions and compounds containing halogen ions; and (6) a solid contact material comprising: (A) cobalt, (B) at least one metal selected from the group consisting of zirconium, zinc, niobium, indium, lead and bismuth, (C) phosphorous, (D) oxygen, (E) at least one material selected from the group consisting of halogen ions and compounds containing halogen ions and, optionally, (F) at least one material selected from the group consisting of Croup IA metals, sulfur, compounds containing sulfur and mixtures thereof and the thus calcined combined compounds are contacted with the material containing at least one halogen, when said contact material is selected from the group consisting of contact materials (1), (2), (3), (4) and (5), and with at least one of the material containing at least one halogen and the material containing at least one reducing agent, when said contact material is contact material (6).

Claim 64

A method in accordance with claim 24 wherein the calcined combined compounds are thus contacted with a material containing at least one halogen, when said contact material is selected from the group consisting of contact materials (1), (2), (3), (4) and (5), and with at least one of the material containing at least one halogen, and with the material containing at least one reducing agent, when said contact material is contact material (6), in a reaction zone in which the feed organic compounds are to be conveited to the product organie c ompounds.

Claim 65

26, A method in accordance with claim 24 wherein the selected contact material is contact material (6) and said contact material is thus contacted with the material containing at least one reducing agent.

Claim 66

A method in accordance with claim 24 wherein the selected contact material is contact material (6) and said contact material is thus contacted with the material containing at least one halogen and the material containing at least one reducing agent.