High aspect ratio catalytic reactor and catalyst inserts therefor

• US 9,938,146 B2
• Filed: 12/28/2015
• Issued: 04/10/2018
• Est. Priority Date: 12/28/2015
• Status: Active Grant

• Current Assignee: Praxair Technology Incorporated (Linde Plc)
• Original Assignee: Praxair Technology Incorporated (Linde Plc)
• Inventors: Lin, Jiefeng, Kelly, Sean M.
• Primary Examiner(s): Slifka, Colin W.
• Application Number:
  US14/979,790
• Publication Number:
  US 20170183228A1
• Time in Patent Office: 834 Days
• CPC Class Codes: B01J 15/005 in the presence of catalytically active bodies, e.g. porous plates
• CPC Class Codes: B01J 19/2415 Tubular reactors
• CPC Class Codes: B01J 19/242 in series
• CPC Class Codes: B01J 19/243 spirally, concentrically or zigzag wound
• CPC Class Codes: B01J 19/2485 Monolithic reactors
• CPC Class Codes: B01J 19/249 Plate-type reactors
• CPC Class Codes: B01J 19/32 Packing elements in the form of grids or built-up elements for forming a unit or module inside the apparatus for mass or heat transfer
• CPC Class Codes: B01J 2219/2428 Catalysts coated on the surface of the monolith channels
• CPC Class Codes: B01J 2219/2454 Plates arranged concentrically
• CPC Class Codes: B01J 2219/2474 Mixing means, e.g. fins or baffles attached to the plates
• CPC Class Codes: B01J 2219/2479 Catalysts coated on the surface of plates or inserts
• CPC Class Codes: B01J 2219/2482 Catalytically active foils; Plates having catalytically activity on their own
• CPC Class Codes: B01J 2219/2485 Metals or alloys
• CPC Class Codes: B01J 2219/2487 Ceramics
• CPC Class Codes: B01J 2219/2495 the plates being assembled interchangeably or in a disposable way
• CPC Class Codes: B01J 2219/2496 Means for assembling modules together, e.g. casings, holders, fluidic connectors
• CPC Class Codes: B01J 2219/30292 rolled up
• CPC Class Codes: B01J 2219/30475 comprising catalytically active material
• CPC Class Codes: B01J 2219/32248 Sheets comprising areas that are raised or sunken from the plane of the sheet
• CPC Class Codes: B01J 2219/32251 Dimples, bossages, protrusions
• CPC Class Codes: B01J 2219/32408 : Metal
• CPC Class Codes: B01J 2219/32425 : Ceramic
• CPC Class Codes: B01J 2219/32466 : comprising catalytically active material
• CPC Class Codes: B01J 23/894 : with rare earths or actinides
• CPC Class Codes: B01J 35/40 : characterised by dimensions, e.g. grain size in a colloidal state B01J35/23; crystallite size B01J35/77
• CPC Class Codes: B01J 35/56 : Foraminous structures having flow-through passages or channels, e.g. grids or three-dimensional monoliths
• CPC Class Codes: C01B 2203/0233 : the reforming step being a steam reforming step
• CPC Class Codes: C01B 2203/085 : by electric heating
• CPC Class Codes: C01B 2203/1023 : Catalysts in the form of a monolith or honeycomb
• CPC Class Codes: C01B 2203/1058 : Nickel catalysts
• CPC Class Codes: C01B 2203/1064 : Platinum group metal catalysts
• CPC Class Codes: C01B 2203/1241 : Natural gas or methane
• CPC Class Codes: C01B 2203/1614 : Controlling the temperature
• CPC Class Codes: C01B 3/384 : the catalyst being continuously externally heated
• CPC Class Codes: Y02P 20/10 : Process efficiency
• CPC Class Codes: Y02P 20/52 : using catalysts, e.g. selective catalysts

Abstract

The present invention relates to high efficient tubular catalytic steam reforming reactor configured from about 0.2 inch to about 2 inch inside diameter high temperature metal alloy tube or pipe and loaded with a plurality of rolled catalyst inserts comprising metallic monoliths. The catalyst insert substrate is formed from a single metal foil without a central supporting structure in the form of a spiral monolith. The single metal foil is treated to have 3-dimensional surface features that provide mechanical support and establish open gas channels between each of the rolled layers. This unique geometry accelerates gas mixing and heat transfer and provides a high catalytic active surface area. The small diameter, high aspect ratio tubular catalytic steam reforming reactors loaded with rolled catalyst inserts can be arranged in a multi-pass non-vertical parallel configuration thermally coupled with a heat source to carry out steam reforming of hydrocarbon-containing feeds. The rolled catalyst inserts are self-supported on the reactor wall and enable efficient heat transfer from the reactor wall to the reactor interior, and lower pressure drop than known particulate catalysts. The heat source can be oxygen transport membrane reactors.

Claims

1. A catalyst insert for a tubular catalytic steam reforming reactor comprising a metal substrate, an interfacial catalyst layer containing an active ingredient capable of catalyzing endothermic reforming reactions;

the metal substrate is a metal foil having a 3-D pattern of surface features comprising a plurality of peaks and grooves and said foil rolled into a spiral monolith;

the spiral monolith having a characteristic length “

L_m”

, an innermost diameter “

d_i”

, an outermost diameter “

d_m”

;

a characteristic spacing “

h_m”

between layers;

wherein the ratio “

L_m/d_m”

is greater than two and the ratio “

d_i/h_m”

is less than three, wherein said 3-D pattern of surface features form about 75 peaks per square inch to about 200 peaks per square inch, and wherein said spiral monolith has a porosity of from about 50% to about 85%.

2. The catalyst insert of claim 1 wherein said active ingredient comprises at least one of Ni or Rh.

3. The catalyst insert of claim 1 wherein said interfacial catalyst layer has a thickness in the range of about 10 microns to about 80 microns.

4. The catalyst insert of claim 3 wherein said interfacial catalyst layer has a thickness in the range of about 40 microns to about 80 microns.

5. A catalytic reactor comprising a plurality of catalyst inserts according to claim 1;

the reactor having an inlet, an outlet, an exterior surface to receive heat, an interior volume defining a fluid flow passageway of length “

L”

between the inlet and the outlet;

the outlet is spaced apart from the inlet at a vertical distance “

H”

;

wherein the ratio “

H/L”

is less than 0.5; and

the ratio of the lengths of plurality of catalyst inserts to the reactor length is at least 0.8.

6. The reactor of claim 5 wherein said catalyst insert is formed from a metal foil having defined surface patterns comprising a plurality of peaks and grooves, said foil rolled into a multi-layer spiral monolith, wherein said plurality of peaks and groves provide mechanical support for each rolled layer of said spiral and establish open channels through which gas can pass between the multi-layers of said spiral, wherein said rolled multi-layer spiral has a porosity of from about 50% to about 85%.

7. A process for endothermic reforming of a methane containing feed gas utilizing the catalyst inserts of claim 1, comprising:

providing a plurality of high efficient tubular reactors arranged in a non-vertical orientation;

said reactors containing said plurality of catalyst inserts;

each of said reactors having an inlet, an outlet, an exterior surface to receive heat, an interior volume defining a passageway for fluid flow from the inlet to the outlet;

providing heat and heating said reactors exterior surface to a temperature of from about 650°

C. to about 950°

C.;

passing a feed stream containing methane and steam at a GHSV in the range of about 200,000 cm³/(hr g-cat) to about 500,000 cm³/(hr g-cat);

wherein the reformed product leaving the reactor at 850°

C. has an approach to equilibrium of less than 5°

C.

8. The process of claim 7 wherein said tubular reactor receives heat at a volumetric heat flux of from about 15,000 kW/m³ to about 25,000 kW/m³.

9. The process of claim 7 where in the heat source comprises an oxygen transport membrane reactor.