DETAILED ACTION
Notice of Pre-AIA or AIA Status
The present application, filed on or after March 16, 2013, is being examined under the first inventor to file provisions of the AIA .
Response to Amendment
Applicant’s amendment filed on February 19, 2026 has been received. Claims 1-20 are under consideration. Claims 21-30 are withdrawn from further consideration.
Response to Arguments
Applicant’s arguments filed on February 19, 2026 have been fully considered. In particular, Applicant argues that the prior art fails to disclose or teach the new limitation in the amended independent claims 1, 10, 13, and 16, which recites:
“a catalyst in which one-third of the catalyst is an acid catalyst and two-thirds of the catalyst is a reforming catalyst”.
The argument is persuasive, and therefore, the rejections under 35 U.S.C. 102 and 103 have been withdrawn. However, upon further consideration, new grounds of rejection are made in view of the newly discovered prior art to Faungnawakij et al. (Applied Catalysis A: General 304 (2006) 40-48). Faungnawakij et al. discloses a catalyst for steam reforming dimethyl ether to hydrogen, wherein the catalyst (see 2.1 Catalyst preparation) comprises an acid catalyst (i.e., a solid acid catalyst, such as alumina or zeolite) and a reforming catalyst (i.e., a Cu-based spinel oxide catalyst), of which one-third is the acid catalyst and two-thirds is the reforming catalyst (i.e., “The Cu-based spinel was mechanically mixed with the solid-acid catalyst at a fixed weight ratio of 2:1” see page 41, second column, second paragraph).
Claim Objections
Claim 9 is objected to because “allows” (at line 2) should be changed to, for instance, --that allows--. Appropriate correction is required.
Claim Rejections - 35 USC § 112
The following is a quotation of 35 U.S.C. 112(b):
(b) CONCLUSION.—The specification shall conclude with one or more claims particularly pointing out and distinctly claiming the subject matter which the inventor or a joint inventor regards as the invention.
The following is a quotation of 35 U.S.C. 112 (pre-AIA ), second paragraph:
The specification shall conclude with one or more claims particularly pointing out and distinctly claiming the subject matter which the applicant regards as his invention.
Claims 10-12 and 18 are rejected under 35 U.S.C. 112(b) or 35 U.S.C. 112 (pre-AIA ), second paragraph, as being indefinite for failing to particularly point out and distinctly claim the subject matter which the inventor or a joint inventor (or for applications subject to pre-AIA 35 U.S.C. 112, the applicant), regards as the invention.
Regarding claim 10, the limitation “circulating steam in the reactor” (at line 3) is unclear because the claim does not recite where, in the reactor, the steam is circulated. Also, the relationship between the “heat” (twice, at lines 4 and 6) and “steam” (at line 3) is unclear.
Regarding claim 11, the further limitation with respect to “powering a plurality of electric heating elements inside the casing and outside the plurality of tubes” (at lines 3-4) is unclear because the reactor embodiment in which heat is provided by steam circulating in the reactor, as set forth in claim 10, and the reactor embodiment in which heat is provided by electric heating elements inside of the casing appear to be mutually exclusive reactor embodiments, based on the disclosure.
Regarding claim 12, the further limitations with respect to “a refractory surface along an inside portion of the casing” and “a layer of insulation between the refractory surface and an outside portion of each of the plurality of tubes” are unclear because the reactor embodiment in which heat is provided by steam circulating in the reactor, as set forth in claim 10, and the reactor embodiment in which a refractory surface and a layer of insulation are provided inside the casing appear to be mutually exclusive reactor embodiments, based on the disclosure.
Regarding claim 18, the recitation of “the reaction chamber” (at line 1), which is drawn to a single reaction chamber, renders the claim indefinite because claim 16 set forth a reactor comprising a plurality of reaction chambers (i.e., a reaction chamber for each of the plurality of tubes).
Claim Rejections - 35 USC § 103
The following is a quotation of 35 U.S.C. 103 which forms the basis for all obviousness rejections set forth in this Office action:
A patent for a claimed invention may not be obtained, notwithstanding that the claimed invention is not identically disclosed as set forth in section 102, if the differences between the claimed invention and the prior art are such that the claimed invention as a whole would have been obvious before the effective filing date of the claimed invention to a person having ordinary skill in the art to which the claimed invention pertains. Patentability shall not be negated by the manner in which the invention was made.
Claims 1-9 are rejected under 35 U.S.C. 103 as being unpatentable over Yamada et al. (JP 2008-273795 A) in view of Tonkovich et al. (US 6,540,975) and Faungnawakij et al. (Applied Catalysis A: General 304 (2006) 40-48).
Regarding claim 1, Yamada et al. discloses a method for generating hydrogen using a reactor (i.e., a method for generating hydrogen using a reforming reactor 1; see FIG. 2 and translation, in particular, at the underlined portions), the method comprising:
circulating steam in the reactor (i.e., circulating a heat medium 21 such as water vapor (steam) in the reactor 1; see translation at page 5, fifth paragraph), the reactor including:
an outer tube (i.e., an outer housing of the reactor 1) including a steam inlet configured to receive the steam 21, the outer tube 1 configured to contain the steam 21, and the outer tube 1 having an outer tube dimension;
an inner tube (i.e., a reaction tube 102) situated inside an outer tube 1, the inner tube 102 configured to conduct heat from the steam contained by the outer tube 1, the inner tube 102 having an inner tube dimension smaller than the outer tube dimension, the inner tube 102 having a first end (i.e., an upper end) and a second end (i.e., a lower end), the inner tube 102 forming a reaction chamber between the first end and the second end, the reaction chamber having a catalyst (i.e., a catalyst layer 101);
a feed line (i.e., a line for introducing a DME/steam mixed gas 13) coupled to the first end (i.e., the upper end) of the inner tube 102, the feed line configured to pass dimethyl ether and steam 13 to the inner tube 102; and
a reactor outlet (i.e., an outlet for hydrogen-rich reformed gas 15) proximate to the second end (i.e., the lower end) of the inner tube 102, the reactor outlet configured to collect hydrogen from the inner tube 102 and output the hydrogen 15.
Yamada et al. does not specifically state that the outer tube 1 dimension is an outer tube diameter and the inner tube 102 dimension is an inner tube diameter.
Tonkovich et al. discloses a reactor suitable for use in a method for generating hydrogen via a steam reforming reaction (see column 1, lines 19-24 and 51-59; Example 2), wherein the reactor (i.e., a reactor configured with nested chambers; see FIG. 1b; column 3, lines 16-25) comprises: an outer tube (i.e., a vessel 100 defining an outer chamber 102 as a heat transfer chamber), the outer tube having an outer tube diameter (i.e., the vessel 100 is circular in cross-section); and an inner tube (i.e., a tube comprising a wall 106 defining an inner chamber 104 as a reaction chamber for containing a catalyst) situated inside the outer tube, the inner tube having an inner tube diameter (i.e., the tube 106 is circular in cross-section), where the inner tube diameter is smaller than the outer tube diameter; and wherein the inner tube 106 is configured to conduct heat from a heat medium contained by the outer tube 100 (i.e., in the chamber 102) (see column 2, lines 23-32; column 3, lines 62-67).
It would have been obvious for one of ordinary skill in the art before the effective filing date of the claimed invention to configure the outer tube and the inner tube in the reactor used in the method of Yamada et al. to respectively comprise an outer tube diameter and an inner tube diameter, wherein the inner tube diameter is smaller than the outer tube diameter, because the reactor configuration would have resulted in efficient transfer of heat across the wall of the inner tube, between the heat medium contained in the outer tube and the catalyst contained in the inner tube, as taught by Tonkovich et al.
Yamada et al. further discloses that the catalyst 101 catalyzes the steam reforming reaction of dimethyl ether to hydrogen. Yamada, however, fails to disclose that one-third of the catalyst 101 is an acid catalyst and two-thirds of the catalyst is a reforming catalyst.
Faungnawakij et al. discloses a method for generating hydrogen using a reactor (i.e., a method for producing hydrogen via steam reforming of dimethyl ether (DME SR), expressed as Eq. (3) on page 41, wherein the method uses a conventional flow reactor; see 2.3. Catalytic-activity evaluation); wherein the reactor defines a reaction chamber containing a catalyst (i.e., a composite catalyst; see 2.1 Catalyst preparation), the catalyst including an acid catalyst (i.e., a solid acid catalyst, such as alumina or zeolite, for the DME hydrolysis reaction, expressed as Eq. (1)) and a reforming catalyst (i.e., a Cu-based spinel oxide catalyst for the methanol steam reforming (MeOH SR) reaction, expressed as Eq. (2)). Specifically, Faungnawakij et al. discloses that one-third of the catalyst is the acid catalyst and two-thirds of the catalyst is the reforming catalyst (i.e., “The Cu-based spinel was mechanically mixed with the solid-acid catalyst at a fixed weight ratio of 2:1 in this study.” see page 41, second column, second paragraph).
It would have been obvious for one of ordinary skill in the art before the effective filing date of the claimed invention to substitute the catalyst of Faungnawakij et al. for the catalyst used in the method of Yamada et al. because the catalyst, having a 2:1 weight ratio of the reforming catalyst to the acid catalyst, would have exhibited high activity for the steam reforming reaction of dimethyl ether for the production of hydrogen, as taught by Faungnawakij et al. (see Abstract and 4. Conclusions).
Regarding claim 2, Yamada et al. (see FIG. 2) further discloses the catalyst 101 receives heat from the steam 21 contained by the outer tube.
Regarding claim 3, Yamada et al. (see FIG. 2) further discloses that the method comprises: adding dimethyl ether and steam (i.e., DME/steam mixed gas 13) to the reaction chamber 102 with the catalyst 101 heated by the steam 21 contained by the outer tube; wherein the reaction chamber 102 produces hydrogen (i.e., hydrogen-rich reformed gas 15) in response to a coordinated reaction of the dimethyl ether and steam with the catalyst 101. In the modified method of Yamada et al., the coordinated reaction of the dimethyl ether and steam would be performed in the presence of the catalyst taught by Faungnawakij et al.
Regarding claim 4, Faungnawakij et al. further discloses feeding dimethyl ether and steam to the reaction chamber as a gas composition of 15% DME, 45% steam, and N2 balance, having a steam-to-carbon molar ratio (S/C) = 1.5 (see 2.3. Catalytic-activity evaluation; also, the descriptions under FIG. 1-7). Dimethyl ether (CH3OCH3) contains 2 moles of carbon per 1 mole of the compound. Thus, the molar ratio of steam-to-dimethyl ether equals 3. It would have been obvious for one of ordinary skill in the art before the effective filing date of the claimed invention to feed the steam and dimethyl ether to the reaction chamber at a steam-to-dimethyl ether molar ratio between 2 to 4 in the modified method of Yamada et al. because a molar ratio within this range—specifically, a molar ratio equal to 3, was shown to be a suitable for effecting the steam reforming reaction of dimethyl ether in the presence of the described catalysts for the production of hydrogen, as taught by Faungnawakij et al.
Regarding claim 5, Faungnawakij et al. (see page 41) further discloses that methanol is produced by a hydrolysis of the dimethyl ether over the acid catalyst (i.e., via DME hydrolysis, expressed as Eq. (1)), and a steam reforming of the methanol is performed by the reforming catalyst (i.e., via MeOH SR, expressed as Eq. (2)).
Regarding claim 6, Yamada et al. (see FIG. 2) further discloses that the inner tube 102 is configured to heat the catalyst 101 in response to conducting heat from the steam 21 contained by the outer tube 1.
Regarding claim 7, Faungnawakij et al. discloses that the catalyst (i.e., the zeolite-based composite catalyst; see 3.2.2. Zeolite-type catalysts as acidic catalyst) catalyzes the steam reforming reaction of dimethyl ether to hydrogen at a temperature in the range of 200 to 275 °C, with hydrogen production increasing as the temperature increases from 200 °C to approx. 275 °C, and the temperature being generally limited at or below 300 °C (see Abstract, FIG. 3(b), and 4. Conclusions). Therefore, it would have been obvious for one of ordinary skill in the art before the effective filing date of the claimed invention to heat the reaction chamber to a temperature between 225 and 300 °C using the steam in the modified method of Yamada et al. because a temperature within this range was shown to be optimal for carrying out the steam reforming reaction of dimethyl ether in the presence of the zeolite-based catalyst for the production of hydrogen, as taught by Faungnawakij et al.
Regarding claim 8, Yamada et al. (see FIG. 2) further discloses that the outer tube 1 comprises a steam condensate outlet (i.e., an outlet for removing condensed water vapor as the spent heat medium 23).
Regarding claim 9, Yamada et al. (see FIG. 2) further discloses that the reactor comprises a spacing between the outer tube 1 and the inner tube 102 that allows the steam 21 to circulate and condense inside the outer tube 1.
Claim 10 is rejected under 35 U.S.C. 103 as being unpatentable over Yamada et al. (JP 2008-273795 A) in view of Faungnawakij et al. (Applied Catalysis A: General 304 (2006) 40-48).
Yamada et al. discloses a method for generating hydrogen using a reactor (i.e., a method for generating hydrogen using a reforming reactor 1; see FIG. 2 and translation, in particular, at the underlined portions), the method comprising:
circulating steam in the reactor (i.e., circulating a heat medium 21, such as water vapor (steam) in the reactor 1; see translation at page 5, fifth paragraph), the reactor including:
a casing configured to contain heat (i.e., an outer casing of the reforming reactor 1, through which the heat medium 21 flows);
a plurality of tubes situated inside the casing (i.e., a reaction tube 102 as shown, wherein a plurality of the reaction tubes 102 can be provided in parallel in the reforming reactor 1; see translation at page 5, second to last paragraph), the tubes 102 each having a first end (i.e., an upper end) and a second end (i.e., a lower end), the tubes 102 each forming a reaction chamber between the first end and the second end of each of the tubes 102, and each reaction chamber having a catalyst (i.e., a catalyst layer 101);
a feed line (i.e., a line for introducing a DME/steam mixed gas 13) coupled to each of the first end (i.e., the upper end) of the plurality of tubes 102, the feed line configured to pass dimethyl ether and steam 13 to the plurality of tubes 102; and
a reactor outlet (i.e., an outlet for hydrogen-rich reformed gas 15) proximate to each of the second end (i.e., the lower end) of the plurality of tubes 102, the reactor outlet configured to collect hydrogen from the tubes 102 and output the hydrogen 15.
Yamada et al. discloses that the catalyst 101 catalyzes the steam reforming reaction of dimethyl ether to hydrogen. Yamada, however, fails to disclose that one-third of the catalyst 101 is an acid catalyst and two-thirds of the catalyst is a reforming catalyst.
Faungnawakij et al. discloses a method for generating hydrogen using a reactor (i.e., a method for producing hydrogen via steam reforming of dimethyl ether (DME SR), expressed as Eq. (3) on page 41, wherein the method uses a conventional flow reactor; see 2.3. Catalytic-activity evaluation); wherein the reactor defines a reaction chamber containing a catalyst (i.e., a composite catalyst; see 2.1 Catalyst preparation), the catalyst including an acid catalyst (i.e., a solid acid catalyst, such as alumina or zeolite, for DME hydrolysis, expressed as Eq. (1)) and a reforming catalyst (i.e., a Cu-based spinel oxide catalyst for methanol steam reforming (MeOH SR), expressed as Eq. (2)). Specifically, Faungnawakij et al. discloses that one-third of the catalyst is the acid catalyst and two-thirds of the catalyst is the reforming catalyst (i.e., “The Cu-based spinel was mechanically mixed with the solid-acid catalyst at a fixed weight ratio of 2:1 in this study.” see page 41, second column, second paragraph).
It would have been obvious for one of ordinary skill in the art before the effective filing date of the claimed invention to substitute the catalyst of Faungnawakij et al. for the catalyst in the method of Yamada et al. because the catalyst, having a 2:1 weight ratio of reforming catalyst to acid catalyst, would have exhibited high activity for the steam reforming reaction of dimethyl ether for the production of hydrogen, as taught by Faungnawakij et al. (see Abstract and 4. Conclusions).
Claims 10 and 13-15 are rejected under 35 U.S.C. 103 as being unpatentable over Pierce (US 2,667,410) in view of Faungnawakij et al. (Applied Catalysis A: General 304 (2006) 40-48).
Regarding claim 10, Pierce discloses a method for generating hydrogen using a reactor (i.e., a method for generating hydrogen using an apparatus for steam reforming hydrocarbons such as natural gas; see Figure; column 5, lines 7-50), the method comprising:
circulating steam in the reactor (i.e., steam in excess of the stoichiometric amount is supplied to the reactor, through line 20), the reactor including:
a casing (i.e., a furnace 28) configured to contain heat (i.e., heat generated by a plurality of burners 40);
a plurality of tubes (i.e., catalyst tubes 26) situated inside the casing, the plurality of tubes 26 configured to conduct heat contained by the casing 28, the plurality of tubes 26 each having a first end (i.e., an upper end) and a second end (i.e., a lower end), the plurality of tubes 26 each forming a reaction chamber between the first end and the second end of each of the tubes, each reaction chamber containing a reforming catalyst (see column 2, lines 36-38);
a feed line (i.e., a manifold 24) coupled to each of the first end (i.e., the upper end) of the plurality of tubes 26, the feed line 24 configured to pass a hydrocarbon (i.e., natural gas that has been treated for the removal of hydrogen sulfide and organic sulphur is supplied to the reactor via line 10; see column 2, lines 30-38) and steam (i.e., supplied via the line 20) to the plurality of tubes 26; and
a reactor outlet (i.e., a line 30 withdrawing reformed gas) proximate to each of the second end (i.e., the lower end) of the plurality of tubes 26, the reactor outlet 30 configured to collect hydrogen from the plurality of tubes and output the hydrogen (i.e., the reformed gas contains hydrogen).
Pierce discloses that the method generates hydrogen by steam reforming hydrocarbons such as natural gas, where the natural gas has been treated for the removal of hydrogen sulfide and organic sulphur (see column 2, lines 20-34). Pierce fails to disclose a method for generating hydrogen by steam reforming dimethyl ether, instead of natural gas, wherein each reaction chamber of the reactor contains a catalyst in which one-third of the catalyst is an acid catalyst and two-thirds of the catalyst is a reforming catalyst.
Faungnawakij et al. discloses a method for generating hydrogen using a reactor (i.e., a method for producing hydrogen via steam reforming of dimethyl ether (DME SR), expressed as Eq. (3) on page 41, wherein the method uses a conventional flow reactor; see 2.3. Catalytic-activity evaluation); wherein the reactor defines a reaction chamber containing a catalyst (i.e., a composite catalyst; see 2.1 Catalyst preparation), the catalyst including an acid catalyst (i.e., a solid acid catalyst, such as alumina or zeolite, for the DME hydrolysis reaction, expressed as Eq. (1)) and a reforming catalyst (i.e., a Cu-based spinel oxide catalyst for the methanol steam reforming (MeOH SR) reaction, expressed as Eq. (2)). Specifically, Faungnawakij et al. discloses that one-third of the catalyst is the acid catalyst and two-thirds of the catalyst is the reforming catalyst (i.e., “The Cu-based spinel was mechanically mixed with the solid-acid catalyst at a fixed weight ratio of 2:1 in this study.” see page 41, second column, second paragraph).
It would have been obvious for one of ordinary skill in the art before the effective filing date of the claimed invention to modify the reactor in the method of Pierce so that the reactor was used to generate hydrogen via steam reforming of dimethyl ether, instead of natural gas, with each reaction chamber containing a catalyst having one-third acid catalyst and two-thirds reforming catalyst, because i) dimethyl ether has a high hydrogen-to-carbon ratio and a high energy density, is non-toxic, and can be easily handled, stored, and transported; ii) unlike natural gas, dimethyl ether does not require prior desulfurization; iii) the steam reforming reaction of dimethyl ether can be conducted at a lower temperature than the conventional steam reforming reaction of natural gas; and iv) a high activity for the dimethyl ether steam reforming reaction can be attained through the use of the described catalysts, in which one-third of the catalyst is an acid catalyst and two-thirds of the catalyst is a reforming catalyst, as taught by Faungnawakij et al. (see Abstract, 1. Introduction, and 4. Conclusions).
Regarding claim 13, Pierce discloses a reactor (i.e., an apparatus for reforming hydrocarbons such as natural gas; see Figure; column 5, lines 7-50) comprising:
a shell (i.e., a furnace 28) configured to contain heat (i.e., heat is generated by a plurality of burners 40);
a plurality of tubes (i.e., catalyst tubes 26) nested inside the shell 28, the tubes 26 configured to conduct heat from the heat contained inside the shell 28, the tubes 26 each having a first end (i.e., an upper end) and a second end (i.e., a lower end), and the tubes 26 each forming a reaction chamber between the first end and the second end, each reaction chamber containing a reforming catalyst (see column 2, lines 36-38);
a feed line (i.e., a manifold 24) coupled to each of the first end (i.e., upper end) of the plurality of tubes 26, the feed line 24 configured to receive the hydrocarbons (i.e., natural gas from line 10) and steam (i.e., from line 20); and
a reactor outlet (i.e., a line 30 withdrawing reformed gas) proximate to each of the second end (i.e., the lower end) of the plurality of tubes 26, the reactor outlet 30 configured to collect hydrogen from the plurality of tubes and output the hydrogen (i.e., the reformed gas contains hydrogen).
Pierce discloses that the reactor generates hydrogen by steam reforming hydrocarbons such as natural gas, where the natural gas has been treated for the removal of hydrogen sulfide and organic sulphur (see column 2, lines 20-34). Pierce fails to disclose that the reactor is configured to generate hydrogen by steam reforming dimethyl ether, instead of natural gas, wherein each reaction chamber contains a catalyst in which one-third of the catalyst is an acid catalyst and two-thirds of the catalyst is a reforming catalyst.
Faungnawakij et al. discloses a reactor (i.e., a conventional flow reactor, see 2.3. Catalytic-activity evaluation; where the reactor produces hydrogen via steam reforming of dimethyl ether, expressed as Eq. (3) on page 41); the reactor defining a reaction chamber containing a catalyst (i.e., a composite catalyst; see 2.1 Catalyst preparation) including an acid catalyst (i.e., a solid acid catalyst, such as alumina or zeolite, for DME hydrolysis, expressed as Eq. (1)) and a reforming catalyst (i.e., a Cu-based spinel oxide catalyst for methanol steam reforming, expressed as Eq. (2)). Specifically, Faungnawakij et al. discloses that one-third of the catalyst is the acid catalyst and two-thirds of the catalyst is the reforming catalyst (i.e., “The Cu-based spinel was mechanically mixed with the solid-acid catalyst at a fixed weight ratio of 2:1 in this study.” see page 41, second column, second paragraph).
It would have been obvious for one of ordinary skill in the art before the effective filing date of the claimed invention to modify the reactor of Pierce so that the reactor was configured to generate hydrogen by steam reforming of dimethyl ether, instead of natural gas, with each reaction chamber containing a catalyst that was one-third acid catalyst and two-thirds reforming catalyst, because i) dimethyl ether has a high hydrogen-to-carbon ratio and a high energy density, is non-toxic, and can be easily handled, stored, and transported; ii) unlike natural gas, dimethyl ether does not require prior desulfurization; iii) the steam reforming reaction of dimethyl ether can be conducted at a lower temperature than the conventional steam reforming reaction of natural gas; and iv) a high activity for the dimethyl ether steam reforming reaction can be attained through the use of the described catalysts, in which one-third of the catalyst is an acid catalyst and two-thirds of the catalyst is a reforming catalyst, as taught by Faungnawakij et al. (see Abstract, 1. Introduction, and 4. Conclusions).
Regarding claim 14, Pierce discloses that the reactor comprises a plurality of burners 40 inside the shell 28, the burners configured to generate the heat contained inside the shell; and a shell outlet configured to output flue gas (i.e., an outlet opening 44 for combustion gases).
Regarding claim 15, Pierce discloses that the plurality of burners is configured to turn on simultaneously for maintaining uniform temperature (i.e., each burner 40 is connected to a common fuel gas line 38, such that the burners 40 can be turned on simultaneously); and the shell is a fire box (i.e., the furnace 28 is a box which contains the flames of the burners 40).
Claim 11 is rejected under 35 U.S.C. 103 as being unpatentable over Pierce (US 2,667,410) in view of Faungnawakij et al. (Applied Catalysis A: General 304 (2006) 40-48), as applied to claim 10 above, and further in view of van der Ploeg (US 2021/0113980).
Pierce fails to disclose that the method further comprises: powering a plurality of electric heating elements inside the casing 28 and outside the plurality of tubes 26, wherein the plurality of tubes 26 is configured to conduct the heat contained by the casing, with the heat being provided by the electric heating elements. In contrast, Pierce discloses a plurality of burners 40 for providing the heat in the casing 28.
van der Ploeg discloses a method for generating hydrogen using a reactor (i.e., a method for generating hydrogen by reforming hydrocarbons an electrically heated reactor; see FIG. 1, 3; paragraph [0048]-[0049]), wherein the reactor comprising a casing configured to contain heat (i.e., a furnace defined by a furnace outer wall); a plurality of tubes inside the casing (see paragraph [0030]), the tubes configured to conduct heat contained by the casing; a feed line (i.e., a line coupled to an upper end of the tubes) configured to pass hydrocarbons and steam to the tubes, and a reactor outlet (i.e., a line coupled to a lower end of the tubes) to collect hydrogen from the tubes and output the hydrogen. Specifically, van der Ploeg discloses that the method comprises: powering a plurality of electric heating elements inside the casing and outside the tubes (i.e., powering a plurality of resistance-based heating elements; see FIG. 1, 3; paragraphs [0019]-[0026]), wherein the tubes conduct the heat contained by the casing.
It would have been obvious for one of ordinary skill in the art before the effective filing date of the claimed invention to modify the reactor as used in the modified method of Pierce to power a plurality of electric heating elements inside the casing and outside the tubes because the catalyst in the tubes could be heated by means of electrical heating, instead of by burning fuel, with the result that the production of CO2, which is a greenhouse gas, would be significantly reduced, as taught by van der Ploeg (see paragraphs [0002], [0038]).
Claim 12 is rejected under 35 U.S.C. 103 as being unpatentable over Pierce (US 2,667,410) in view of Faungnawakij et al. (Applied Catalysis A: General 304 (2006) 40-48), as applied to claim 10 above, and further in view of Meumann (US 4,840,131).
Pierce discloses that the casing comprises a refractory surface along an inside portion of the casing (i.e., the furnace 28 is made of or lined with fire and heat resistant refractories; see column 4, lines 21-24; column 5, lines 27-28). Pierce, however, fails to disclose that the casing 28 further comprises a layer of insulation between the refractory surface and an outside portion of each of the plurality of tubes 26.
Meumann discloses an apparatus (i.e., a gas-fired furnace; see FIG. 1; column 3, lines 6-23) comprising: a casing configured to contain heat (i.e., a casing of the furnace); wherein the casing comprises a refractory surface along an inside portion of the casing (i.e., a refractory surface of a board 3 made of refractory material), and the casing further comprises a layer of insulation (i.e., a further board 2 made of refractory heat-insulating material) between the refractory surface and a space within which a material or article is to be heated.
It would have been obvious for one of ordinary skill in the art before the effective filing date of the claimed invention to configure the casing of the reactor used in the modified method of Pierce to comprise a refractory surface along an inside portion of the casing and to further comprise a layer of insulation between the refractory surface and an outside portion of the tubes because the multiple layers of refractory material and insulation would have ensured that the casing was adequately insulated, as taught by Meumann.
Claims 16-18 and 20 are rejected under 35 U.S.C. 103 as being unpatentable over Miyake et al. (JP 2003-073104 A) in view of Faungnawakij et al. (Applied Catalysis A: General 304 (2006) 40-48).
Regarding claim 16, Miyake et al. discloses a reactor (i.e., a conventional steam reformer 101 used for steam-reforming a gaseous reforming raw material, such as dimethyl ether; see FIG. 3 and translation at paragraphs [0002]-[0004], [0018]) comprising:
a shell (i.e., a heat medium container 103) configured to contain heat (i.e., a heat medium, introduced into the heat medium container via an inlet 104 and discharged from the heat medium container via an outlet 105);
a top tube plate coupled to a top portion of the shell (i.e., a horizontal plate coupled to an upper end of the heat medium container 103, as shown), the top tube plate including a plurality of top tube plate apertures (i.e., the apertures respectively receiving the upper ends of circular tubes 102);
a bottom tube plate coupled to a bottom portion of the shell (i.e., a horizontal plate coupled to a lower end of the heat medium container 103, as shown), the bottom tube plate including a plurality of bottom tube plate apertures (i.e., the apertures respectively receiving the lower ends of circular tubes 102);
a plurality of tubes (i.e., the circular tubes 102) configured to extend between the top tube plate and the bottom tube plate, each of the tubes 102 configured to be inserted inside a top tube plate aperture of the plurality of top tube plate apertures and a bottom tube plate aperture of the plurality of bottom tube plate apertures (as shown); the plurality of tubes 102 configured to conduct heat from the heat contained inside the shell 103 (i.e., the inside of each circular tube 102 serves as a catalyst filling chamber, and the catalyst filling chamber is heated by the heat medium in the heat medium container 103), the tubes 102 each forming a reaction chamber (i.e., a catalyst filling chamber) between the top tube plate and the bottom tube plate;
a feed line (i.e., an inlet 106 for introducing the gaseous reforming raw material together with steam) proximate to the top portion of the shell 103, the feed line 106 being configured to pass dimethyl ether (i.e., dimethyl ether as the gaseous reforming raw material) and steam to the plurality of tubes 102; and
a reactor outlet (i.e., an outlet 107) proximate to the bottom portion of the shell 103, the reactor outlet 107 configured to collect hydrogen from the plurality of tubes 102 (i.e., a reformed gas comprising hydrogen) and output the hydrogen.
Miyake et al. discloses that each reaction chamber contains a catalyst for steam reforming dimethyl ether to hydrogen. Miyake et al., however, fails to disclose that one-third of the catalyst is an acid catalyst and two-thirds of the catalyst is a reforming catalyst.
Faungnawakij et al. discloses a catalyst for steam reforming dimethyl ether to produce hydrogen (i.e., dimethyl ether steam reforming (DME SR), expressed as Eq. (3) on page 41); wherein the catalyst (i.e., a composite catalyst; see 2.1 Catalyst preparation) includes an acid catalyst (i.e., a solid acid catalyst, such as alumina or zeolite, for DME hydrolysis, expressed as Eq. (1)) and a reforming catalyst (i.e., a Cu-based spinel oxide catalyst for methanol steam reforming (MeOH SR), expressed as Eq. (2)). Specifically, Faungnawakij et al. discloses that one-third of the catalyst is the acid catalyst and two-thirds of the catalyst is the reforming catalyst (i.e., “The Cu-based spinel was mechanically mixed with the solid-acid catalyst at a fixed weight ratio of 2:1 in this study.” see page 41, second column, second paragraph).
It would have been obvious for one of ordinary skill in the art before the effective filing date of the claimed invention to substitute the catalyst of Faungnawakij et al. for the catalyst in the reactor of Miyake et al. because the catalyst, having a 2:1 weight ratio of the reforming catalyst to the acid catalyst, would have exhibited high activity for the steam reforming reaction of dimethyl ether for the production of hydrogen, as taught by Faungnawakij et al. (see Abstract and 4. Conclusions).
Regarding claim 17, Miyake et al. (see FIG. 3; paragraph [0002]) discloses that the catalyst is configured to receive the heat contained by the plurality of tubes (i.e., the catalyst within the circular tubes 102 receives heat transferred from the surrounding heat medium in the heat medium container 103 through the walls of the circular tubes 102).
Regarding claim 18, Faungnawakij et al. (see page 41) discloses that methanol is produced by a hydrolysis of the dimethyl ether over the acid catalyst (i.e., via DME hydrolysis, expressed as Eq. (1)), and a steam reforming of the methanol is performed by the reforming catalyst (i.e., via MeOH SR, expressed as Eq. (2)).
Regarding claim 20, Miyake et al. (see FIG. 3) discloses a spacing between the shell 103 and the tubes 102, wherein the spacing allows a heating oil (i.e., a heat medium such as synthetic oil, see translation at page 5, fifth paragraph) to circulate inside the shell 103.
Claim 19 is rejected under 35 U.S.C. 103 as being unpatentable over Miyake et al. (JP 2003-073104 A) in view of Faungnawakij et al. (Applied Catalysis A: General 304 (2006) 40-48), as applied to claim 17 above, and further in view of Yamada et al. (JP 2008-273795 A).
Miyake et al. (see FIG. 3) discloses that the plurality of tubes 102 are configured to heat the catalyst (i.e., inside the tubes 102) in response to conducting heat from the heat medium (i.e., introduced via inlet 104) contained by the shell 103. Miyake mentions the use of heating oil for the heat medium (i.e., synthetic oil; see translation at page 5, fifth paragraph). Miyake et al., however, fails to disclose steam for the heat medium.
Yamada et al. discloses a reactor (i.e., a reforming reactor 1; see FIG. 2; translation, in particular, at underlined portions), comprising: a shell configured to contain heat (i.e., an outer shell of the reforming reactor 1, receiving a heat medium 21); a plurality of tubes inside the shell 1 (i.e., a reaction tube 102 as shown, wherein a plurality of reaction tubes 102 can be provided in the reforming reactor 1; see translation at page 5, second to last paragraph), the tubes 102 being configured to conduct heat from the heat 21 contained inside the shell 1, the tubes 102 each forming a reaction chamber containing a catalyst (i.e., a catalyst layer 101); a feed line (i.e., a line for introducing a DME/steam mixed gas 13) to pass dimethyl ether and steam 13 to the tubes 102; and a reactor outlet (i.e., an outlet for hydrogen-rich reformed gas 15) to collect hydrogen from the tubes 102 and output the hydrogen 15. Specifically, Yamada et al. discloses that the heat can be provided by a heat medium such as steam (water vapor) or heating oil (heat medium oil) (see translation at page 5, underlined).
It would have been obvious for one of ordinary skill in the art before the effective filing date of the claimed invention to configure the plurality of tubes to heat the catalyst in response to conducting heat from steam contained by the shell in the modified reactor of Mikyake et al. because either steam or heating oil would have been considered a suitable source of heat for heating the catalyst in the tubes to a temperature that was sufficient to carry out the steam reforming reaction of dimethyl ether to produce hydrogen, as taught by Yamada et al.
Conclusion
The prior art made of record and not relied upon is considered pertinent to applicant's disclosure: Faungnawakij et al. (Applied Catalysis A: General 333 (2007) 114-121) is cited to further illustrate the state of the art.
Applicant's amendment necessitated the new ground(s) of rejection presented in this Office action. Accordingly, THIS ACTION IS MADE FINAL. See MPEP § 706.07(a). Applicant is reminded of the extension of time policy as set forth in 37 CFR 1.136(a).
A shortened statutory period for reply to this final action is set to expire THREE MONTHS from the mailing date of this action. In the event a first reply is filed within TWO MONTHS of the mailing date of this final action and the advisory action is not mailed until after the end of the THREE-MONTH shortened statutory period, then the shortened statutory period will expire on the date the advisory action is mailed, and any nonprovisional extension fee (37 CFR 1.17(a)) pursuant to 37 CFR 1.136(a) will be calculated from the mailing date of the advisory action. In no event, however, will the statutory period for reply expire later than SIX MONTHS from the mailing date of this final action.
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/JENNIFER A LEUNG/Primary Examiner, Art Unit 1774
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