CN115318285A - Self-activating Pt-based catalyst for hydrogen production by reforming bioethanol and preparation method thereof - Google Patents
Self-activating Pt-based catalyst for hydrogen production by reforming bioethanol and preparation method thereof Download PDFInfo
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- CN115318285A CN115318285A CN202211128909.6A CN202211128909A CN115318285A CN 115318285 A CN115318285 A CN 115318285A CN 202211128909 A CN202211128909 A CN 202211128909A CN 115318285 A CN115318285 A CN 115318285A
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
- B01J23/38—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals
- B01J23/54—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals combined with metals, oxides or hydroxides provided for in groups B01J23/02 - B01J23/36
- B01J23/56—Platinum group metals
- B01J23/63—Platinum group metals with rare earths or actinides
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
- B01J23/002—Mixed oxides other than spinels, e.g. perovskite
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- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B3/00—Hydrogen; Gaseous mixtures containing hydrogen; Separation of hydrogen from mixtures containing it; Purification of hydrogen
- C01B3/02—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen
- C01B3/32—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air
- C01B3/323—Catalytic reaction of gaseous or liquid organic compounds other than hydrocarbons with gasifying agents
- C01B3/326—Catalytic reaction of gaseous or liquid organic compounds other than hydrocarbons with gasifying agents characterised by the catalyst
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J2523/00—Constitutive chemical elements of heterogeneous catalysts
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- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
- C01B2203/02—Processes for making hydrogen or synthesis gas
- C01B2203/0205—Processes for making hydrogen or synthesis gas containing a reforming step
- C01B2203/0227—Processes for making hydrogen or synthesis gas containing a reforming step containing a catalytic reforming step
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- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
- C01B2203/12—Feeding the process for making hydrogen or synthesis gas
- C01B2203/1205—Composition of the feed
- C01B2203/1211—Organic compounds or organic mixtures used in the process for making hydrogen or synthesis gas
- C01B2203/1217—Alcohols
- C01B2203/1229—Ethanol
Abstract
The invention discloses a self-activating Pt-based catalyst for hydrogen production by reforming bioethanol, which comprises Al 2 O 3 A matrix of microspheres of said Al 2 O 3 The microsphere matrix is loaded with a composite solid solution; the composite solid solution contains three metal elements of Ce, la and Pt, presents a cerium oxide fluorite cubic structure and is recorded as: ce 1‑x‑y La x Pt y O 2‑δ (ii) a Wherein x is more than or equal to 0.3 and less than or equal to 0.4; y is more than or equal to 0.03 and less than or equal to 0.10; delta is more than or equal to 0.15 and less than or equal to 0.3; h gradually generated by self-activating Pt-based catalyst in process of hydrogen production by reforming bioethanol 2 Reduction, pt species from CeO 2 Precipitating in crystal lattice, reducing into metal particles to form Pt/Ce 1‑x La x O 2‑δ /Al 2 O 3 A catalyst. Said catalyst is cheap, and has good methane dry-method and wet-method reforming performance, and possesses the advantages of high activity and high selectivityThe efficiency of hydrogen production by reforming bioethanol is effectively improved.
Description
Technical Field
The invention relates to the technical field of hydrogen production by reforming bioethanol, in particular to a self-activating Pt-based catalyst for hydrogen production by reforming bioethanol and a preparation method thereof.
Background
The biological ethanol reforming hydrogen production adopts an efficient chemical process, utilizes mature renewable energy sources, is a green hydrogen preparation technology which is expected to quickly realize industrialization, and in the biological ethanol reforming hydrogen production reaction process, ethanol is used as C2+ alcohol, so that the energy density is higher, the toxicity and the corrosivity are lower, but the C-C bond activation energy is higher than that of a C-H bond and a C-O bond, so that the conversion efficiency of the C2+ alcohol is easily limited, more organic byproducts are produced, and the carbon deposition is more serious. Therefore, a catalyst with high activity and high selectivity is needed to improve the efficiency of hydrogen production by reforming bioethanol.
The related catalysts for hydrogen production by reforming bioethanol are various in types, and precious metals such as Rh, ru, au, pd, pt and Ir, and non-precious metals such as Cu, ni and Co can be used as active components of the catalyst for hydrogen production by reforming bioethanol. Among them, rh is good in performance but expensive, and the reaction of the high-temperature section for hydrogen production by ethanol reforming is mainly methane dry reforming and wet reforming, and Rh is not the most suitable active component; while other cheap active components such as Ni can be used as active components for bioethanol reforming and methane reforming, ni-based catalysts generally have poor carbon deposition resistance and are difficult to have potential for industrial application in a short period. Therefore, it is necessary to develop a catalyst with high activity, high selectivity and relatively low cost to improve the efficiency of hydrogen production by reforming bioethanol.
Disclosure of Invention
The invention aims to provide a self-activating Pt-based catalyst for hydrogen production by bioethanol reforming and a preparation method thereof, wherein the catalyst is low in price, good in methane dry-method and wet-method reforming performances, high in activity and high in selectivity, and can effectively improve the hydrogen production efficiency by bioethanol reforming.
The purpose of the invention is realized by the following technical scheme:
a self-activating Pt-based catalyst for bioethanol reforming hydrogen production, the self-activating Pt-based catalyst comprising: al (Al) 2 O 3 A matrix of microspheres of said Al 2 O 3 The microsphere matrix is loaded with a composite solid solution;
the composite solid solution contains three metal elements of Ce, la and Pt, presents a cerium oxide fluorite cubic structure and is recorded as:
Ce 1-x-y La x Pt y O 2-δ ；
wherein x is more than or equal to 0.3 and less than or equal to 0.4; y is more than or equal to 0.03 and less than or equal to 0.10; delta is more than or equal to 0.15 and less than or equal to 0.3; the three parameters x, y, δ are calculated as follows:
x＝mol(La)/[mol(Ce)+mol(La)+mol(Pt)]
y＝mol(Pt)/[mol(Ce)+mol(La)+mol(Pt)]
δ＝2*(1-mol(Ce 4+ ))/[mol(Ce)+mol(La)+mol(Pt)]
wherein mol (Ce), mol (La), mol (Pt) and mol (Ce) 4+ ) Respectively Ce, la, pt and Ce 4+ The molar amount of (c); δ is the oxygen hole concentration;
h generated by the self-activated Pt-based catalyst gradually in the process of hydrogen production reaction by reforming bioethanol 2 Reduction, pt species from CeO 2 Precipitating in crystal lattice, reducing into metal particles to form Pt/Ce 1-x La x O 2-δ /Al 2 O 3 A catalyst; on the Pt/Ce formed 1-x La x O 2-δ /Al 2 O 3 In the catalyst, pt is highly dispersed in Ce 1-x La x O 2-δ Surface, ce 1-x La x O 2-δ In Al 2 O 3 The surface was spread.
The technical scheme provided by the invention shows that the catalyst is low in price, and the methane dry-method and wet-method reforming performance is good, so that the catalyst has the advantages of high activity and high selectivity, and can effectively improve the efficiency of hydrogen production by reforming bioethanol.
Drawings
In order to more clearly illustrate the technical solutions of the embodiments of the present invention, the drawings needed to be used in the description of the embodiments are briefly introduced below, and it is obvious that the drawings in the following description are only some embodiments of the present invention, and it is obvious for those skilled in the art to obtain other drawings based on the drawings without creative efforts.
FIG. 1 is an X-ray diffraction (XRD) pattern of a composite solid solution according to an embodiment of the present invention;
fig. 2 is a schematic flow chart of a preparation process of a self-activated Pt-based catalyst for hydrogen production by bioethanol reforming according to an embodiment of the present invention.
Detailed Description
The technical solutions in the embodiments of the present invention are clearly and completely described below with reference to the drawings in the embodiments of the present invention, and it is obvious that the described embodiments are only a part of the embodiments of the present invention, rather than all of the embodiments, and this does not limit the present invention. All other embodiments, which can be derived by a person skilled in the art from the embodiments of the present invention without making any creative effort, shall fall within the protection scope of the present invention.
The application provides a self-activating Pt-based catalyst for hydrogen production by bioethanol reforming, which comprises: al (Al) 2 O 3 A matrix of microspheres of said Al 2 O 3 The microsphere matrix is loaded with a composite solid solution;
the composite solid solution contains three metal elements of Ce, la and Pt, presents a cerium oxide fluorite cubic structure, as shown in figure 1, an XRD (X-ray diffraction) pattern of the composite solid solution in the embodiment of the invention is shown, and a sample tested in figure 1 is Ce 0.65 La 0.3 Pt 0.05 O 1.78 /Al 2 O 3 ，Ce 0.65 La 0.3 Pt 0.05 O 1.72 /Al 2 O 3 (mol/mol) =17mol.%, the XRD spectrum shows a typical cubic structure of ceria fluorite, there is no La and Pt related peaks in the spectrum, which can be explained by the La and Pt ions having been doped into the ceria lattice to form a solid solution, no significant Al is present 2 O 3 The peak indicates that the composite solid solution is in Al 2 O 3 The surface is highly dispersed;
is recorded as:
Ce 1-x-y La x Pt y O 2-δ ；
wherein x is more than or equal to 0.3 and less than or equal to 0.4; y is more than or equal to 0.03 and less than or equal to 0.10; delta is more than or equal to 0.15 and less than or equal to 0.3; the three parameters x, y, δ are calculated as follows:
x＝mol(La)/[mol(Ce)+mol(La)+mol(Pt)]
y＝mol(Pt)/[mol(Ce)+mol(La)+mol(Pt)]
δ＝2*(1-mol(Ce 4+ ))/[mol(Ce)+mol(La)+mol(Pt)]
wherein mol (Ce), mol (La), mol (Pt) and mol (Ce) 4+ ) Respectively Ce, la, pt and Ce 4+ The molar amount of (a); δ is the oxygen hole concentration.
The self-activated Pt-based catalyst is gradually generated into H in the process of hydrogen production reaction by reforming bioethanol 2 Reduction, pt species from CeO 2 Precipitating in crystal lattice, reducing into metal particles to form Pt/Ce 1-x La x O 2-δ /Al 2 O 3 A catalyst; on the formed Pt/Ce 1-x La x O 2-δ /Al 2 O 3 In the catalyst, pt is highly dispersed in Ce 1-x La x O 2-δ Surface, ce 1-x La x O 2-δ In Al 2 O 3 Spreading the surface;
in the specific implementation, in the self-activating Pt-based catalyst, 14mol% or more of Ce 1-x-y La x Pt y O 2-δ /Al 2 O 3 The content of (A) is less than or equal to 18mol percent; wherein, ce 1-x-y La x Pt y O 2-δ /Al 2 O 3 The content of (A) = [ mol (Ce) + mol (La) + mol (Pt) ]]/mol(Al 2 O 3 )。
The embodiment of the invention also provides a preparation method of the self-activated Pt-based catalyst for hydrogen production by bioethanol reforming, and as shown in FIG. 2, the preparation method provided by the embodiment of the invention has a schematic flow chart, and the method comprises the following steps:
step 1, preparing a mixed solution of cerium salt, lanthanum salt and platinum salt according to a set molar ratio, wherein the concentration is 1mol/L; wherein, ce: la: pt = 0.6;
step 2, adding 20gAl 2 O 3 Adding the microspheres into 12mL of mixed solution while stirring, wherein the amount of the added mixed solution is slightly higher than that of Al 2 O 3 The water absorption capacity of the microspheres;
among them, 20gAl 2 O 3 The water absorption of the microspheres is about 10mL, and the amount of the added mixed solution is slightly higher than that of Al 2 O 3 Compared with an initial impregnation method and a traditional impregnation method, the loading method has the advantages that the prepared sample metal proportion is more accurate, and the uniformity is higher;
and 4, roasting the catalyst for 5 hours at 600 ℃ in a muffle furnace to obtain the self-activating Pt-based catalyst.
It is noted that those skilled in the art will recognize that embodiments of the present invention are not described in detail herein.
The catalyst prepared by the method is low in price, and good in methane dry-method and wet-method reforming performances, although the activity of hydrogen production by low-temperature reforming is slightly lower than that of the rhodium-based catalyst, the catalyst has the advantages of high activity and high selectivity at higher temperature, can effectively improve the efficiency of hydrogen production by bioethanol reforming, and is more suitable for industrial application.
The above description is only for the preferred embodiment of the present invention, but the scope of the present invention is not limited thereto, and any changes or substitutions that can be easily conceived by those skilled in the art within the technical scope of the present invention are included in the scope of the present invention. Therefore, the protection scope of the present invention shall be subject to the protection scope of the claims. The information disclosed in this background section is only for enhancement of understanding of the general background of the invention and should not be taken as an acknowledgement or any form of suggestion that this information forms the prior art already known to a person skilled in the art.
Claims (4)
1. One kind is usedThe self-activation Pt-based catalyst for hydrogen production by reforming bioethanol is characterized by comprising the following components in parts by weight: al (aluminum) 2 O 3 A matrix of microspheres of said Al 2 O 3 The microsphere matrix is loaded with a composite solid solution;
the composite solid solution contains three metal elements of Ce, la and Pt, presents a cerium oxide fluorite cubic structure and is recorded as:
Ce 1-x-y La x Pt y O 2-δ ；
wherein x is more than or equal to 0.3 and less than or equal to 0.4; y is more than or equal to 0.03 and less than or equal to 0.10; delta is more than or equal to 0.15 and less than or equal to 0.3; the three parameters x, y, δ are calculated as follows:
x＝mol(La)/[mol(Ce)+mol(La)+mol(Pt)]
y＝mol(Pt)/[mol(Ce)+mol(La)+mol(Pt)]
δ＝2*(1-mol(Ce 4+ ))/[mol(Ce)+mol(La)+mol(Pt)]
wherein mol (Ce), mol (La), mol (Pt) and mol (Ce) 4+ ) Respectively Ce, la, pt and Ce 4+ The molar amount of (c); δ is the oxygen hole concentration;
the self-activated Pt-based catalyst is gradually generated into H in the process of hydrogen production reaction by reforming bioethanol 2 Reduction, pt species from CeO 2 Precipitating in crystal lattice, reducing into metal particles to form Pt/Ce 1-x La x O 2-δ /Al 2 O 3 A catalyst; on the Pt/Ce formed 1-x La x O 2-δ /Al 2 O 3 In the catalyst, pt is highly dispersed in Ce 1-x La x O 2-δ Surface, ce 1-x La x O 2-δ In Al 2 O 3 The surface was spread.
2. The self-activating Pt-based catalyst for hydrogen production by bioethanol reforming according to claim 1, wherein,
in the self-activating Pt-based catalyst, the Ce is more than or equal to 14mol percent 1-x-y La x Pt y O 2-δ /Al 2 O 3 The content of (A) is less than or equal to 18mol percent;
wherein, ce 1-x-y La x Pt y O 2-δ /Al 2 O 3 In an amount of = [ mol (Ce) + mol (La) + mol (Pt) ]]/mol(Al 2 O 3 )。
3. A method for preparing a self-activating Pt-based catalyst for hydrogen production by bioethanol reforming, the method comprising:
step 1, preparing a mixed solution of cerium salt, lanthanum salt and platinum salt according to a set molar ratio, wherein the concentration is 1mol/L;
step 2, adding 20gAl 2 O 3 Adding the microspheres into 12mL of mixed solution while stirring, wherein the amount of the added mixed solution is slightly higher than that of Al 2 O 3 The water absorption capacity of the microspheres;
step 3, heating and stirring in air until the materials are not sticky, and then drying in an oven at 110 ℃ for 12 hours;
and 4, roasting the catalyst for 5 hours at 600 ℃ in a muffle furnace to obtain the self-activating Pt-based catalyst.
4. The preparation method of the self-activating Pt-based catalyst for hydrogen production by bioethanol reforming according to claim 3, wherein in step 1, the molar ratio of cerium, lanthanum and platinum is as follows:
Ce：La：Pt＝0.6:0.35:0.05。
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Citations (6)
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| TW201429546A (en) * | 2013-01-25 | 2014-08-01 | Univ Nat Chiao Tung | Ethanol reforming catalyst composition and preparation method of ethanol reforming catalyst |
| CN114160148A (en) * | 2021-12-08 | 2022-03-11 | 中国科学院生态环境研究中心 | Cu-based catalyst for hydrogen production by methanol reforming and preparation method and application thereof |
| CN115382542A (en) * | 2022-09-16 | 2022-11-25 | 北京石油化工学院 | Double-catalyst for hydrogen production by biological ethanol reforming and preparation method thereof |
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2022
- 2022-09-16 CN CN202211128909.6A patent/CN115318285A/en active Pending
Patent Citations (6)
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| CN1674328A (en) * | 2004-03-25 | 2005-09-28 | 中国科学院大连化学物理研究所 | CO carbon monoxide water-vapour conversion catalyst and producing process and application |
| WO2008153826A2 (en) * | 2007-05-31 | 2008-12-18 | Corning Incorporated | Catalyst for hydrogen production by autothermal reforming, method of making same and use thereof |
| CN102513105A (en) * | 2011-12-16 | 2012-06-27 | 中国科学院生态环境研究中心 | Hydrogen production catalyst |
| TW201429546A (en) * | 2013-01-25 | 2014-08-01 | Univ Nat Chiao Tung | Ethanol reforming catalyst composition and preparation method of ethanol reforming catalyst |
| CN114160148A (en) * | 2021-12-08 | 2022-03-11 | 中国科学院生态环境研究中心 | Cu-based catalyst for hydrogen production by methanol reforming and preparation method and application thereof |
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