CN104888765A - Cage porous platinum-palladium composite nanoparticle having excellent catalysis performance on methanol, and preparation method thereof - Google Patents
Cage porous platinum-palladium composite nanoparticle having excellent catalysis performance on methanol, and preparation method thereof Download PDFInfo
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Abstract
The invention relates to a cage porous platinum-palladium composite nanoparticle and a preparation method thereof. The cage porous platinum-palladium composite nanoparticle has the characteristics of uniform scale, high specific surface area and good catalytic activity, and the components of the nanoparticle can be effectively regulated in a large range (a Pt/Pd molar ratio of 3-19). The complete preparation method of the nanoparticle comprises the following steps: 1, sequentially sodium tetrachloroplatinate, potassium tetrachloropalladate, hydrochloric acid, polyoxyethylene-polyoxypropylene-polyoxyethylene (P123) and ascorbic acid into an aqueous solution to obtain a reaction precursor solution; and 2, carrying out ultrasonic treatment on the precursor solution at 35DEG C for 4h, centrifuging at a rotating speed of 7000-10000r/min, and separating to obtain a black precipitate which is the platinum-palladium composite nanoparticle. The cage porous platinum-palladium composite nanoparticle prepared in the invention has important application values and wide application prospect in fuel cells, industrial catalysis, automobile tail gas purification, water splitting and carbon monoxide catalytic oxidation.
Description
Technical field
The present invention relates to a kind of to methyl alcohol caged porous platinum palladium composite nanoparticle with excellent catalytic performance and preparation method thereof.
Background technology
Noble metal platinum (Pt), as important catalyst, is widely used in fields such as Industrial Catalysis, fuel cell, purifying vehicle exhaust, water-splitting, catalyzing carbon monoxide oxidations.Especially at catalytic field, platinum is the active component being difficult to be substituted.As in low-temperature fuel cell, the most effective catalyst of electrochemical reaction rates accelerated at present by platinum or its alloy.In addition, platinum is also the platinum group metal uniquely bearing sour environment in low-temperature fuel cell.But platinum is rare noble metal, and price is very expensive, causes low-temperature fuel cell high cost, limits low-temperature fuel cell and extensively, on a large scale applies.The more important thing is, its catalytic activity is very easily poisoned by carbon monoxide (CO) and causes its catalytic performance sharply to reduce.There are some researches show, acted synergistically by intermetallic, constructing platinum palladium composite nanoparticle is a kind of effective minimizing platinum consumption in the catalyst, reduces catalyst cost, improves the method for its catalytic activity and stability.Therefore, the preparation of platinum palladium composite nanoparticle enjoys the concern of people recently.At present, people have been developed chemical reduction method, seed mediated growth method, electrochemical process, have been gone alloyage, the multiple platinum palladium composite nanoparticle synthetic route such as displacement method, reverse micelle method, polyalcohol co-reducing process, successfully prepare the platinum palladium composite nanoparticle at interior different morphologies such as dendritic, flower-shaped, wire in the liquid phase.But as far as we know, adopting existing synthetic route, people are difficult to prepare the caged platinum palladium composite nanoparticle with loose structure.We know, metal nano particle catalysis reaction generally occurs in the surface of particle.Obviously, compared with solid platinum palladium composite nanoparticle, the caged platinum palladium composite nanoparticle of loose structure has higher specific area, and therefore it will have more excellent catalytic performance.As previously mentioned, the synthesis of caged porous platinum palladium composite nanoparticle is still faced with numerous challenge, and its preparation were established rarely has report.
Summary of the invention
The technical problem to be solved in the present invention prepares caged porous platinum palladium composite nanoparticle One-step Synthesis method easily and effectively for proposing one, controls a series of caged porous platinum palladium composite nanoparticle methyl alcohol to excellent catalytic performance of synthesis.
In the present invention, caged porous platinum palladium composite nanoparticle exemplary synthesis under ultrasound condition, controls uniform temperature reduce Tetrachloroplatinate sodium (Na using polyoxyethylene-poly-oxypropylene polyoxyethylene (P123) as surfactant, with ascorbic acid (AA)
2ptCl
4) and potassium chloropalladite (K
2pdCl
4), adopt one kettle way to realize the preparation of caged porous platinum palladium composite nanoparticle.
The preparation method of involved caged porous platinum palladium composite nanoparticle, comprises following concrete steps:
(1) in 18.25 megaohm deionized waters, Tetrachloroplatinate sodium (Na is added successively
2ptCl
4) and potassium chloropalladite (K
2pdCl
4), hydrochloric acid (HCl), polyoxyethylene-poly-oxypropylene polyoxyethylene (P123) aqueous solution, obtain mixed solution after concussion evenly;
(2) to add in the mixed solution configured (1) ascorbic acid (AA) afterwards concuss shake up, obtain reaction precursor liquid solution, wherein, Tetrachloroplatinate sodium (Na
2ptCl
4), potassium chloropalladite (K
2pdCl
4), the ultimate density of hydrochloric acid (HCl) and polyoxyethylene-poly-oxypropylene polyoxyethylene (P123) is respectively 0.0075-0.0095 mol/L, 0.0005-0.0025 mol/L, 0.06 mol/L, 0.0004 mol/L, 0.05 mol/L;
(3), at reaction precursor liquid solution (2) being placed in 35 DEG C after ultrasonic 4 hours, obtained solution color is the caged porous platinum palladium composite nanoparticle colloidal solution of black;
(4) the caged porous platinum palladium composite nanoparticle colloidal solution supercentrifuge centrifugation obtained, after centrifugal 10-20 minute at rotating speed 7000-10000 rev/min, removes colourless solution in centrifuge tube, obtains black precipitate product;
(5) with the black precipitate product that solvent supersonic cleaning obtains, obtained caged porous platinum palladium composite nanoparticle.
Beneficial effect of the present invention
(1) product that prepared by the method is platinum palladium composite nanoparticle, and its shape is caged loose structure, and particle scale is even, and specific area is high;
(2) not only productive rate is high for the caged porous platinum palladium composite nanoparticle prepared of the method, and its composition is by Control release parameter (Pt/Pd molar ratio: 3 ~ 19) Effective Regulation on a large scale;
(3) by utilizing electrochemical workstation to test methanol oxidation performance to prepared caged porous platinum palladium composite nanoparticle, test result shows, compared to commercialization platinum catalyst (load capacity 20%), platinum palladium composite nanoparticle prepared by the present invention has more excellent catalytic performance in methanol oxidation, therefore will have very large application prospect at fuel cell and Industrial Catalysis field;
(4) preparation of the present invention only needs the conventional equipment that laboratory is commonly used, and do not need special equipment, technical process is simple to operation;
(5) the present invention is raw materials used abundant, preparation temperature is low, and caged porous platinum palladium composite nanoparticle productive rate is high, is particularly suitable in enormous quantities, the low cost preparation of caged porous platinum palladium composite nanoparticle, not only be applicable to industrialized large-scale production, be also easy to business-like application.
Accompanying drawing explanation
Fig. 1 be to after reaction system fore-and-aft observing with one of multiple optical photographs of camera shooting, Fig. 1 a is the precursor solution before reaction, and color be light yellow, and Fig. 1 b reacts the platinum palladium composite nanoparticle colloidal solution after terminating, and color is black;
Fig. 2 is one of multiple transmission electron microscope photos (TEM image) taken after the nano particle NEC JEOL-1400 transmission electron microscope observation to preparation, wherein, Fig. 2 a is low power TEM image, Fig. 2 b is high power TEM image, can be seen by Fig. 2 a and Fig. 2 b, product is the nano particle of caged porous, particle size uniformity, its yardstick is 75 nm, and productive rate is high;
Fig. 3 is the X-ray energy spectrum figure (EDX) the caged porous platinum palladium composite nanoparticle Inca. Oxford type X-ray energy spectrometer prepared by embodiment 1 being tested to rear acquisition, and wherein, ordinate is intensity, and abscissa is energy.Known by EDX collection of illustrative plates, obtain product component except platinum (Pd), palladium (Pd) two kinds of elements (copper is from Electronic Speculum copper mesh), there is no other any impurity.Be 81.6:18.4 to the atomic ratio of platinum palladium in atlas analysis known caged porous platinum palladium composite nanoparticle further, close with the concentration ratio (80:20) of platinum, palladium presoma, platinum, palladium presoma complete reaction in this preparation method of deducibility thus;
Fig. 4 is one of multiple stereoscan photographs (FESEM image) taken the photograph after observing with FEI Sirion 200 type field emission scanning electron microscope, and as seen from the figure, product morphology is caged loose structure, and particle scale is even;
Fig. 5 is one of multiple transmission electron microscopes (TEM) photo taken after the caged porous platinum palladium composite nanoparticle JEOL-1400 transmission electron microscope observing of different platinum palladium atomic ratio, wherein, the caged porous platinum palladium composite nanoparticle of Fig. 5 a to be platinum palladium atomic ratio be 75:25, the caged porous platinum palladium composite nanoparticle of Fig. 5 b to be platinum palladium atomic ratio be 95:5, the caged porous platinum palladium composite nanoparticle of Fig. 5 c to be platinum palladium atomic ratio be 85:15, the caged porous platinum palladium composite nanoparticle of Fig. 5 d to be platinum palladium atomic ratio be 90:10.As can be seen from Fig. 3, Fig. 5 a, Fig. 5 b, Fig. 5 c and Fig. 5 d, the method can prepare the caged porous platinum palladium composite nanoparticle of different platinum palladium atomic ratio;
Obtained caged porous platinum palladium composite nanoparticle evenly drips to be coated onto after on slide by Fig. 6, with Philips X'Pert type x-ray diffractometer, the X-ray diffracting spectrum (XRD) obtained is tested to it, wherein, ordinate is relative intensity, and abscissa is the angle of diffraction.Through comparing with the platinum card of the JCPDS of standard, the known prepared XRD diffraction maximum peak position of sample and the face-centered cubic diffraction maximum peak position of platinum fit like a glove, because platinum and palladium have the diffraction maximum that therefore close lattice parameter does not observe independent palladium in XRD collection of illustrative plates;
Fig. 7 a is " caged porous " Pt
80pd
20to the cyclic voltammetry curve (CV) of methanol oxidation, (perchloric acid and methanol concentration are 1 M, and the total load amount (Pd+Pt) of metal on carbon is 20 % in acid condition for composite nanoparticle and business Pt/C catalyst (platinum load capacity 20%); The consumption of the PtPd NPs/C on test electrode is 15 ug); Fig. 7 b is that " caged porous platinum palladium composite nanoparticle is to methanol oxidation catalytic activity for heterogeneity.Known by Fig. 7 a, b, the caged porous platinum palladium composite nanoparticle prepared by the present invention has more excellent catalytic performance than commercialization platinum C catalyst (load capacity 20%) in methanol oxidation.
Specific embodiments
Tetrachloroplatinate sodium (the Na that the present invention uses
2ptCl
4), potassium chloropalladite (K
2pdCl
4), ascorbic acid (AA), hydrochloric acid (HCl), polyoxyethylene-poly-oxypropylene polyoxyethylene (P123) directly buy from the market, without the need to doing any purification process before using.Specific embodiments prepared by caged porous platinum palladium composite nanoparticle comprises:
(1) 18.25 megaohm deionized water configuration Tetrachloroplatinate sodium (Na are utilized
2ptCl
4), potassium chloropalladite (K
2pdCl
4), ascorbic acid (AA), hydrochloric acid (HCl), polyoxyethylene-poly-oxypropylene polyoxyethylene (P123) aqueous solution, wherein Tetrachloroplatinate sodium (Na
2ptCl
4), potassium chloropalladite (K
2pdCl
4), ascorbic acid (AA), hydrochloric acid (HCl), polyoxyethylene-poly-oxypropylene polyoxyethylene (P123) concentration is respectively 0.125 mol/L, 0.125 mol/L, 1 mol/L, 5 mol/L, 0.005 mol/L;
(2) configuration of reaction precursor liquid solution: first add Tetrachloroplatinate sodium (Na successively in 18 megaohm deionized waters
2ptCl
4), potassium chloropalladite (K
2pdCl
4), hydrochloric acid (HCl), polyoxyethylene-poly-oxypropylene polyoxyethylene (P123) aqueous solution obtain mixed solution, then add rapidly ascorbic acid (AA) and shake up, obtain reaction precursor liquid solution;
(3) under ultrasound condition, one kettle way is adopted by reaction precursor liquid solution to prepare caged porous platinum palladium composite nanoparticle.
Below in conjunction with specific embodiment, content of the present invention is described in further details, but the invention is not restricted to the following specific examples enumerated.
embodiment 1
the preparation (platinum atomic percent palladium 80:20) of caged porous platinum palladium composite nanoparticle
First successively in 18.25 megaohm deionized waters, Tetrachloroplatinate sodium (Na is added
2ptCl
4), potassium chloropalladite (K
2pdCl
4), hydrochloric acid (HCl), polyoxyethylene-poly-oxypropylene polyoxyethylene (P123) aqueous solution, obtain mixed solution after fully shaking up; Then add rapidly ascorbic acid (AA) and obtain reaction precursor liquid solution, Tetrachloroplatinate sodium (Na in precursor solution
2ptCl
4), potassium chloropalladite (K
2pdCl
4), hydrochloric acid (HCl), polyoxyethylene-poly-oxypropylene polyoxyethylene (P123), ascorbic acid (AA) concentration is followed successively by 0.008 mol/L, 0.002 mol/L, 0.06 mol/L, 0.00007 mol/L, 0.05 mol/L; Precursor solution is transferred in KQ2200DA type numerical control Ultrasound Instrument, within ultrasonic 4 hours at 35 DEG C, caged porous platinum palladium nano-sized colloidal solution can be obtained; , remove centrifuge tube colourless solution at the middle and upper levels, obtain black precipitate product after centrifugal 10 minutes with supercentrifuge under rotating speed 7000 revs/min of conditions; By deionized water to black precipitate product ultrasonic cleaning 3-5 time, the obtained platinum atomic percent palladium 80:20 caged porous platinum palladium composite nanoparticle being similar to Fig. 3.
embodiment 2
the preparation (platinum atomic percent palladium 75:25) of caged porous platinum palladium composite nanoparticle
First successively in 18.25 megaohm deionized waters, Tetrachloroplatinate sodium (Na is added
2ptCl
4), potassium chloropalladite (K
2pdCl
4), hydrochloric acid (HCl), polyoxyethylene-poly-oxypropylene polyoxyethylene (P123) aqueous solution, obtain mixed solution after fully shaking up; Then add rapidly ascorbic acid (AA) and obtain reaction precursor liquid solution, Tetrachloroplatinate sodium (Na in precursor solution
2ptCl
4), potassium chloropalladite (K
2pdCl
4), hydrochloric acid (HCl), three embedding polymer P luronic P123, ascorbic acid (AA) concentration is followed successively by 0.0075 mol/L, 0.0025 mol/L, 0.06 mol/L, 0.00007 mol/L, 0.05 mol/L; Precursor solution is transferred in KQ2200DA type numerical control Ultrasound Instrument, within ultrasonic 4 hours at 35 DEG C, caged porous platinum palladium nano-sized colloidal solution can be obtained; , remove centrifuge tube colourless solution at the middle and upper levels, obtain black precipitate product after centrifugal 10 minutes with supercentrifuge under rotating speed 7000 revs/min of conditions; By deionized water to black precipitate product ultrasonic cleaning 3-5 time, the obtained caged porous platinum palladium composite nanoparticle being similar to the platinum atomic percent palladium 75:25 of Fig. 5 a.
embodiment 3
the preparation (platinum atomic percent palladium 95:5) of caged porous platinum palladium composite nanoparticle
First successively in 18.25 megaohm deionized waters, Tetrachloroplatinate sodium (Na is added
2ptCl
4), potassium chloropalladite (K
2pdCl
4), hydrochloric acid (HCl), polyoxyethylene-poly-oxypropylene polyoxyethylene (P123) aqueous solution, obtain mixed solution after fully shaking up; Then add rapidly ascorbic acid (AA) and obtain reaction precursor liquid solution, Tetrachloroplatinate sodium (Na in precursor solution
2ptCl
4), potassium chloropalladite (K
2pdCl
4), hydrochloric acid (HCl), polyoxyethylene-poly-oxypropylene polyoxyethylene (P123), ascorbic acid (AA) concentration is followed successively by 0.0095 mol/L, 0.0005 mol/L, 0.06 mol/L, 0.00007 mol/L, 0.05 mol/L; Precursor solution is transferred in KQ2200DA type numerical control Ultrasound Instrument, within ultrasonic 4 hours at 35 DEG C, caged porous platinum palladium nano-sized colloidal solution can be obtained; , remove centrifuge tube colourless solution at the middle and upper levels, obtain black precipitate product after centrifugal 15 minutes with supercentrifuge under rotating speed 8000 revs/min of conditions; ; By deionized water to black precipitate product ultrasonic cleaning 3-5 time, the obtained caged porous platinum palladium composite nanoparticle being similar to the platinum atomic percent palladium 95:5 of Fig. 5 b.
embodiment 4
the preparation (platinum atomic percent palladium 85:15) of caged porous platinum palladium composite nanoparticle
First successively in 18.25 megaohm deionized waters, Tetrachloroplatinate sodium (Na is added
2ptCl
4), potassium chloropalladite (K
2pdCl
4), hydrochloric acid (HCl), polyoxyethylene-poly-oxypropylene polyoxyethylene (P123) aqueous solution, obtain mixed solution after fully shaking up; Then add rapidly ascorbic acid (AA) and obtain reaction precursor liquid solution, Tetrachloroplatinate sodium (Na in precursor solution
2ptCl
4), potassium chloropalladite (K
2pdCl
4), hydrochloric acid (HCl), polyoxyethylene-poly-oxypropylene polyoxyethylene (P123), ascorbic acid (AA) concentration is followed successively by 0.0085 mol/L, 0.0015 mol/L, 0.06 mol/L, 0.00007 mol/L, 0.05 mol/L; Precursor solution is transferred in KQ2200DA type numerical control ultrasonic cleaner, within ultrasonic 4 hours at 35 DEG C, caged platinum palladium nano-sized colloidal solution can be obtained; , remove centrifuge tube colourless solution at the middle and upper levels, obtain black precipitate product after centrifugal 10 minutes with supercentrifuge under rotating speed 8000 revs/min of conditions; By deionized water to black precipitate product ultrasonic cleaning 3-5 time, obtain and be similar to the platinum atomic percent palladium shown in Fig. 5 c
85:15caged porous platinum palladium composite nanoparticle.
execute example 5
the preparation (platinum atomic percent palladium 90:10) of caged porous platinum palladium composite nanoparticle
First successively in 18.25 megaohm deionized waters, Tetrachloroplatinate sodium (Na is added
2ptCl
4), potassium chloropalladite (K
2pdCl
4), hydrochloric acid (HCl), polyoxyethylene-poly-oxypropylene polyoxyethylene (P123) aqueous solution, obtain mixed solution after fully shaking up; Then add rapidly ascorbic acid (AA) and obtain reaction precursor liquid solution, Tetrachloroplatinate sodium (Na in precursor solution
2ptCl
4), potassium chloropalladite (K
2pdCl
4), hydrochloric acid (HCl), polyoxyethylene-poly-oxypropylene polyoxyethylene (P123), ascorbic acid (AA) concentration is followed successively by 0.009 mol/L, 0.001 mol/L, 0.06 mol/L, 0.00007 mol/L, 0.05 mol/L; Precursor solution is transferred in KQ2200DA type numerical control ultrasonic cleaner, within ultrasonic 4 hours at 35 DEG C, caged porous platinum palladium nano-sized colloidal solution can be obtained; , remove centrifuge tube colourless solution at the middle and upper levels, obtain black precipitate product after centrifugal 15 minutes with supercentrifuge under rotating speed 10000 revs/min of conditions; By deionized water to black precipitate product ultrasonic cleaning 3-5 time, the obtained caged porous platinum palladium composite nanoparticle being similar to the platinum atomic percent palladium 90:10 shown in Fig. 5 d.
Claims (7)
1. methyl alcohol is had to a caged porous platinum palladium composite nanoparticle for excellent catalytic performance, it is characterized in that:
(1) said caged porous platinum palladium composite nanoparticle refers to the nano particle with caged loose structure, and its particle scale is even, productive rate high (99%);
(2) preparation temperature of caged porous platinum palladium composite nanoparticle is lower, and preparation method is simple and easy to operate;
(3) in caged porous platinum palladium composite nanoparticle its composition can on a large scale (Pt/Pd molar ratio: 3 ~ 19) Effective Regulation;
(4) compared to existing commercialization platinum/C catalyst (load capacity 20%), caged porous platinum palladium composite nanoparticle prepared by the present invention has more excellent catalytic performance in methanol oxidation, will have significant application value and broad prospect of application in fuel cell, Industrial Catalysis, purifying vehicle exhaust, water-splitting, catalyzing carbon monoxide oxidation etc.
2. complete preparation method methyl alcohol to the caged porous platinum palladium composite nanoparticle of excellent catalytic performance according to claim 1, is characterized in that comprising the following steps:
(1) in 18.25 megaohm deionized waters, Tetrachloroplatinate sodium (Na is added successively
2ptCl
4), potassium chloropalladite (K
2pdCl
4), hydrochloric acid (HCl), polyoxyethylene-poly-oxypropylene polyoxyethylene (P123) aqueous solution, obtain mixed solution after fully shaking up;
(2) be rapidly in mixed solution and add reducing agent ascorbic acid (AA) and obtain reaction precursor liquid solution, Tetrachloroplatinate sodium (Na in precursor solution
2ptCl
4), potassium chloropalladite (K
2pdCl
4), hydrochloric acid (HCl), polyoxyethylene-poly-oxypropylene polyoxyethylene (P123), ascorbic acid (AA) concentration is followed successively by 0.0075-0.0095 mol/L, 0.0025-0.0005 mol/L, 0.06 mol/L, 0.00007 mol/L, 0.05 mol/L;
(3) transferred to by precursor solution in KQ2200DA type numerical control Ultrasound Instrument, ultrasonic power is 80%, and temperature control 35 degrees centigrade ultrasonic 4 hours obtained solution colors are the caged porous platinum palladium composite nanoparticle colloidal solution of black;
(4), remove centrifuge tube colourless solution at the middle and upper levels, obtain black precipitate product after centrifugal 10-15 minute with supercentrifuge under rotating speed 7000-10000 rev/min condition;
(5) black precipitated product is cleaned with solvent supersonic, obtained caged porous platinum palladium composite nanoparticle.
3. preparation method according to claim 2, is characterized in that utilizing one kettle way to synthesize caged porous platinum palladium composite nanoparticle methyl alcohol to excellent catalytic performance by comparatively gentle condition in aqueous.
4. preparation method according to claim 2, the temperature of required preparation caged porous platinum palladium composite nanoparticle is 35 DEG C.
5. preparation method according to claim 2, is characterized in that reaction system ultimate density is respectively Tetrachloroplatinate sodium (Na
2ptCl
4), potassium chloropalladite (K
2pdCl
4), hydrochloric acid (HCl), polyoxyethylene-poly-oxypropylene polyoxyethylene (P123), ascorbic acid (AA) concentration is followed successively by 0.0075-0.0095 mol/L, 0.0025-0.0005 mol/L, 0.06 mol/L, 0.00007 mol/L, 0.05 mol/L.
6. preparation method according to claim 2, the reducing agent that it is characterized in that in precursors is the ascorbic acid (AA) to human body close friend, i.e. vitamin C.
7. preparation method according to claim 2, is characterized in that the solvent of washing and precipitating product is 18.25 megaohm deionized water or distilled water.
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| CN109364964A (en) * | 2018-11-27 | 2019-02-22 | 浙江工业大学 | A kind of platinum palladium nickel-phosphorus alloy porous nano microballoon and preparation method thereof of catalytic oxidation-reduction reaction |
| CN109659573A (en) * | 2018-11-27 | 2019-04-19 | 浙江工业大学 | A kind of mesoporous platinum porpezite elctro-catalyst and preparation method thereof |
| CN111293323A (en) * | 2020-02-25 | 2020-06-16 | 安徽师范大学 | Porous platinum-palladium nano cubic material, preparation method thereof and application thereof in catalyzing methanol oxidation |
| CN112973676A (en) * | 2019-12-16 | 2021-06-18 | 中国科学院大连化学物理研究所 | Preparation method of supported porous nano platinum catalyst |
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| CN109364964A (en) * | 2018-11-27 | 2019-02-22 | 浙江工业大学 | A kind of platinum palladium nickel-phosphorus alloy porous nano microballoon and preparation method thereof of catalytic oxidation-reduction reaction |
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| CN111293323A (en) * | 2020-02-25 | 2020-06-16 | 安徽师范大学 | Porous platinum-palladium nano cubic material, preparation method thereof and application thereof in catalyzing methanol oxidation |
| CN111293323B (en) * | 2020-02-25 | 2023-03-07 | 安徽师范大学 | Porous platinum-palladium nano cubic material, preparation method thereof and application thereof in catalyzing methanol oxidation |
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