CN101711979A - Method for preparing platinum-zirconium/carbon dioxide composite electro-catalyst - Google Patents
Method for preparing platinum-zirconium/carbon dioxide composite electro-catalyst Download PDFInfo
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- CN101711979A CN101711979A CN200910153974A CN200910153974A CN101711979A CN 101711979 A CN101711979 A CN 101711979A CN 200910153974 A CN200910153974 A CN 200910153974A CN 200910153974 A CN200910153974 A CN 200910153974A CN 101711979 A CN101711979 A CN 101711979A
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Abstract
The invention discloses a method for preparing a platinum-zirconium/carbon dioxide composite electro-catalyst. The method comprises: dissolving chloroplatinic acid in glycol to prepare 0.002 to 0.005 mol/L of chloroplatinic acid and glycol solution; adding aqueous solution of zirconium nitrate to the chloroplatinic acid and glycol solution; adding stabilizing agent; using sodium hydroxide to regulate pH to be between 12 and 14; adding nanometer carbon as a carrier to the obtained solution; ultrasonically mixing well; putting the mixture in a microwave oven with a reflux device to heat the mixture for 5 to 20 minutes; cooling and then filtering the obtained product; using acetone and deionized water to fully wash and dry the obtained product; and obtaining the platinum-zirconium/carbon dioxide composite electro-catalyst, wherein the mass fraction of platinum in the catalyst is 10 to 20 percent, and the molar ratio of platinum to zirconium is between 1:1 and 3:1. The platinum-zirconium/carbon dioxide composite electro-catalyst prepared by the method has higher electro-catalytic activity to the electro-oxidation of methanol than platinum/carbon catalysts, has improved performance of resisting CO poisoning, and has extensive application as the catalyst for direct alcohol fuel cells.
Description
Technical field
That the present invention relates to is a kind of preparation method of platinum-zirconium/carbon dioxide composite electro-catalyst, belongs to catalyst preparation technical field and electrochemical energy technical field.
Background technology
The noble metal platinum nano particle of carbon load high dispersive has good catalytic action, has obtained extensive studies and application in fuel cell.But because noble metal platinum costs an arm and a leg, reserves are low, and simple platinum is easy to be subjected to intermediate product in catalyzing alcohols fuel cell process, as the poisoning effect of CO, so synthesizing efficient rate, high catalytic activity and to have the fuel-cell catalyst that anti-CO poisons be the previous challenging research topic of order.Synthesize this anti-CO fouled catalyst that has, usually be divided into two aspects: the one, in platinum/C catalyst, add another metal, as Ru, Sn, Ni, Re, Co, Cr etc.; The 2nd, in platinum/C catalyst, add some transition metal oxides, as RuO
2, SnO
2, WO
3And TiO
2Deng, can improve the electrocatalytic oxidation property of methyl alcohol or oxidation of ethanol.Recent study is found in the catalyst that transition metal oxide mixes, wherein ceria and zirconium dioxide are because its good oxygen storage capacity, the intermediate product that produces in can the oxidized fuel cell catalytic process, thereby raising electrocatalysis characteristic, therefore be commonly used to the eelctro-catalyst that synthetic this class is mixed, but the synthetic method of bibliographical information all be in two steps or multistep finish.
The microwave radiation has been applied to the synthetic of chemical reaction and multiple nano material widely as a kind of heating technique fast, simply and efficiently.But up to the present, also Shang Weijian has the document that utilizes one step of microwave method to synthesize platinum-zirconium/carbon dioxide composite electro-catalyst openly to report.
Summary of the invention
The preparation method who the purpose of this invention is to provide a kind of platinum-zirconium/carbon dioxide composite electro-catalyst.The preparation method of platinum-zirconium/carbon dioxide composite electro-catalyst of the present invention, its step is as follows:
1) chloroplatinic acid is dissolved in the ethylene glycol, is mixed with the chloroplatinic acid ethylene glycol solution of 0.002～0.005mol/L;
2) add the zirconium nitrate aqueous solution in the chloroplatinic acid ethylene glycol solution, making the platinum in the solution and the mol ratio of zirconium is 1: 1～3: 1, adds stabilizing agent then, and regulating pH with NaOH is 12～14;
3) in step 2) add nano-sized carbon as carrier in the solution of gained, after ultrasonic the mixing, put into the micro-wave oven that has reflux and heat 5～20min, after the cooling after filtration, fully wash with acetone and deionized water, oven dry obtains platinum-zirconium/carbon dioxide composite electro-catalyst, the mass fraction of platinum in catalyst is 10～20%, and the mol ratio of platinum and zirconium was at 1: 1～3: 1.
The said stabilizing agent of the present invention is polyvinylpyrrolidone or polyethylene glycol.Said nano-sized carbon is XC-72 carbon or CNT.
In order to strengthen the load effect of metal nanoparticle, with CNT 60 ℃ of reflow treatment 16h in red fuming nitric acid (RFNA) before use in carbon nano tube surface.
Method of the present invention compared with prior art has following outstanding advantage:
The present invention utilizes microwave heating method one step preparation platinum-zirconium/carbon dioxide composite electro-catalyst, compares with existing method to have quick, simple, efficient and energy-saving advantages.
And nano platinum particle has tiny and uniform particle diameter in the prepared catalyst of the present invention, and average grain diameter is 3.0～3.5nm.
The platinum-zirconium/carbon dioxide composite electro-catalyst of the present invention preparation has higher electro catalytic activity than platinum/C catalyst to the electroxidation of methyl alcohol, and has the anti-CO poisoning performance of improvement, has widely as the catalyst of direct alcohol fuel battery and uses.
The specific embodiment
Embodiment 1:
Chloroplatinic acid is dissolved in the ethylene glycol, is mixed with the solution that concentration is 0.002mol/L.Get this solution of 50mL, adding 10mL concentration is the 10mmol/L zirconium nitrate aqueous solution, and the mol ratio of platinum and zirconium is 1: 1 in the solution, adds the polyethylene glycol aqueous solution of 5mL 1% again.With sodium hydroxide solution regulator solution pH value is 12.The XC-72 carbon that in this synthetic solvent, adds 63mg again, and ultrasonic mixing.Final mixture is transferred in the round-bottomed flask of 250mL, and is placed in the micro-wave oven, adds reflux, microwave 15min.After the cooling, solid product fully washs after filtration and with acetone and deionized water, 80 ℃ of oven dry, obtains platinum-zirconium dioxide/XC-72 carbon composite electrocatalyst.(mass fraction of platinum is 20% in the catalyst, mol ratio platinum: zirconium=1: 1).Nano platinum particle has uniform particle diameter in the transmission electron microscope observing catalyst, and average grain diameter is 3.1nm.
As a comparison, in synthetic solvent, do not add zirconium nitrate solution, with the synthetic platinum/C catalyst (mass fraction of platinum is 20%) of similar method.The nano platinum particle particle diameter is 3.0nm in transmission electron microscope observing platinum/carbon eelctro-catalyst.
To methanol oxidation electrocatalysis characteristic test relatively: the Nafion solution and the deionized water of a spot of catalyst and an amount of 5% are mixed under the ultrasonic wave effect, should be coated on the glassy carbon electrode by uniform mixture, dry the back down as measuring working electrode at 80 ℃.Reference electrode is saturated calomel electrode (SCE) during measurement, and electrolyte is 2mol/L methyl alcohol+1mol/L sulfuric acid, and platinized platinum is to electrode.With cyclic voltammetry (sweep speed 20mV/s, 30 ℃) and constant potential chronoamperometry (polarization potential 0.4V vs.SCE, time 1h) experimental evaluation catalyst electro catalytic activity to methanol electrooxidation.Test result shows under the same terms: (platinum: zirconium=1: 1) take-off potential and the peak current to methanol oxidation is respectively 0.30V and 12.4mA to platinum-zirconium dioxide/XC-72 carbon composite electrocatalyst, and platinum/C catalyst is respectively 0.40V and 8.5mA to the take-off potential and the peak current of methanol oxidation, and platinum-zirconium dioxide/XC-72 carbon composite electrocatalyst (platinum: zirconium=1: 1) than platinum/C catalyst methanol oxidation is had higher electro catalytic activity of the present invention's preparation is described; After the constant potential polarization 1h, platinum-zirconium dioxide/XC-72 carbon composite electrocatalyst (platinum: zirconium=1: 1) to the electric current of methanol oxidation be 1.06mA (for initial value 78%), and platinum/C catalyst to the electric current of methanol oxidation only be 0.80mA (for initial value 65%), platinum-zirconium dioxide/XC-72 carbon composite electrocatalyst (platinum: zirconium=1: 1) than platinum/C catalyst methanol oxidation is had the stable and anti-CO poisoning performance of better electro-catalysis of the present invention's preparation be described.
Embodiment 2:
Chloroplatinic acid is dissolved in the ethylene glycol, is mixed with the solution that concentration is 0.004mol/L.Get this solution of 50mL, adding 10mL concentration is the 10mmol/L zirconium nitrate aqueous solution, and the mol ratio of platinum and zirconium is 2: 1 in the solution, adds the polyethylene glycol aqueous solution of 10mL 1% again.With sodium hydroxide solution regulator solution pH value is 12.The XC-72 carbon that in this synthetic solvent, adds 143mg again, and ultrasonic mixing.Final mixture is transferred in the round-bottomed flask of 250mL, and is placed in the micro-wave oven, adds reflux, microwave 15min.After the cooling, solid product fully washs after filtration and with acetone and deionized water, 80 ℃ of oven dry, obtains platinum-zirconium dioxide/XC-72 carbon composite electrocatalyst.(mass fraction of platinum is 20% in the catalyst, mol ratio platinum: zirconium=2: 1).Nano platinum particle has uniform particle diameter in the transmission electron microscope observing catalyst, and average grain diameter is 3.0nm.
As a comparison, in synthetic solvent, do not add zirconium nitrate solution, with the synthetic platinum/C catalyst (mass fraction of platinum is 20%) of similar method.The nano platinum particle particle diameter is 3.0nm in transmission electron microscope observing platinum/carbon eelctro-catalyst.
According to 1 pair of methanol oxidation electrocatalysis characteristic test of embodiment relatively.Test result shows under the same terms: (platinum: zirconium=2: 1) take-off potential and the peak current to methanol oxidation is respectively 0.32V and 14.3mA to platinum-zirconium dioxide/XC-72 carbon composite electrocatalyst, and platinum/C catalyst is respectively 0.40V and 9.0mA to the take-off potential and the peak current of methanol oxidation, and platinum-zirconium dioxide/XC-72 carbon composite electrocatalyst (platinum: zirconium=2: 1) than platinum/C catalyst methanol oxidation is had higher electro catalytic activity of the present invention's preparation is described; Again after the constant potential polarization 1h, platinum-zirconium dioxide/XC-72 carbon composite electrocatalyst (platinum: zirconium=2: 1) to the electric current of methanol oxidation be 1.27mA (for initial value 80%), and platinum/C catalyst to the electric current of methanol oxidation only be 0.83mA (for initial value 69%), platinum-zirconium dioxide/XC-72 carbon composite electrocatalyst (platinum: zirconium=2: 1) than platinum/C catalyst methanol oxidation is had the stable and anti-CO poisoning performance of better electro-catalysis of the present invention's preparation be described.
Embodiment 3:
Chloroplatinic acid is dissolved in the ethylene glycol, is mixed with the solution that concentration is 0.002mol/L.Get this solution of 50mL, adding 10mL concentration is the 10mmol/L zirconium nitrate aqueous solution, and the mol ratio of platinum and zirconium is 1: 1 in the solution, adds the polyethylene glycol aqueous solution of 5mL 1% again.With sodium hydroxide solution regulator solution pH value is 12.The CNT that in this synthetic solvent, adds 63mg again, and ultrasonic mixing.Final mixture is transferred in the round-bottomed flask of 250mL, and is placed in the micro-wave oven, adds reflux, microwave 15min.After the cooling, solid product fully washs after filtration and with acetone and deionized water, 80 ℃ of oven dry, obtains platinum-zirconium/carbon dioxide nanotube composite electrocatalyst.(mass fraction of platinum is 20% in the catalyst, mol ratio platinum: zirconium=1: 1).Nano platinum particle has uniform particle diameter in the transmission electron microscope observing catalyst, and average grain diameter is 3.0nm.
As a comparison, in synthetic solvent, do not add zirconium nitrate solution, with the synthetic platinum/carbon nano-tube catalyst (mass fraction of platinum is 20%) of similar method.The nano platinum particle particle diameter is 3.1nm in the transmission electron microscope observing platinum/carbon nano-tube eelctro-catalyst.
According to 1 pair of methanol oxidation electrocatalysis characteristic test of embodiment relatively.Test result shows under the same terms: (platinum: zirconium=1: 1) take-off potential and the peak current to methanol oxidation is respectively 0.31V and 11.3mA to platinum-zirconium/carbon dioxide nanotube composite electrocatalyst, and the platinum/carbon nano-tube catalyst is respectively 0.40V and 9.5mA to the take-off potential and the peak current of methanol oxidation, and platinum-zirconium/carbon dioxide nanotube composite electrocatalyst (platinum: zirconium=1: 1) than platinum/carbon nano-tube catalyst methanol oxidation is had higher electro catalytic activity of the present invention's preparation is described; Again after the constant potential polarization 1h, platinum-zirconium/carbon dioxide nanotube composite electrocatalyst (platinum: zirconium=1: 1) to the electric current of methanol oxidation be 0.98mA (for initial value 81%), and the platinum/carbon nano-tube catalyst to the electric current of methanol oxidation only be 0.90mA (for initial value 71%), platinum-zirconium/carbon dioxide nanotube composite electrocatalyst (platinum: zirconium=1: 1) than platinum/carbon nano-tube catalyst methanol oxidation is had the stable and anti-CO poisoning performance of better electro-catalysis of the present invention's preparation be described.
Embodiment 4:
Chloroplatinic acid is dissolved in the ethylene glycol, is mixed with the solution that concentration is 0.004mol/L.Get this solution of 50mL, adding 10mL concentration is the 10mmol/L zirconium nitrate aqueous solution, and the mol ratio of platinum and zirconium is 2: 1 in the solution, adds the polyethylene glycol aqueous solution of 10mL 1% again.With sodium hydroxide solution regulator solution pH value is 12.The CNT that in this synthetic solvent, adds 143mg again, and ultrasonic mixing.Final mixture is transferred in the round-bottomed flask of 250mL, and is placed in the micro-wave oven, adds reflux, microwave 15min.After the cooling, solid product fully washs after filtration and with acetone and deionized water, 80 ℃ of oven dry, obtains platinum-zirconium/carbon dioxide nanotube composite electrocatalyst.(mass fraction of platinum is 20% in the catalyst, mol ratio platinum: zirconium=2: 1).Nano platinum particle has uniform particle diameter in the transmission electron microscope observing catalyst, and average grain diameter is 3.1nm.
As a comparison, in synthetic solvent, do not add zirconium nitrate solution, with the synthetic platinum/carbon nano-tube catalyst (mass fraction of platinum is 20%) of similar method.The nano platinum particle particle diameter is 3.2nm in the transmission electron microscope observing platinum/carbon nano-tube eelctro-catalyst.
According to 1 pair of methanol oxidation electrocatalysis characteristic test of embodiment relatively.Test result shows under the same terms: (platinum: zirconium=2: 1) take-off potential and the peak current to methanol oxidation is respectively 0.33V and 12.8mA to platinum-zirconium/carbon dioxide nanotube composite electrocatalyst, and the platinum/carbon nano-tube catalyst is respectively 0.40V and 9.8mA to the take-off potential and the peak current of methanol oxidation, and platinum-zirconium/carbon dioxide nanotube composite electrocatalyst (platinum: zirconium=2: 1) than platinum/carbon nano-tube catalyst methanol oxidation is had higher electro catalytic activity of the present invention's preparation is described; Again after the constant potential polarization 1h, platinum-zirconium/carbon dioxide nanotube composite electrocatalyst (platinum: zirconium=2: 1) to the electric current of methanol oxidation be 1.02mA (for initial value 82%), and the platinum/carbon nano-tube catalyst to the electric current of methanol oxidation only be 0.96mA (for initial value 75%), platinum-zirconium/carbon dioxide nanotube composite electrocatalyst (platinum: zirconium=2: 1) than platinum/carbon nano-tube catalyst methanol oxidation is had the stable and anti-CO poisoning performance of better electro-catalysis of the present invention's preparation be described.
Embodiment 5:
Chloroplatinic acid is dissolved in the ethylene glycol, is mixed with the solution that concentration is 0.005mol/L.Get this solution of 60mL, adding 10mL concentration is the 10mmol/L zirconium nitrate aqueous solution, and the mol ratio of platinum and zirconium is 3: 1 in the solution, adds the polyethylene glycol aqueous solution of 15mL 1% again.With sodium hydroxide solution regulator solution pH value is 12.The XC-72 carbon that in this synthetic solvent, adds 183mg again, and ultrasonic mixing.Final mixture is transferred in the round-bottomed flask of 250mL, and is placed in the micro-wave oven, adds reflux, microwave 15min.After the cooling, solid product fully washs after filtration and with acetone and deionized water, 80 ℃ of oven dry, obtains platinum-zirconium dioxide/XC-72 carbon composite electrocatalyst.(mass fraction of platinum is 20% in the catalyst, mol ratio platinum: zirconium=3: 1).Nano platinum particle has uniform particle diameter in the transmission electron microscope observing catalyst, and average grain diameter is 3.0nm.
As a comparison, in synthetic solvent, do not add zirconium nitrate solution, with the synthetic platinum/C catalyst (mass fraction of platinum is 20%) of similar method.The nano platinum particle particle diameter is 3.1nm in transmission electron microscope observing platinum/carbon eelctro-catalyst.
According to 1 pair of methanol oxidation electrocatalysis characteristic test of embodiment relatively.Test result shows under the same terms: (platinum: zirconium=3: 1) take-off potential and the peak current to methanol oxidation is respectively 0.35V and 13.8mA to platinum-zirconium dioxide/XC-72 carbon composite electrocatalyst, and platinum/C catalyst is respectively 0.40V and 9.2mA to the take-off potential and the peak current of methanol oxidation, and platinum-zirconium dioxide/XC-72 carbon composite electrocatalyst (platinum: zirconium=3: 1) than platinum/C catalyst methanol oxidation is had higher electro catalytic activity of the present invention's preparation is described; Again after the constant potential polarization 1h, platinum-zirconium dioxide/XC-72 carbon composite electrocatalyst (platinum: zirconium=3: 1) to the electric current of methanol oxidation be 1.04mA (for initial value 81%), and platinum/C catalyst to the electric current of methanol oxidation only be 0.88mA (for initial value 73%), platinum-zirconium dioxide/XC-72 carbon composite electrocatalyst (platinum: zirconium=3: 1) than platinum/C catalyst methanol oxidation is had the stable and anti-CO poisoning performance of better electro-catalysis of the present invention's preparation be described.
Embodiment 6:
Chloroplatinic acid is dissolved in the ethylene glycol, is mixed with the solution that concentration is 0.002mol/L.Get this solution of 50mL, adding 10mL concentration is the 10mmol/L zirconium nitrate aqueous solution, and the mol ratio of platinum and zirconium is 1: 1 in the solution, adds the polyvinylpyrrolidone aqueous solution of 5mL 1% again.With sodium hydroxide solution regulator solution pH value is 12.The CNT that in this synthetic solvent, adds 63mg again, and ultrasonic mixing.Final mixture is transferred in the round-bottomed flask of 250mL, and is placed in the micro-wave oven, adds reflux, microwave 15min.After the cooling, solid product fully washs after filtration and with acetone and deionized water, 80 ℃ of oven dry, obtains platinum-zirconium/carbon dioxide nanotube composite electrocatalyst.(mass fraction of platinum is 20% in the catalyst, mol ratio platinum: zirconium=1: 1).Nano platinum particle has uniform particle diameter in the transmission electron microscope observing catalyst, and average grain diameter is 3.0nm.
As a comparison, in synthetic solvent, do not add zirconium nitrate solution, with the synthetic platinum/carbon nano-tube catalyst (mass fraction of platinum is 20%) of similar method.The nano platinum particle particle diameter is 3.1nm in the transmission electron microscope observing platinum/carbon nano-tube eelctro-catalyst.
According to 1 pair of methanol oxidation electrocatalysis characteristic test of embodiment relatively.Test result shows under the same terms: (platinum: zirconium=1: 1) take-off potential and the peak current to methanol oxidation is respectively 0.31V and 11.5mA to platinum-zirconium/carbon dioxide nanotube composite electrocatalyst, and the platinum/carbon nano-tube catalyst is respectively 0.40V and 9.4mA to the take-off potential and the peak current of methanol oxidation, and platinum-zirconium/carbon dioxide nanotube composite electrocatalyst (platinum: zirconium=1: 1) than platinum/carbon nano-tube catalyst methanol oxidation is had higher electro catalytic activity of the present invention's preparation is described; Again after the constant potential polarization 1h, platinum-zirconium/carbon dioxide nanotube composite electrocatalyst (platinum: zirconium=1: 1) to the electric current of methanol oxidation be 1.00mA (for initial value 82%), and the platinum/carbon nano-tube catalyst to the electric current of methanol oxidation only be 0.91mA (for initial value 73%), platinum-zirconium/carbon dioxide nanotube composite electrocatalyst (platinum: zirconium=1: 1) than platinum/carbon nano-tube catalyst methanol oxidation is had the stable and anti-CO poisoning performance of better electro-catalysis of the present invention's preparation be described.
Claims (3)
1. the preparation method of a platinum-zirconium/carbon dioxide composite electro-catalyst is characterized in that following steps:
1) chloroplatinic acid is dissolved in the ethylene glycol, is mixed with the chloroplatinic acid ethylene glycol solution of 0.002～0.005mol/L;
2) add the zirconium nitrate aqueous solution in the chloroplatinic acid ethylene glycol solution, making the platinum in the solution and the mol ratio of zirconium is 1: 1～3: 1, adds stabilizing agent then, and regulating pH with NaOH is 12～14;
3) in step 2) add nano-sized carbon as carrier in the solution of gained, after ultrasonic the mixing, put into the micro-wave oven that has reflux and heat 5～20min, after the cooling after filtration, fully wash with acetone and deionized water, oven dry obtains platinum-zirconium/carbon dioxide composite electro-catalyst, the mass fraction of platinum in catalyst is 10～20%, and the mol ratio of platinum and zirconium was at 1: 1～3: 1.
2. the preparation method of a kind of platinum-zirconium/carbon dioxide composite electro-catalyst according to claim 1 is characterized in that said stabilizing agent is polyvinylpyrrolidone or polyethylene glycol.
3. the preparation method of a kind of platinum-zirconium/carbon dioxide composite electro-catalyst according to claim 1 is characterized in that said nano-sized carbon is XC-72 carbon or CNT.
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Cited By (5)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN104716347A (en) * | 2015-03-15 | 2015-06-17 | 北京工业大学 | CeO2 containing Pt-based fuel cell catalyst and preparation method thereof |
| CN111342067A (en) * | 2020-03-10 | 2020-06-26 | 中国原子能科学研究院 | Platinum-based catalyst and preparation method thereof |
| CN111710878A (en) * | 2020-05-29 | 2020-09-25 | 新疆大学 | Preparation method of metal organic framework derived Co embedded nitrogen-doped carbon nanotube modified mesoporous carbon supported platinum catalyst |
| CN112736260A (en) * | 2020-12-09 | 2021-04-30 | 中国科学院福建物质结构研究所 | Composite material and preparation method and application thereof |
| CN113877574A (en) * | 2021-11-11 | 2022-01-04 | 河北工业大学 | Preparation method and application of zirconium dioxide nanotube array immobilized monatomic catalyst |
-
2009
- 2009-11-30 CN CN200910153974A patent/CN101711979A/en active Pending
Cited By (6)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN104716347A (en) * | 2015-03-15 | 2015-06-17 | 北京工业大学 | CeO2 containing Pt-based fuel cell catalyst and preparation method thereof |
| CN111342067A (en) * | 2020-03-10 | 2020-06-26 | 中国原子能科学研究院 | Platinum-based catalyst and preparation method thereof |
| CN111710878A (en) * | 2020-05-29 | 2020-09-25 | 新疆大学 | Preparation method of metal organic framework derived Co embedded nitrogen-doped carbon nanotube modified mesoporous carbon supported platinum catalyst |
| CN112736260A (en) * | 2020-12-09 | 2021-04-30 | 中国科学院福建物质结构研究所 | Composite material and preparation method and application thereof |
| CN113877574A (en) * | 2021-11-11 | 2022-01-04 | 河北工业大学 | Preparation method and application of zirconium dioxide nanotube array immobilized monatomic catalyst |
| CN113877574B (en) * | 2021-11-11 | 2024-02-02 | 河北工业大学 | Preparation method and application of zirconium dioxide nanotube array immobilized monoatomic catalyst |
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Open date: 20100526 |