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CN-121976245-A - Selenium monoatomic coupling PtNiMoPdRh alloy catalyst and preparation method and application thereof

CN121976245ACN 121976245 ACN121976245 ACN 121976245ACN-121976245-A

Abstract

The invention provides a selenium single-atom coupling PtNiMoPdRh alloy catalyst and a preparation method and application thereof, belonging to the technical field of metal nano catalysts. The invention firstly carries out constant temperature heat treatment on carbon-selenium mixed powder at 680-700 ℃ to obtain a carbon-selenium compound, then uniformly mixes a metal source, a surfactant, a reducing agent and the carbon-selenium compound in a solvent, and then carries out reaction at 200-240 ℃ to obtain the selenium monoatomic coupling PtNiMoPdRh alloy catalyst. The selenium monoatomic coupling PtNiMoPdRh alloy catalyst has the advantages of high conductivity, strong metal-carrier interaction, sufficient active site, high structural stability, high catalytic activity and the like, can be used for catalyzing water to produce hydrogen, and has the advantages of simplicity, easiness in operation, short reaction time, low cost and good popularization and application prospects.

Inventors

  • WANG JIKE
  • WEI MIN
  • LI ZITING

Assignees

  • 武汉大学

Dates

Publication Date
20260505
Application Date
20260121

Claims (10)

  1. 1. The preparation method of the selenium monoatomic coupling PtNiMoPdRh alloy catalyst is characterized by comprising the following steps of: The method comprises the steps of uniformly mixing raw materials comprising a metal source, a surfactant, a reducing agent and a carbon-selenium compound in a solvent 1, then placing the raw materials in a temperature of 200-240 ℃ for reaction, and washing, centrifuging and drying the raw materials to obtain the selenium monoatomic coupling PtNiMoPdRh alloy catalyst, wherein the metal source comprises a platinum source, a nickel source, a molybdenum source, a palladium source and a rhodium source.
  2. 2. The preparation method of the selenium single-atom coupling PtNiMoPdRh alloy catalyst according to claim 1 is characterized by comprising the steps of mixing carbon powder and selenium powder in a solvent 2, performing ball milling treatment to obtain carbon-selenium mixed powder, performing thermal treatment on the carbon-selenium mixed powder at 680-700 ℃ in an inert gas atmosphere, and cooling to obtain the carbon-selenium composite.
  3. 3. The method for preparing the selenium monoatomic coupling PtNiMoPdRh alloy catalyst according to claim 2, wherein the mass ratio of the carbon powder to the selenium powder is (1-10): 1.
  4. 4. The method for preparing the selenium monatomic coupling PtNiMoPdRh alloy catalyst according to claim 1, wherein in the selenium monatomic coupling PtNiMoPdRh alloy catalyst, the atomic ratio of platinum, nickel, molybdenum, palladium and rhodium is (24-28): 28-30): 1-3): 24-26: 16-20, selenium exists in the form of a single atom, and the selenium atom accounts for 1% -0.1%.
  5. 5. The method for preparing a selenium monatomic coupling PtNiMoPdRh alloy catalyst according to claim 4, wherein the mass ratio of the platinum source, the surfactant, the reducing agent and the carbon-selenium composite is 4:240:24:1.
  6. 6. The method for preparing a selenium monoatomic coupling PtNiMoPdRh alloy catalyst according to claim 5, wherein the molar ratio of the platinum source, the nickel source, the molybdenum source, the palladium source and the rhodium source is 1:4:5:1:1.
  7. 7. The method for preparing the selenium monoatomic coupling PtNiMoPdRh alloy catalyst according to claim 6, wherein the platinum source is platinum acetylacetonate, the nickel source is nickel acetylacetonate, nickel acetate or nickel chloride, the molybdenum source is molybdenum hexacarbonyl, the palladium source is palladium acetylacetonate, and the rhodium source is rhodium acetylacetonate.
  8. 8. The method for preparing the selenium single-atom-coupled PtNiMoPdRh alloy catalyst according to claim 5, wherein the surfactant is benzyl triethyl ammonium chloride and the reducing agent is glucose.
  9. 9. Selenium monoatomic coupling PtNiMoPdRh alloy catalyst prepared by the preparation method of any one of claims 1 to 8.
  10. 10. Use of the selenium monoatomic coupling PtNiMoPdRh alloy catalyst of claim 9 in catalyzing hydrogen evolution reactions.

Description

Selenium monoatomic coupling PtNiMoPdRh alloy catalyst and preparation method and application thereof Technical Field The invention relates to the technical field of metal nano catalysts, in particular to a selenium single-atom coupling PtNiMoPdRh alloy catalyst, a preparation method and application thereof. Background With the deep global energy transformation, efficient and clean hydrogen energy becomes a key driving force for future development. The high performance catalyst can significantly accelerate the development of hydrogen energy. Among existing catalysts, platinum (Pt) exhibits excellent activity in Hydrogen Evolution Reaction (HER) due to its unique electronic structure. However, its high cost limits its further industrial application. More and more methods are exploring to improve catalytic activity by adjusting the d-electron structure of Pt, thereby reducing consumption. High entropy alloys become potential catalysts due to their four major effects. Therefore, the Pt-based high-entropy alloy material improves the catalytic activity and simultaneously obviously reduces the dosage of Pt. In addition to alloying, regulating the electronic interactions between the metal and the support is a key strategy to improve catalytic activity. In the graphene supported metal catalyst, pi electrons of a carbon carrier are hybridized with d orbitals of metal to generate charge transfer, and d band centers of the metal move downwards, so that adsorption energy of molecules such as carbon monoxide, hydrogen and the like is regulated, and the reaction energy barrier is remarkably reduced. Meanwhile, in sulfur-doped carbon-supported platinum nanoclusters, carbon transfer to platinum electrons creates electron-rich platinum sites, thereby enhancing H-adsorption and accelerating the kinetics of hydrogen evolution reactions. In addition to d-band center modulation, heteroatom doping also alters the conductivity of the support. The enhancement effectively reduces the electron transfer impedance and the potential gradient, ensures the rapid and uniform electron acquisition/release of the electrode/catalytic site, and improves the catalytic activity and the kinetic reaction. The d-band center of the active site can be obviously influenced by reasonably regulating and controlling the electronic structure of the carrier, and the electronic tuning effectively optimizes the adsorption/desorption behavior of the key reaction intermediate. The catalytic performance of the metal-carrier interaction system can be optimized by regulating and controlling the charge on the interface, and the bonding strength of the reaction intermediate can be accurately regulated by regulating the electron density around the active center so as to achieve the optimal balance between adsorption and desorption. On one hand, the d-band center of the metal is changed by alloy to actively participate in electron interaction so as to adjust the d-electron structure of the active site to be beneficial to the occurrence of catalytic reaction, and on the other hand, the introduction of hetero atoms into the carbon-based carrier can not only effectively change the local charge and the conductivity, but also generate selective charge polarization in the metal-carrier. The introduction of the heteroatom-enhanced metal-support interaction interface engineering provides a powerful and versatile strategy for optimizing reaction energetics and accelerating catalytic kinetics. 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 of ordinary skill in the art. Disclosure of Invention Aiming at the defects of the prior art, the invention provides the selenium single-atom coupling PtNiMoPdRh alloy catalyst with stable structure, high activity and low cost, and the preparation method and the application thereof. In order to achieve the above purpose, the specific technical scheme of the invention is as follows: in a first aspect of the present invention, a method for preparing a selenium monatomic coupling PtNiMoPdRh alloy catalyst is provided, comprising the steps of: Uniformly mixing a metal source, a surfactant, a reducing agent and a carbon-selenium compound in a solvent 1, then placing the mixture in a condition of 200-240 ℃ for reaction, and washing, centrifuging and drying the mixture to obtain the selenium monoatomic coupling PtNiMoPdRh alloy catalyst, wherein the metal source comprises a platinum source, a nickel source, a molybdenum source, a palladium source and a rhodium source. The preparation method of the carbon-selenium compound comprises the steps of mixing carbon (C) powder and selenium (Se) powder in a solvent 2, performing ball milling treatment to obtain carbon-selenium mixed powder, performing heat treatment on the carbon-s