Rui Zhou, Hongjiang Li, Shenmin Li, Yingna Cui, Xinping Wang
{"title":"将Pt原子锚定在MFI分子筛骨架Zn上,构建稳定、活性丙烷脱氢催化剂","authors":"Rui Zhou, Hongjiang Li, Shenmin Li, Yingna Cui, Xinping Wang","doi":"10.1016/j.micromeso.2025.113676","DOIUrl":null,"url":null,"abstract":"<div><div>Constructing an efficient Pt intermetallic alloy (IMA) species inside the zeolite intrinsic micropore is highly desired for propane dehydrogenation (PDH) process. Typical impregnation method often results in inhomogeneous dispersion of metal species on the zeolite surface. Herein, we report a strategy of constructing PtZn IMA species within the silicalite-1 (S-1) zeolite crystals by introducing Pt (NH<sub>3</sub>)<sub>4</sub><sup>2+</sup> ions into the ZnS-1 zeolite channels via ion-exchange. It allowed all of the Pt in the catalyst to anchored at the framework Zn and eventually transform to atomic PtZn IMA species after reduction over there. The Pt@2ZnS-1 catalyst containing 0.073 wt% Pt and 2 wt% Zn exhibited an initial propylene formation rate of 214.2 mol<sub>C3H6</sub>∙g<sub>Pt</sub><sup>−1</sup>∙h<sup>−1</sup> and a deactivation rate 0.00023 h<sup>−1</sup> at 550 °C in 600 h' reaction in feed gas C<sub>3</sub>H<sub>8</sub>/H<sub>2</sub>/N<sub>2</sub> = 1/1/4 (V/V/V), and initial propylene formation rate of 301 mol<sub>C3H6</sub>∙g<sub>Pt</sub><sup>−1</sup>∙h<sup>−1</sup> and deactivation rate 0.00217 h<sup>−1</sup> in 100 h’ reaction in feed gas C<sub>3</sub>H<sub>8</sub>/N<sub>2</sub> = 1/4 (V/V).</div></div>","PeriodicalId":392,"journal":{"name":"Microporous and Mesoporous Materials","volume":"394 ","pages":"Article 113676"},"PeriodicalIF":4.8000,"publicationDate":"2025-05-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Anchoring atomic Pt on MFI zeolite framework Zn to construct stable and active propane dehydrogenation catalyst\",\"authors\":\"Rui Zhou, Hongjiang Li, Shenmin Li, Yingna Cui, Xinping Wang\",\"doi\":\"10.1016/j.micromeso.2025.113676\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>Constructing an efficient Pt intermetallic alloy (IMA) species inside the zeolite intrinsic micropore is highly desired for propane dehydrogenation (PDH) process. Typical impregnation method often results in inhomogeneous dispersion of metal species on the zeolite surface. Herein, we report a strategy of constructing PtZn IMA species within the silicalite-1 (S-1) zeolite crystals by introducing Pt (NH<sub>3</sub>)<sub>4</sub><sup>2+</sup> ions into the ZnS-1 zeolite channels via ion-exchange. It allowed all of the Pt in the catalyst to anchored at the framework Zn and eventually transform to atomic PtZn IMA species after reduction over there. The Pt@2ZnS-1 catalyst containing 0.073 wt% Pt and 2 wt% Zn exhibited an initial propylene formation rate of 214.2 mol<sub>C3H6</sub>∙g<sub>Pt</sub><sup>−1</sup>∙h<sup>−1</sup> and a deactivation rate 0.00023 h<sup>−1</sup> at 550 °C in 600 h' reaction in feed gas C<sub>3</sub>H<sub>8</sub>/H<sub>2</sub>/N<sub>2</sub> = 1/1/4 (V/V/V), and initial propylene formation rate of 301 mol<sub>C3H6</sub>∙g<sub>Pt</sub><sup>−1</sup>∙h<sup>−1</sup> and deactivation rate 0.00217 h<sup>−1</sup> in 100 h’ reaction in feed gas C<sub>3</sub>H<sub>8</sub>/N<sub>2</sub> = 1/4 (V/V).</div></div>\",\"PeriodicalId\":392,\"journal\":{\"name\":\"Microporous and Mesoporous Materials\",\"volume\":\"394 \",\"pages\":\"Article 113676\"},\"PeriodicalIF\":4.8000,\"publicationDate\":\"2025-05-05\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Microporous and Mesoporous Materials\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S1387181125001908\",\"RegionNum\":3,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, APPLIED\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Microporous and Mesoporous Materials","FirstCategoryId":"88","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S1387181125001908","RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, APPLIED","Score":null,"Total":0}
Anchoring atomic Pt on MFI zeolite framework Zn to construct stable and active propane dehydrogenation catalyst
Constructing an efficient Pt intermetallic alloy (IMA) species inside the zeolite intrinsic micropore is highly desired for propane dehydrogenation (PDH) process. Typical impregnation method often results in inhomogeneous dispersion of metal species on the zeolite surface. Herein, we report a strategy of constructing PtZn IMA species within the silicalite-1 (S-1) zeolite crystals by introducing Pt (NH3)42+ ions into the ZnS-1 zeolite channels via ion-exchange. It allowed all of the Pt in the catalyst to anchored at the framework Zn and eventually transform to atomic PtZn IMA species after reduction over there. The Pt@2ZnS-1 catalyst containing 0.073 wt% Pt and 2 wt% Zn exhibited an initial propylene formation rate of 214.2 molC3H6∙gPt−1∙h−1 and a deactivation rate 0.00023 h−1 at 550 °C in 600 h' reaction in feed gas C3H8/H2/N2 = 1/1/4 (V/V/V), and initial propylene formation rate of 301 molC3H6∙gPt−1∙h−1 and deactivation rate 0.00217 h−1 in 100 h’ reaction in feed gas C3H8/N2 = 1/4 (V/V).
期刊介绍:
Microporous and Mesoporous Materials covers novel and significant aspects of porous solids classified as either microporous (pore size up to 2 nm) or mesoporous (pore size 2 to 50 nm). The porosity should have a specific impact on the material properties or application. Typical examples are zeolites and zeolite-like materials, pillared materials, clathrasils and clathrates, carbon molecular sieves, ordered mesoporous materials, organic/inorganic porous hybrid materials, or porous metal oxides. Both natural and synthetic porous materials are within the scope of the journal.
Topics which are particularly of interest include:
All aspects of natural microporous and mesoporous solids
The synthesis of crystalline or amorphous porous materials
The physico-chemical characterization of microporous and mesoporous solids, especially spectroscopic and microscopic
The modification of microporous and mesoporous solids, for example by ion exchange or solid-state reactions
All topics related to diffusion of mobile species in the pores of microporous and mesoporous materials
Adsorption (and other separation techniques) using microporous or mesoporous adsorbents
Catalysis by microporous and mesoporous materials
Host/guest interactions
Theoretical chemistry and modelling of host/guest interactions
All topics related to the application of microporous and mesoporous materials in industrial catalysis, separation technology, environmental protection, electrochemistry, membranes, sensors, optical devices, etc.