• 文献检索
  • 文档翻译
  • 深度研究
  • 学术资讯
  • Suppr Zotero 插件Zotero 插件
  • 邀请有礼
  • 套餐&价格
  • 历史记录
应用&插件
Suppr Zotero 插件Zotero 插件浏览器插件Mac 客户端Windows 客户端微信小程序
定价
高级版会员购买积分包购买API积分包
服务
文献检索文档翻译深度研究API 文档MCP 服务
关于我们
关于 Suppr公司介绍联系我们用户协议隐私条款
关注我们

Suppr 超能文献

核心技术专利:CN118964589B侵权必究
粤ICP备2023148730 号-1Suppr @ 2026

文献检索

告别复杂PubMed语法,用中文像聊天一样搜索,搜遍4000万医学文献。AI智能推荐,让科研检索更轻松。

立即免费搜索

文件翻译

保留排版,准确专业,支持PDF/Word/PPT等文件格式,支持 12+语言互译。

免费翻译文档

深度研究

AI帮你快速写综述,25分钟生成高质量综述,智能提取关键信息,辅助科研写作。

立即免费体验

亚纳米级铂簇作为丙烷氧化脱氢的高活性和高选择性催化剂。

Subnanometre platinum clusters as highly active and selective catalysts for the oxidative dehydrogenation of propane.

作者信息

Vajda Stefan, Pellin Michael J, Greeley Jeffrey P, Marshall Christopher L, Curtiss Larry A, Ballentine Gregory A, Elam Jeffrey W, Catillon-Mucherie Stephanie, Redfern Paul C, Mehmood Faisal, Zapol Peter

机构信息

Chemical Sciences and Engineering Division, Argonne National Laboratory, 9700 South Cass Avenue, Argonne, Illinois 60439, USA.

出版信息

Nat Mater. 2009 Mar;8(3):213-6. doi: 10.1038/nmat2384. Epub 2009 Feb 8.

DOI:10.1038/nmat2384
PMID:19202544
Abstract

Small clusters are known to possess reactivity not observed in their bulk analogues, which can make them attractive for catalysis. Their distinct catalytic properties are often hypothesized to result from the large fraction of under-coordinated surface atoms. Here, we show that size-preselected Pt(8-10) clusters stabilized on high-surface-area supports are 40-100 times more active for the oxidative dehydrogenation of propane than previously studied platinum and vanadia catalysts, while at the same time maintaining high selectivity towards formation of propylene over by-products. Quantum chemical calculations indicate that under-coordination of the Pt atoms in the clusters is responsible for the surprisingly high reactivity compared with extended surfaces. We anticipate that these results will form the basis for development of a new class of catalysts by providing a route to bond-specific chemistry, ranging from energy-efficient and environmentally friendly synthesis strategies to the replacement of petrochemical feedstocks by abundant small alkanes.

摘要

已知小团簇具有其块状类似物中未观察到的反应活性,这使得它们对催化具有吸引力。人们常常推测,它们独特的催化性能源于大量配位不足的表面原子。在这里,我们表明,负载在高比表面积载体上的尺寸预选的Pt(8 - 10)团簇,对于丙烷的氧化脱氢反应,其活性比先前研究的铂和钒催化剂高40 - 100倍,同时对丙烯生成的选择性高于副产物。量子化学计算表明,与延展表面相比,团簇中Pt原子的配位不足是导致其惊人高反应活性的原因。我们预计,这些结果将为开发新型催化剂奠定基础,通过提供一条通向键特异性化学的途径,从节能和环境友好的合成策略到用丰富的小烷烃替代石化原料。

相似文献

1
Subnanometre platinum clusters as highly active and selective catalysts for the oxidative dehydrogenation of propane.亚纳米级铂簇作为丙烷氧化脱氢的高活性和高选择性催化剂。
Nat Mater. 2009 Mar;8(3):213-6. doi: 10.1038/nmat2384. Epub 2009 Feb 8.
2
Serendipity in Catalysis Research: Boron-Based Materials for Alkane Oxidative Dehydrogenation.催化研究中的意外发现:用于烷烃氧化脱氢的硼基材料
Acc Chem Res. 2018 Oct 16;51(10):2556-2564. doi: 10.1021/acs.accounts.8b00330. Epub 2018 Oct 4.
3
Ethane and Propane Dehydrogenation on Small Platinum Clusters Supported on Silica: An Ab Initio Molecular Dynamics and DFT Study.二氧化硅负载的小铂团簇上乙烷和丙烷的脱氢反应:从头算分子动力学和密度泛函理论研究
Chempluschem. 2024 Feb;89(2):e202300347. doi: 10.1002/cplu.202300347. Epub 2023 Nov 29.
4
Thermally Stable and Regenerable Platinum-Tin Clusters for Propane Dehydrogenation Prepared by Atom Trapping on Ceria.通过铈上原子捕获制备用于丙烷脱氢的热稳定和可再生的铂锡簇。
Angew Chem Int Ed Engl. 2017 Jul 24;56(31):8986-8991. doi: 10.1002/anie.201701115. Epub 2017 Jun 28.
5
Reactive Force Field Development for Propane Dehydrogenation on Platinum Surfaces.铂表面丙烷脱氢反应力场的开发
J Phys Chem C Nanomater Interfaces. 2024 Feb 9;128(7):2844-2855. doi: 10.1021/acs.jpcc.3c07126. eCollection 2024 Feb 22.
6
Tailoring Single-Atom Platinum for Selective and Stable Catalysts in Propane Dehydrogenation.定制用于丙烷脱氢的选择性和稳定催化剂的单原子铂
Chempluschem. 2022 Apr;87(4):e202100560. doi: 10.1002/cplu.202100560. Epub 2022 Feb 14.
7
Reactivity of chemisorbed oxygen atoms and their catalytic consequences during CH4-O2 catalysis on supported Pt clusters.担载 Pt 团簇上 CH4-O2 催化反应中化学吸附氧原子的反应性及其催化后果。
J Am Chem Soc. 2011 Oct 12;133(40):15958-78. doi: 10.1021/ja202411v. Epub 2011 Sep 15.
8
Subnanometer Bimetallic Platinum-Zinc Clusters in Zeolites for Propane Dehydrogenation.用于丙烷脱氢的沸石中的亚纳米双金属铂 - 锌簇
Angew Chem Int Ed Engl. 2020 Oct 26;59(44):19450-19459. doi: 10.1002/anie.202003349. Epub 2020 May 11.
9
DFT study of propane dehydrogenation on Pt catalyst: effects of step sites.DFT 研究丙烷在 Pt 催化剂上的脱氢反应:台阶位的影响。
Phys Chem Chem Phys. 2011 Feb 28;13(8):3257-67. doi: 10.1039/c0cp00341g. Epub 2011 Jan 21.
10
Regioselective generation and reactivity control of subnanometric platinum clusters in zeolites for high-temperature catalysis.用于高温催化的沸石中亚纳米级铂簇的区域选择性生成及反应性控制
Nat Mater. 2019 Aug;18(8):866-873. doi: 10.1038/s41563-019-0412-6. Epub 2019 Jul 1.

引用本文的文献

1
Synthesis and functionalization of polymeric materials based on organic borazine.基于有机硼嗪的高分子材料的合成与功能化
RSC Adv. 2025 Sep 2;15(38):31416-31446. doi: 10.1039/d5ra04671h. eCollection 2025 Aug 29.
2
Atomically Precise Platinum Nanoclusters: History and Recent Advances in Synthesis, Structure, and Properties.原子精确的铂纳米团簇:合成、结构和性质的历史与最新进展
Precis Chem. 2025 May 2;3(8):401-423. doi: 10.1021/prechem.5c00003. eCollection 2025 Aug 25.
3
Comprehensive Atomistic Simulations of Fischer-Tropsch in Outer Space: Astrocatalysis by Fe-Supported Nanoclusters on SiO.

本文引用的文献

1
Selective propene epoxidation on immobilized au(6-10) clusters: the effect of hydrogen and water on activity and selectivity.固定化金(6 - 10)团簇上的选择性丙烯环氧化:氢气和水对活性及选择性的影响
Angew Chem Int Ed Engl. 2009;48(8):1467-71. doi: 10.1002/anie.200804154.
2
Methane activation on Pt and Pt4: a density functional theory study.铂及Pt4上的甲烷活化:一项密度泛函理论研究
J Phys Chem B. 2007 Feb 22;111(7):1657-63. doi: 10.1021/jp065288e. Epub 2007 Feb 1.
3
Thermodynamic equilibrium compositions, structures, and reaction energies of Pt(x)O(y) (x = 1-3) clusters predicted from first principles.
外太空费托合成的综合原子模拟:SiO上铁负载纳米团簇的星催化作用
J Phys Chem C Nanomater Interfaces. 2025 May 20;129(22):10069-10082. doi: 10.1021/acs.jpcc.5c01472. eCollection 2025 Jun 5.
4
Unlocking CO conversion potential with single atom catalysts and machine learning in energy application.利用单原子催化剂和机器学习在能源应用中释放一氧化碳转化潜力。
iScience. 2025 Mar 28;28(6):112306. doi: 10.1016/j.isci.2025.112306. eCollection 2025 Jun 20.
5
The Tiara Nickel Cluster Story from Theory to Catalytic Applications.从理论到催化应用的钛镍簇故事
Precis Chem. 2025 Jan 9;3(4):157-171. doi: 10.1021/prechem.4c00087. eCollection 2025 Apr 28.
6
Low-Temperature Direct Oxidation of Propane to Propylene Oxide Using Supported Subnanometer Cu Clusters.使用负载型亚纳米铜簇将丙烷低温直接氧化为环氧丙烷
ACS Catal. 2025 Mar 24;15(7):5760-5769. doi: 10.1021/acscatal.4c07577. eCollection 2025 Apr 4.
7
Light-driven propane dehydrogenation by a single-atom catalyst under near-ambient conditions.近环境条件下单原子催化剂光驱动丙烷脱氢
Nat Chem. 2025 Jun;17(6):890-896. doi: 10.1038/s41557-025-01766-3. Epub 2025 Mar 21.
8
Role and regulation of surface oxygen vacancies in vanadium-based oxides for chemical looping oxidative dehydrogenation of propane.钒基氧化物表面氧空位在丙烷化学链氧化脱氢中的作用与调控
Chem Sci. 2025 Jan 22;16(11):4710-4717. doi: 10.1039/d4sc07811j. eCollection 2025 Mar 12.
9
Synergistic effect of scattered rare metals on Pt/CeO for propane oxidative dehydrogenation with CO.分散的稀有金属对Pt/CeO用于丙烷与CO氧化脱氢的协同效应。
RSC Adv. 2025 Jan 23;15(4):2319-2328. doi: 10.1039/d4ra08481k.
10
Theoretical study of the electronic and optical properties of a composite formed by the zeolite NaA and a magnetite cluster.由沸石NaA和磁铁矿簇形成的复合材料的电子和光学性质的理论研究。
Beilstein J Nanotechnol. 2025 Jan 17;16:44-53. doi: 10.3762/bjnano.16.5. eCollection 2025.
基于第一性原理预测的Pt(x)O(y)(x = 1 - 3)团簇的热力学平衡组成、结构和反应能量。
J Phys Chem B. 2006 Aug 24;110(33):16591-9. doi: 10.1021/jp0614446.
4
Clusters, surfaces, and catalysis.团簇、表面与催化作用。
Proc Natl Acad Sci U S A. 2006 Jul 11;103(28):10577-83. doi: 10.1073/pnas.0507691103. Epub 2006 Jun 1.
5
Quantum chemical study of mechanisms for oxidative dehydrogenation of propane on vanadium oxide.钒氧化物上丙烷氧化脱氢反应机理的量子化学研究
J Phys Chem B. 2006 Apr 27;110(16):8363-71. doi: 10.1021/jp056228w.
6
Landing of size-selected Agn+ clusters on single crystal TiO2 (110)-(1x1) surfaces at room temperature.在室温下,尺寸选择的Agn+团簇沉积在单晶TiO2(110)-(1x1)表面上。
J Chem Phys. 2005 Feb 22;122(8):81102. doi: 10.1063/1.1859271.
7
Charging effects on bonding and catalyzed oxidation of CO on Au8 clusters on MgO.电荷对MgO上Au8团簇上CO的键合和催化氧化的影响。
Science. 2005 Jan 21;307(5708):403-7. doi: 10.1126/science.1104168.
8
Physics. The active site in nanoparticle gold catalysis.物理学。纳米颗粒金催化中的活性位点。
Science. 2004 Oct 8;306(5694):234-5. doi: 10.1126/science.1104246.
9
The structure of catalytically active gold on titania.二氧化钛上具有催化活性的金的结构。
Science. 2004 Oct 8;306(5694):252-5. doi: 10.1126/science.1102420. Epub 2004 Aug 26.
10
Theoretical study of the H(2) reaction with a Pt(4) (111) cluster.H₂与Pt₄(111)团簇反应的理论研究。
J Chem Phys. 2004 Apr 1;120(13):6222-8. doi: 10.1063/1.1630298.