Bimetallic Fe x Pt100-x Nanoparticles Immobilized on Supported Ionic Liquid Phases as Hydrogenation and Hydrodeoxygenation Catalysts: Influence of the Metal Content on Activity and Selectivity

被引：5

作者：

Marchenko, Nataliia ^{[1
]}

Lacroix, Lise-Marie ^{[1
,2
]}

Ratel-Ramond, Nicolas ^{[1
]}

Leitner, Walter ^{[3
,4
]}

Bordet, Alexis ^{[3
]}

Tricard, Simon ^{[1
]}

机构：

[1] Univ Toulouse, LPCNO, INSA, CNRS, F-31077 Toulouse, France

[2] Inst Univ France IUF, F-75005 Paris, France

[3] Max Planck Inst Chem Energy Convers, D-45470 Mulheim, Germany

[4] Rhein Westfal TH Aachen, Inst Tech & Makromol Chem, D-52074 Aachen, Germany

来源：

ACS APPLIED NANO MATERIALS | 2023年 / 6卷 / 21期

关键词：

bimetallic nanoparticles; supported ionic liquid phases; platinum; iron; hydrogenation; hydrodeoxygenation; catalysis; magnetism; REDUCTION; PLATINUM; SURFACES; PTFE; PD; OXIDATION; KETONES; SYSTEM; ALLOYS; ACID;

D O I：

10.1021/acsanm.3c03996

中图分类号：

TB3 [工程材料学];

学科分类号：

0805 ; 080502 ;

摘要：

Iron-platinum nanoparticles of tunable Fe/Pt ratios were immobilized on an imidazolium-based supported ionic liquid phase (SILP). The resulting FexPt100-x @SILP materials were characterized and applied in catalysis. Electron microscopy confirmed the formation of small, well-dispersed, bimetallic nanoparticles in all the investigated materials. Magnetometry measurements evidenced a clear influence of the Fe/Pt ratio on the oxidation state of Fe in FexPt100-x @SILP. In particular, Fe appeared in the metallic state at x <= 40, whereas partial oxidation was observed at x >= 60. The catalytic properties of FexPt100-x @SILP materials were probed using the reduction of benzylic ketones with H-2 as a model reaction. The Fe/Pt ratio of the nanoparticles was found to have a critical influence on the observed activity and selectivity, with clear synergistic effects. In particular, by diluting Pt with Fe sites, the ability of FexPt100-x @SILP catalysts to hydrogenate 6-membered aromatic rings was shut down for x >= 40, while C=O hydrogenation activity was preserved. In addition, Fe40Pt60@SILP showed excellent hydrodeoxygenation activity and selectivity with acetophenone derivatives in the absence of acid additives. This remarkable reactivity, out of reach for monometallic Pt@SILP, is attributed to the enhanced oxophilicity of Fe in FePt catalysts favoring C=O activation and cleavage.

引用

页码：20231 / 20239

页数：9

共 63 条

[1] Can the state of platinum species be unambiguously determined by the stretching frequency of an adsorbed CO probe molecule? [J].

Aleksandrov, Hristiyan A. ;

Neyman, Konstantin M. ;

Hadjiivanov, Konstantin I. ;

Vayssilov, Georgi N. .

PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2016, 18 (32) :22108-22121

[2] Hydrodeoxygenation Using Magnetic Induction: High-Temperature Heterogeneous Catalysis in Solution [J].

Asensio, Juan M. ;

Miguel, Ana B. ;

Fazzini, Pier-Francesco ;

van Leeuwen, Piet W. N. M. ;

Chaudret, Bruno .

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2019, 58 (33) :11306-11310

[3] Multicomponent Pt-Based Zigzag Nanowires as Selectivity Controllers for Selective Hydrogenation Reactions [J].

Bai, Shuxing ;

Bu, Lingzheng ;

Shao, Qi ;

Zhu, Xing ;

Huang, Xiaoqing .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2018, 140 (27) :8384-8387

[4] Metal Nanoparticles Immobilized on Molecularly Modified Surfaces: Versatile Catalytic Systems for Controlled Hydrogenation and Hydrogenolysis [J].

Bordet, Alexis ;

Leitner, Walter .

ACCOUNTS OF CHEMICAL RESEARCH, 2021, 54 (09) :2144-2157

[5] Molecular Control of the Catalytic Properties of Rhodium Nanoparticles in Supported Ionic Liquid Phase (SILP) Systems [J].

Bordet, Alexis ;

Moos, Gilles ;

Welsh, Calum ;

Licence, Peter ;

Luska, Kylie L. ;

Leitner, Walter .

ACS CATALYSIS, 2020, 10 (23) :13904-13912

[6] Properties of alumina supported Pd-Fe and Pt-Fe catalysts prepared using surface organometallic chemistry [J].

Crabb, EM ;

Marshall, R .

APPLIED CATALYSIS A-GENERAL, 2001, 217 (1-2) :41-53

[7] Selective Hydrogenation of Functionalized Alkynes to (E)-Alkenes, Using Ordered Alloys as Catalysts [J].

Furukawa, Shinya ;

Komatsu, Takayuki .

ACS CATALYSIS, 2016, 6 (03) :2121-2125

[8] Unsupported Nanoporous Platinum-Iron Bimetallic Catalyst for the Chemoselective Hydrogenation of Halonitrobenzenes to Haloanilines [J].

Geng, Yuxuan ;

Chen, Chong ;

Gao, Zhanming ;

Feng, Xiujuan ;

Liu, Wei ;

Li, Yanhui ;

Jin, Tienan ;

Shi, Yantao ;

Zhang, Wei ;

Bao, Ming .

ACS APPLIED MATERIALS & INTERFACES, 2021, 13 (20) :23655-23661

[9] Selective hydrodeoxygenation of acetophenone derivatives using a Fe25Ru75@SILP catalyst: a practical approach to the synthesis of alkyl phenols and anilines [J].

Goclik, Lisa ;

Walschus, Henrik ;

Bordet, Alexis ;

Leitner, Walter .

GREEN CHEMISTRY, 2022, 24 (07) :2937-2945

[10] Selective hydrodeoxygenation of hydroxyacetophenones to ethyl-substituted phenol derivatives using a FeRu@SILP catalyst [J].

Goclik, Lisa ;

Offner-Marko, Lisa ;

Bordet, Alexis ;

Leitner, Walter .

CHEMICAL COMMUNICATIONS, 2020, 56 (66) :9509-9512

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