Single Pt Coordinated with Framework Fe in MWW-Type Ferrisilicate toward Efficient Propane Dehydrogenation

Longkang Zhang; Xinyu Chen; Yue Ma; Shaojia Song; Hao Xu; Yejun Guan; Weiyu Song; Jiangwei Zhang; Peng Wu

doi:10.1021/acscatal.4c02091

Single Pt Coordinated with Framework Fe in MWW-Type Ferrisilicate toward Efficient Propane Dehydrogenation

Longkang Zhang
, Xinyu Chen
, Yue Ma
, Shaojia Song
, Hao Xu^*
, Yejun Guan^*
, Weiyu Song^*
, Jiangwei Zhang^*
, Peng Wu^*

^*Corresponding author for this work

School of Chemistry and Molecular Engineering

Research output: Contribution to journal › Article › peer-review

17 Scopus citations

Abstract

Single atom catalysts have been widely studied due to their high metal dispersity and remarkable catalytic performance. However, stabilizing single-atom metals remains challenging because of the high surface free energy. In this work, framework Fe atom-stabilized single atom Pt were successfully confined into MWW zeolite (Pt@Fe-MWW) by a one-pot synthesis strategy. The isolated skeleton Fe served as anchoring site and promoter to stabilize the single atom Pt via Pt-O-Fe coordination as identified by the in situ CO-IR spectra and XAFS analysis, enabling Pt@Fe-MWW with satisfied activity for the PDH reaction with trace Pt content (<0.01 wt %). A linear relationship between the quantities of Pt-O-Fe coordinated species and the propylene formation rate further confirmed the synergistic catalysis of Pt and skeleton Fe species. A recorded propylene formation rate of Pt (FR_C3H6/Pt) of 1100 mol/g_Pt/h was achieved with a Pt content of 0.006 wt %. DFT calculations revealed that the formation of Pt-O-Fe species reduced the dissociation energy of the C-H bonds and facilitated the desorption of H₂, enabling efficient propane dehydrogenation.

Original language	English
Pages (from-to)	9431-9439
Number of pages	9
Journal	ACS Catalysis
Volume	14
Issue number	12
DOIs	https://doi.org/10.1021/acscatal.4c02091
State	Published - 21 Jun 2024

Keywords

Fe-MWW zeolite
Pt−O−Fe coordination
Trace Pt
propane dehydrogenation
single atom catalyst

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10.1021/acscatal.4c02091

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@article{f5af08b589d44432a88cd760e797dd64,

title = "Single Pt Coordinated with Framework Fe in MWW-Type Ferrisilicate toward Efficient Propane Dehydrogenation",

abstract = "Single atom catalysts have been widely studied due to their high metal dispersity and remarkable catalytic performance. However, stabilizing single-atom metals remains challenging because of the high surface free energy. In this work, framework Fe atom-stabilized single atom Pt were successfully confined into MWW zeolite (Pt@Fe-MWW) by a one-pot synthesis strategy. The isolated skeleton Fe served as anchoring site and promoter to stabilize the single atom Pt via Pt-O-Fe coordination as identified by the in situ CO-IR spectra and XAFS analysis, enabling Pt@Fe-MWW with satisfied activity for the PDH reaction with trace Pt content (<0.01 wt \%). A linear relationship between the quantities of Pt-O-Fe coordinated species and the propylene formation rate further confirmed the synergistic catalysis of Pt and skeleton Fe species. A recorded propylene formation rate of Pt (FRC3H6/Pt) of 1100 mol/gPt/h was achieved with a Pt content of 0.006 wt \%. DFT calculations revealed that the formation of Pt-O-Fe species reduced the dissociation energy of the C-H bonds and facilitated the desorption of H2, enabling efficient propane dehydrogenation.",

keywords = "Fe-MWW zeolite, Pt−O−Fe coordination, Trace Pt, propane dehydrogenation, single atom catalyst",

author = "Longkang Zhang and Xinyu Chen and Yue Ma and Shaojia Song and Hao Xu and Yejun Guan and Weiyu Song and Jiangwei Zhang and Peng Wu",

note = "Publisher Copyright: {\textcopyright} 2024 American Chemical Society.",

year = "2024",

month = jun,

day = "21",

doi = "10.1021/acscatal.4c02091",

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TY - JOUR

T1 - Single Pt Coordinated with Framework Fe in MWW-Type Ferrisilicate toward Efficient Propane Dehydrogenation

AU - Zhang, Longkang

AU - Chen, Xinyu

AU - Ma, Yue

AU - Song, Shaojia

AU - Xu, Hao

AU - Guan, Yejun

AU - Song, Weiyu

AU - Zhang, Jiangwei

AU - Wu, Peng

PY - 2024/6/21

Y1 - 2024/6/21

N2 - Single atom catalysts have been widely studied due to their high metal dispersity and remarkable catalytic performance. However, stabilizing single-atom metals remains challenging because of the high surface free energy. In this work, framework Fe atom-stabilized single atom Pt were successfully confined into MWW zeolite (Pt@Fe-MWW) by a one-pot synthesis strategy. The isolated skeleton Fe served as anchoring site and promoter to stabilize the single atom Pt via Pt-O-Fe coordination as identified by the in situ CO-IR spectra and XAFS analysis, enabling Pt@Fe-MWW with satisfied activity for the PDH reaction with trace Pt content (<0.01 wt %). A linear relationship between the quantities of Pt-O-Fe coordinated species and the propylene formation rate further confirmed the synergistic catalysis of Pt and skeleton Fe species. A recorded propylene formation rate of Pt (FRC3H6/Pt) of 1100 mol/gPt/h was achieved with a Pt content of 0.006 wt %. DFT calculations revealed that the formation of Pt-O-Fe species reduced the dissociation energy of the C-H bonds and facilitated the desorption of H2, enabling efficient propane dehydrogenation.

AB - Single atom catalysts have been widely studied due to their high metal dispersity and remarkable catalytic performance. However, stabilizing single-atom metals remains challenging because of the high surface free energy. In this work, framework Fe atom-stabilized single atom Pt were successfully confined into MWW zeolite (Pt@Fe-MWW) by a one-pot synthesis strategy. The isolated skeleton Fe served as anchoring site and promoter to stabilize the single atom Pt via Pt-O-Fe coordination as identified by the in situ CO-IR spectra and XAFS analysis, enabling Pt@Fe-MWW with satisfied activity for the PDH reaction with trace Pt content (<0.01 wt %). A linear relationship between the quantities of Pt-O-Fe coordinated species and the propylene formation rate further confirmed the synergistic catalysis of Pt and skeleton Fe species. A recorded propylene formation rate of Pt (FRC3H6/Pt) of 1100 mol/gPt/h was achieved with a Pt content of 0.006 wt %. DFT calculations revealed that the formation of Pt-O-Fe species reduced the dissociation energy of the C-H bonds and facilitated the desorption of H2, enabling efficient propane dehydrogenation.

KW - Fe-MWW zeolite

KW - Pt−O−Fe coordination

KW - Trace Pt

KW - propane dehydrogenation

KW - single atom catalyst

UR - https://www.scopus.com/pages/publications/85195597190

U2 - 10.1021/acscatal.4c02091

DO - 10.1021/acscatal.4c02091

M3 - 文章

AN - SCOPUS:85195597190

SN - 2155-5435

VL - 14

SP - 9431

EP - 9439

JO - ACS Catalysis

JF - ACS Catalysis

IS - 12

ER -

Single Pt Coordinated with Framework Fe in MWW-Type Ferrisilicate toward Efficient Propane Dehydrogenation

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