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Title: Self-assembly of noble metal monolayers on transition metal carbide nanoparticle catalysts

Abstract

Here, we demonstrated the self-assembly of transition metal carbide nanoparticles coated with atomically thin noble metal monolayers by carburizing mixtures of noble metal salts and transition metal oxides encapsulated in removable silica templates. This approach allows for control of the final core-shell architecture, including particle size, monolayer coverage, and heterometallic composition. Carbon-supported Ti0.1W0.9C nanoparticles coated with Pt or bimetallic PtRu monolayers exhibited enhanced resistance to sintering and CO poisoning, achieving an order of magnitude increase in specific activity over commercial catalysts for methanol electrooxidation after 10,000 cycles. These core-shell materials provide a new direction to reduce the loading, enhance the activity, and increase the stability of noble metal catalysts.

Authors:
 [1];  [1];  [2];  [1];  [3];  [1]
  1. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
  2. Univ. of Wisconsin-Madison, Madison, WI (United States); Univ. of Toledo, Toledo, OH (United States)
  3. Univ. of Wisconsin-Madison, Madison, WI (United States)
Publication Date:
Research Org.:
Univ. of Wisconsin, Madison, WI (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Contributing Org.:
Extreme Science and Engineering Discovery Environment (XSEDE) and the University of Wisconsin Materials Research Science and Engineering Center
OSTI Identifier:
1434319
Grant/Contract Number:  
SC0014058
Resource Type:
Accepted Manuscript
Journal Name:
Science
Additional Journal Information:
Journal Volume: 352; Journal Issue: 6288; Journal ID: ISSN 0036-8075
Publisher:
AAAS
Country of Publication:
United States
Language:
English
Subject:
77 NANOSCIENCE AND NANOTECHNOLOGY

Citation Formats

Hunt, Sean T., Milina, Maria, Alba-Rubio, Ana C., Hendon, Christopher H., Dumesic, James A., and Roman-Leshkov, Yuriy. Self-assembly of noble metal monolayers on transition metal carbide nanoparticle catalysts. United States: N. p., 2016. Web. doi:10.1126/science.aad8471.
Hunt, Sean T., Milina, Maria, Alba-Rubio, Ana C., Hendon, Christopher H., Dumesic, James A., & Roman-Leshkov, Yuriy. Self-assembly of noble metal monolayers on transition metal carbide nanoparticle catalysts. United States. https://doi.org/10.1126/science.aad8471
Hunt, Sean T., Milina, Maria, Alba-Rubio, Ana C., Hendon, Christopher H., Dumesic, James A., and Roman-Leshkov, Yuriy. Fri . "Self-assembly of noble metal monolayers on transition metal carbide nanoparticle catalysts". United States. https://doi.org/10.1126/science.aad8471. https://www.osti.gov/servlets/purl/1434319.
@article{osti_1434319,
title = {Self-assembly of noble metal monolayers on transition metal carbide nanoparticle catalysts},
author = {Hunt, Sean T. and Milina, Maria and Alba-Rubio, Ana C. and Hendon, Christopher H. and Dumesic, James A. and Roman-Leshkov, Yuriy},
abstractNote = {Here, we demonstrated the self-assembly of transition metal carbide nanoparticles coated with atomically thin noble metal monolayers by carburizing mixtures of noble metal salts and transition metal oxides encapsulated in removable silica templates. This approach allows for control of the final core-shell architecture, including particle size, monolayer coverage, and heterometallic composition. Carbon-supported Ti0.1W0.9C nanoparticles coated with Pt or bimetallic PtRu monolayers exhibited enhanced resistance to sintering and CO poisoning, achieving an order of magnitude increase in specific activity over commercial catalysts for methanol electrooxidation after 10,000 cycles. These core-shell materials provide a new direction to reduce the loading, enhance the activity, and increase the stability of noble metal catalysts.},
doi = {10.1126/science.aad8471},
journal = {Science},
number = 6288,
volume = 352,
place = {United States},
year = {Fri May 20 00:00:00 EDT 2016},
month = {Fri May 20 00:00:00 EDT 2016}
}

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Recent Progress in the Design and Synthesis of Nitrides for Mesoscopic and Perovskite Solar Cells
journal, January 2019


Golden single-atomic-site platinum electrocatalysts
journal, September 2018


New design for highly durable infrared-reflective coatings
journal, December 2017

  • Hu, Chaoquan; Liu, Jian; Wang, Jianbo
  • Light: Science & Applications, Vol. 7, Issue 4
  • DOI: 10.1038/lsa.2017.175

W 2 C nanorods with various amounts of vacancy defects: determination of catalytic active sites in the hydrodeoxygenation of benzofuran
journal, January 2017

  • Liu, Rong; Pang, Min; Chen, Xiaozhen
  • Catalysis Science & Technology, Vol. 7, Issue 6
  • DOI: 10.1039/c6cy02702d

A general synthesis approach for amorphous noble metal nanosheets
journal, October 2019


Metallic tungsten carbide nanoparticles as a near-infrared-driven photocatalyst
journal, January 2019

  • Huang, Weicheng; Meng, Hongxue; Gao, Yan
  • Journal of Materials Chemistry A, Vol. 7, Issue 31
  • DOI: 10.1039/c9ta03151k

Highly active zigzag-like Pt-Zn alloy nanowires with high-index facets for alcohol electrooxidation
journal, April 2019


Engineering High-Energy Interfacial Structures for High-Performance Oxygen-Involving Electrocatalysis
journal, March 2017

  • Guo, Chunxian; Zheng, Yao; Ran, Jingrun
  • Angewandte Chemie International Edition, Vol. 56, Issue 29
  • DOI: 10.1002/anie.201701531

MOF-derived nanostructured catalysts for low-temperature ammonia synthesis
journal, January 2020

  • Luz, Ignacio; Parvathikar, Sameer; Carpenter, Michael
  • Catalysis Science & Technology, Vol. 10, Issue 1
  • DOI: 10.1039/c9cy01303b

Density functional study on the high catalytic performance of single metal atoms on the NbC(001) surface
journal, January 2018

  • Kan, Dongxiao; Zhang, Xilin; Fu, Zhaoming
  • Physical Chemistry Chemical Physics, Vol. 20, Issue 15
  • DOI: 10.1039/c8cp00069g

Interface Engineered W x C@WS 2 Nanostructure for Enhanced Hydrogen Evolution Catalysis
journal, January 2017

  • Wang, Fengmei; He, Peng; Li, Yuanchang
  • Advanced Functional Materials, Vol. 27, Issue 7
  • DOI: 10.1002/adfm.201605802

Highly Efficient, Low-Cost, and Magnetically Recoverable FePt–Ag Nanocatalysts: Towards Green Reduction of Organic Dyes
journal, May 2018

  • Liu, Yang; Zhang, Yuanyuan; Kou, Qiangwei
  • Nanomaterials, Vol. 8, Issue 5
  • DOI: 10.3390/nano8050329

Recent Progress in Photocatalytic CO 2 Reduction Over Perovskite Oxides
journal, September 2017


Ni-based bimetallic heterogeneous catalysts for energy and environmental applications
journal, January 2016

  • De, Sudipta; Zhang, Jiaguang; Luque, Rafael
  • Energy & Environmental Science, Vol. 9, Issue 11
  • DOI: 10.1039/c6ee02002j

Surface-clean, phase-pure multi-metallic carbides for efficient electrocatalytic hydrogen evolution reaction
journal, January 2019

  • Gao, Shuang; Chen, Hui; Liu, Yipu
  • Inorganic Chemistry Frontiers, Vol. 6, Issue 4
  • DOI: 10.1039/c8qi01360h