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Highly Active Subnano Palladium Clusters Embedded in i-Motif DNA

Highly active subnano Pd clusters were synthesized using i-motif DNA as the template through characterization via ESI MS, DLS, XPS, UV-vis, and FTIR. It is indicated that Pd sub(1)-Pd sub(5) clusters are generated at a [Pd]/[base] ratio of 0.2, Pd sub(8) to Pd sub(9) clusters are generated at a [Pd]... Full description

Journal Title: Langmuir Nov 26, 2013, Vol.29(47), pp.14345-14350-14345-14350
Main Author: Zhang, Jinli
Other Authors: Wang, Xian , Fu, Yan , Han, You , Cheng, Jingyao , Zhang, Yanqing , Li, Wei
Format: Electronic Article Electronic Article
Language: English
Subjects:
DNA
ID: ISSN: 0743-7463 ; E-ISSN: 1520-5827 ; DOI: 10.1021/la402153b
Link: http://search.proquest.com/docview/1534830251/
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title: Highly Active Subnano Palladium Clusters Embedded in i-Motif DNA
format: Article
creator:
  • Zhang, Jinli
  • Wang, Xian
  • Fu, Yan
  • Han, You
  • Cheng, Jingyao
  • Zhang, Yanqing
  • Li, Wei
subjects:
  • Ions
  • Cytosine
  • Palladium
  • Heavy Metals
  • DNA
  • Catalysts
  • Nanoparticles
  • Scaffolds
  • Miscellaneous
ispartof: Langmuir, Nov 26, 2013, Vol.29(47), pp.14345-14350-14345-14350
description: Highly active subnano Pd clusters were synthesized using i-motif DNA as the template through characterization via ESI MS, DLS, XPS, UV-vis, and FTIR. It is indicated that Pd sub(1)-Pd sub(5) clusters are generated at a [Pd]/[base] ratio of 0.2, Pd sub(8) to Pd sub(9) clusters are generated at a [Pd]/[base] ratio of 0.5, and large nanoparticles with the size about 2.6 nm are formed at a [Pd]/[base] ratio of 2.0. The i-motif-stabilized Pd sub(8)-Pd sub(9) clusters show high catalytic activity toward the reduction of 4-nitrophenol with a relative rate constant value of 2034 min super(-1) (mM Pd) super(-1). DFT calculations disclose that the unique structure of the i-motif with consecutive hemiprotonated CH super(+).C pairs can efficiently ligate Pd ions at the N3 sites of cytosines and that the synthesized Pd clusters consist of metallic Pd atoms as well as positively charged Pd that is ligated by nucleobases, which is capable of facilitating the activation of the nitryl group of 4-nitrophenol. This work suggests a promising pathway to preparing subnano metal catalysts with enhanced catalytic activity using programmable DNA scaffolds.
language: eng
source:
identifier: ISSN: 0743-7463 ; E-ISSN: 1520-5827 ; DOI: 10.1021/la402153b
fulltext: fulltext
issn:
  • 07437463
  • 0743-7463
  • 15205827
  • 1520-5827
url: Link


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titleHighly Active Subnano Palladium Clusters Embedded in i-Motif DNA
creatorZhang, Jinli ; Wang, Xian ; Fu, Yan ; Han, You ; Cheng, Jingyao ; Zhang, Yanqing ; Li, Wei
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ispartofLangmuir, Nov 26, 2013, Vol.29(47), pp.14345-14350-14345-14350
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subjectIons ; Cytosine ; Palladium ; Heavy Metals ; DNA ; Catalysts ; Nanoparticles ; Scaffolds ; Miscellaneous
descriptionHighly active subnano Pd clusters were synthesized using i-motif DNA as the template through characterization via ESI MS, DLS, XPS, UV-vis, and FTIR. It is indicated that Pd sub(1)-Pd sub(5) clusters are generated at a [Pd]/[base] ratio of 0.2, Pd sub(8) to Pd sub(9) clusters are generated at a [Pd]/[base] ratio of 0.5, and large nanoparticles with the size about 2.6 nm are formed at a [Pd]/[base] ratio of 2.0. The i-motif-stabilized Pd sub(8)-Pd sub(9) clusters show high catalytic activity toward the reduction of 4-nitrophenol with a relative rate constant value of 2034 min super(-1) (mM Pd) super(-1). DFT calculations disclose that the unique structure of the i-motif with consecutive hemiprotonated CH super(+).C pairs can efficiently ligate Pd ions at the N3 sites of cytosines and that the synthesized Pd clusters consist of metallic Pd atoms as well as positively charged Pd that is ligated by nucleobases, which is capable of facilitating the activation of the nitryl group of 4-nitrophenol. This work suggests a promising pathway to preparing subnano metal catalysts with enhanced catalytic activity using programmable DNA scaffolds.
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abstractHighly active subnano Pd clusters were synthesized using i-motif DNA as the template through characterization via ESI MS, DLS, XPS, UV-vis, and FTIR. It is indicated that Pd sub(1)-Pd sub(5) clusters are generated at a [Pd]/[base] ratio of 0.2, Pd sub(8) to Pd sub(9) clusters are generated at a [Pd]/[base] ratio of 0.5, and large nanoparticles with the size about 2.6 nm are formed at a [Pd]/[base] ratio of 2.0. The i-motif-stabilized Pd sub(8)-Pd sub(9) clusters show high catalytic activity toward the reduction of 4-nitrophenol with a relative rate constant value of 2034 min super(-1) (mM Pd) super(-1). DFT calculations disclose that the unique structure of the i-motif with consecutive hemiprotonated CH super(+).C pairs can efficiently ligate Pd ions at the N3 sites of cytosines and that the synthesized Pd clusters consist of metallic Pd atoms as well as positively charged Pd that is ligated by nucleobases, which is capable of facilitating the activation of the nitryl group of 4-nitrophenol. This work suggests a promising pathway to preparing subnano metal catalysts with enhanced catalytic activity using programmable DNA scaffolds.
doi10.1021/la402153b
urlhttp://search.proquest.com/docview/1534830251/
date2013-11-26