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01.12.2009

From Ultrafine Thiolate-Capped Copper Nanoclusters toward Copper Sulfide Nanodiscs: A Thermally Activated Evolution Route





  • Derrick Mott, Jun Yin, Mark Engelhard, Rameshwori Loukrakpam, Paul Chang, George Miller§, In-Tae Bae, Narayan Chandra Das, Chongmin Wang, Jin Luo and Chuan-Jian Zhong*




    Department of Chemistry, State University of New York at Binghamton, Binghamton, New York 13902

    Environmental and Molecular Sciences Laboratory, Pacific Northwest National Laboratory, Richland, Washington 99352

    § AFRL/RHPG, Brooks City-Base, San Antonio, Texas

     SIP Analytical and Diagnostics Laboratory, State University of New York at Binghamton, Binghamton, New York 13902


    Chem. Mater., Article ASAP

    DOI: 10.1021/cm903038w

    Publication Date (Web): November 30, 2009

    Copyright © 2009 American Chemical Society

    *To whom correspondence should be addressed. E-mail: cjzhong@binghamton.edu.




    Abstract



     

    This report shows that the size, shape, and composition of presynthesized copper nanoparticles can be nanoengineered through exploiting concurrent interparticle aggregative growth and interfacial carbon−sulfur cleavage in a thermally activated evolution route. This is demonstrated by thermally activated processing of ultrafine copper nanoclusters encapsulated with thiolate monolayer (Cun(SR)m) toward semiconducting copper sulfide (Cu2S) nanodiscs with controllable sizes and shapes. Under controlled temperatures (120−150 °C), the ultrafine Cun(SR)m nanoclusters, with a size of 0.5 nm evidenced by TEM, SAXS-WAXS, DCP-AES, and MALDI-TOF measurements, were shown to evolve into thiolate-capped Cu2S nanodiscs via thermally activated coalescence and copper-catalyzed interfacial C−S cleavage reactivities. The Cu2S nanodiscs, as confirmed by XPS and HRTEM analyses, exhibited controllable and monodispersed sizes depending on the thermal processing parameters, ranging from 5 to 35 nm in the disk dimension and 3−6 nm in the thickness dimension. These nanodiscs are stable and display remarkable 1D/2D ordering upon self-assembly. This process is not a simple digestive ripening of smaller particles because it involves an aggregative nucleation and growth process distinctively different from traditional ripening and a reactive carbon−sulfur bond cleavage controlled by the catalytic effect of copper under the specified temperatures. The coupling of the thermally activated coalescence and C−S bond cleavage to convert the ultrafine Cu nanoclusters toward the formation of Cu2S nanodiscs is highly effective for tuning nanoscale size, shape, and composition, and could find applications in nanoengineering a variety of semiconducting nanocrystals for applications in nanostructured electronic, sensing, and photochemical devices.




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  • Chen Wev .  honorary member of ISSC science council

  • Harton Vladislav Vadim  honorary member of ISSC science council

  • Lichtenstain Alexandr Iosif  honorary member of ISSC science council

  • Novikov Dimirtii Leonid  honorary member of ISSC science council

  • Yakushev Mikhail Vasilii  honorary member of ISSC science council

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