Skip to main content Accessibility help

We use cookies to distinguish you from other users and to provide you with a better experience on our websites. Close this message to accept cookies or find out how to manage your cookie settings.

Close cookie message
×
Home
Hostname: page-component-768dbb666b-6zkrn Total loading time: 0.336 Render date: 2023-02-05T20:41:59.075Z Has data issue: true Feature Flags: { "useRatesEcommerce": false } hasContentIssue true
  • English
Microscopy and Microanalysis Microscopy and Microanalysis

Article contents

Unique Structural Characteristics of Catalytic Palladium/Gold Nanoparticles on Graphene

Published online by Cambridge University Press:  30 January 2019

Kavita Meduri Open the ORCID record for Kavita Meduri[Opens in a new window] ,
Candice Stauffer ,
Graham O'Brien Johnson ,
Paolo Longo ,
Paul G. Tratnyek  and
Jun Jiao
Kavita Meduri
Affiliation:
Department of Mechanical & Materials Engineering, Portland State University, Portland, OR 97207USA
Candice Stauffer
Affiliation:
Department of Physics, Portland State University, Portland, OR 97207USA
Graham O'Brien Johnson
Affiliation:
School of Public Health Oregon Health & Science University, Portland, OR 97239, USA
Paolo Longo
Affiliation:
Gatan Inc, Pleasanton, CA 94566, USA
Paul G. Tratnyek
Affiliation:
School of Public Health Oregon Health & Science University, Portland, OR 97239, USA
Jun Jiao*
Affiliation:
Department of Mechanical & Materials Engineering, Portland State University, Portland, OR 97207USA Department of Physics, Portland State University, Portland, OR 97207USA
*
*Author for correspondence: Jun Jiao, E-mail: jiaoj@pdx.edu
Get access

Abstract

Adding Au to Pd nanoparticles (NPs) can impart high catalytic activity with respect to hydrogenation of a wide range of substances. These materials are often synthesized by reducing metallic precursors; hence, sonochemical and solvothermal processes are commonly used to anchor these bimetals onto thin supports, including graphene. Although similar NPs have been studied reasonably well, a clear understanding of structural characteristics relative to their synthesis parameters is lacking, due to limitations in characterization techniques, which may prevent optimization of this very promising catalyst. In this report, a strategic approach has been used to identify this structural and material synthesis correlation, starting with controlled sample preparation and followed by detailed characterization. This includes advanced scanning transmission electron microscopy and electron energy loss spectroscopy; the latter using a state-of-the-art instrumentation to map the distribution of Pd and Au, and to identify chemical state of the Pd NPs, which has not been previously reported. Results show that catalytic bimetal NP clusters were made of small zero-valent Pd NPs aggregating to form a shell around an Au core. Not only can the described characterization approach be applied to similar material systems, but the results can guide the optimization of the synthesis procedures.

Keywords

bimetal core–shell nanoparticlesdirect detectionEDSEELSelectron microscopygold and graphenepalladiumSEMTEM
Type
Materials Science Applications
Information
Microscopy and Microanalysis , Volume 25 , Issue 1 , February 2019 , pp. 80 - 91
Copyright
Copyright © Microscopy Society of America 2019 

Access options

Get access to the full version of this content by using one of the access options below. (Log in options will check for institutional or personal access. Content may require purchase if you do not have access.)

References

Akita, T, Hase, N, Taguchi, N, Tanaka, S, Kohyama, M & Hori, F (2008). Analytical TEM study of the core-shell structure of Au-Pd nano-particles prepared by sonochemical technique. J Phys Conf Ser 100, 1–4.CrossRefGoogle Scholar
Bang, JH & Suslick, KS (2010). Applications of ultrasound to the synthesis of nanostructured materials. Adv Mater 22, 1039–1059.CrossRefGoogle ScholarPubMed
Caruso, RA, Ashokkumar, M & Grieser, F (2002). Sonochemical formation of gold sols. Langmuir 18, 7831–7836.CrossRefGoogle Scholar
Chaplin, BP, Reinhard, M, Schneider, WF, Schu, C, Shapley, JR, Strathmann, TJ & Werth, CJ (2012). Critical review of Pd-based catalytic treatment of priority contaminants in water. Environ Sci Technol 46, 3655–3670.CrossRefGoogle ScholarPubMed
Demazeau, G (2010). Solvothermal processes: Definition, Key factors governing the involved chemical reactions and new trends. Zeitschrift fur Naturforschung - Section B J Chem. Sci. 65, 999–1006.CrossRefGoogle Scholar
Edwards, JK, Solsona, BE, Landon, P, Carley, AF, Herzing, A, Kiely, CJ & Hutchings, GJ (2005). Direct synthesis of hydrogen peroxide from H2 and O2 using TiO2-supported Au-Pd catalysts. J Catal 236, 69–79.CrossRefGoogle Scholar
Edwards, JK, Thomas, A, Carley, AF, Herzing, AA, Kiely, CJ & Hutchings, GJ (2008). Au–Pd supported nanocrystals as catalysts for the direct synthesis of hydrogen peroxide from H2 and O2. Green Chem 10, 388.CrossRefGoogle Scholar
Enache, DI, Edwards, JK, Landon, P, Solsona-Espriu, B, Carley, AF, Herzing, AA, Watanabe, M, Kiely, CJ, Knight, DW & Hutchings, GJ (2006). Solvent-free oxidation of primary alcohols to aldehydes using. Science 311, 362–366.CrossRefGoogle Scholar
Ferrando, R, Jellinek, J & Johnston, RL (2008). Nanoalloys: From theory to applications of alloy clusters and nanoparticles. Chem Rev 108, 845–910.CrossRefGoogle ScholarPubMed
Gersten, B (2004). Solvothermal synthesis of nanoparticles. Chemfiles 5. https://www.sigmaaldrich.com/content/dam/sigma-aldrich/articles/chemfiles/volume5a13/Solvothermal_Synthesis_of_Nanoparticles.pdf (accessed July 9, 2018).Google Scholar
Hart, JL, Lang, AC, Leff, AC, Longo, P, Trevor, C, Twesten, RD & Taheri, ML (2017). Direct detection electron energy-loss spectroscopy: A method to push the limits of resolution and sensitivity. Sci Rep 7, 1–14.CrossRefGoogle ScholarPubMed
Huang, Y, Ferhan, AR, Dandapat, A, Yoon, CS, Song, JE, Cho, EC & Kim, D (2015). A strategy for the formation of gold–palladium supra-nanoparticles from gold nanoparticles of various shapes and their application to high-performance H2O2 sensing. J Phys Chem C 119, 26164–26170.CrossRefGoogle Scholar
Ji, W, Zhang, C, Li, F, Li, P, Wang, P, Ren, M & Yuan, M (2014). First-principles study of small Pd–Au alloy clusters on graphene. RSC Adv 4, 55781–55789.CrossRefGoogle Scholar
Lee, AF, Baddeley, CJ, Hardacre, C, Ormerod, RM, Lambert, RM, Schmid, G & West, H (1995). Structural and catalytic properties of novel Au/Pd bimetallic colloid particles: EXAFS, XRD, and acetylene coupling. J Phys Chem 99, 6096–6102.CrossRefGoogle Scholar
Li, S, Fang, YL, Romanczuk, CD, Jin, Z, Li, T & Wong, MS (2012). Establishing the trichloroethene dechlorination rates of palladium-based catalysts and iron-based reductants. Appl Catal B 125, 95–102.CrossRefGoogle Scholar
Lim, B, Kobayashi, H, Yu, T, Wang, J, Kim, MJ, Li, ZY, Rycenga, M & Xia, Y (2010). Synthesis of pd-au bimetallic nanocrystals via controlled overgrowth. J Am Chem Soc 132, 2506–2507.CrossRefGoogle ScholarPubMed
Liu, HB, Pal, U, Medina, A, Maldonado, C & Ascencio, JA (2005). Structural incoherency and structure reversal in bimetallic Au-Pd nanoclusters. Phys Rev B Condensed Matter Mater Phys 71, 075403–1–075403-6.Google Scholar
Meduri, K, Barnum, A, Johnson, GOB, Tratnyek, PG & Jiao, J (2016). Characterization of palladium and gold nanoparticles on granular activated carbon as an efficient catalyst for hydrodechlorination of trichloroethylene. Microsc Microanal 22, 332–333.CrossRefGoogle Scholar
Meduri, K, Stauffer, C, Lindner, T, Johnson, GOB, Tratnyek, PG & Jiao, J (2017). Effect of synthesis temperature on the formation GAC supported Pd and Au NPs. Microsc Microanal 23, 1916–1917.CrossRefGoogle Scholar
Meduri, K, Stauffer, C, Qian, W, Zietz, O, Barnum, A, O'brien Johnson, G, Fan, D, Ji, W, Zhang, C, Tratnyek, P & Jiao, J (2018). Palladium and gold nanoparticles on carbon supports as highly efficient catalysts for effective removal of trichloroethylene. J Mater Res 33, 2404–2413.CrossRefGoogle Scholar
Mizukoshi, Y, Fujimoto, T, Nagata, Y, Oshima, R & Maeda, Y (2000). Characterization and catalytic activity of core−shell structured gold/palladium bimetallic nanoparticles synthesized by the sonochemical method. J Phys Chem B 104, 6028–6032.CrossRefGoogle Scholar
Mizukoshi, Y, Okitsu, K, Maeda, Y, Yamamoto, TA, Oshima, R & Nagata, Y (1997). Sonochemical preparation of bimetallic nanoparticles of gold/palladium in aqueous solution. J Phys Chem B 101, 7033–7037.CrossRefGoogle Scholar
Nagata, Y, Mizukoshi, Y, Okitsu, K & Maeda, Y (1996). Sonochemical formation of gold particles in aqueous solution. Radiat Res 146, 333–338.CrossRefGoogle ScholarPubMed
Nutt, MO, Hughes, JB & Wong, MS (2005). Designing Pd-on-Au bimetallic nanoparticle catalysts for trichloroethene hydrodechlorination. Environ Sci Technol 39, 1346–1353.CrossRefGoogle ScholarPubMed
Okitsu, K, Mizukoshi, Y, Bandow, H, Yamamoto, TA, Nagata, Y & Maeda, Y (1997). Synthesis of palladium nanoparticles with interstitial carbon by sonochemical reduction of tetrachloropalladate(II) in aqueous solution. J Phys Chem B 101, 5470–5472.CrossRefGoogle Scholar
Qian, H, Zhao, Z, Velazquez, JC, Pretzer, LA, Heck, KN & Wong, MS (2014). Supporting palladium metal on gold nanoparticles improves its catalysis for nitrite reduction. Nanoscale 6, 358–364.CrossRefGoogle Scholar
Riesz, P, Berdahi, D & Christman, CL (1985). Free radical generation by ultrasound in aqueous and nonaqueous solutions. Environ Health Perspect 64, 233–252.CrossRefGoogle ScholarPubMed
Schmid, G, Maihack, V, Lantermann, F & Peschel, S (1996). Ligand-stabilized metal clusters and colloids: Properties and applications. J Chem Soc, Dalton Trans 0, 589–595.CrossRefGoogle Scholar
Shi, L, Wang, A, Zhang, T, Zhang, B, Su, D, Li, H & Song, Y (2013). One-step synthesis of Au-pd alloy nanodendrites and their catalytic activity. J Phys Chem C 117, 12526–12536.CrossRefGoogle Scholar
Tauber, A, Mark, G, Schuchmann, H & Sonntag, C (1999). Sonolysis of tert-butyl alcohol in aqueous solution. J Chem Soc Perkin Trans 2 0, 1129–1135.CrossRefGoogle Scholar
Zhang, K, Shen, M, Liu, H, Shang, S, Wang, D & Liimatainen, H (2018). Facile synthesis of palladium and gold nanoparticles by using dialdehyde nanocellulose as template and reducing agent. Carbohydr Polym 186, 132–139.CrossRefGoogle ScholarPubMed

Save article to Kindle

To save this article to your Kindle, first ensure coreplatform@cambridge.org is added to your Approved Personal Document E-mail List under your Personal Document Settings on the Manage Your Content and Devices page of your Amazon account. Then enter the ‘name’ part of your Kindle email address below. Find out more about saving to your Kindle.

Note you can select to save to either the @free.kindle.com or @kindle.com variations. ‘@free.kindle.com’ emails are free but can only be saved to your device when it is connected to wi-fi. ‘@kindle.com’ emails can be delivered even when you are not connected to wi-fi, but note that service fees apply.

Find out more about the Kindle Personal Document Service.

Unique Structural Characteristics of Catalytic Palladium/Gold Nanoparticles on Graphene
Available formats
×

Save article to Dropbox

To save this article to your Dropbox account, please select one or more formats and confirm that you agree to abide by our usage policies. If this is the first time you used this feature, you will be asked to authorise Cambridge Core to connect with your Dropbox account. Find out more about saving content to Dropbox.

Unique Structural Characteristics of Catalytic Palladium/Gold Nanoparticles on Graphene
Available formats
×

Save article to Google Drive

To save this article to your Google Drive account, please select one or more formats and confirm that you agree to abide by our usage policies. If this is the first time you used this feature, you will be asked to authorise Cambridge Core to connect with your Google Drive account. Find out more about saving content to Google Drive.

Unique Structural Characteristics of Catalytic Palladium/Gold Nanoparticles on Graphene
Available formats
×
×

Reply to: Submit a response

Please enter your response.

Your details

Please enter a valid email address.

Conflicting interests

Do you have any conflicting interests? *