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Title: Accumulation-Driven Surfactant-Free Synthesis of Architectured Immiscible Metallic Nanoalloys with Enhanced Catalysis

Abstract

Accumulation-mediated chemical reactions are a ubiquitous phenomenon in nature. In this work, we explore microbubble-induced accumulation of precursor ions to achieve surfactant-free synthesis of immiscible metallic nanoalloys and simultaneously pattern the nanoalloys into targeted architectures for their enhanced catalytic applications. Additionally, our unified spatiotemporal synthesis and structuring (US3) strategy, whereby millisecond-scale accumulation of the ions takes place in a highly confined laser-mediated microbubble trap (MBT), drives ultrafast alloy synthesis in sync with the structuring process. As a case in point, we employ the US3 strategy for the in situ surfactant-free synthesis and patterning of traditionally immiscible rhodium-gold (RhAu) nanoalloys. Stochastic random walk simulations justify the millisecond-scale accumulation process, leading to a 3-order reduction in synthesis time. The catalytic activity and structure-property relationship were evaluated using the reduction of p-nitrophenol with NaBH4. Our in situ synthesis and structuring strategy can be translated for high-throughput production and screening of multimetallic systems with tailored catalytic, optoelectronic, and magnetic functions.

Authors:
 [1];  [2];  [3];  [3];  [4];  [5];  [1];  [6];  [3];  [3];  [6]
  1. Univ. of Texas, Austin, TX (United States). Texas Materials Inst.
  2. Univ. of Texas, Austin, TX (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  3. Univ. of Texas, Austin, TX (United States)
  4. Univ. of Texas, Austin, TX (United States). Texas Materials Inst.; Sungkyunkwan Univ., Suwon (South Korea)
  5. ExxonMobil Research and Engineering Co., Annandale, NJ (United States)
  6. Univ. of Texas, Austin, TX (United States). Texas Materials Inst.; Univ. of Texas, Austin, TX (United States)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE); National Science Foundation (NSF); National Aeronautics and Space Administration (NASA); National Research Foundation of Korea (NRF)
OSTI Identifier:
1658000
Grant/Contract Number:  
AC05-00OR22725; CMMI-1761743; UTA17-000828; 80NSSC17K0520; CHE-1807847; 2016R1A6A3A11934734
Resource Type:
Accepted Manuscript
Journal Name:
Social Science Research Network (SSRN)
Additional Journal Information:
Journal Name: Social Science Research Network (SSRN); Journal Volume: 1; Journal Issue: 6; Journal ID: ISSN 1556-5068
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Rajeeva, Bharath Bangalore, Kunal, Pranaw, Kollipara, Pavana Siddhartha, Acharya, Palash V., Joe, Minwoong, Ide, Matthew S., Jarvis, Karalee, Liu, Yuanyue, Bahadur, Vaibhav, Humphrey, Simon M., and Zheng, Yuebing. Accumulation-Driven Surfactant-Free Synthesis of Architectured Immiscible Metallic Nanoalloys with Enhanced Catalysis. United States: N. p., 2019. Web. https://doi.org/10.2139/ssrn.3372970.
Rajeeva, Bharath Bangalore, Kunal, Pranaw, Kollipara, Pavana Siddhartha, Acharya, Palash V., Joe, Minwoong, Ide, Matthew S., Jarvis, Karalee, Liu, Yuanyue, Bahadur, Vaibhav, Humphrey, Simon M., & Zheng, Yuebing. Accumulation-Driven Surfactant-Free Synthesis of Architectured Immiscible Metallic Nanoalloys with Enhanced Catalysis. United States. https://doi.org/10.2139/ssrn.3372970
Rajeeva, Bharath Bangalore, Kunal, Pranaw, Kollipara, Pavana Siddhartha, Acharya, Palash V., Joe, Minwoong, Ide, Matthew S., Jarvis, Karalee, Liu, Yuanyue, Bahadur, Vaibhav, Humphrey, Simon M., and Zheng, Yuebing. Wed . "Accumulation-Driven Surfactant-Free Synthesis of Architectured Immiscible Metallic Nanoalloys with Enhanced Catalysis". United States. https://doi.org/10.2139/ssrn.3372970. https://www.osti.gov/servlets/purl/1658000.
@article{osti_1658000,
title = {Accumulation-Driven Surfactant-Free Synthesis of Architectured Immiscible Metallic Nanoalloys with Enhanced Catalysis},
author = {Rajeeva, Bharath Bangalore and Kunal, Pranaw and Kollipara, Pavana Siddhartha and Acharya, Palash V. and Joe, Minwoong and Ide, Matthew S. and Jarvis, Karalee and Liu, Yuanyue and Bahadur, Vaibhav and Humphrey, Simon M. and Zheng, Yuebing},
abstractNote = {Accumulation-mediated chemical reactions are a ubiquitous phenomenon in nature. In this work, we explore microbubble-induced accumulation of precursor ions to achieve surfactant-free synthesis of immiscible metallic nanoalloys and simultaneously pattern the nanoalloys into targeted architectures for their enhanced catalytic applications. Additionally, our unified spatiotemporal synthesis and structuring (US3) strategy, whereby millisecond-scale accumulation of the ions takes place in a highly confined laser-mediated microbubble trap (MBT), drives ultrafast alloy synthesis in sync with the structuring process. As a case in point, we employ the US3 strategy for the in situ surfactant-free synthesis and patterning of traditionally immiscible rhodium-gold (RhAu) nanoalloys. Stochastic random walk simulations justify the millisecond-scale accumulation process, leading to a 3-order reduction in synthesis time. The catalytic activity and structure-property relationship were evaluated using the reduction of p-nitrophenol with NaBH4. Our in situ synthesis and structuring strategy can be translated for high-throughput production and screening of multimetallic systems with tailored catalytic, optoelectronic, and magnetic functions.},
doi = {10.2139/ssrn.3372970},
journal = {Social Science Research Network (SSRN)},
number = 6,
volume = 1,
place = {United States},
year = {2019},
month = {11}
}

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