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

Journal Article · 06 November 2019 · Social Science Research Network (SSRN)

DOI: https://doi.org/10.2139/ssrn.3372970 · OSTI ID:1658000

Rajeeva, Bharath Bangalore ^[1]; Kunal, Pranaw ^[2]; Kollipara, Pavana Siddhartha ^[3]; Acharya, Palash V. ^[3]; Joe, Minwoong ^[4]; Ide, Matthew S. ^[5]; Jarvis, Karalee ^[1]; Liu, Yuanyue ^[6]; Bahadur, Vaibhav ^[3]; Humphrey, Simon M. ^[3]; Zheng, Yuebing ^[6]

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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)

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.

• Research Organization: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
• Sponsoring Organization: USDOE; 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)
• Grant/Contract Number: AC05-00OR22725; CMMI-1761743; UTA17-000828; 80NSSC17K0520; CHE-1807847; 2016R1A6A3A11934734
• OSTI ID: 1658000
• Journal Information: Social Science Research Network (SSRN), Vol. 1, Issue 6; ISSN 1556-5068
• Publisher: ElsevierCopyright Statement
• Country of Publication: United States
• Language: English