Overcoming immiscibility toward bimetallic catalyst library
A general nonequilibrium synthesis strategy is reported to address the bimetallic immiscibility challenge for catalysis. Bimetallics are emerging as important materials that often exhibit distinct chemical properties from monometallics. However, there is limited access to homogeneously alloyed bimet...
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| Published in | Science advances Vol. 6; no. 17; p. eaaz6844 |
|---|---|
| Main Authors | , , , , , , , , , , , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
United States
AAAS
24.04.2020
American Association for the Advancement of Science |
| Subjects | |
| Online Access | Get full text |
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| Abstract | A general nonequilibrium synthesis strategy is reported to address the bimetallic immiscibility challenge for catalysis.
Bimetallics are emerging as important materials that often exhibit distinct chemical properties from monometallics. However, there is limited access to homogeneously alloyed bimetallics because of the thermodynamic immiscibility of the constituent elements. Overcoming the inherent immiscibility in bimetallic systems would create a bimetallic library with unique properties. Here, we present a nonequilibrium synthesis strategy to address the immiscibility challenge in bimetallics. As a proof of concept, we synthesize a broad range of homogeneously alloyed Cu-based bimetallic nanoparticles regardless of the thermodynamic immiscibility. The nonequilibrated bimetallic nanoparticles are further investigated as electrocatalysts for carbon monoxide reduction at commercially relevant current densities (>100 mA cm
−2
), in which Cu
0.9
Ni
0.1
shows the highest multicarbon product Faradaic efficiency of ~76% with a current density of ~93 mA cm
−2
. The ability to overcome thermodynamic immiscibility in multimetallic synthesis offers freedom to design and synthesize new functional nanomaterials with desired chemical compositions and catalytic properties. |
|---|---|
| AbstractList | A general nonequilibrium synthesis strategy is reported to address the bimetallic immiscibility challenge for catalysis.
Bimetallics are emerging as important materials that often exhibit distinct chemical properties from monometallics. However, there is limited access to homogeneously alloyed bimetallics because of the thermodynamic immiscibility of the constituent elements. Overcoming the inherent immiscibility in bimetallic systems would create a bimetallic library with unique properties. Here, we present a nonequilibrium synthesis strategy to address the immiscibility challenge in bimetallics. As a proof of concept, we synthesize a broad range of homogeneously alloyed Cu-based bimetallic nanoparticles regardless of the thermodynamic immiscibility. The nonequilibrated bimetallic nanoparticles are further investigated as electrocatalysts for carbon monoxide reduction at commercially relevant current densities (>100 mA cm
−2
), in which Cu
0.9
Ni
0.1
shows the highest multicarbon product Faradaic efficiency of ~76% with a current density of ~93 mA cm
−2
. The ability to overcome thermodynamic immiscibility in multimetallic synthesis offers freedom to design and synthesize new functional nanomaterials with desired chemical compositions and catalytic properties. Bimetallics are emerging as important materials that often exhibit distinct chemical properties from monometallics. However, there is limited access to homogeneously alloyed bimetallics because of the thermodynamic immiscibility of the constituent elements. Overcoming the inherent immiscibility in bimetallic systems would create a bimetallic library with unique properties. Here, we present a nonequilibrium synthesis strategy to address the immiscibility challenge in bimetallics. As a proof of concept, we synthesize a broad range of homogeneously alloyed Cu-based bimetallic nanoparticles regardless of the thermodynamic immiscibility. The nonequilibrated bimetallic nanoparticles are further investigated as electrocatalysts for carbon monoxide reduction at commercially relevant current densities (>100 mA cm-2), in which Cu0.9Ni0.1 shows the highest multicarbon product Faradaic efficiency of ~76% with a current density of ~93 mA cm-2. The ability to overcome thermodynamic immiscibility in multimetallic synthesis offers freedom to design and synthesize new functional nanomaterials with desired chemical compositions and catalytic properties.Bimetallics are emerging as important materials that often exhibit distinct chemical properties from monometallics. However, there is limited access to homogeneously alloyed bimetallics because of the thermodynamic immiscibility of the constituent elements. Overcoming the inherent immiscibility in bimetallic systems would create a bimetallic library with unique properties. Here, we present a nonequilibrium synthesis strategy to address the immiscibility challenge in bimetallics. As a proof of concept, we synthesize a broad range of homogeneously alloyed Cu-based bimetallic nanoparticles regardless of the thermodynamic immiscibility. The nonequilibrated bimetallic nanoparticles are further investigated as electrocatalysts for carbon monoxide reduction at commercially relevant current densities (>100 mA cm-2), in which Cu0.9Ni0.1 shows the highest multicarbon product Faradaic efficiency of ~76% with a current density of ~93 mA cm-2. The ability to overcome thermodynamic immiscibility in multimetallic synthesis offers freedom to design and synthesize new functional nanomaterials with desired chemical compositions and catalytic properties. Bimetallics are emerging as important materials that often exhibit distinct chemical properties from monometallics. However, there is limited access to homogeneously alloyed bimetallics because of the thermodynamic immiscibility of the constituent elements. Overcoming the inherent immiscibility in bimetallic systems would create a bimetallic library with unique properties. Here, we present a nonequilibrium synthesis strategy to address the immiscibility challenge in bimetallics. As a proof of concept, we synthesize a broad range of homogeneously alloyed Cu-based bimetallic nanoparticles regardless of the thermodynamic immiscibility. The nonequilibrated bimetallic nanoparticles are further investigated as electrocatalysts for carbon monoxide reduction at commercially relevant current densities (>100 mA cm-2), in which Cu0.9Ni0.1shows the highest multicarbon product Faradaic efficiency of ~76% with a current density of ~93 mA cm-2. The ability to overcome thermodynamic immiscibility in multimetallic synthesis offers freedom to design and synthesize new functional nanomaterials with desired chemical compositions and catalytic properties. |
| Author | Wang, Xizheng Hu, Liangbing Ko, Byung Hee Yang, Chunpeng Dai, Jiaqi Hwang, Sooyeon Su, Dong Luc, Wesley Malkani, Arnav S. Xu, Bingjun Li, Tangyuan Jiao, Feng Cui, Mingjin Liu, Zhenyu Wang, Guofeng Yao, Yonggang |
| Author_xml | – sequence: 1 givenname: Chunpeng orcidid: 0000-0001-7075-3356 surname: Yang fullname: Yang, Chunpeng organization: Department of Materials Science and Engineering, University of Maryland, College Park, MD 20742, USA – sequence: 2 givenname: Byung Hee orcidid: 0000-0002-0934-5182 surname: Ko fullname: Ko, Byung Hee organization: Center for Catalytic Science and Technology, Department of Chemical and Biomolecular Engineering, University of Delaware, Newark, DE 19716, USA – sequence: 3 givenname: Sooyeon orcidid: 0000-0001-5606-6728 surname: Hwang fullname: Hwang, Sooyeon organization: Center for Functional Nanomaterials, Brookhaven National Laboratory, Upton, NY 11973, USA – sequence: 4 givenname: Zhenyu orcidid: 0000-0003-2893-5396 surname: Liu fullname: Liu, Zhenyu organization: Department of Mechanical Engineering and Materials Science, University of Pittsburgh, Pittsburgh, PA 15261, USA – sequence: 5 givenname: Yonggang orcidid: 0000-0002-9191-2982 surname: Yao fullname: Yao, Yonggang organization: Department of Materials Science and Engineering, University of Maryland, College Park, MD 20742, USA – sequence: 6 givenname: Wesley surname: Luc fullname: Luc, Wesley organization: Center for Catalytic Science and Technology, Department of Chemical and Biomolecular Engineering, University of Delaware, Newark, DE 19716, USA – sequence: 7 givenname: Mingjin orcidid: 0000-0002-9254-0949 surname: Cui fullname: Cui, Mingjin organization: Department of Materials Science and Engineering, University of Maryland, College Park, MD 20742, USA – sequence: 8 givenname: Arnav S. orcidid: 0000-0002-5984-3382 surname: Malkani fullname: Malkani, Arnav S. organization: Center for Catalytic Science and Technology, Department of Chemical and Biomolecular Engineering, University of Delaware, Newark, DE 19716, USA – sequence: 9 givenname: Tangyuan surname: Li fullname: Li, Tangyuan organization: Department of Materials Science and Engineering, University of Maryland, College Park, MD 20742, USA – sequence: 10 givenname: Xizheng surname: Wang fullname: Wang, Xizheng organization: Department of Materials Science and Engineering, University of Maryland, College Park, MD 20742, USA – sequence: 11 givenname: Jiaqi surname: Dai fullname: Dai, Jiaqi organization: Department of Materials Science and Engineering, University of Maryland, College Park, MD 20742, USA – sequence: 12 givenname: Bingjun orcidid: 0000-0002-2303-257X surname: Xu fullname: Xu, Bingjun organization: Center for Catalytic Science and Technology, Department of Chemical and Biomolecular Engineering, University of Delaware, Newark, DE 19716, USA – sequence: 13 givenname: Guofeng orcidid: 0000-0001-8249-4101 surname: Wang fullname: Wang, Guofeng organization: Department of Mechanical Engineering and Materials Science, University of Pittsburgh, Pittsburgh, PA 15261, USA – sequence: 14 givenname: Dong orcidid: 0000-0002-1921-6683 surname: Su fullname: Su, Dong organization: Center for Functional Nanomaterials, Brookhaven National Laboratory, Upton, NY 11973, USA – sequence: 15 givenname: Feng orcidid: 0000-0002-3335-3203 surname: Jiao fullname: Jiao, Feng organization: Center for Catalytic Science and Technology, Department of Chemical and Biomolecular Engineering, University of Delaware, Newark, DE 19716, USA – sequence: 16 givenname: Liangbing orcidid: 0000-0002-9456-9315 surname: Hu fullname: Hu, Liangbing organization: Department of Materials Science and Engineering, University of Maryland, College Park, MD 20742, USA |
| BackLink | https://www.osti.gov/servlets/purl/1619249$$D View this record in Osti.gov |
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| Copyright | Copyright © 2020 The Authors, some rights reserved; exclusive licensee American Association for the Advancement of Science. No claim to original U.S. Government Works. Distributed under a Creative Commons Attribution NonCommercial License 4.0 (CC BY-NC). Copyright © 2020 The Authors, some rights reserved; exclusive licensee American Association for the Advancement of Science. No claim to original U.S. Government Works. Distributed under a Creative Commons Attribution NonCommercial License 4.0 (CC BY-NC). 2020 The Authors |
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| Snippet | A general nonequilibrium synthesis strategy is reported to address the bimetallic immiscibility challenge for catalysis.
Bimetallics are emerging as important... Bimetallics are emerging as important materials that often exhibit distinct chemical properties from monometallics. However, there is limited access to... |
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| Title | Overcoming immiscibility toward bimetallic catalyst library |
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