Highly Crystalline Multimetallic Nanoframes with Three-Dimensional Electrocatalytic Surfaces
Control of structure at the atomic level can precisely and effectively tune catalytic properties of materials, enabling enhancement in both activity and durability. We synthesized a highly active and durable class of electrocatalysts by exploiting the structural evolution of platinum-nickel (Pt-Ni)...
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| Published in | Science (American Association for the Advancement of Science) Vol. 343; no. 6177; pp. 1339 - 1343 |
|---|---|
| Main Authors | , , , , , , , , , , , , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
United States
American Association for the Advancement of Science
21.03.2014
The American Association for the Advancement of Science AAAS |
| Subjects | |
| Online Access | Get full text |
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| Abstract | Control of structure at the atomic level can precisely and effectively tune catalytic properties of materials, enabling enhancement in both activity and durability. We synthesized a highly active and durable class of electrocatalysts by exploiting the structural evolution of platinum-nickel (Pt-Ni) bimetallic nanocrystals. The starting material, crystalline PtNi3 polyhedra, transforms in solution by interior erosion into Pt3Ni nanoframes with surfaces that offer three-dimensional molecular accessibility. The edges of the Pt-rich PtNi3 polyhedra are maintained in the final Pt3Ni nanoframes. Both the interior and exterior catalytic surfaces of this open-framework structure are composed of the nanosegregated Pt-skin structure, which exhibits enhanced oxygen reduction reaction (ORR) activity. The Pt3Ni nanoframe catalysts achieved a factor of 36 enhancement in mass activity and a factor of 22 enhancement in specific activity, respectively, for this reaction (relative to state-of-the-art platinum-carbon catalysts) during prolonged exposure to reaction conditions. |
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| AbstractList | Giving Electrocatalysts an Edge Platinum (Pt) is an excellent catalyst for the oxygen-reduction reaction (ORR) in fuel cells and electrolyzers, but it is too expensive and scarce for widespread deployment, even when dispersed as Pt nanoparticles on carbon electrode supports (Pt/C). Alternatively, Chen et al. (p. 1339, published online 27 February; see the Perspective by Greer) made highly active ORR catalysts by dissolving away the interior of rhombic dodecahedral PtNi ₃ nanocrystals to leave Pt-rich Pt ₃Ni edges. These nanoframe catalysts are durable—remaining active after 10,000 rounds of voltage cycling—and are far more active than Pt/C. Platinum (Pt) is an excellent catalyst for the oxygen-reduction reaction (ORR) in fuel cells and electrolyzers, but it is too expensive and scarce for widespread deployment, even when dispersed as Pt nanoparticles on carbon electrode supports (Pt/C). Alternatively, Chen et al. (p. 1339, published online 27 February; see the Perspective by Greer) made highly active ORR catalysts by dissolving away the interior of rhombic dodecahedral PtNi3 nanocrystals to leave Pt-rich Pt3Ni edges. These nanoframe catalysts are durable--remaining active after 10,000 rounds of voltage cycling--and are far more active than Pt/C. [PUBLICATION ABSTRACT] Control of structure at the atomic level can precisely and effectively tune catalytic properties of materials, enabling enhancement in both activity and durability. We synthesized a highly active and durable class of electrocatalysts by exploiting the structural evolution of platinum-nickel (Pt-Ni) bimetallic nanocrystals. The starting material, crystalline PtNi3 polyhedra, transforms in solution by interior erosion into Pt3Ni nanoframes with surfaces that offer three-dimensional molecular accessibility. The edges of the Pt-rich PtNi3 polyhedra are maintained in the final Pt3Ni nanoframes. Both the interior and exterior catalytic surfaces of this open-framework structure are composed of the nanosegregated Pt-skin structure, which exhibits enhanced oxygen reduction reaction (ORR) activity. The Pt3Ni nanoframe catalysts achieved a factor of 36 enhancement in mass activity and a factor of 22 enhancement in specific activity, respectively, for this reaction (relative to state-of-the-art platinum-carbon catalysts) during prolonged exposure to reaction conditions. [PUBLICATION ABSTRACT] Control of structure at the atomic level can precisely and effectively tune catalytic properties of materials, enabling enhancement in both activity and durability. We synthesized a highly active and durable class of electrocatalysts by exploiting the structural evolution of platinum-nickel (Pt-Ni) bimetallic nanocrystals. The starting material, crystalline PtNi3 polyhedra, transforms in solution by interior erosion into Pt3Ni nanoframes with surfaces that offer three-dimensional molecular accessibility. The edges of the Pt-rich PtNi3 polyhedra are maintained in the final Pt3Ni nanoframes. Both the interior and exterior catalytic surfaces of this open-framework structure are composed of the nanosegregated Pt-skin structure, which exhibits enhanced oxygen reduction reaction (ORR) activity. The Pt3Ni nanoframe catalysts achieved a factor of 36 enhancement in mass activity and a factor of 22 enhancement in specific activity, respectively, for this reaction (relative to state-of-the-art platinum-carbon catalysts) during prolonged exposure to reaction conditions. Control of structure at the atomic level can precisely and effectively tune catalytic properties of materials, enabling enhancement in both activity and durability. We synthesized a highly active and durable class of electrocatalysts by exploiting the structural evolution of platinum-nickel (Pt-Ni) bimetallic nanocrystals. The starting material, crystalline PtNi3 polyhedra, transforms in solution by interior erosion into Pt3Ni nanoframes with surfaces that offer three-dimensional molecular accessibility. The edges of the Pt-rich PtNi3 polyhedra are maintained in the final Pt3Ni nanoframes. Both the interior and exterior catalytic surfaces of this open-framework structure are composed of the nanosegregated Pt-skin structure, which exhibits enhanced oxygen reduction reaction (ORR) activity. The Pt3Ni nanoframe catalysts achieved a factor of 36 enhancement in mass activity and a factor of 22 enhancement in specific activity, respectively, for this reaction (relative to state-of-the-art platinum-carbon catalysts) during prolonged exposure to reaction conditions.Control of structure at the atomic level can precisely and effectively tune catalytic properties of materials, enabling enhancement in both activity and durability. We synthesized a highly active and durable class of electrocatalysts by exploiting the structural evolution of platinum-nickel (Pt-Ni) bimetallic nanocrystals. The starting material, crystalline PtNi3 polyhedra, transforms in solution by interior erosion into Pt3Ni nanoframes with surfaces that offer three-dimensional molecular accessibility. The edges of the Pt-rich PtNi3 polyhedra are maintained in the final Pt3Ni nanoframes. Both the interior and exterior catalytic surfaces of this open-framework structure are composed of the nanosegregated Pt-skin structure, which exhibits enhanced oxygen reduction reaction (ORR) activity. The Pt3Ni nanoframe catalysts achieved a factor of 36 enhancement in mass activity and a factor of 22 enhancement in specific activity, respectively, for this reaction (relative to state-of-the-art platinum-carbon catalysts) during prolonged exposure to reaction conditions. Platinum (Pt) is an excellent catalyst for the oxygen-reduction reaction (ORR) in fuel cells and electrolyzers, but it is too expensive and scarce for widespread deployment, even when dispersed as Pt nanoparticles on carbon electrode supports (Pt/C). Alternatively, Chen et al. (p. 1339 , published online 27 February; see the Perspective by Greer ) made highly active ORR catalysts by dissolving away the interior of rhombic dodecahedral PtNi 3 nanocrystals to leave Pt-rich Pt 3 Ni edges. These nanoframe catalysts are durable—remaining active after 10,000 rounds of voltage cycling—and are far more active than Pt/C. Highly active electrocatalysts are created by eroding away all but the edges of platinum-nickel nanocrystals. [Also see Perspective by Greer ] Control of structure at the atomic level can precisely and effectively tune catalytic properties of materials, enabling enhancement in both activity and durability. We synthesized a highly active and durable class of electrocatalysts by exploiting the structural evolution of platinum-nickel (Pt-Ni) bimetallic nanocrystals. The starting material, crystalline PtNi 3 polyhedra, transforms in solution by interior erosion into Pt 3 Ni nanoframes with surfaces that offer three-dimensional molecular accessibility. The edges of the Pt-rich PtNi 3 polyhedra are maintained in the final Pt 3 Ni nanoframes. Both the interior and exterior catalytic surfaces of this open-framework structure are composed of the nanosegregated Pt-skin structure, which exhibits enhanced oxygen reduction reaction (ORR) activity. The Pt 3 Ni nanoframe catalysts achieved a factor of 36 enhancement in mass activity and a factor of 22 enhancement in specific activity, respectively, for this reaction (relative to state-of-the-art platinum-carbon catalysts) during prolonged exposure to reaction conditions. |
| Author | Li, Yadong Kang, Yijin Mavrikakis, Manos Somorjai, Gabor A. Huang, Wenyu Xin, Huolin L. Li, Dongguo Chen, Chen Snyder, Joshua D. Zhu, Zhongwei Markovic, Nenad M. Huo, Ziyang Yang, Peidong Herron, Jeffrey A. Chi, Miaofang More, Karren L. Stamenkovic, Vojislav R. |
| Author_xml | – sequence: 1 givenname: Chen surname: Chen fullname: Chen, Chen – sequence: 2 givenname: Yijin surname: Kang fullname: Kang, Yijin – sequence: 3 givenname: Ziyang surname: Huo fullname: Huo, Ziyang – sequence: 4 givenname: Zhongwei surname: Zhu fullname: Zhu, Zhongwei – sequence: 5 givenname: Wenyu surname: Huang fullname: Huang, Wenyu – sequence: 6 givenname: Huolin L. surname: Xin fullname: Xin, Huolin L. – sequence: 7 givenname: Joshua D. surname: Snyder fullname: Snyder, Joshua D. – sequence: 8 givenname: Dongguo surname: Li fullname: Li, Dongguo – sequence: 9 givenname: Jeffrey A. surname: Herron fullname: Herron, Jeffrey A. – sequence: 10 givenname: Manos surname: Mavrikakis fullname: Mavrikakis, Manos – sequence: 11 givenname: Miaofang surname: Chi fullname: Chi, Miaofang – sequence: 12 givenname: Karren L. surname: More fullname: More, Karren L. – sequence: 13 givenname: Yadong surname: Li fullname: Li, Yadong – sequence: 14 givenname: Nenad M. surname: Markovic fullname: Markovic, Nenad M. – sequence: 15 givenname: Gabor A. surname: Somorjai fullname: Somorjai, Gabor A. – sequence: 16 givenname: Peidong surname: Yang fullname: Yang, Peidong – sequence: 17 givenname: Vojislav R. surname: Stamenkovic fullname: Stamenkovic, Vojislav R. |
| BackLink | https://www.ncbi.nlm.nih.gov/pubmed/24578531$$D View this record in MEDLINE/PubMed https://www.osti.gov/biblio/1149771$$D View this record in Osti.gov |
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| Snippet | Control of structure at the atomic level can precisely and effectively tune catalytic properties of materials, enabling enhancement in both activity and... Platinum (Pt) is an excellent catalyst for the oxygen-reduction reaction (ORR) in fuel cells and electrolyzers, but it is too expensive and scarce for... Giving Electrocatalysts an Edge Platinum (Pt) is an excellent catalyst for the oxygen-reduction reaction (ORR) in fuel cells and electrolyzers, but it is too... |
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