Effects of carboxylate stabilizers on the structure and activity of carbon-supported Pt–Cu nanoparticles towards methanol oxidation
Carbon-supported Pt–Cu nanoparticles were prepared by alcohol reduction method in the presence of carboxylate stabilizers with different molecular structure (malonate, succinate, adipate, and citrate). The longer was the carbon chain of stabilizer, the smaller dispersed Pt–Cu alloy crystallites and...
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| Published in: | International journal of hydrogen energy Vol. 42; no. 5; pp. 2984 - 2995 |
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| Main Authors: | , , , , , |
| Format: | Journal Article |
| Language: | English |
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02-02-2017
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| Abstract | Carbon-supported Pt–Cu nanoparticles were prepared by alcohol reduction method in the presence of carboxylate stabilizers with different molecular structure (malonate, succinate, adipate, and citrate). The longer was the carbon chain of stabilizer, the smaller dispersed Pt–Cu alloy crystallites and fewer aggregates were obtained, which was attributed to steric effect of the molecular backbone to protect fine dispersed crystallites. Dispersed nanoparticles were Pt-rich and aggregates were high-Cu crystallites due to competitive chemisorption of carboxylate and Cu2+ on metal surface in the course of nanoparticle formation. Citrate gave aggregates of several low-Cu alloy crystallites dispersed on carbon support, which was attributed to strong chemisorption of citrate on metal surface via tridentate coordination. The length of molecular backbone of stabilizer mainly affected size and dispersivity of Pt–Cu nanoparticles while the chemisorption strength of stabilizer on metal surface affected the degree of alloying. The Pt–Cu prepared with succinate showed the highest methanol oxidation activity, which was attributed to moderate size and moderate alloying degree leading to a moderate chemisorption strength of reactants and intermediates.
•The structure of Pt–Cu nanoparticles depends on molecular structure of stabilizer.•Steric factor of stabilizer affects dispersivity of Pt–Cu nanoparticles.•Chemisorption strength of stabilizer on metal surface affects the degree of alloying.•Pt–Cu prepared with succinate showed the highest activity for methanol oxidation.•The high activity was attributed to moderate chemisorption strength of reactants. |
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| AbstractList | Carbon-supported Pt–Cu nanoparticles were prepared by alcohol reduction method in the presence of carboxylate stabilizers with different molecular structure (malonate, succinate, adipate, and citrate). The longer was the carbon chain of stabilizer, the smaller dispersed Pt–Cu alloy crystallites and fewer aggregates were obtained, which was attributed to steric effect of the molecular backbone to protect fine dispersed crystallites. Dispersed nanoparticles were Pt-rich and aggregates were high-Cu crystallites due to competitive chemisorption of carboxylate and Cu2+ on metal surface in the course of nanoparticle formation. Citrate gave aggregates of several low-Cu alloy crystallites dispersed on carbon support, which was attributed to strong chemisorption of citrate on metal surface via tridentate coordination. The length of molecular backbone of stabilizer mainly affected size and dispersivity of Pt–Cu nanoparticles while the chemisorption strength of stabilizer on metal surface affected the degree of alloying. The Pt–Cu prepared with succinate showed the highest methanol oxidation activity, which was attributed to moderate size and moderate alloying degree leading to a moderate chemisorption strength of reactants and intermediates.
•The structure of Pt–Cu nanoparticles depends on molecular structure of stabilizer.•Steric factor of stabilizer affects dispersivity of Pt–Cu nanoparticles.•Chemisorption strength of stabilizer on metal surface affects the degree of alloying.•Pt–Cu prepared with succinate showed the highest activity for methanol oxidation.•The high activity was attributed to moderate chemisorption strength of reactants. |
| Author | Seino, Satoshi Yamamoto, Takao A. Nakagawa, Takashi Kugai, Junichiro Tanaka, Shingo Okazaki, Tomohisa |
| Author_xml | – sequence: 1 givenname: Junichiro surname: Kugai fullname: Kugai, Junichiro email: jkugai@kobe-kosen.ac.jp organization: Department of Applied Chemistry, Kobe City College of Technology, 8-3 Gakuen-higashimachi Nishi-ku, Kobe, Hyogo 651-2194, Japan – sequence: 2 givenname: Tomohisa surname: Okazaki fullname: Okazaki, Tomohisa organization: Graduate School of Engineering, Osaka University, 2-1 Yamadaoka, Suita, Osaka 565-0871, Japan – sequence: 3 givenname: Satoshi surname: Seino fullname: Seino, Satoshi organization: Graduate School of Engineering, Osaka University, 2-1 Yamadaoka, Suita, Osaka 565-0871, Japan – sequence: 4 givenname: Takashi surname: Nakagawa fullname: Nakagawa, Takashi organization: Graduate School of Engineering, Osaka University, 2-1 Yamadaoka, Suita, Osaka 565-0871, Japan – sequence: 5 givenname: Takao A. surname: Yamamoto fullname: Yamamoto, Takao A. organization: Graduate School of Engineering, Osaka University, 2-1 Yamadaoka, Suita, Osaka 565-0871, Japan – sequence: 6 givenname: Shingo surname: Tanaka fullname: Tanaka, Shingo organization: Research Institute of Electrochemical Energy, National Institute of Advanced Industrial Science and Technology (AIST), 1-8-31 Midorigaoka, Ikeda, Osaka 563-8577, Japan |
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| CitedBy_id | crossref_primary_10_1016_j_ijhydene_2019_06_170 crossref_primary_10_1149_2_1151908jes crossref_primary_10_1007_s11581_020_03608_3 crossref_primary_10_1016_j_ijhydene_2018_05_158 crossref_primary_10_1016_j_jelechem_2021_115596 crossref_primary_10_1039_C8NR09005J crossref_primary_10_1016_j_jechem_2021_05_003 crossref_primary_10_1007_s11581_021_04311_7 crossref_primary_10_1016_j_ijhydene_2017_07_113 crossref_primary_10_1007_s11581_018_2590_7 |
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| Keywords | Nanoparticles CO stripping Alcohol reduction Stabilizer Pt–Cu Methanol oxidation |
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