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| Author | Search for: Li, Yueying1; Search for: Dang, Ngoc Kim; Search for: Gao, Guorui; Search for: Shin, Homin1ORCID identifier: https://orcid.org/0000-0001-9300-6898; Search for: Sharma, Shriya; Search for: Wu, Xiaohua1ORCID identifier: https://orcid.org/0000-0002-4206-0103; Search for: Kodra, Oltion2; Search for: Zborowski, Andre2; Search for: Malenfant, Patrick R. L.1ORCID identifier: https://orcid.org/0000-0001-5391-2300; Search for: Ding, Jianfu1ORCID identifier: https://orcid.org/0000-0003-2440-0968; Search for: Dinh, Cao-Thang; Search for: Ouyang, Jianying1ORCID identifier: https://orcid.org/0000-0001-5700-9506 |
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| Affiliation | - National Research Council of Canada. Quantum and Nanotechnologies
- National Research Council of Canada. Clean Energy Innovation
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| Format | Text, Article |
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| Subject | Au nanocrystals; SWCNTs; bipyridine; in situ reduction; electrochemical CO₂ reduction; high mass activity |
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| Abstract | Metal nanocrystals (NCs) have been synthesized and used as highly efficient electrocatalysts for the electrocatalytic CO₂ reduction reaction (eCO₂RR) in recent years. Electrocatalysts with various metal sizes and morphologies have achieved remarkable improvement in the CO₂ reduction. However, the syntheses are typically energy-demanding and the catalysts exhibit low mass activity. Ultrasmall metal NCs synthesized by a one-step process at room temperature and an ambient environment stand out because of cost-effectiveness in materials and energy. Here, we report a facile synthesis to produce 1 nm gold nanocrystals in ambient conditions, which was realized by an in situ reduction of AuCl₃ on a semiconducting single-walled carbon nanotube (sc-SWCNT) surface. In addition, the bipyridine (BPy) units in tube-wrapped polymers function as chelating sites for anchoring Au3+ and AuNCs. The ultrasmall size of AuNCs was achieved by fast AuCl₃ diffusion and the anchoring function of BPy units. A slow diffusion or absence of BPy units resulted in AuNCs in larger sizes. The NC density was controlled by AuCl₃ feed amounts by varying the Au-to-BPy molar ratios. Density functional theory was applied to simulate the Au-BPy coordination. The fabricated nanocomposites exhibited a high Faradaic CO selectivity up to 86% at 25 mA/cm² and a high mass activity up to 5.61 A/mg (Au) at 100 mA/cm², which is the highest value reported so far in AuNC electrocatalysts for CO₂ reduction. |
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| Publication date | 2025-04-18 |
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| Publisher | American Chemical Society |
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| Language | English |
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| In press | Yes |
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| Peer reviewed | Yes |
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| Identifier | 10.1021/acsanm.5c01797 |
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| Export citation | Export as RIS |
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| Report a correction | Report a correction (opens in a new tab) |
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| Record identifier | 14531f51-424d-41ba-8c8d-9a078dce26ea |
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| Record created | 2025-04-30 |
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| Record modified | 2025-04-30 |
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