A Polymer Encapsulation Strategy to Synthesize Porous Nitrogen‐Doped Carbon‐Nanosphere‐Supported Metal Isolated‐Single‐Atomic‐Site Catalysts |
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Authors: | Aijuan Han Wenxing Chen Shaolong Zhang Maolin Zhang Yunhu Han Jian Zhang Shufang Ji Lirong Zheng Yu Wang Lin Gu Chen Chen Qing Peng Dingsheng Wang Yadong Li |
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Affiliation: | 1. Department of Chemistry, Tsinghua University, Beijing, China;2. Beijing Synchrotron Radiation Facility, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing, China;3. Shanghai Synchrotron Radiation Facility, Shanghai Institute of Applied Physics, Chinese Academy of Sciences, Shanghai, China;4. Institute of Physics, Chinese Academy of Sciences, Beijing, China |
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Abstract: | A novel polymer encapsulation strategy to synthesize metal isolated‐single‐atomic‐site (ISAS) catalysts supported by porous nitrogen‐doped carbon nanospheres is reported. First, metal precursors are encapsulated in situ by polymers through polymerization; then, metal ISASs are created within the polymer‐derived p‐CN nanospheres by controlled pyrolysis at high temperature (200–900 °C). Transmission electron microscopy and N2 sorption results reveal this material to exhibit a nanospheric morphology, a high surface area (≈380 m2 g?1), and a porous structure (with micropores and mesopores). Characterization by aberration‐corrected high‐angle annular dark‐field scanning transmission electron microscopy and X‐ray absorption fine structure confirms the metal to be present as metal ISASs. This methodology is applicable to both noble and nonprecious metals (M‐ISAS/p‐CN, M = Co, Ni, Cu, Mn, Pd, etc.). In particular, the Co‐ISAS/p‐CN nanospheres obtained using this method show comparable (E1/2 = 0.838 V) electrochemical oxygen reduction activity to commercial Pt/C with 20 wt% Pt loading (E1/2 = 0.834 V) in alkaline media, superior methanol tolerance, and outstanding stability, even after 5000 cycles. |
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Keywords: | isolated‐single‐atomic‐site oxygen reduction reaction polymer porous nitrogen‐doped carbon |
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