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<p>Single-atom catalysts are highly active for specific reactions; however, their sinter-resistance and clean surfaces make it difficult to impart them with a “smart” property. Herein we design a thermosensitive single-atom Rh<sub>1</sub>-Pd nanosheets (NSs) by employing amino functionalized poly(<i>N</i>-isopropylacrylamide) as thermal responsive gate for the “open”/“closed” control of electro-catalytic activity. Using formic acid electro-oxidation as model reaction, the thermosensitive Rh<sub>1</sub>-Pd NSs exhibit high mass activity (2.29 A mg<sub>PGM</sub><sup>-1</sup>), strong poisoning resistance, and reversible thermo-responsibility at a lower critical solution temperature (LCST) of 35 <sup>o</sup>C. In-situ spectroscopy and theoretical investigations reveal that the d-electron deficient Rh<sub>1</sub>-Pd NSs favor the direct formate pathway and weaken the binding of self-poisonous species, contributing to the high activity and anti-self-poisoning talent. Most importantly, for the direct formic acid fuel cells (DFAFCs), the thermosensitive Rh<sub>1</sub>-Pd NSs exhibit a high power density operated below the LCST, while the power drops sharply once above the LCST, realizing the intelligent battery thermal protection for DFAFCs.</p>

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Thermal responsive Rh1-Pd single-atom catalyst for controlling activity in direct formic acid fuel cells

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年12月13日

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  • Keying Su,
  • Shan Yang,
  • Yujia Liang,
  • Dongmei Sun,
  • Mingxing Gong,
  • Yawen Tang,
  • Xiaoyu Qiu

摘要

Single-atom catalysts are highly active for specific reactions; however, their sinter-resistance and clean surfaces make it difficult to impart them with a “smart” property. Herein we design a thermosensitive single-atom Rh1-Pd nanosheets (NSs) by employing amino functionalized poly(N-isopropylacrylamide) as thermal responsive gate for the “open”/“closed” control of electro-catalytic activity. Using formic acid electro-oxidation as model reaction, the thermosensitive Rh1-Pd NSs exhibit high mass activity (2.29 A mgPGM-1), strong poisoning resistance, and reversible thermo-responsibility at a lower critical solution temperature (LCST) of 35 oC. In-situ spectroscopy and theoretical investigations reveal that the d-electron deficient Rh1-Pd NSs favor the direct formate pathway and weaken the binding of self-poisonous species, contributing to the high activity and anti-self-poisoning talent. Most importantly, for the direct formic acid fuel cells (DFAFCs), the thermosensitive Rh1-Pd NSs exhibit a high power density operated below the LCST, while the power drops sharply once above the LCST, realizing the intelligent battery thermal protection for DFAFCs.