4.8 Article

Breaking the symmetry of single-atom catalysts enables an extremely low energy barrier and high stability for large-current-density water splitting

Journal

ENERGY & ENVIRONMENTAL SCIENCE
Volume 15, Issue 10, Pages 4048-4057

Publisher

ROYAL SOC CHEMISTRY
DOI: 10.1039/d2ee01337a

Keywords

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Funding

  1. National Natural Science Foundation of China (NSFC) [21501096, 22075223]
  2. Natural Science Foundation of Jiangsu [BK20150086, BK20201120]
  3. Foundation of the Jiangsu Education Committee [15KJB150020]
  4. Six Talent Peaks Project in Jiangsu Province [JY-087]
  5. Innovation Project of Jiangsu Province
  6. Excellent Scientific and Technological Innovation Team of Colleges and Universities of Jiangsu Province [SUJIAOKE 2021, 1]
  7. Key Subject of Ecology of Jiangsu Province [SUJIAOYANHAN 2022, 2]
  8. Scientific and Technological Innovation Team of Nanjing [NINGJIAOGAOSHI 2021, 16]

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The Ru single-atom system constructed on an iron-cobalt layered double hydroxide exhibits low overpotentials and high stability, surpassing commercial RuO2. Its mass activity is significantly higher than Ru and FeCo-LDH. The formation of an in situ Ru-O-TM nanocompound promotes O-O coupling and suppresses heteroatomic interface instability.
The instability and low large-current-density efficiency for a single atomic metal species system have aroused widespread concern. Herein, the Ru single-atom system constructed on an iron-cobalt layered double hydroxide (Ru(x)SACs@FeCo-LDH) exhibits extremely low oxygen evolution reaction (OER) overpotentials of 194 and 246 mV at current densities of 10 and 1000 mA cm(-2), respectively, and a high stability greater than 1000 h at 1000 mA cm(-2), all of which far surpass the values obtained for commercial RuO2. Moreover, its mass activity is similar to 2 and 6 times higher than those of Ru and FeCo-LDH, respectively. Extraordinarily, it only needs 1.52 V to achieve a 1000 mA cm(-2) current density for water splitting, and it is almost unchanged after 1000 h, as the highest performance reported so far. Experimental and theoretical calculation results show that, after an activation process, an in situ Ru-O-TM (Fe, Co, and Ni)-like nanocompound is formed on the atom-scale symmetry breaking interfaces of the FeCo-LDH surface, promoting O-O coupling at the Ru-O active sites for OER and beneficial for suppressing multiple heteroatomic interface instability for large-current-density water splitting. Our strategy opens up opportunities for boosting the single-atom stability in industrial-scale hydrogen production from water splitting.

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