<p>Efficient ammonia decomposition is crucial for hydrogen economy, but inexpensive Ni catalysts require excessively high temperatures due to limited N-N coupling. Here, we overcome this challenge by constructing a photothermal catalyst with closely interfaced, defect-rich CeO<sub>2-x</sub> nanodomains and electron-rich Ni nanoparticles on carbon nanotubes. The Ni-CeO<sub>2-x</sub>/CNTs catalyst achieves a hydrogen production rate of 298.4 mmol g<sub>cat</sub><sup>-1</sup> min<sup>-1</sup> under full-spectrum light irradiation, which exceeds that of most reported Ru catalysts, and maintained stable activity for over 50 h in continuous-flow operation. The high performance arises from the synergistic effect of thermally promoted photocatalytic N-H bond cleavage and a largely reduced N-N coupling barrier, enabled by efficient photothermal conversion of carbon nanotubes and the up-shifted d-band center of the Ce-Ov-Ni interface (Ov = oxygen vacancy).</p>

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Breakthrough photothermal ammonia decomposition via low-barrier Ni-CeO2-x interfaces on carbon nanotubes

  • Ruike Tan,
  • Xiaowei Mu,
  • Xinhui Wang,
  • Yuxiang Kong,
  • Qing Ji,
  • Qingyun Zhan,
  • Qingchuan Xiong,
  • Lu Li

摘要

Efficient ammonia decomposition is crucial for hydrogen economy, but inexpensive Ni catalysts require excessively high temperatures due to limited N-N coupling. Here, we overcome this challenge by constructing a photothermal catalyst with closely interfaced, defect-rich CeO2-x nanodomains and electron-rich Ni nanoparticles on carbon nanotubes. The Ni-CeO2-x/CNTs catalyst achieves a hydrogen production rate of 298.4 mmol gcat-1 min-1 under full-spectrum light irradiation, which exceeds that of most reported Ru catalysts, and maintained stable activity for over 50 h in continuous-flow operation. The high performance arises from the synergistic effect of thermally promoted photocatalytic N-H bond cleavage and a largely reduced N-N coupling barrier, enabled by efficient photothermal conversion of carbon nanotubes and the up-shifted d-band center of the Ce-Ov-Ni interface (Ov = oxygen vacancy).