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<p>Electrocatalytic nitric oxide (NO) reduction reaction (NORR) is a promising and sustainable process that can simultaneously realize green ammonia (NH<sub>3</sub>) synthesis and hazardous NO removal. However, current NORR performances are far from practical needs due to the lack of efficient electrocatalysts. Engineering the lattice of metal-based nanomaterials via phase control has emerged as an effective strategy to modulate their intrinsic electrocatalytic properties. Herein, we realize boron (B)-insertion-induced phase regulation of rhodium (Rh) nanocrystals to obtain amorphous Rh<sub>4</sub>B nanoparticles (NPs) and hexagonal close-packed (<i>hcp</i>) RhB NPs through a facile wet-chemical method. A high Faradaic efficiency (92.1 ± 1.2%) and NH<sub>3</sub> yield rate (629.5 ± 11.0&#xa0;µmol&#xa0;h<sup>−1</sup>&#xa0;cm<sup>−2</sup>) are achieved over <i>hcp</i> RhB NPs, far superior to those of most reported NORR nanocatalysts. In situ spectro-electrochemical analysis and density functional theory simulations reveal that the excellent electrocatalytic performances of <i>hcp</i> RhB NPs are attributed to the upshift of d-band center, enhanced NO adsorption/activation profile, and greatly reduced energy barrier of the rate-determining step. A demonstrative Zn–NO battery is assembled using <i>hcp</i> RhB NPs as the cathode and delivers a peak power density of 4.33&#xa0;mW&#xa0;cm<sup>−2</sup>, realizing simultaneous NO removal, NH<sub>3</sub> synthesis, and electricity output.</p>

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Boron-Insertion-Induced Lattice Engineering of Rh Nanocrystals Toward Enhanced Electrocatalytic Conversion of Nitric Oxide to Ammonia

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年10月5日

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  • Peng Han,
  • Xiangou Xu,
  • Weiwei Chen,
  • Long Zheng,
  • Chen Ma,
  • Gang Wang,
  • Lei Xu,
  • Ping Gu,
  • Wenbin Wang,
  • Qiyuan He,
  • Zhiyuan Zeng,
  • Jinlan Wang,
  • Dong Su,
  • Chongyi Ling,
  • Zhengxiang Gu,
  • Ye Chen

摘要

Electrocatalytic nitric oxide (NO) reduction reaction (NORR) is a promising and sustainable process that can simultaneously realize green ammonia (NH3) synthesis and hazardous NO removal. However, current NORR performances are far from practical needs due to the lack of efficient electrocatalysts. Engineering the lattice of metal-based nanomaterials via phase control has emerged as an effective strategy to modulate their intrinsic electrocatalytic properties. Herein, we realize boron (B)-insertion-induced phase regulation of rhodium (Rh) nanocrystals to obtain amorphous Rh4B nanoparticles (NPs) and hexagonal close-packed (hcp) RhB NPs through a facile wet-chemical method. A high Faradaic efficiency (92.1 ± 1.2%) and NH3 yield rate (629.5 ± 11.0 µmol h−1 cm−2) are achieved over hcp RhB NPs, far superior to those of most reported NORR nanocatalysts. In situ spectro-electrochemical analysis and density functional theory simulations reveal that the excellent electrocatalytic performances of hcp RhB NPs are attributed to the upshift of d-band center, enhanced NO adsorption/activation profile, and greatly reduced energy barrier of the rate-determining step. A demonstrative Zn–NO battery is assembled using hcp RhB NPs as the cathode and delivers a peak power density of 4.33 mW cm−2, realizing simultaneous NO removal, NH3 synthesis, and electricity output.