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<p>The chlorine evolution reaction (CER) serves as the cornerstone and crucial step in the conversion of chloride ions to chlorine gas, while accompanied by the occurrence of the oxygen evolution reaction (OER) in practical processes that lead to difficulty in achieving the purity requirements of the product Cl<sub>2</sub> for industrial applications. Pd-doped Co<sub>3</sub>O<sub>4</sub> nanoneedles (Pd-Co<sub>3</sub>O<sub>4</sub> NNs) were synthesized via hydrothermal-calcination methods. Pd sites induce electron delocalization, creating asymmetric active Co sites in Co<sub>3</sub>O<sub>4</sub>, enhancing CER performance. The unique nanoneedle arrays of the designed catalysts increase the number of exposed active sites, facilitating electron transfer and endowing the Pd-Co<sub>3</sub>O<sub>4</sub> NNs with a tip catalytic effect, further optimizing the catalytic reaction kinetics of CER with an overpotential of 118 mV at 100 mA cm<sup>−2</sup> and a Tafel slope of 53.93 mV dec<sup>−1</sup>. The density functional theory (DFT) calculations reveal that Pd incorporation at octahedral sites triggers charge redistribution and d-band center downshift, weakening intermediate adsorption and sustaining catalytic activity. This work offers new insights into noble-metal-doped spinel oxides, highlighting their potential for industrial applications.</p>

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Pd sites induced electron delocalization and oxygen vacancies in Co3O4 nanoneedles improving the chlorine production by seawater electrolysis

  • 期刊论文

  • 发表日期：

    2025年10月27日

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  • Ruixue Zhang,
  • Yu Miao,
  • Shuhan Wei,
  • Shuai He,
  • Jiayi Li,
  • Qiyan Sun,
  • Lei Wang,
  • Guang-rui Xu

摘要

The chlorine evolution reaction (CER) serves as the cornerstone and crucial step in the conversion of chloride ions to chlorine gas, while accompanied by the occurrence of the oxygen evolution reaction (OER) in practical processes that lead to difficulty in achieving the purity requirements of the product Cl2 for industrial applications. Pd-doped Co3O4 nanoneedles (Pd-Co3O4 NNs) were synthesized via hydrothermal-calcination methods. Pd sites induce electron delocalization, creating asymmetric active Co sites in Co3O4, enhancing CER performance. The unique nanoneedle arrays of the designed catalysts increase the number of exposed active sites, facilitating electron transfer and endowing the Pd-Co3O4 NNs with a tip catalytic effect, further optimizing the catalytic reaction kinetics of CER with an overpotential of 118 mV at 100 mA cm−2 and a Tafel slope of 53.93 mV dec−1. The density functional theory (DFT) calculations reveal that Pd incorporation at octahedral sites triggers charge redistribution and d-band center downshift, weakening intermediate adsorption and sustaining catalytic activity. This work offers new insights into noble-metal-doped spinel oxides, highlighting their potential for industrial applications.