<p>Tungsten oxides with oxygen vacancies, particularly W<sub>18</sub>O<sub>49</sub>, hold promise for pseudocapacitive energy storage but are often limited by moderate conductivity and insufficient structural stability under high-rate operation. In this work, a Ni-doped W<sub>18</sub>O<sub>49</sub> electrode with an urchin-like architecture directly grown on nickel foam (Ni-W<sub>18</sub>O<sub>49</sub>/NF) is reported via a one-step solvothermal method. This unique interconnected microsphere morphology provides abundant active sites, facilitates electrolyte penetration, and ensures efficient charge transport. The capacitive behaviors of Ni-W<sub>18</sub>O<sub>49</sub>/NF electrode in different electrolytes were compared and screened. As a result, when evaluated in 1&#xa0;M AlCl<sub>3</sub> electrolyte, the electrode delivers a specific capacitance of 625 mF cm<sup>− 2</sup> at a high current density of 20&#xa0;mA cm<sup>− 2</sup>. Moreover, it exhibits a high Coulombic efficiency of 99.76% and excellent capacitance retention of 99.33% after 3000 cycles at 15&#xa0;mA·cm<sup>− 2</sup>. This is confirmed to be attributed to the pseudo-capacitance contribution generated by the smaller Al<sup>3+</sup> diameter embedded in the Ni-W<sub>18</sub>O<sub>49</sub> lattice. The doped Ni element extends the diameters of these tunnels and generates additional potential defects, thereby providing more sites for the incorporation of Al<sup>3+</sup>. This work provides a scalable design strategy for durable, high-rate supercapacitor electrodes by combining transition-metal doping, oxygen-defect engineering, and electrolyte design.</p>

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In-situ Ni-doped W18O49/NF compatible with Al3+ electrolyte for high-rate performance in supercapacitors

  • Boya Wang,
  • Junkai Li,
  • Chen Zhu,
  • Jin Hu,
  • Shizhao Xiong,
  • Kaizhao Wang

摘要

Tungsten oxides with oxygen vacancies, particularly W18O49, hold promise for pseudocapacitive energy storage but are often limited by moderate conductivity and insufficient structural stability under high-rate operation. In this work, a Ni-doped W18O49 electrode with an urchin-like architecture directly grown on nickel foam (Ni-W18O49/NF) is reported via a one-step solvothermal method. This unique interconnected microsphere morphology provides abundant active sites, facilitates electrolyte penetration, and ensures efficient charge transport. The capacitive behaviors of Ni-W18O49/NF electrode in different electrolytes were compared and screened. As a result, when evaluated in 1 M AlCl3 electrolyte, the electrode delivers a specific capacitance of 625 mF cm− 2 at a high current density of 20 mA cm− 2. Moreover, it exhibits a high Coulombic efficiency of 99.76% and excellent capacitance retention of 99.33% after 3000 cycles at 15 mA·cm− 2. This is confirmed to be attributed to the pseudo-capacitance contribution generated by the smaller Al3+ diameter embedded in the Ni-W18O49 lattice. The doped Ni element extends the diameters of these tunnels and generates additional potential defects, thereby providing more sites for the incorporation of Al3+. This work provides a scalable design strategy for durable, high-rate supercapacitor electrodes by combining transition-metal doping, oxygen-defect engineering, and electrolyte design.