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<p>Photoelectrochemical (PEC) seawater splitting faces challenges including limited light absorption, rapid charge recombination, and chloride corrosion. This study addresses these issues by constructing a p-n heterojunction composite photoanode (Ni-ZIF/TNTAs) through solvothermal integration of nickel-based zeolitic imidazolate framework (Ni-ZIF) onto anodized TiO<sub>2</sub> nanotube arrays (TNTAs). The synergy between Ni-ZIF (bandgap: 2.23&#xa0;eV) and TNTAs narrows the composite bandgap to 2.72&#xa0;eV, extending light absorption to 450&#xa0;nm. The optimized Ni-ZIF/TNTAs (NT-0.01) achieves a photocurrent density of 2.2&#xa0;mA/cm² at 1.23&#xa0;V vs. RHE in simulated seawater (3.5 wt% NaCl), fivefold higher than pristine TNTAs (0.44&#xa0;mA/cm²), alongside a hydrogen evolution rate of 117.5 µmol/cm². Mott-Schottky and UV-vis analyses confirm a built-in electric field at the p-n junction interface, facilitating charge separation and doubling the incident photon-to-current efficiency (IPCE) to 30% at 365&#xa0;nm. Remarkably, the composite retains 96% hydrogen yield over four cycles, attributed to dynamically formed surface NiOOH layers that suppress chloride penetration while maintaining 87% oxygen evolution reaction (OER) selectivity. This work pioneers the application of Ni-ZIF/TiO<sub>2</sub> heterojunctions in seawater splitting, offering a scalable strategy to reduce freshwater dependency in solar-driven hydrogen production. The design merges visible-light harvesting, corrosion resistance, and efficient charge transport, advancing sustainable energy solutions.</p> Graphical Abstract <p></p>

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Development of a p-n Ni-ZIF/TiO2 Heterojunction for Photoelectrocatalytic Hydrogen Generation from Seawater

  • 期刊论文

  • 发表日期：

    2025年7月9日

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  • Daxiang Jin,
  • Wanggang Zhang,
  • Jian Wang,
  • Xiaohong Li,
  • Yiming Liu

摘要

Photoelectrochemical (PEC) seawater splitting faces challenges including limited light absorption, rapid charge recombination, and chloride corrosion. This study addresses these issues by constructing a p-n heterojunction composite photoanode (Ni-ZIF/TNTAs) through solvothermal integration of nickel-based zeolitic imidazolate framework (Ni-ZIF) onto anodized TiO2 nanotube arrays (TNTAs). The synergy between Ni-ZIF (bandgap: 2.23 eV) and TNTAs narrows the composite bandgap to 2.72 eV, extending light absorption to 450 nm. The optimized Ni-ZIF/TNTAs (NT-0.01) achieves a photocurrent density of 2.2 mA/cm² at 1.23 V vs. RHE in simulated seawater (3.5 wt% NaCl), fivefold higher than pristine TNTAs (0.44 mA/cm²), alongside a hydrogen evolution rate of 117.5 µmol/cm². Mott-Schottky and UV-vis analyses confirm a built-in electric field at the p-n junction interface, facilitating charge separation and doubling the incident photon-to-current efficiency (IPCE) to 30% at 365 nm. Remarkably, the composite retains 96% hydrogen yield over four cycles, attributed to dynamically formed surface NiOOH layers that suppress chloride penetration while maintaining 87% oxygen evolution reaction (OER) selectivity. This work pioneers the application of Ni-ZIF/TiO2 heterojunctions in seawater splitting, offering a scalable strategy to reduce freshwater dependency in solar-driven hydrogen production. The design merges visible-light harvesting, corrosion resistance, and efficient charge transport, advancing sustainable energy solutions.

Graphical Abstract