Phosphorus ligand induced electron-energy synergetic enhancing simultaneous pollutant degradation and hydrogen production in a novel full spectrum heterostructure photocatalyst

Solar-driven hydrogen production coupled with water purification is an ideal way to resolve energy environmental problems together. In this study, we designed a novel full-spectrum heterostructure photocatalyst like a pseudo photocatalytic fuel cell (pseudo-PFC) for simultaneous water splitting and pollutant degradation. The core-shell heterostructure NaYF 4 :Yb,Er@TpMA-COF is fabricated through mechanical combination of near-infrared upconversion fluorescent material and covalent organic frameworks (COFs) with Alendronate as covalent linker. The bonded Alendronate not only acts as charge-transport bridges, but also reinforces the fluorescence resonance energy transfer (FRTE) process from NaYF 4 :Yb,Er to COF component, thus further enhancing the synergism of high and low-energy photons. Additionally, the Alendronate introduces abundant Brönsted acid/base sites for the selective formation of free ·OH radicals on photoanode, suppressing the O 2 evolution. Benefiting from the synergistic effect and selectivity, the optimal photocatalyst NYF@COF20 achieves excellent rates of 913 μmol h −1 g −1 for H 2 production (without extra sacrificial agents) and 0.235 min −1 g-cat. −1 for sulfamethoxazole (SMX, C 0 =10 mg L −1 ) degradation under the simulated sunlight provided by 300 W Xe light source, which is outstanding among similar photocatalysts. This work opens a new avenue for developing efficient photocatalysts in wastewater resource utilization and provides in-depth insights into the near-infrared mediated photocatalytic mechanism.