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Unbiased Photoelectrochemical H2O2 Production Using Boron Nitride for Both Photogenerated Hole Extraction and Oxygen
Qi Sui1, Hui Li1, Jiarui Xia2
1College of Chemistry, Liaoning University, Shenyang, Liaoning, 110036, China.
None:
Unbiased photoelectrochemical (PEC) H2O2 production offers a sustainable alternative to the energy-intensive anthraquinone process, yet faces critical bottlenecks: inefficient charge separation, uncontrolled two-electron oxygen reduction reaction (2e- ORR) pathways, and high-purity O2 requirements. Herein, we report an efficient unbiased PEC system for H2O2 production under ambient air. The key innovation involves the strategic implementation of boron nitride (BN) serves a dual role as a charge transfer mediator and ORR pathway modulator. At the photoanode, BN functions as a hole-extraction layer, because of elevating the valence band position of BiVO4 (BVO), effectively suppressing interfacial charge recombination between the BVO photoanode and the FeNiOOH cocatalyst, resulting in a photocurrent density achieving 6.08 mA cm-2 at 1.23 VRHE. At the cathode, BN acts as a "reaction helmsman", tuning the binding energy of the *OOH intermediate and enabling the CoPc + BN to achieve 97% 2e- ORR selectivity at -0.3 VAg/AgCl. As a result, the integrated system delivers a sustained H2O2 production rate of 1.22 ± 0.14 mM cm-2 h-1 over 16 consecutive cycles. This study provides an innovative solution to address the key challenges in bias-free H2O2 production.
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