Precise O-doping across dual-Fe sites directed by pulsed laser optimized via Taguchi method for pH-universal H2O2 electrosynthesis
At present, over 95 % of H 2 O 2 is produced via the anthraquinone process that requires large infrastructure, generates organic pollution, and poses safety issues. Electrochemical H 2 O 2 generation through oxygen reduction can serve as an alternative, reliable, and decentralized production method if affordable and high-performance electrocatalysts can be developed. Herein, a two-step process is used to prepare an Fe-based complex as a non-precious metal electrocatalyst to facilitate oxygen reduction reaction (ORR) and produce an alkaline H 2 O 2 solution. The Fe complex of benzene-1,3,5-tricarboxylate (FeBTC) is first synthesized using a hydrothermal method and then activated via a pulsed laser treatment process that is optimized via the Taguchi method. The pulse-laser-treated FeBTC (PL-FeBTC) lowers the H 2 O 2 electrosynthesis overpotential by 50 mV at −0.1 mA/cm 2 and exhibits a 25 % increase in H 2 O 2 product selectivity at 0.4 V vs. RHE. The experimental results indicate that the O 2 -to-H 2 O 2 turnover frequency and electrocatalytic yield of the Fe-based metal–organic framework are enhanced simultaneously through solid-to-solid pulsed laser conversion. Through a series of X-ray photoelectron spectroscopy, elemental analysis, Raman spectroscopy, X-ray absorption spectroscopy, and control atmospheric experiments, the origin of the improvement in catalytic performance is rationalized through the formation of an oxo-bridge across the di–Fe active site via an oxygen-doping mechanism, thus providing a systematic laser methodology for precise structure-performance tuning. Beyond H 2 O 2 generation, this study further lays the foundation for the development of cost-effective and scalable electrocatalysts that are central to other commodity manufacturing and sustainable resourcification processes.
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