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Lattice Hydrogen Engineering Unlocks Inert TiO2 for H2O2 Electrosynthesis in Neutral Media
Nannan Hou1, Ke Ye2, Mingzhou Wang1
1State Key Laboratory of Advanced Environmental Technology, Department of Environmental Science and Engineering, Key Laboratory of Precision and Intelligent Chemistry, Hefei National Research Center for Physical Sciences at the Microscale, Center for Micro and Nanoscale Research and Fabrication, University of Science & Technology of China, Hefei, Anhui, 230026, P. R. China.
None:
Electrochemical H2O2 production through the two-electron oxygen reduction reaction (2e- ORR) represents a transformative route for sustainable and decentralized chemical synthesis. Nevertheless, conventional catalysts struggle to achieve optimal intermediates adsorption and efficient proton-coupled electron transfer (PCET) under neutral conditions, as the sluggish dissociation of water imposes a severe kinetic bottleneck. Herein, we introduce a lattice hydrogen engineering strategy that confers unprecedented catalytic functionality to traditionally inert metal oxides. Through precise hydrogen implantation into the TiO2 lattice, we establish Ti-O2C-H active centers-a dual-function motif that simultaneously achieves near-ideal OOH* adsorption (positioned at the Sabatier volcano apex) and intrinsic proton reservoir capability. This atomically engineered H-TiO2 catalyst delivers > 95% H2O2 selectivity, operating stably for over 100 h at an industrial current density of 200 mA cm-2. This robust operation yields a high H2O2 production rate of 13,968 mmol g-1 h-1 with an energy efficiency of 41.3%. Crucially, the universality of lattice hydrogen engineering is demonstrated through the activation of WO3, MoO3, and Nb2O5, yielding comparable performance enhancements for neutral 2e- ORR. By unlocking metal oxides as a robust catalyst platform for H2O2 electrosynthesis, this work establishes a scalable pathway toward scalable, green and cost-effective peroxide production.
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