Plasmon Polarization Induced Multi-Field Coupling in Molybdenum-Oxide Based Heterojunctions to Efficiently Hydrolyze Ammonia Borane

Rapid recombination of photogenerated carriers and weak driving forces to inject hot electrons are critical bottlenecks in solar-driven ammonia borane (AB) hydrolysis. Herein, aided by machine learning, a strategy is developed in a molybdenum-oxide based system to enhance AB hydrolytic activity, by plasmon polarization induced multi-field coupling. The reconstructed surface unsaturated metal (Mo ^δ+ ) active sites exhibit excellent activity and high stability over 100 hours in AB hydrolysis, which deliver a turnover frequency up to 5806 min ^-1 , surpassing non-noble and noble-metal based analogues ever reported. It is verified that the polarized electric field (PEF) facilitates carrier separation through incorporating polarization components (O _v and -OH), thereby promoting electron accumulation around Mo ^δ+ active sites. Meanwhile, the local electric field (LEF) enables highly delocalized hot electrons through plasmon oscillation, thus lowering the reaction barrier between Mo ^δ+ and AB. Accordingly, the hot electrons are efficiently channeled via an enhanced feedback pathway, facilitating their transfer into B-H antibonding orbitals toward boosted AB hydrolysis.