Direct and Sustainable Ammonia Synthesis from Air and Water with Sulfur-Deficient MoS₂ Piezocatalysts

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High Resolution Image Download MS PowerPoint Slide Eco-friendly ammonia (NH 3 ) production is critical for advancing sustainable agriculture and industry. This study introduces a sustainable, cleaner approach using MoS 2 nanoflowers (NFs) to synthesize NH 3 directly from water and air without the need for sacrificial agents. The advanced design leverages double sulfur vacancies (V2s) in MoS 2 NFs (V2s-MoS 2 NFs) and their piezoelectric properties, achieving a noteworthy production efficiency of 8374.8 ± 140.1 μmol L –1 g –1 h –1 (absolute production rate of 0.84 ± 0.01 μmol h –1 ). This outperforms most existing photocatalysts and piezocatalysts and rivals advanced electrocatalysts. The catalyst demonstrated exceptional stability, producing 36.55 mmol L –1 g –1 (equivalent to an absolute yield of 3.655 μmol) with N 2 and 26.03 mmol L –1 g –1 (equivalent to an absolute yield of 2.603 μmol) with air over 8 h. In situ Raman spectroscopy revealed intensifying peaks at ∼819 and 993 cm –1 under N 2 gas, attributed to Mo–N stretching vibrations. Additionally, in situ diffuse reflectance infrared Fourier-transform spectroscopy showed N 2 adsorption configurations, including side-on adsorption, indicative of N≡N bond elongation on the catalyst surface. Density functional theory calculations corroborated these findings, illustrating how unpaired Mo d orbital electrons near sulfur vacancies activate N 2 dissociation via backdonation to N 2 ’s antibonding π orbitals. This research highlights the transformative potential of piezocatalytic systems for nitrogen reduction reactions using atmospheric N 2 and water, providing a basis for sustainable energy solutions.