Light induced ammonia synthesis by crystalline polyoxometalate-based hybrid frameworks coupled with the Sv-1T MoS2 cocatalyst,Inorganic Chemistry Frontiers

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Light induced ammonia synthesis by crystalline polyoxometalate-based hybrid frameworks coupled with the Sv-1T MoS2 cocatalyst
Inorganic Chemistry Frontiers ( IF 6.1 ) Pub Date : 2022-06-08 , DOI: 10.1039/d2qi01003h
Fengrui Li ₁ , Hongru Liu ₁ , Weichao Chen _{1,

2} , Ying Su ₁ , Weilin Chen ₁ , Jingjing Zhi ₁ , Yangguang Li ₁

Affiliation

The exploration of efficient and stable composite-materials as nitrogen reduction photocatalysts featuring wide spectrum absorption and nitrogen fixation active sites has become specifically significant. In this work, a series of mixed-addendum PMoV-based organic–inorganic hybrid materials coupled with rich sulfur vacancy 1T MoS₂ (Sv-1T MoS₂) through a hydrothermal growth strategy are presented towards green NH₃ production. The intervalence electron transfer of the reduced polyoxometalates, as well as the construction of a Ni-trinuclear cluster-based framework, is responsible for the capable light-harvesting performance of the well-defined PMo₈V₆–Ni crystalline material, and Sv-1T MoS₂ which serves as a cocatalyst can facilitate electron–hole separation of the light absorbers, which further promotes the ammonia production capacity of the composite materials. As expected, the ammonia generation rate of Sv-1T MoS₂/PMo₈V₆–Ni (80.6 μmol h⁻¹ g⁻¹) is much higher than that of either PMo₈V₆–Ni (9.7 μmol h⁻¹ g⁻¹) or Sv-1T MoS₂ (8.6 μmol h⁻¹ g⁻¹) component. Such a noble-metal-free system therefore shows an apparent quantum efficiency (AQE) of 0.368% at 550 nm. The “working-in-tandem” mechanism established by sulfur vacancies as nitrogen active sites and polyoxometalate crystalline photosensitizers are extremely crucial for facilitating N₂ chemisorption and NH₃ formation. This work provides a fresh perspective for the rational design of photocatalyst composite materials with energetic electrons towards efficient nitrogen fixation.

中文翻译：

基于结晶多金属氧酸盐的杂化框架与 Sv-1T MoS2 助催化剂耦合的光诱导氨合成

探索高效稳定的复合材料作为具有广谱吸收和固氮活性位点的氮还原光催化剂具有特别重要的意义。在这项工作中，通过水热生长策略将一系列混合添加剂 PMoV 基有机-无机杂化材料与富硫空位 1T MoS ₂ (Sv-1T MoS _{2 ) 相结合，用于绿色 NH}₃生产。还原的多金属氧酸盐的间隔电子转移，以及基于 Ni-三核簇的框架的构建，是定义明确的 PMo ₈ V ₆ -Ni 晶体材料和 Sv- 1T_二硫化钼作为助催化剂，可以促进光吸收剂的电子-空穴分离，从而进一步提高复合材料的产氨能力。_{正如预期的那样，Sv-1T MoS 2} /PMo ₈ V ₆ -Ni (80.6 μmol h ^-1 g ^-1 )的氨生成率远高于PMo ₈ V ₆ -Ni (9.7 μmol h ^-1 g )。 ^-1 ) 或 Sv-1T MoS ₂ (8.6 μmol h ^-1 g ^-1）零件。因此，这种不含贵金属的系统在 550 nm 处显示出 0.368% 的表观量子效率 (AQE)。_{由硫空位作为氮活性位点和多金属氧酸盐结晶光敏剂建立的“串联工作”机制对于促进 N 2}化学吸附和 NH ₃形成至关重要。这项工作为合理设计具有高能电子的光催化剂复合材料以实现高效固氮提供了新的视角。

更新日期：2022-06-08

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