Prospects for Aerobic Photocatalytic Nitrogen Fixation
Prospects for Aerobic Photocatalytic Nitrogen Fixation
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DOI：
10.1021/acsenergylett.1c02260
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发表时间：
2022-01-14
影响因子：
22
通讯作者：
Hatzell, Marta C.
中科院分区：
文献类型：
--
作者：
Liu, Yu-Hsuan;Fernandez, Carlos A.;Hatzell, Marta C.
通过光催化固氮的脱碳氨生产是有吸引力的，因为它可以允许使用地球丰富的原料，能源和催化剂进行农场规模的肥料生产。然而，分散式氨生产系统的可行性在很大程度上取决于达到哈伯-博世平价点的完整光催化系统的成本。在这里，我们证明了农场规模的低成本光催化氨合成系统的空气分离单元可以占总系统成本的70%。这种高成本取决于空气分离装置的类型和氮气的纯度。这促进了对催化剂的需求，该催化剂可以耐受痕量氧或甚至可以在有氧条件下操作以实现Haber-Bosch成本平价。我们进一步证明了在有氧和厌氧条件下的原型未掺杂和金属掺杂的二氧化钛光催化剂的催化活性的变化。在各种金属掺杂的二氧化钛光催化剂中，钒和铈掺杂的二氧化钛在有氧条件下没有表现出性能下降。
Decarbonized ammonia production through photocatalytic nitrogen fixation is appealing, as it may allow for farm-scale fertilizer production using earth-abundant feedstocks, energy, and catalysts. Yet, the viability of decentralized ammonia production systems is largely dependent on the cost of a complete photocatalytic system reaching a Haber-Bosch parity point. Here, we demonstrate that an air separation unit for a farm-scale low-cost photocatalytic ammonia synthesis system can account for 70% of the total system cost. This high cost depends on the type of air separation unit and the purity of nitrogen. This promotes the need for a catalyst, which can tolerate trace oxygen or can even operate under aerobic conditions to attain Haber-Bosch cost parity. We further demonstrate the change in catalytic activity of prototypical undoped and metal-doped titania photocatalysts under aerobic and anaerobic conditions. Among various metal-doped titania photocatalyst, vanadium- and ruthenium-doped titania demonstrated no performance decline under aerobic conditions.