Despite more than a century of advances in catalyst and production plant design, the Haber-Bosch process for industrial ammonia (NH₃) synthesis still requires energy-intensive high temperatures and pressures. We propose taking advantage of sunlight conversion into surface plasmon resonances in Au nanoparticles to enhance the rate of the N₂ dissociation reaction, which is the bottleneck in NH₃ production. We predict that this can be achieved through Mo doping of the Au surface based on embedded multireference correlated wave function calculations. The Au component serves as a light-harvesting antenna funneling energy onto the Mo active site, whereby excited-state channels (requiring 1.4 to 1.45 eV, near-infrared-to-visible plasmon resonances) may be accessed. This effectively lowers the energy barriers to 0.44 to 0.77 eV/N₂ (43 to 74 kJ/mol N₂) from 3.5 eV/N₂ (335 kJ/mol N₂) in the ground state. The overall process requires three successive surface excitation events, which could be facilitated by amplified resonance energy transfer due to plasmon local field enhancement.

中文翻译：

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利用近红外到可见光纳米等离子体技术预测低温N2解离催化剂。

尽管在催化剂和生产装置的设计上已有一百多年的进步，但用于工业氨（NH ₃）合成的哈伯-博世（Haber-Bosch）工艺仍然需要耗能大量的高温和高压。我们建议利用Au纳米颗粒中的阳光转化为表面等离振子共振来提高N ₂解离反应的速率，这是NH ₃的瓶颈生产。我们预测这可以通过基于嵌入的多参考相关波函数计算的Au表面的Mo掺杂来实现。Au组分用作将能量集中到Mo活性位点上的集光天线，从而可以访问激发态通道（需要1.4到1.45 eV，近红外到可见的等离振子共振）。这有效地降低了能量壁垒0.44到0.77电子伏特/ N ₂（43至74千焦耳/摩尔的N ₂从为3.5eV / N）₂（335千焦耳/摩尔的N ₂在基态）。整个过程需要三个连续的表面激发事件，由于等离激元局部场增强，可以通过放大的共振能量转移来促进这些事件。