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Regulating the Scaling Relations in Ammonia Synthesis Through a Light‐driven Bendable Seesaw Effect on Tailored Iron Catalyst

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION(2024)

Huazhong Agr Univ

Cited 2|Views90
Abstract
Advancing the energy‐intensive Haber‐Bosch process faces significant challenges due to the intrinsic constraints of scaling relations in heterogeneous catalysis. Herein, we reported an approach of bending the “seesaw effect” to regulate the scaling relations over a tailored α‐Fe metallic material (α‐Fe‐110s), realizing highly efficient light‐driven thermal catalytic ammonia synthesis rate of 1260 μmol gcatalyst−1 h−1 without additional heating. Specifically, the thermal catalytic activity of α‐Fe‐110s was significantly enhanced by the novel stepped {110} surface, exhibiting a 3.8‐fold increase compared to the commercial fused‐iron catalyst with promoters at 350 °C. The photo‐induced hot electron transfer further accelerates the dinitrogen dissociation and hydrogenation simultaneously, effectively overcoming the limitation of scaling relation over identical sites. Consequently, the ammonia production rate of α‐Fe‐110s was further enhanced by 30 times at the same temperature with irradiation. This work designs an efficient and sustainable system for ammonia synthesis and provides a novel approach for regulating the scaling relations in heterogeneous catalysis.
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photothermal catalysis,ammonia synthesis,scaling relations,hot electron transfer,alpha-Fe catalyst
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要点】:本文通过光驱动可弯曲的“跷跷板效应”在定制α-Fe催化剂上调控了氨合成过程中的尺度关系,实现了高效的热催化氨合成。

方法】:采用特殊设计的α-Fe-110s催化剂,利用其阶梯状{110}表面增强热催化活性,并通过光诱导热电子转移加速氮气和氢气的分解和氢化过程。

实验】:在无额外加热条件下,α-Fe-110s催化剂在350°C时的氨合成速率达到1260 μmol gcatalyst−1 h−1,是商业促进铁催化剂的3.8倍;在光照下,同一温度下的氨产量提高了30倍。实验使用了α-Fe-110s催化剂,具体数据集名称未提及。