Yang Yi, Wang Pei, Zhang Xiaohu, Wang Shengyao, Ding Xing, Ma Hongshan, Wang He, Li Yuanzhi, Jiang Bo, Song Hui, Hai Xiao, Lu Yue, Chen Hao, Ye Jinhua
College of Chemistry, Huazhong Agricultural University, Wuhan, 430070, P. R. China.
International Center for Materials Nanoarchitectonics (WPI-MANA), National Institute for Materials Science (NIMS), 1-1 Namiki, Tsukuba, Ibaraki, 305-0044, Japan.
Angew Chem Int Ed Engl. 2024 Oct 24;63(44):e202408309. doi: 10.1002/anie.202408309. Epub 2024 Sep 23.
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 with a rate of 1260 μmol g h 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.
由于多相催化中尺度关系的内在限制,推进能源密集型的哈伯-博施法面临重大挑战。在此,我们报道了一种扭转“跷跷板效应”的方法,以调控定制的α-Fe金属材料(α-Fe-110s)上的尺度关系,实现了无需额外加热、速率为1260 μmol g⁻¹ h⁻¹的高效光驱动热催化氨合成。具体而言,新型阶梯状{110}表面显著增强了α-Fe-110s的热催化活性,在350 °C时,与含促进剂的商业熔铁催化剂相比,活性提高了3.8倍。光诱导热电子转移进一步同时加速了氮气解离和氢化,有效克服了相同位点上尺度关系的限制。因此,在相同温度下光照时,α-Fe-110s的氨生成速率进一步提高了30倍。这项工作设计了一种高效且可持续的氨合成系统,并为调控多相催化中的尺度关系提供了一种新方法。