查找使用阿拉丁产品的科研文献

Tuning clusters-metal oxide promoters electronic interaction of Ru-based catalyst for ammonia synthesis under mild conditions

Tianhua Zhang,Haihui Hu,Jiaxin Li,Yinglong Gao,Lingling Li,Mingyuan Zhang,Xuanbei Peng,Yanliang Zhou,Jun Ni,Bingyu Lin,Jianxin Lin,Bing Zhu,Dongshuang Wu,Linjie Zhang,Lili Han,Lirong Zheng,Xiuyun Wang,Lilong Jiang

Ammonia (NH 3 ) is an excellent candidate for hydrogen storage and transport. However, producing NH 3 under mild conditions is a long-term, arduous task. Atomic cluster catalysts (ACCs) have been shown to be effective for catalytic N 2 -to-NH 3 conversion, opening the door to the development of efficient catalysts under mild conditions. Still, ACC formation with thermally stable catalytic sites remains a challenge because of their high surface free energy . Herein, we report anchoring Ba and/or Ce onto Ru ACCs (2 wt% Ru atomic clusters supported on N-doped carbon) to form so-called clusters–metal oxide promoters electronic interaction (CMEI) to stabilize the Ru atomic clusters. The resulting Ba/Ce/Ru ACCs significantly boost the NH 3 synthesis rate to 56.2 mmol NH3 g cat −1 h −1 at 400 °C and 1 MPa, which is 7.5-fold higher than that of Ru ACC. The strengthened CMEI between the Ba/Ce and Ru atomic clusters across the Ba/Ce/Ru ACC enables electron transfer from Ba and/or Ce to Ru atomic clusters. As such, the electron-enriched Ru atom could facilitate electron transfer to N≡N bond π* orbitals, which would weaken the N≡N bond and drive the eventual conversion of N 2 to NH 3 . This study offers insight into the role of CMEI in Ru ACCs and provides an effective approach for designing stable atomic cluster catalysts for NH 3 synthesis.