Balanced nitrogen and hydrogen chemisorption by [RuH6] catalytic center favors low-temperature NH3 synthesis

被引:7
|
作者
Pan, Jaysree [1 ]
Wang, Qianru [2 ,3 ]
Guo, Jianping [2 ,3 ]
Hansen, Heine Anton [1 ]
Chen, Ping [2 ,3 ,4 ]
Vegge, Tejs [1 ]
机构
[1] Tech Univ Denmark, Dept Energy Convers & Storage, DK-2800 Lyngby, Denmark
[2] Chinese Acad Sci, Dalian Inst Chem Phys, Dalian Natl Lab Clean Energy, Dalian 116023, Peoples R China
[3] Univ Chinese Acad Sci, Beijing 100049, Peoples R China
[4] State Key Lab Catalysis, Dalian 116023, Peoples R China
来源
CELL REPORTS PHYSICAL SCIENCE | 2022年 / 3卷 / 07期
基金
国家重点研发计划; 中国国家自然科学基金;
关键词
AMMONIA-SYNTHESIS; CO OXIDATION; REDUCTION; MECHANISM; HYDRIDES;
D O I
10.1016/j.xcrp.2022.100970
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Ammonia is a central vector in sustainable global growth, but the usage of fossil feedstocks and centralized Haber-Bosch synthesis conditions causes >1.4% of global anthropogenic CO2 emissions. While nitrogenase enzymes convert atmospheric N-2 to ammonia at ambient conditions, even the most active manmade inorganic catalysts fail due to low activity and parasitic hydrogen evolution at low temperatures. Here, we show that the [RuH6] catalytic center in ternary ruthenium complex hydrides (Li4RuH6) activates N-2 preferentially and avoids hydrogen over-saturation at low temperatures and near ambient pressure by delicately balancing H-2 chemisorption and N-2 activation. The active [RuH6] catalytic center is capable of achieving high yield at low temperatures via a shift in the rate-determining reaction intermediates and transition states, where the reaction orders in hydrogen and ammonia change dramatically. Temperature-dependent atomic-scale understanding of this unique mechanism is obtained with synchronized experimental and density functional theory investigations.
引用
收藏
页数:14
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