Entropy‐Driven Stabilization of Noble Metal Single Atoms: Advancing Ammonia Synthesis and Energy Output in Zinc‐Nitrate Batteries
Abstract
Abstract Noble metal single atoms (NMSA) offer exceptional atom utilization and catalytic activity but face challenges like limited stability, low atomic loading, and complex synthesis. This study presents an innovative entropy‐driven strategy to stabilize Ru single atoms (SA) on a (CePrYZrHf)O x high‐entropy oxide substrate (Ru α% ‐HEO). Due to their defect‐rich structure and significant lattice distortion, HEO substrates can accommodate and stabilize more Ru SA than traditional low‐entropy oxides (LEO) like CeO 2 . This strategy is also effective for achieving high loadings of other NMSAs, such as Pd and Pt. Ru 3% ‐HEO, as an electrocatalyst for nitrate reduction, achieves a high ammonia yield (5.79 mg h −1 mg cat. −1 ) and a Faradaic efficiency (FE) of 91.3%. Density functional theory (DFT) calculations reveal that Ru 3% ‐HEO exhibits favorable thermodynamics for nitrate reduction, with a lower energy barrier for the rate‐determining step of first hydrogenation ( * NO + H + + e⁻ → * NOH) and stronger intermediates adsorption compared to RuO 2 , enhancing its catalytic efficiency. As a cathode material in a zinc‐nitrate battery, Ru 3% ‐HEO demonstrates a high NH 3 yield rate (1.11 mg h −1 cm −2 ) and FE value (93.4%). This study provides an efficient strategy to produce stable and high‐loading SA using high‐entropy materials, showcasing their broad applicability in advanced electrocatalysis.
Article Details
Authors (16)
Hele Guo
Key Laboratory of Synthetic and Biological Colloids, Ministry of Education, School of Chemical and Material Engineering, International Joint Research Laboratory for Nano Energy Composites
Zhongyuan Guo
Guohao Xue
The Key Laboratory of Synthetic and Biological Colloids Ministry of Education School of Chemical and Material Engineering Jiangnan University Wuxi 214122 P. R. China
Haifeng Wang
Jiaming Gong
State Key Laboratory of Metal Matrix Composites School of Materials Science and Engineering Shanghai Jiao Tong University Shanghai 200240 P.R. China
Kaibin Chu
Key Laboratory of Synthetic and Biological Colloids, Ministry of Education, School of Chemical and Material Engineering, International Joint Research Laboratory for Nano Energy Composites
Jingjing Qin
The Key Laboratory of Synthetic and Biological Colloids, Ministry of Education, School of Chemical and Material Engineering, Jiangnan University, Wuxi 214122, China
Yawen Guan
State Key Laboratory of Metal Matrix Composites School of Materials Science and Engineering Shanghai Jiao Tong University Shanghai 200240 P. R. China
Hongliang Dong
Center for High Pressure Science and Technology Advanced Research
Yujie Chen
Yue‐E Miao
State Key Laboratory of Advanced Fiber Materials College of Materials Science and Engineering Donghua University Shanghai 201620 P.R. China
Chao Zhang
Hezhou Liu
Tianxi Liu
Key Laboratory of Synthetic and Biological Colloids, Ministry of Education, School of Chemical and Material Engineering
Johan Hofkens
Department of Chemistry, KU Leuven, Celestijnenlaan 200F, B-3001 Leuven, Belgium
Feili Lai
Department of Chemistry, KU Leuven, Celestijnenlaan 200F, Leuven 3001, Belgium