Oxygen-Bridged Copper-Iron Atomic Pair as Dual-Metal Active Sites for Boosting Electrocatalytic NO Reduction

被引:58
作者
Wang, Dongdong [1 ]
Zhu, Xiaorong [2 ]
Tu, Xiaojin [1 ]
Zhang, Xiaoran [1 ]
Chen, Chen [1 ]
Wei, Xiaoxiao [1 ]
Li, Yafei [3 ]
Wang, Shuangyin [1 ]
机构
[1] Hunan Univ, Coll Chem & Chem Engn, State Key Lab Chemo, Biosensing & Chemometr, Changsha 410082, Peoples R China
[2] Nantong Univ, Sch Chem & Chem Engn, Nantong 226019, Peoples R China
[3] Nanjing Normal Univ, Coll Chem & Mat Sci, Nanjing 210023, Peoples R China
基金
中国国家自然科学基金;
关键词
dual-site catalysts; electrocatalysis; NH3; synthesis; NO reduction; synergistic effect;
D O I
10.1002/adma.202304646
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Electrocatalytic reduction of nitric oxide (NO) to ammonia (NH3) is a promising approach to NH3 synthesis. However, due to the lack of efficient electrocatalysts, the performance of electrocatalytic NO reduction reaction (NORR) is far from satisfactory. Herein, it is reported that an atomic copper-iron dual-site electrocatalyst bridged by an axial oxygen atom (O-Fe-N-6-Cu) is anchored on nitrogen-doped carbon (CuFe DS/NC) for NORR. The CuFe DS/NC can significantly enhance the electrocatalytic NH3 synthesis performance (Faraday efficiency, 90%; yield rate, 112.52 & mu;mol cm(-2) h(-1)) at -0.6 V versus RHE, which is dramatically higher than the corresponding Cu single-atom, Fe single-atom and all NORR single-atom catalysts in the literature so far. Moreover, an assembled proof-of-concept Zn-NO battery using CuFe DS/NC as the cathode outputs a power density of 2.30 mW cm(-2) and an NH3 yield of 45.52 & mu;g h(-1) mg(cat)(-1). The theoretical calculation result indicates that bimetallic sites can promote electrocatalytic NORR by changing the rate-determining step and accelerating the protonation process. This work provides a flexible strategy for efficient sustainable NH3 synthesis.
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页数:7
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