Constructing Ru single-atomic sites through potential-induced self-reconstruction to accelerate electrocatalytic nitrate reduction for ammonia production

被引:8
|
作者
Cao, Huiqun [1 ]
Liang, Bin [1 ]
Ye, Shenghua [1 ,2 ,3 ,4 ]
Zhuang, Ziqiong [1 ]
Zheng, Lirong [5 ]
Chen, Wenda [1 ]
Chen, Weibin [1 ]
Zhang, Jie [1 ]
Zhang, Qinghao [1 ]
Liu, Jianhong [1 ,4 ]
Yan, Xueqing [2 ,3 ]
Zhang, Qianling [1 ]
机构
[1] Shenzhen Univ, Coll Chem & Environm Engn, Graphene Composite Res Ctr, Shenzhen 518060, Peoples R China
[2] Peking Univ, State Key Lab Nucl Phys & Technol, Beijing 100871, Peoples R China
[3] Peking Univ, Key Lab HEDP, CAPT, Minist Educ, Beijing 100871, Peoples R China
[4] Shenzhen Eigen Equat Graphene Technol Co Ltd, Shenzhen 518000, Peoples R China
[5] Chinese Acad Sci, Inst High Energy Phys, Beijing 100049, Peoples R China
基金
中国国家自然科学基金;
关键词
Nitrate reduction reaction; Ammonia; Single atomic catalysts; Self-reconstruction;
D O I
10.1016/j.cej.2024.151883
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Conversion of NO3--to-NH3 via the electrocatalytic nitrate reduction reaction (NO3-RR) is an emerging strategy for ammonia production and storage of "green hydrogen", but is limited by the dissatisfactory activity and selectivity. In this study, we discovered that cobalt carbonate hydroxide (Co-2(OH)(2)CO3) underwent a potential-induced self-reconstruction to cobalt hydroxide (Co(OH)(2)) during NO3-RR. The incorporation of Ru into Co-2(OH)(2)CO3 expedited the aforementioned self-reconstruction process and resulted in the formation of Ru single-atomic sites (Ru SASs) anchored on Co(OH)(2) nanosheets. This structure is reported as a highly efficient electrocatalyst for NO3--to-NH3 conversion and exhibits exceptional electrochemical performance in zinc-NO3- batteries. Theoretical analysis revealed that the conversion of NO3--to-NH3 occurred on Ru SASs through an N-end pathway with *NO as a characteristic intermediate. Furthermore, Ru SASs facilitated the thermodynamic-determining step of *NH2-to-*NH3, thus promoting the overall NO3--to-NH3 conversion process.
引用
收藏
页数:8
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