Concave-convex surface oxide layers over copper nanowires boost electrochemical nitrate-to-ammonia conversion

被引:199
作者
Ren, Tianlun [1 ]
Ren, Kaili [1 ]
Wang, Mingzhen [1 ]
Liu, Mengying [1 ]
Wang, Ziqiang [1 ]
Wang, Hongjing [1 ]
Li, Xiaonian [1 ]
Wang, Liang [1 ]
Xu, You [1 ]
机构
[1] Zhejiang Univ Technol, Coll Chem Engn, State Key Lab Breeding Base Green Chem Synth Tech, Hangzhou 310014, Peoples R China
基金
中国国家自然科学基金;
关键词
Cu nanowires; Nitrate reduction reaction; Ammonium synthesis; Electrocatalysis; Selectivity; ELECTROCATALYTIC REDUCTION; ULTRATHIN NANOSHEETS; METAL-ELECTRODES; N-2; REDUCTION; PERSPECTIVES; NANOTUBES; CATALYST; REMOVAL; NH3;
D O I
10.1016/j.cej.2021.130759
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
The room-temperature nitrate electroreduction to ammonia recycles the fixed nitrogen and offers an appealing ammonia-synthesis scenario. Electrocatalyst engineering is of vital importance to accelerate the reaction kinetics and increase the product selectivity during nitrate electroreduction to ammonia. In this work, Cu nanowires with concave-convex surface Cu2+1O layers (Cu@Cu2+1O NWs) were fabricated by a facile surface engineering strategy. Interior metallic Cu components allow for efficient electronic transmission capability along the nanowire structure, while exterior concave-convex Cu2+1O layers endow abundant catalytically active sites. Furthermore, the electronic interaction and interface effect between Cu/Cu2+1O enable tuning of the Cu d-band center and modulating the adsorption energies of intermediates. Consequently, the electroreduction ability of nitrate-to-ammonia over the Cu@Cu2+1O NWs is substantially improved, evident by the high nitrate-N conversion rate (78.57%), ammonia yield rate (576.53 mu g h(-1) mg(cat)(-1)) and ammonia Faradaic efficiency (87.07%) at the optimal applied potential (-1.2 V vs. saturated calomel electrode) for 2 h. The findings in the study are worth reference to tailor surface/interface properties and atom structure towards highly efficient electrocatalysts.
引用
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页数:8
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