Uniting Synergistic Effect of Single-Ni Site and Electric Field of B- Bridged-N for Boosted Electrocatalytic Nitrate Reduction to Ammonia

被引:23
作者
Ajmal, Saira [1 ]
Kumar, Anuj [2 ]
Mushtaq, Muhammad Asim [1 ]
Tabish, Mohammad [3 ]
Zhao, Yulin [4 ]
Zhang, Wenbin [1 ]
Khan, Abdul Sammed [1 ]
Saad, Ali [5 ,6 ]
Yasin, Ghulam [1 ]
Zhao, Wei [1 ]
机构
[1] Shenzhen Univ, Inst Adv Study, Shenzhen 518060, Guangdong, Peoples R China
[2] GLA Univ, Dept Chem, Nanotechnol Res Lab, Mathura 281406, Uttar Pradesh, India
[3] Beijing Univ Chem Technol, Coll Mat Sci & Engn, Beijing 100029, Peoples R China
[4] Southwest Univ Sci & Technol, Sch Mat & Chem, Mianyang 621010, Peoples R China
[5] Aarhus Univ, Ctr Water Technol WATEC, Universitetsbyen 36, DK-8000 Aarhus, Denmark
[6] Aarhus Univ, Dept Biol & Chem Engn, Universitetsbyen 36, DK-8000 Aarhus, Denmark
基金
中国国家自然科学基金;
关键词
ammonia synthesis; boron-spanning microenvironment engineering; Ni single atom; nitrate reduction; synergistic electrocatalysis; ELECTROCHEMICAL REDUCTION; NICKEL SITES; NANOPARTICLES;
D O I
10.1002/smll.202310082
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Electrochemical conversion of nitrate, a prevalent water pollutant, to ammonia (NH3) is a delocalized and green path for NH3 production. Despite the existence of different nitrate reduction pathways, selectively directing the reaction pathway on the road to NH3 is now hindered by the absence of efficient catalysts. Single-atom catalysts (SACs) are extensively investigated in a wide range of catalytic processes. However, their application in electrocatalytic nitrate reduction reaction (NO3-RR) to NH3 is infrequent, mostly due to their pronounced inclination toward hydrogen evolution reaction (HER). Here, Ni single atoms on the electrochemically active carrier boron, nitrogen doped-graphene (BNG) matrix to modulate the atomic coordination structure through a boron-spanning strategy to enhance the performance of NO3-RR is designed. Density functional theory (DFT) study proposes that BNG supports with ionic characteristics, offer a surplus electric field effect as compared to N-doped graphene, which can ease the nitrate adsorption. Consistent with the theoretical studies, the as-obtained NiSA@BNG shows higher catalytic activity with a maximal NH3 yield rate of 168 mu g h-1 cm-2 along with Faradaic efficiency of 95% and promising electrochemical stability. This study reveals novel ways to rationally fabricate SACs' atomic coordination structure with tunable electronic properties to enhance electrocatalytic performance. A boron-spanning strategy to modulate the atomic coordination structure and construct a single-atom Ni catalyst with a rational structure of NiN4B2 synchronized with boron-bridged nitrogen on graphene nanosheets is reported. The Ni SAs on the electrochemically active carrier due to the electronegativity difference between B and N atoms induced a local electric field and prompted a synergistic effect, facilitating the highly efficient nitrate reduction. image
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页数:10
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