A Robust n-n Heterojunction: Cu-N and B-N Boosting for Ambient Electrocatalytic Nitrogen Reduction to Ammonia

被引:14
作者
Liu, Jiameng [1 ]
He, Linghao [1 ]
Zhao, Shuangrun [1 ]
Hu, Lijun [1 ]
Li, Sizhuan [1 ]
Zhang, Zhihong [1 ]
Du, Miao [1 ]
机构
[1] Zhengzhou Univ Light Ind, Coll Mat & Chem Engn, Inst New Energy Sci & Technol, Zhengzhou 450001, Peoples R China
基金
中国国家自然科学基金;
关键词
ammonia synthesis; conductive metal-organic frameworks; electrochemical nitrogen reduction; hexagonal boron nitride; n-n heterojunction; METAL-ORGANIC FRAMEWORK; BORON-NITRIDE; STRATEGIES;
D O I
10.1002/smll.202302600
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
An n-n type heterojunction comprising with Cu-N and B-N dual active sites is synthesized via in situ growth of a conductive metal-organic framework (MOF) [Cu-3(HITP)(2)] (HITP = 2,3,6,7,10,11-hexaiminotriphenylene) on hexagonal boron nitride (h-BN) nanosheets (hereafter denoted as Cu-3(HITP)(2)@h-BN) for the electrocatalytic nitrogen reduction reaction (eNRR). The optimized Cu-3(HITP)(2)@h-BN shows the outstanding eNRR performance with the NH3 production of 146.2 mu g h(-1) mg(cat)(-1) and the Faraday efficiency of 42.5% due to high porosity, abundant oxygen vacancies, and Cu-N/B-N dual active sites. The construction of the n-n heterojunction efficiently modulates the state density of active metal sites toward the Fermi level, facilitating the charge transfer at the interface between the catalyst and reactant intermediates. Additionally, the pathway of NH3 production catalyzed by the Cu-3(HITP)(2)@h-BN heterojunction is illustrated by in situ FT-IR spectroscopy and density functional theory calculation. This work presents an alternative approach to design advanced electrocatalysts based on conductive MOFs.
引用
收藏
页数:9
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