Photoelectrochemical N2 -to-NH3 Fixation with High Efficiency and Rates via Optimized Si-Based System at Positive Potential versus Li0/

© 2023 The Authors. Advanced Materials published by Wiley-VCH GmbH.

Détails bibliographiques
Publié dans:Advanced materials (Deerfield Beach, Fla.). - 1998. - 35(2023), 21 vom: 05. Mai, Seite e2211894
Auteur principal: Zhang, Xiaoran (Auteur)
Autres auteurs: Lyu, Yanhong, Zhou, Huaijuan, Zheng, Jianyun, Huang, Aibin, Ding, Jingjing, Xie, Chao, De Marco, Roland, Tsud, Nataliya, Kalinovych, Viacheslav, Jiang, San Ping, Dai, Liming, Wang, Shuangyin
Format: Article en ligne
Langue:English
Publié: 2023
Accès à la collection:Advanced materials (Deerfield Beach, Fla.)
Sujets:Journal Article N2-to-NH3 fixation lithium-mediated nitrogen reduction reaction photoelectrochemical nitrogen reduction reaction reaction mechanism
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520 |a As a widely used commodity chemical, ammonia is critical for producing nitrogen-containing fertilizers and serving as the promising zero-carbon energy carrier. Photoelectrochemical nitrogen reduction reaction (PEC NRR) can provide a solar-powered green and sustainable route for synthesis of ammonia (NH3 ). Herein, an optimum PEC system is reported with an Si-based hierarchically-structured PdCu/TiO2 /Si photocathode and well-thought-out trifluoroethanol as the proton source for lithium-mediated PEC NRR, achieving a record high NH3 yield of 43.09 µg cm-2 h-1 and an excellent faradaic efficiency of 46.15% under 0.12 MPa O2 and 3.88 MPa N2 at 0.07 V versus lithium(0/+) redox couple (vs Li0/+ ). PEC measurements coupled with operando characterization reveal that the PdCu/TiO2 /Si photocathode under N2 pressures facilitate the reduction of N2 to form lithium nitride (Li3 N), which reacts with active protons to produce NH3 while releasing the Li+ to reinitiate the cycle of the PEC NRR. The Li-mediated PEC NRR process is further enhanced by introducing small amount of O2 or CO2 under pressure by accelerating the decomposition of Li3 N. For the first time, this work provides mechanistic understanding of the lithium-mediated PEC NRR process and opens new avenues for efficient solar-powered green conversion of N2 -to-NH3 
650 4 |a Journal Article 
650 4 |a N2-to-NH3 fixation 
650 4 |a lithium-mediated nitrogen reduction reaction 
650 4 |a photoelectrochemical nitrogen reduction reaction 
650 4 |a reaction mechanism 
700 1 |a Lyu, Yanhong  |e verfasserin  |4 aut 
700 1 |a Zhou, Huaijuan  |e verfasserin  |4 aut 
700 1 |a Zheng, Jianyun  |e verfasserin  |4 aut 
700 1 |a Huang, Aibin  |e verfasserin  |4 aut 
700 1 |a Ding, Jingjing  |e verfasserin  |4 aut 
700 1 |a Xie, Chao  |e verfasserin  |4 aut 
700 1 |a De Marco, Roland  |e verfasserin  |4 aut 
700 1 |a Tsud, Nataliya  |e verfasserin  |4 aut 
700 1 |a Kalinovych, Viacheslav  |e verfasserin  |4 aut 
700 1 |a Jiang, San Ping  |e verfasserin  |4 aut 
700 1 |a Dai, Liming  |e verfasserin  |4 aut 
700 1 |a Wang, Shuangyin  |e verfasserin  |4 aut 
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