journal article·2023-10-13

Lithium-Mediated Photoelectrochemical Ammonia Synthesis with 95% Selectivity on Silicon Photocathode

Hao Huang, Wenguang Tu, Liping Fang, Yelan Xiao, Feng Niu, Heng Zhu, Xi Zhu, Lu Wang, Yujie Xiong, Jianyong Feng, Huaiguang Li, Mingjian Zhang, Yongcai Zhang, Yingfang Yao, Yong Zhou, Hong Li, Zhigang Zou

ACS Energy Letters· Volume 8· Issue 10
Publisher page

Abstract

Ammonia synthesis via the energy-intensive Haber–Bosch process contributes to ∼1.8% global carbon emission. To this end, photoelectrochemical (PEC) ammonia synthesis using solar energy is an attractive alternative technique to significantly reduce carbon emission. Nevertheless, the PEC process is still limited by the low Faradaic efficiency and insufficient ammonia formation rate. Herein, we report a lithium-mediated PEC device composed of a Si photocathode and Li ions as the reduction mediator to show efficient nitrogen reduction into ammonia with a Faradaic efficiency of 95% and an ammonia yield rate of 52.4 μg cm –2 h –1 under ambient conditions. Our mechanistic studies reveal that the Si photocathode under light illumination provides photogenerated electrons to reduce Li + ions into metallic Li and then initiates the Li-mediated nitrogen reduction process, where the solid electrolyte interphase (SEI) facilitates homogeneous lithium plating. This work offers a promising solar-driven catalytic system for ammonia synthesis under ambient conditions.
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Research context

OpenAlex topics: Ammonia Synthesis and Nitrogen Reduction · Advanced Photocatalysis Techniques · Hydrogen Storage and Materials

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

School of Science and Engineering, The Chinese University of Hong Kong, Shenzhen 518172, Guangdong, People’s Republic of China

School of Chemistry and Materials Science, University of Science and Technology of China, Hefei 230026, Anhui, People’s Republic of China

College of Engineering and Applied Sciences, Nanjing University, Nanjing 210093, Jiangsu, People’s Republic of China

School of Chemistry and Chemical Engineering, Yangzhou University, Yangzhou 225009, Jiangsu, People’s Republic of China

Kunshan Innovation Institute of Nanjing University, Kunshan 215347, Jiangsu, People’s Republic of China

Jiangsu Key Laboratory for Nano Technology, National Laboratory of Solid State Microstructures, Collaborative Innovation Center of Advanced Microstructures, School of Physics, Nanjing University, Nanjing 210093, Jiangsu, People’s Republic of China

School of Chemical and Environmental Engineering, Anhui Polytechnic University, Wuhu 241002, Anhui, People’s Republic of China

School of Mechanical and Aerospace Engineering, Nanyang Technological University, Singapore 639798, Singapore

Funding

Guangdong Province Introduction of Innovative R&D Team · Natural Science Foundation of Shenzhen City · National Natural Science Foundation of China · University Development Fund · Shenzhen Key Laboratory of Eco-materials and Renewable Energy

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