Enhancing Green Ammonia Electrosynthesis Through Tuning Sn Vacancies in Sn-Based MXene/MAX Hybrids

Xinyu Dai; Zhen-Yi Du; Ying Sun; Ping Chen; Xiaoguang Duan; Junjun Zhang; Hui Li; Yang Fu; Baohua Jia; Lei Zhang; Wenhui Fang; Jieshan Qiu; Tianyi Ma

doi:10.1007/s40820-023-01303-2

Enhancing Green Ammonia Electrosynthesis Through Tuning Sn Vacancies in Sn-Based MXene/MAX Hybrids

Nanomicro Lett. 2024 Jan 16;16(1):89. doi: 10.1007/s40820-023-01303-2.

Authors

Xinyu Dai^#¹, Zhen-Yi Du^#², Ying Sun³, Ping Chen⁴, Xiaoguang Duan⁵, Junjun Zhang⁶, Hui Li⁷, Yang Fu⁷, Baohua Jia⁷, Lei Zhang⁸, Wenhui Fang⁹, Jieshan Qiu¹⁰, Tianyi Ma¹¹

Affiliations

¹ Key Laboratory for Green Synthesis and Preparative Chemistry of Advanced Materials of Liaoning Province, College of Chemistry, Institute of Clean Energy Chemistry, Liaoning University, Shenyang, 110036, People's Republic of China.
² State Key Laboratory of Clean and Efficient Coal Utilization, Taiyuan University of Technology, Taiyuan, 030024, People's Republic of China.
³ Key Laboratory for Green Synthesis and Preparative Chemistry of Advanced Materials of Liaoning Province, College of Chemistry, Institute of Clean Energy Chemistry, Liaoning University, Shenyang, 110036, People's Republic of China. yingsun@lnu.edu.cn.
⁴ School of Chemistry and Chemical Engineering, Anhui University, Hefei, 230601, People's Republic of China.
⁵ School of Chemical Engineering, The University of Adelaide, Adelaide, SA, 5005, Australia.
⁶ State Key Laboratory of High-Efficiency Utilization of Coal and Green Chemical Engineering, College of Chemistry and Chemical Engineering, Ningxia University, Yinchuan, 750021, Ningxia, People's Republic of China.
⁷ School of Science, RMIT University, Melbourne, VIC, 3000, Australia.
⁸ Guangdong Provincial Key Laboratory of Advanced Energy Storage Materials, School of Chemistry and Chemical Engineering, South China University of Technology, Guangzhou, 510640, People's Republic of China.
⁹ College of Chemical Engineering, State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, Beijing, 100029, People's Republic of China.
¹⁰ College of Chemical Engineering, State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, Beijing, 100029, People's Republic of China. qiujs@mail.buct.edu.cn.
¹¹ School of Science, RMIT University, Melbourne, VIC, 3000, Australia. tianyi.ma@rmit.edu.au.

^# Contributed equally.

Abstract

Renewable energy driven N₂ electroreduction with air as nitrogen source holds great promise for realizing scalable green ammonia production. However, relevant out-lab research is still in its infancy. Herein, a novel Sn-based MXene/MAX hybrid with abundant Sn vacancies, Sn@Ti₂CT_X/Ti₂SnC-V, was synthesized by controlled etching Sn@Ti₂SnC MAX phase and demonstrated as an efficient electrocatalyst for electrocatalytic N₂ reduction. Due to the synergistic effect of MXene/MAX heterostructure, the existence of Sn vacancies and the highly dispersed Sn active sites, the obtained Sn@Ti₂CT_X/Ti₂SnC-V exhibits an optimal NH₃ yield of 28.4 µg h^-1 mg_cat^-1 with an excellent FE of 15.57% at - 0.4 V versus reversible hydrogen electrode in 0.1 M Na₂SO₄, as well as an ultra-long durability. Noticeably, this catalyst represents a satisfactory NH₃ yield rate of 10.53 µg h^-1 mg^-1 in the home-made simulation device, where commercial electrochemical photovoltaic cell was employed as power source, air and ultrapure water as feed stock. The as-proposed strategy represents great potential toward ammonia production in terms of financial cost according to the systematic technical economic analysis. This work is of significance for large-scale green ammonia production.

Keywords: Green ammonia synthesis; MXene/MAX hybrid; N2 electroreduction; Renewable energy; Sn.