Abstract:
An environmentally friendly alternative synthesis process is desired to produce NH3 with no CO2 emissions and low energy demand in a sustainable and ecological way in the future. The electrochemical method assisted by earth-abundant materials has been widely utilized for the chemical energy conversion. We have developed new earth-abundant layered structure 1T-molybdenum disulfide (MoS2) and iron pyrite (FeS2) based materials as active catalysts for electrochemically nitrogen reduction reaction. From electrochemical analysis, the Faraday efficiency of MoS2 and FeS2 for NRR can be achieve to~20% and 14% with good catalytic stability, respectively. The energy profile of the NRR reaction pathway on the catalysts will be performed by the density functional theoretical (DFT) calculation. Besides, there have been lots of studies on hydrogen evolution reaction (HER) catalytic activity using ultralow loading of Pt catalysts or even Pt single atom catalysts as well. However, Pt single atom deposited on the surface of the carbon or metal oxide material showed some drawbacks, such as high possibility of Pt desorption from the supported material in the electrolyte. Our work demonstrated that gold nanodendrites (Au NDs) with high facet surface was chosen as the supported materials for studying the relation between the low loading amount of Pt atoms and reaction mechanism of HER activity. Overall results provides a feasible approach to morphological control of metal sulfide and atomic deposition of Pt element on the specific substrate as active catalysts for NRR and HER applications, respectively.
Keywords - Nitrogen Reduction Reaction, Hydrogen Evolution Reaction, Molybdenum disulfide, Pt on Au nanodendrite, In-situ XRD analysis, X-ray absorption spectroscopy.
References:
[1] Ying-Huang Lai,* Sin-Ren Li,# Swathi M G,#Hsiao-Tzu Chang,# Yu-Bin Huang, Yen-Ken Li, Yu-Mei Chen, Shivaraj B. Patil, Shu-Yi Chang, Po-Kai Chen, Chia-Che Chang, Yi-Chia Chen, Chih-Wen Pao, Jeng-Lung Chen, Chuan-Yu Wei, I-Kuan Lin, Hung-Lung Chou, Chun-Jen Su, U-Ser Jeng, Tsung-Rong Kuo, Cheng-Yen Wen, Di-Yan Wang* J. Mater. Chem. A, 2021, 9, 22901-22912.
[2] Shivaraj B. Patil, Ting-Ran Liu, Hung-Lung Chou,* Yu‐Bin Huang, Chia-Che Chang, Yi-Chia Chen, Ying-Sheng Lin, Hsin Li, Yi-Cheng Lee, Yuan Jay Chang, Ying-Huang Lai, Cheng-Yen Wen, Di-Yan Wang* J. Phys. Chem. Lett. 2021, 12, 8121-8128.
[3] Shivaraj B. Patil, Hung-Lung Chou, Yu-Mei Chen, Shang-Hsien Hsieh, Chia-Hao Chen, Chia-Che Chang, Shin-Ren Li, Yi-Cheng Lee, Ying-Sheng Lin, Hsin Li,1 Yuan Jay Chang, Ying-Huang Lai, Di-Yan Wang* 2021: Enhanced N2 Affinity of 1T-MoS2 with Unique Pseudo Six-membered Ring Consisting of N—Li—S—Mo—S—Mo for High Ambient Ammonia Electrosynthesis Performance, J. Mater. Chem. A, 2021, 9, 1230–1239.
[4] Shivaraj B. Patil, Hsiang-Ju Liao and Di-Yan Wang* 2020: Challenges and Prospects of Polyatomic Ions Intercalation in the Graphite Layer for Energy Storage Applications, Phys. Chem. Chem. Phys., 2020, 22, 24842-24855. (Invited Review Article)
[5] Chia-Che Chang, Sin-Ren Li, Hung-Lung Chou,* Yi-Cheng Lee, Shivaraj Patil, Ying-Sheng Lin, Chun-Chih Chang, Yuan Jay Chang, and Di-Yan Wang*, 2019: Photoactive Earth-Abundant Iron Pyrite Catalysts for Electrocatalytic Nitrogen Reduction Reaction, Small. 2019, 15, 1904723.