Citation: Zirui Wang, Sihao Shen, Yupeng Han, Weihui Fang, Qiaohong Li, Jian Zhang. Theoretical study on the application of the largest aluminum-pyrazole ring in electrochemical nitrogen reduction reaction[J]. Chinese Chemical Letters, ;2023, 34(12): 108604. doi: 10.1016/j.cclet.2023.108604 shu

Theoretical study on the application of the largest aluminum-pyrazole ring in electrochemical nitrogen reduction reaction

Zirui Wang ^{a, b, d, 1} ,
Sihao Shen ^{a, c, 1} ,
Yupeng Han ^{a, c} ,
Weihui Fang ^{a, c, d, *,} ,
Qiaohong Li ^{a, c, d, *,} ,
Jian Zhang ^{a, c, d}

a.
State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou 350002, China
b.
School of Physical Science and Technology, ShanghaiTech University, Shanghai 201210, China
c.
Chinese Academy of Sciences, University of Chinese Academy of Sciences, Beijing 100049, China
d.
Fujian College, University of Chinese Academy of Sciences, Fuzhou 350002, China

fwh@fjirsm.ac.cn

lqh2382@fjirsm.ac.cn

Received Date: 17 March 2023
Revised Date: 22 May 2023
Accepted Date: 24 May 2023
Available Online: 25 May 2023

Figures(4)

Electrochemical nitrogen reduction reaction (NRR) is a mild and sustainable method for ammonia synthesis. Therefore, developing high activity, selectivity, and economic efficiency catalysts with considering the synergistic effects between catalysts and carriers to design novel structural models is very important. Considering the non-noble metal NRR catalyst, Mo₃, we tried to find a suitable carrier which is stable and economical. Herein, we used the largest atomically precise aluminum-pyrazole ring (AlOC-69) to date (diameter up to 2.3 nm). The larger ring cavities and the presence of abundant hydroxy groups make AlOC-69 an ideal molecular carrier model and provide a basis for studying its structure-activity relationship. The formation energy (−0.76 eV) and stable Mo-O bonds indicate that Mo₃ can be stabilized on the Al₁₀O₁₀ surface. Additionally, N₂ has fully activated due to the strong interaction between the p-orbital of N and the d-orbital of Mo. The low limiting potential (−0.28 V) emerges that Mo₃@Al₁₀O₁₀ has ideal catalytic activity and selectivity. This research provides a promising catalyst model and an understanding of its catalytic process at the atomic level, providing a new approach for the co-design of catalyst and carrier in NRR.
- Nitrogen reduction reaction,
- Hydrogen evolution reaction,
- Electrocatalysts,
- Density functional theory,
- Aluminum-pyrazole ring,
- Metal catalyst
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