纳米花
多金属氧酸盐
石墨烯
电催化剂
双金属片
氧化物
电化学
化学工程
材料科学
水热合成
无机化学
可逆氢电极
金属有机骨架
产量(工程)
氨
氨硼烷
法拉第效率
化学
催化作用
纳米技术
制氢
热液循环
电极
有机化学
吸附
工作电极
冶金
物理化学
工程类
作者
Zemin Feng,Gang Li,Xinming Wang,Carlos J. Gómez‐García,Jianjiao Xin,Huiyuan Ma,Haijun Pang,Kaixiong Gao
标识
DOI:10.1016/j.cej.2022.136797
摘要
The electrocatalytic nitrogen reduction reaction (NRR) provides a promising way for storage and sustainable utilization of ammonia. In order to reduce the cost of ammonia synthesis and promote large-scale production, it is very important to develop stable and highly active electrocatalysts. In this work, we demonstrate an iron-based metal–organic framework (MIL-100) and molybdenum-based polyoxometalate (PMo12) host–guest-assisted strategy for synthesizing nanostructured bimetallic sulfides through a one-pot hydrothermal synthesis process. FeS2/MoS2 particles are evenly distributed on reduced graphene oxide (RGO) with high conductivity, forming a well-defined nanoflower structure. Benefiting from the synergistic effect of FeS2, MoS2 (with inherent rich catalytically active sites and uniform nanoflower structure) and RGO, the as-synthesized FeS2/MoS2@RGO achieves electrocatalytic activity and stability towards NRR in both basic and acidic solutions. The electrochemical results show a high Faradaic efficiency (FE) of 38.6 % and NH3 yield rate of 41.1 μg h−1 mgcat-1 at −0.2 V with respect to a reversible hydrogen electrode (RHE) in acidic potassium sulfate, and FE of 9.62 % and NH3 yield rate of 10.35 μg h−1 mgcat–1 at −0.4 V vs. RHE in alkaline potassium hydroxide solution at room temperature. Density functional theory (DFT) calculation indicates that NRR on FeS2/MoS2 has optimized nitrogen binding and ammonia release which promotes the fast kinetics process through the distal mechanism, and the protonation of N2 to form *N2H species is the rate-determining step (RDS) with the maximum ΔG values (+0.43 eV). This work develop a general and promising method for the design of efficient and low cost pH-universal NRR electrocatalysts.
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