302-01-2Relevant articles and documents
Rational design of bimetallic Rh0.6Ru0.4nanoalloys for enhanced nitrogen reduction electrocatalysis under mild conditions
Zhao, Lei,Liu, Xuejing,Zhang, Shen,Zhao, Jie,Xu, Xiaolong,Du, Yu,Sun, Xu,Zhang, Nuo,Zhang, Yong,Ren, Xiang,Wei, Qin
supporting information, p. 259 - 263 (2021/01/14)
As a carbon-free reaction process, the electrocatalytic nitrogen reduction reaction (eNRR) under mild conditions has broad prospects for green and sustainable NH3 production. In this work, bimetallic RhRu nanoalloys (NAs) with cross-linked curly nanosheets were successfully prepared and exhibited exciting results in the eNRR process. Furthermore, the composition effect of RhRu NAs on eNRR activity was studied systematically, and the results showed that Rh0.6Ru0.4 NAs/CP exhibited the highest NH3 yield rate of 57.75 μg h-1 mgcat.-1 and faradaic efficiency of 3.39%. As an eNRR catalyst with great potential, Rh0.6Ru0.4 NAs extend the possibility of alloy-nanomaterials in the eNRR field and further provide an idea for the precise structure of more effective and stable electrocatalysts.
Enhancing electrocatalytic nitrogen reduction to ammonia with rare earths (La, Y, and Sc) on high-index faceted platinum alloy concave nanocubes
Chen, You-Hu,Jiang, Xin,Liao, Hong-Gang,Liu, Feng,Mao, Yu-Jie,Sheng, Tian,Sun, Shi-Gang,Wei, Lu,Ye, Jin-Yu,Zhao, Xin-Sheng
, p. 26277 - 26285 (2021/12/10)
Surface structure effect is the key subject in electrocatalysis, and consists of the structure dependence of interaction between reaction molecules and the catalyst surface in specifying the surface atomic arrangement, chemical composition and electronic structure. Herein, we develop a controllable synthesis of Pt-RE (RE = La, Y, Sc) alloy concave nanocubes (PtRENCs) with {410} high-index facets (HIFs) by an electrochemical method in a choline chloride-urea based deep eutectic solvent. The PtRENCs are used as an efficient catalyst in electrocatalytic nitrogen reduction to ammonia (NH3). Owing to the high density of low-coordinated Pt step sites (HIF structure) and the unique electronic effect of Pt-RE, the as-prepared PtRENCs exhibit an excellent electrocatalytic performance for the nitrogen reduction reaction (NRR) under ambient conditions. The NH3 yield rate and faradaic efficiency (FE) share the same trend of Pt-La (rNH3: 71.4 μg h-1 μgcat-1, FE: 35.6%) > Pt-Y (rNH3: 65.2 μg h-1 μgcat-1, FE: 26.7%) > Pt-Sc (rNH3: 48.5 μg h-1 μgcat-1, FE: 19%) > Pt (rNH3: 25.8 μg h-1 μgcat-1, FE: 10.7%). Moreover, the PtRENCs demonstrate high selectivity for N2 reduction to NH3 and high stability retaining 90% of the NH3 yield rate and FE values after 12 h continuous NRR tests. Density functional theory (DFT) calculations indicate that the rate determining step of the NRR process is the formation of N2H2? from N2 with the transfer of two proton-coupled electrons, and the upshift of the d-band center boosts the NRR activity by enhancing the bonding strength of reaction intermediates on the high-index faceted Pt-RE (RE = La, Y, Sc) alloying surface. In addition, the introduction of RE (RE = La, Y, Sc) on the Pt step surface can effectively suppress the HER process and provide appropriate sites for the NRR. This journal is
Rigid two-dimensional indium metal-organic frameworks boosting nitrogen electroreduction at all pH values
Chen, Sheng,Ding, Shan,Duan, Jingjing,Sun, Yuntong,Xia, Baokai,Yu, Licheng
supporting information, p. 20040 - 20047 (2021/09/20)
Based on an ion exchange and dissolution-recrystallization mechanism, rigid indium metal-organic framework (In-MOF) nanosheets have been synthesized under mild conditions. The collective advantages of the rigid structure and two-dimensional architecture (thickness: 1.3 nm) enable In-MOF to show great activity during nitrogen electroreduction and excellent stability over a wide pH range. At pH values ?1mg?1(or 4.94 μg h?1cm?2) and faradic efficiency ≥6.72%. At pH values ≥7, 2D In-MOF can operate efficiently with a record NH3yield of 79.20 μg h?1mg?1(or 15.94 μg h?1cm?2) and faradic efficiency of 14.98%, making it one of the most active MOF-based electrocatalysts for nitrogen electroreduction. Furthermore, the reaction mechanism of nitrogen electroreduction has been revealed using density function theory (DFT) simulations, and it follows enzymatic pathways at all pH values, with the potential determining step being *H2NNH2* → *NH2+ NH3. It is expected that the present study will offer valuable clues for the design and fabrication of low-cost and efficient all-pH nitrogen reduction electrocatalysts for industrial applications.
