scholarly journals High-Throughput Screening Single-Atom Alloy for Electroreduction of Dinitrogen to Ammonia

2021 ◽  
Author(s):  
Guokui Zheng ◽  
Ziqi Tian ◽  
Xingwang Zhang ◽  
Liang Chen ◽  
Xu Qian ◽  
...  
Keyword(s):  
High Throughput Screening ◽  
Density Functional ◽  
Ammonia Synthesis ◽  
Density Functional Theory Calculations ◽  
Reduction Reaction ◽  
Single Atom ◽  
Functional Theory ◽  
Metal Doped ◽  
Single Atom Alloy ◽  
Single Atom Alloys

<p></p><p>Exploring electrocatalyst with high activity, selectivity and stability is essential for development of applicable electrocatalytic ammonia synthesis technology. By performing density functional theory calculations, we systematically investigated a series of transition-metal doped Au-based single atom alloys (SAAs) as promising electrocatalysts for nitrogen reduction reaction (NRR). For Au-based electrocatalyst, the first hydrogenation step (*N<sub>2</sub>→*NNH) normally determines the limiting potential of the overall reaction process. Compared with pristine Au(111) surface, introducing single atom can significantly enhance the binding strength of N<sub>2</sub>, leading to decreased energy barrier of the key step, i.e., ΔG(*N<sub>2</sub>→*NNH). According to simulation results, three descriptors were proposed to describe ΔG(*N<sub>2</sub>→*NNH), including ΔG(*NNH), <i>d</i>-band center, and . Eight doped elements (Ti, V, Nb, Ru, Ta, Os, W, and Mo) were initially screened out with limiting potential ranging from -0.75V to -0.30 V. Particularly, Mo- and W-doped systems possess the best activity with limiting potentials of -0.30 V, respectively. Then the intrinsic relationship between structure and the potential performance was further analyzed by using machine-learning. The selectivity, feasibility, stability of these candidates were also evaluated, confirming that SAA containing Mo, Ru ,Ta, and W could be outstanding NRR electrocatalysts. This work not only broadens the understating of SAA application in electrocatalysis, but also devotes to the discovery of novel NRR electrocatalysts.</p><br><p></p>

scholarly journals High-Throughput Screening Single-Atom Alloy for Electroreduction of Dinitrogen to Ammonia

2021 ◽  
Author(s):  
Guokui Zheng ◽  
Ziqi Tian ◽  
Xingwang Zhang ◽  
Liang Chen ◽  
Xu Qian ◽  
...  
Keyword(s):  
High Throughput Screening ◽  
Density Functional ◽  
Ammonia Synthesis ◽  
Density Functional Theory Calculations ◽  
Reduction Reaction ◽  
Single Atom ◽  
Functional Theory ◽  
Metal Doped ◽  
Single Atom Alloy ◽  
Single Atom Alloys

<p></p><p>Exploring electrocatalyst with high activity, selectivity and stability is essential for development of applicable electrocatalytic ammonia synthesis technology. By performing density functional theory calculations, we systematically investigated a series of transition-metal doped Au-based single atom alloys (SAAs) as promising electrocatalysts for nitrogen reduction reaction (NRR). For Au-based electrocatalyst, the first hydrogenation step (*N<sub>2</sub>→*NNH) normally determines the limiting potential of the overall reaction process. Compared with pristine Au(111) surface, introducing single atom can significantly enhance the binding strength of N<sub>2</sub>, leading to decreased energy barrier of the key step, i.e., ΔG(*N<sub>2</sub>→*NNH). According to simulation results, three descriptors were proposed to describe ΔG(*N<sub>2</sub>→*NNH), including ΔG(*NNH), <i>d</i>-band center, and . Eight doped elements (Ti, V, Nb, Ru, Ta, Os, W, and Mo) were initially screened out with limiting potential ranging from -0.75V to -0.30 V. Particularly, Mo- and W-doped systems possess the best activity with limiting potentials of -0.30 V, respectively. Then the intrinsic relationship between structure and the potential performance was further analyzed by using machine-learning. The selectivity, feasibility, stability of these candidates were also evaluated, confirming that SAA containing Mo, Ru ,Ta, and W could be outstanding NRR electrocatalysts. This work not only broadens the understating of SAA application in electrocatalysis, but also devotes to the discovery of novel NRR electrocatalysts.</p><br><p></p>

Two-dimensional metal-organic frameworks Mo3(C2O)12 as promising single-atom catalysts for selective nitrogen-to-ammonia

2022 ◽  
Author(s):  
Zhen Feng ◽  
Zelin Yang ◽  
Xiaowen Meng ◽  
Fachuang Li ◽  
Zhanyong Guo ◽  
...  
Keyword(s):  
Density Functional Theory ◽  
Density Functional ◽  
Metal Organic Frameworks ◽  
Density Functional Theory Calculations ◽  
Reduction Reaction ◽  
Single Atom ◽  
Two Dimensional ◽  
Functional Theory ◽  
New Family ◽  
Metal Organic

The development of single-atom catalysts (SACs) for electrocatalytic nitrogen reduction reaction (NRR) remains a great challenge. Using density functional theory calculations, we design a new family of two-dimensional metal-organic frameworks...

scholarly journals Electrochemical ammonia synthesis via nitrate reduction on Fe single atom catalyst

2021 ◽  
Vol 12 (1) ◽  
Author(s):  
Zhen-Yu Wu ◽  
Mohammadreza Karamad ◽  
Xue Yong ◽  
Qizheng Huang ◽  
David A. Cullen ◽  
...  
Keyword(s):  
Nitrate Reduction ◽  
Density Functional ◽  
Ammonia Synthesis ◽  
Reaction Pathway ◽  
Density Functional Theory Calculations ◽  
Single Atom ◽  
Functional Theory ◽  
Faradaic Efficiency ◽  
Yield Rate ◽  
Water Pollutant

AbstractElectrochemically converting nitrate, a widespread water pollutant, back to valuable ammonia is a green and delocalized route for ammonia synthesis, and can be an appealing and supplementary alternative to the Haber-Bosch process. However, as there are other nitrate reduction pathways present, selectively guiding the reaction pathway towards ammonia is currently challenged by the lack of efficient catalysts. Here we report a selective and active nitrate reduction to ammonia on Fe single atom catalyst, with a maximal ammonia Faradaic efficiency of ~ 75% and a yield rate of up to ~ 20,000 μg h−1 mgcat.−1 (0.46 mmol h−1 cm−2). Our Fe single atom catalyst can effectively prevent the N-N coupling step required for N2 due to the lack of neighboring metal sites, promoting ammonia product selectivity. Density functional theory calculations reveal the reaction mechanisms and the potential limiting steps for nitrate reduction on atomically dispersed Fe sites.

Conductive two-dimensional M3(C6S3O3)2 monolayers as effective electrocatalysts for oxygen reduction reaction

2021 ◽  
Author(s):  
Tianchun Li ◽  
Manman Li ◽  
Xinyue Zhu ◽  
Juan Zhang ◽  
Yu Jing
Keyword(s):  
Oxygen Reduction Reaction ◽  
Oxygen Reduction ◽  
Density Functional ◽  
Metal Organic Frameworks ◽  
Density Functional Theory Calculations ◽  
Reduction Reaction ◽  
Single Atom ◽  
Two Dimensional ◽  
Functional Theory ◽  
Metal Organic

Two dimensional (2D) conjugated metal organic frameworks (MOFs) which feature single atom catalysts are promising electrocatalysts to promote oxygen reduction reaction (ORR). Here, by means of density functional theory calculations...

Ruthenium single-atom catalysis for electrocatalytic nitrogen reduction unveiled by grand canonical density functional theory

2020 ◽  
Vol 8 (39) ◽  
pp. 20402-20407
Author(s):  
Yujin Ji ◽  
Yifan Li ◽  
Huilong Dong ◽  
Lifeng Ding ◽  
Youyong Li
Keyword(s):  
Density Functional Theory ◽  
Density Functional ◽  
Density Functional Theory Calculations ◽  
Catalytic Site ◽  
Single Atom ◽  
Functional Theory ◽  
Nitrogen Reduction ◽  
Grand Canonical

Grand canonical density functional theory calculations reveal that the Ru–N4 motif is the superior catalytic site for eNRR rather than the Ru–N3 motif.

scholarly journals Exposed facet-controlled N2 electroreduction on distinct Pt3Fe nanostructures of nanocubes, nanorods and nanowires

2020 ◽  
Author(s):  
Wu Tong ◽  
Bolong Huang ◽  
Pengtang Wang ◽  
Qi Shao ◽  
Xiaoqing Huang
Keyword(s):  
Density Functional ◽  
Density Functional Theory Calculations ◽  
Active Surface ◽  
Reduction Reaction ◽  
Active Surface Area ◽  
Hydrogen Electrode ◽  
Functional Theory ◽  
Effective Strategies ◽  
Exposed Facet ◽  
Coupling Correlation

Abstract Understanding the correlation between exposed surfaces and performances of controlled nanocatalysts can aid effective strategies to enhance electrocatalysis, but this is as yet unexplored for the nitrogen reduction reaction (NRR). Here, we first report controlled synthesis of well-defined Pt3Fe nanocrystals with tunable morphologies (nanocube, nanorod and nanowire) as ideal model electrocatalysts for investigating the NRR on different exposed facets. The detailed electrocatalytic studies reveal that the Pt3Fe nanocrystals exhibit shape-dependent NRR electrocatalysis. The optimized Pt3Fe nanowires bounded with high-index facets exhibit excellent selectivity (no N2H4 is detected), high activity with NH3 yield of 18.3 μg h−1 mg−1cat (0.52 μg h−1 cm−2ECSA; ECSA: electrochemical active surface area) and Faraday efficiency of 7.3% at −0.05 V versus reversible hydrogen electrode, outperforming the {200} facet-enclosed Pt3Fe nanocubes and {111} facet-enclosed Pt3Fe nanorods. They also show good stability with negligible activity change after five cycles. Density functional theory calculations reveal that, with high-indexed facet engineering, the Fe-3d band is an efficient d-d coupling correlation center for boosting the Pt 5d-electronic exchange and transfer activities towards the NRR.

scholarly journals Composition and electronic structure of Mn3O4 and Co3O4 cathodes in zinc/air batteries: a DFT study

2021 ◽  
Author(s):  
Fernanda Juarez ◽  
Hui Yin ◽  
Axel Gross
Keyword(s):  
Gas Phase ◽  
Density Functional ◽  
Density Functional Theory Calculations ◽  
Reduction Reaction ◽  
Operating Conditions ◽  
Active Centers ◽  
Functional Theory ◽  
Pourbaix Diagrams ◽  
Grand Canonical ◽  
Zinc Air Batteries

The surface structures of promising cathode materials for zinc-air batteries, Mn3O4 and Co3O4, have been systematically studied under operating conditions by density functional theory calculations. The environment has been taken into account using grand-canonical schemes both for gas-phase and electrochemical conditions. By analysing the structures appearing in the calculated phase diagrams and Pourbaix diagrams in detail, we derive the factors underlying their stability in the gas phase and under electrochemical conditions. Changes in charge, oxidation states and spin states of the metal cations on the surface are discussed and their feasibility as active centers for the oxygen evolution and reduction reaction is thoroughly analyzed.

The oxygen reduction reaction mechanism on Pt(111) from density functional theory calculations

2010 ◽  
Vol 55 (27) ◽  
pp. 7975-7981 ◽  
Author(s):  
Vladimir Tripković ◽  
Egill Skúlason ◽  
Samira Siahrostami ◽  
Jens K. Nørskov ◽  
Jan Rossmeisl
Keyword(s):  
Density Functional Theory ◽  
Reaction Mechanism ◽  
Oxygen Reduction Reaction ◽  
Oxygen Reduction ◽  
Density Functional ◽  
Density Functional Theory Calculations ◽  
Reduction Reaction ◽  
Functional Theory

The synergetic effect of aqua ligand and metal site on performance of single-atom catalysts in H2O2 synthesis: a Density Functional Theory Study

2022 ◽  
Author(s):  
Xin-Chen Zhu ◽  
Wei Zhang ◽  
Qian Xia ◽  
Anfu Hu ◽  
Jian Jiang ◽  
...  
Keyword(s):  
Density Functional Theory ◽  
Density Functional ◽  
Rational Design ◽  
Synergetic Effect ◽  
Density Functional Theory Calculations ◽  
Single Atom ◽  
Density Functional Theory Study ◽  
Functional Theory ◽  
Metal Site ◽  
Coordination Field

To study the effect of coordination field on catalytic property is critical for rational design of outstanding electrocatalyst for H2O2 synthesis. Herein, via density functional theory calculations, we built an...

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