scholarly journals Boosting Electrochemical Nitrogen Reduction Performance over Binuclear Mo Atoms on N-Doped Nanoporous Graphene: A Theoretical Investigation

Molecules ◽  
2019 ◽  
Vol 24 (9) ◽  
pp. 1777 ◽  
Author(s):  
Ruijie Guo ◽  
Min Hu ◽  
Weiqing Zhang ◽  
Jia He
Keyword(s):  
Free Energy ◽  
Binding Free Energy ◽  
Product Yield ◽  
Reduction Reaction ◽  
Ambient Conditions ◽  
Present Contribution ◽  
Faradaic Efficiency ◽  
Nitrogen Reduction ◽  
Mo Catalyst ◽  
Nanoporous Graphene

Exploration of efficient catalysts is a priority for the electrochemical nitrogen reduction reaction (NRR) in order to receive a high product yield rate and faradaic efficiency of NH3, under ambient conditions. In the present contribution, the binding free energy of N2, NNH, and NH2 were used as descriptors to screen the potential NRR electrocatalyst among different single or binuclear transition metal atoms on N-doped nanoporous graphene. Results showed that the binuclear Mo catalyst might exhibit the highest catalytic activity. Further free energy profiles confirmed that binuclear Mo catalysts possess the lowest potential determining step (hydrogenation of NH2* to NH3). The improved activities could be ascribed to a down-shift of the density of states for Mo atoms. This investigation could contribute to the design of a highly active NRR electrocatalyst.

Highly efficient electrochemical ammonia synthesis via nitrogen reduction reactions on a VN nanowire array under ambient conditions

2018 ◽  
Vol 54 (42) ◽  
pp. 5323-5325 ◽  
Author(s):  
Xiaoping Zhang ◽  
Rong-Mei Kong ◽  
Huitong Du ◽  
Lian Xia ◽  
Fengli Qu
Keyword(s):  
High Performance ◽  
Ammonia Synthesis ◽  
Nanowire Array ◽  
Reduction Reaction ◽  
Carbon Cloth ◽  
Ambient Conditions ◽  
Faradaic Efficiency ◽  
Nitrogen Reduction ◽  
Highly Efficient ◽  
High Ammonia

A VN nanowire array on carbon cloth (VN/CC) as a high-performance catalyst for the nitrogen reduction reaction (NRR) affords high ammonia yield (2.48 × 10−10 mol−1 s−1 cm−2) and faradaic efficiency (3.58%) at −0.3 V versus RHE in 0.1 M HCl.

scholarly journals Mechanistic Insight into High Yield Electrochemical Nitrogen Reduction to Ammonia using Lithium Ions

2019 ◽  
Author(s):  
Anku Guha ◽  
Sreekanth Narayanru ◽  
Nisheal M. Kaley ◽  
D. Krishna Rao ◽  
Jagannath Mondal ◽  
...  
Keyword(s):  
Hydrogen Generation ◽  
Reduction Reaction ◽  
High Yield ◽  
Ambient Conditions ◽  
Faradaic Efficiency ◽  
Nitrogen Reduction ◽  
Mechanistic Insight ◽  
Working Electrode ◽  
Hydrogen Carrier ◽  
Scientific Attention

<p>Development of methods for economically feasible greener ammonia (NH<sub>3</sub>) production is gaining tremendous scientific attention. NH<sub>3</sub> has its importance in fertilizer industry and it is envisaged as a safer liquid hydrogen carrier for futuristic energy resources. Here, an aqueous electrolysis based NH<sub>3</sub> production in ambient conditions is reported, which yields high faradaic efficiency (~12%) NH<sub>3 </sub><i>via</i> nitrogen reduction reaction (NRR) at lower over potentials (~ -0.6V <i>vs.</i> RHE or -1.1V <i>vs.</i> Ag/AgCl). Polycrystalline copper (Cu) and gold (Au) are used as electrodes for electrochemical NRR, where the electrolyte which yields high amount of NH<sub>3 </sub>(~41 µmol/L) is 5M LiClO<sub>4</sub> in water with Cu as working electrode. A detailed study conducted here establishes the role of Li<sup>+</sup> in stabilizing nitrogen near to the working electrode - augmenting the NRR in comparison to its competitor - hydrogen evolution reaction, and a mechanistic insight in to the phenomenon is provided. <sup>15</sup>N<sub>2</sub> assisted labeling experiments are also conducted to confirm the formation of ammonia <i>via</i> NRR. This study opens up the possibilities of developing economically feasible electrodes for electrochemical NRR at lower energies with only transient modifications of electrodes during the electrolysis, unlike the studies reported on complex electrodes or electrolytes designed for NRR in aqueous medium to suppress the hydrogen generation. </p>

Mechanistic Insight into High Yield Electrochemical Nitrogen Reduction to Ammonia using Lithium Ions

2019 ◽  
Author(s):  
Anku Guha ◽  
Sreekanth Narayanru ◽  
Nisheal M. Kaley ◽  
D. Krishna Rao ◽  
Jagannath Mondal ◽  
...  
Keyword(s):  
Hydrogen Generation ◽  
Reduction Reaction ◽  
High Yield ◽  
Ambient Conditions ◽  
Faradaic Efficiency ◽  
Nitrogen Reduction ◽  
Mechanistic Insight ◽  
Working Electrode ◽  
Hydrogen Carrier ◽  
Scientific Attention

<p>Development of methods for economically feasible greener ammonia (NH<sub>3</sub>) production is gaining tremendous scientific attention. NH<sub>3</sub> has its importance in fertilizer industry and it is envisaged as a safer liquid hydrogen carrier for futuristic energy resources. Here, an aqueous electrolysis based NH<sub>3</sub> production in ambient conditions is reported, which yields high faradaic efficiency (~12%) NH<sub>3 </sub><i>via</i> nitrogen reduction reaction (NRR) at lower over potentials (~ -0.6V <i>vs.</i> RHE or -1.1V <i>vs.</i> Ag/AgCl). Polycrystalline copper (Cu) and gold (Au) are used as electrodes for electrochemical NRR, where the electrolyte which yields high amount of NH<sub>3 </sub>(~41 µmol/L) is 5M LiClO<sub>4</sub> in water with Cu as working electrode. A detailed study conducted here establishes the role of Li<sup>+</sup> in stabilizing nitrogen near to the working electrode - augmenting the NRR in comparison to its competitor - hydrogen evolution reaction, and a mechanistic insight in to the phenomenon is provided. <sup>15</sup>N<sub>2</sub> assisted labeling experiments are also conducted to confirm the formation of ammonia <i>via</i> NRR. This study opens up the possibilities of developing economically feasible electrodes for electrochemical NRR at lower energies with only transient modifications of electrodes during the electrolysis, unlike the studies reported on complex electrodes or electrolytes designed for NRR in aqueous medium to suppress the hydrogen generation. </p>

Zr-doped α-FeOOH with High Faradaic Efficiency for Electrochemical Nitrogen Reduction Reaction

2021 ◽  
pp. 150801
Author(s):  
Jiabin Tan ◽  
Xiaobo H ◽  
Fengxiang Yin ◽  
Xin Liang ◽  
Guoru Li ◽  
...  
Keyword(s):  
Reduction Reaction ◽  
Faradaic Efficiency ◽  
Nitrogen Reduction

scholarly journals Communication—Partial Oxidation of MnS for Synergistic Electrocatalysis of N2-to-NH3 Fixation at Ambient Conditions

2021 ◽  
Author(s):  
Peiei Li ◽  
Dan Cheng ◽  
Xiaohua Zhu ◽  
Meiling Liu ◽  
Youyu Zhang
Keyword(s):  
Partial Oxidation ◽  
Reduction Reaction ◽  
Ambient Conditions ◽  
Faradaic Efficiency ◽  
Bosch Process ◽  
Ambient Nh3 ◽  
Reaction Performance ◽  
Excellent Selectivity

Abstract Compared with the traditional Haber-Bosch process, electrochemical N2-to-NH3 reduction affords an eco-friendly and sustainable alternative to ambient NH3 synthesis with the aid of efficient electrocatalysts. In this work, partial oxidation of MnS to obtain the MnS-Mn3O4 is proved as a promising noble-free electrocatalysts of N2to NH3 fixation at ambient conditions. When tested in 0.1 M Na2SO4, the electrochemical N2 reduction reaction performance of MnS-Mn3O4 is improved comparing with the MnS, which achieves large NH3 yield of 16.74 μg h–1 mgcat.–1 and a high Faradaic efficiency of 5.72%. It also exhibits excellent selectivity of N2-to-NH3 and strong long-term electrochemical stabil

scholarly journals Adsorption-regulated precise synthesis of atomically-dispersed bimetallic Fe-Co sites on carbon for electrocatalytic nitrogen reduction reaction

2021 ◽  
Author(s):  
Shengbo Zhang ◽  
Miaomiao Han ◽  
Tongfei Shi ◽  
Haimin Zhang ◽  
Yue Lin ◽  
...  
Keyword(s):  
Bacterial Cellulose ◽  
Reduction Reaction ◽  
Single Atom ◽  
Synthetic Approach ◽  
New Paradigm ◽  
Faradaic Efficiency ◽  
Nitrogen Reduction ◽  
Site Density

Abstract The intriguing features of single-atom catalysts (SACs) could bring catalysis into a new paradigm, however, controllably synthesising SACs with desired SA loadings and coordination forms are challenging. Here, we report an adsorption-regulated approach to precisely control the synthesis of bimetallic Fe-Co SAs on carbon. Bacterial cellulose (BC) is utilised as an adsorption regulator to controllably impregnate Fe3+/Co2+ on BC and through carbonisation to anchor Fe-Co SAs on BC-derived carbon via bimetallic [(O-C2)3Fe-Co(O-C2)3] coordination with desired Fe/Co contents and atomic ratios. Under electrocatalytic nitrogen reduction reaction (NRR) conditions, [(O-C2)3Fe-Co(O-C2)3] is operando transformed to [(O-C2)3Fe-Co(O-C)C2] that promotes and sustains NRR performance. A superb ammonia yield of 574.8 ± 35.3 μg h-1 mgcat.-1 with an exceptional faradaic efficiency of 73.2 ± 4.6% are obtained from an electrocatalyst with the highest bimetallic Fe-Co site density. The exemplified synthetic approach would be of generically applicable to controllably anchor SAs on carbon that enables meaningfully investigate and rationally design SACs.

p-Block Element-doped Silicon Nanowires for Nitrogen Reduction Reaction: A DFT Study

Nanoscale ◽  
2021 ◽  
Author(s):  
Zhongyuan Guo ◽  
Lakshitha Jasin Arachchige ◽  
Siyao Qiu ◽  
Xiao Li Zhang ◽  
Yongjun Xu ◽  
...  
Keyword(s):  
Silicon Nanowires ◽  
Reduction Reaction ◽  
Dft Study ◽  
Block Element ◽  
Ambient Conditions ◽  
Nitrogen Reduction ◽  
Green Route ◽  
Doped Silicon

Photocatalytic nitrogen reduction reaction (NRR) is a promising, green route to chemically reducing N2 into NH3 under ambient conditions, correlating to the N2 fixation process of nitrogenase enzymes. To achieve...

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