Boron and nitrogen dual-doped carbon nanospheres for efficient electrochemical reduction of N2 to NH3

2020 ◽  
Vol 56 (3) ◽  
pp. 446-449 ◽  
Author(s):  
Shenglin Xiao ◽  
Fang Luo ◽  
Hao Hu ◽  
Zehui Yang
Keyword(s):  
Electrochemical Reduction ◽  
Reduction Reaction ◽  
Carbon Nanospheres ◽  
Faradaic Efficiency ◽  
Nitrogen Reduction ◽  
Yield Rate ◽  
Acidic Electrolyte

Boron and nitrogen dual-doped carbon nanospheres show exceptional nitrogen reduction reaction activity, with an NH3 yield rate of 15.7 μgNH3 h−1 mgcat.−1 and Faradaic efficiency of 8.1% at −0.4 V vs. RHE in acidic electrolyte.

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 Efficient electrocatalytic nitrogen reduction to ammonia with aqueous silver nanodots

2021 ◽  
Vol 4 (1) ◽  
Author(s):  
Wenyi Li ◽  
Ke Li ◽  
Yixing Ye ◽  
Shengbo Zhang ◽  
Yanyan Liu ◽  
...  
Keyword(s):  
Active Sites ◽  
Theoretical Calculations ◽  
Current Collector ◽  
Electrochemical Reactor ◽  
Reduction Reaction ◽  
Solution Ph ◽  
Faradaic Efficiency ◽  
Yield Rate ◽  
Silver Nanodots ◽  
Ti Mesh

AbstractThe electrocatalytic nitrogen (N2) reduction reaction (NRR) relies on the development of highly efficient electrocatalysts and electrocatalysis systems. Herein, we report a non-loading electrocatalysis system, where the electrocatalysts are dispersed in aqueous solution rather than loading them on electrode substrates. The system consists of aqueous Ag nanodots (AgNDs) as the catalyst and metallic titanium (Ti) mesh as the current collector for electrocatalytic NRR. The as-synthesized AgNDs, homogeneously dispersed in 0.1 M Na2SO4 solution (pH = 10.5), can achieve an NH3 yield rate of 600.4 ± 23.0 μg h−1 mgAg−1 with a faradaic efficiency (FE) of 10.1 ± 0.7% at −0.25 V (vs. RHE). The FE can be further improved to be 20.1 ± 0.9% at the same potential by using Ti mesh modified with oxygen vacancy-rich TiO2 nanosheets as the current collector. Utilizing the aqueous AgNDs catalyst, a Ti plate based two-electrode configured flow-type electrochemical reactor was developed to achieve an NH3 yield rate of 804.5 ± 30.6 μg h−1 mgAg−1 with a FE of 8.2 ± 0.5% at a voltage of −1.8 V. The designed non-loading electrocatalysis system takes full advantage of the AgNDs’ active sites for N2 adsorption and activation, following an alternative hydrogenation mechanism revealed by theoretical calculations.

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.

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 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.

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>

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