Cr3C2 Nanoparticles-Embedded Carbon Nanofiber for Artificial Synthesis of NH3 through N2 Fixation under Ambient Conditions.

Industrial production of NH3 heavily depends on the conventional Haber-Bosch process under rigorous conditions with a large amount of energy consumption and carbon emissions. Electrocatalysis exhibits an intriguing prospect for the N2 reduction reaction (NRR) at ambient conditions. Wherein, a high-efficiency and low-cost catalyst is paramount. In this letter, Cr3C2 nanoparticles and carbon nanofiber composite (Cr3C2@C NF) is proposed as a noble metal-free NRR electrocatalyst for converting N2 to NH3 c with an excellent selectivity. The optimal faradic efficiency and NH3 yield rate achieve as high as 8.6% and 23.9 μg h-1 mgcat.-1 at -0.3 V vs. reversible hydrogen electrode (RHE) in 0.1 M HCl. Theoretical calculations show a low reaction barrier of merely 0.53 eV in the enzymatic route for this catalyst.

[1]  Zhiming M. Wang,et al.  Recent progress in the electrochemical ammonia synthesis under ambient conditions , 2019, EnergyChem.

[2]  Tingshuai Li,et al.  Electrochemical synthesis of ammonia by zirconia-based catalysts at ambient conditions , 2019, Applied Catalysis A: General.

[3]  Hongyu Chen,et al.  Boron Nanosheet: An Elemental Two-Dimensional (2D) Material for Ambient Electrocatalytic N2-to-NH3 Fixation in Neutral Media , 2019, ACS Catalysis.

[4]  Song Gao,et al.  Fabricating hierarchically porous and Fe3C-embeded nitrogen-rich carbon nanofibers as exceptional electocatalysts for oxygen reduction , 2019, Carbon.

[5]  Haihui Wang,et al.  Efficient Electrocatalytic N2 Fixation with MXene under Ambient Conditions , 2019, Joule.

[6]  Abdullah M. Asiri,et al.  High-Performance N2-to-NH3 Conversion Electrocatalyzed by Mo2C Nanorod , 2018, ACS central science.

[7]  B. Tang,et al.  Electrocatalytic Hydrogenation of N2 to NH3 by MnO: Experimental and Theoretical Investigations , 2018, Advanced science.

[8]  M. Shao,et al.  Chromium Oxynitride Electrocatalysts for Electrochemical Synthesis of Ammonia Under Ambient Conditions , 2018, Small Methods.

[9]  Haihui Wang,et al.  Molybdenum Carbide Nanodots Enable Efficient Electrocatalytic Nitrogen Fixation under Ambient Conditions , 2018, Advanced materials.

[10]  B. Tang,et al.  High-performance artificial nitrogen fixation at ambient conditions using a metal-free electrocatalyst , 2018, Nature Communications.

[11]  M. Shu,et al.  Achieving a Record‐High Yield Rate of 120.9 μgNH3  mgcat.−1  h−1 for N2 Electrochemical Reduction over Ru Single‐Atom Catalysts , 2018, Advanced materials.

[12]  Sajanlal R. Panikkanvalappil,et al.  Enhancing the rate of electrochemical nitrogen reduction reaction for ammonia synthesis under ambient conditions using hollow gold nanocages , 2018, Nano Energy.

[13]  Xiaoguang Liu,et al.  Green preparation of in situ Cr3C2 nano-coatings on graphite surface and their water-wettability and rheological properties , 2018, Ceramics International.

[14]  Yu Ding,et al.  An Amorphous Noble-Metal-Free Electrocatalyst that Enables Nitrogen Fixation under Ambient Conditions. , 2018, Angewandte Chemie.

[15]  H. Xin,et al.  Ambient ammonia synthesis via palladium-catalyzed electrohydrogenation of dinitrogen at low overpotential , 2018, Nature Communications.

[16]  Jianguo Wang,et al.  Highly Efficient Ammonia Synthesis Electrocatalyst: Single Ru Atom on Naturally Nanoporous Carbon Materials , 2018 .

[17]  Q. Jiang,et al.  Amorphizing of Au Nanoparticles by CeOx–RGO Hybrid Support towards Highly Efficient Electrocatalyst for N2 Reduction under Ambient Conditions , 2017, Advanced materials.

[18]  Jun-min Yan,et al.  Au Sub‐Nanoclusters on TiO2 toward Highly Efficient and Selective Electrocatalyst for N2 Conversion to NH3 at Ambient Conditions , 2017, Advanced materials.

[19]  Zongping Shao,et al.  A Perovskite Nanorod as Bifunctional Electrocatalyst for Overall Water Splitting , 2017 .

[20]  Claudio Ampelli,et al.  Electrocatalytic Synthesis of Ammonia at Room Temperature and Atmospheric Pressure from Water and Nitrogen on a Carbon-Nanotube-Based Electrocatalyst. , 2017, Angewandte Chemie.

[21]  Leijiang Zhang,et al.  Understanding the growth mechanism of vertically aligned graphene and control of its wettability , 2016 .

[22]  J. Tu,et al.  Transition Metal Carbides and Nitrides in Energy Storage and Conversion , 2016, Advanced science.

[23]  R. Hamers,et al.  Photo-illuminated diamond as a solid-state source of solvated electrons in water for nitrogen reduction. , 2013, Nature materials.

[24]  Sheng-Chang Wang,et al.  Carbothermal reduction process for synthesis of nanosized chromium carbide via metal-organic vapor deposition , 2010 .

[25]  F. Armstrong,et al.  Uncoupling nitrogenase: catalytic reduction of hydrazine to ammonia by a MoFe protein in the absence of Fe protein-ATP. , 2010, Journal of the American Chemical Society.

[26]  M. Koper,et al.  Nitrogen cycle electrocatalysis. , 2009, Chemical reviews.

[27]  G. Henkelman,et al.  A fast and robust algorithm for Bader decomposition of charge density , 2006 .

[28]  Vaclav Smil,et al.  Detonator of the population explosion , 1999, Nature.

[29]  D. Rees,et al.  Nitrogenase and biological nitrogen fixation. , 1994, Biochemistry.

[30]  G. Watt,et al.  Spectrophotometric Method for Determination of Hydrazine , 1952 .

[31]  R. Service.  Chemistry. New recipe produces ammonia from air, water, and sunlight. , 2014, Science.