Metal-organic framework-derived nitrogen-doped highly disordered carbon for electrochemical ammonia synthesis using N2 and H2O in alkaline electrolytes

Ambient Electrosynthesis of Ammonia on a Core–Shell‐Structured Au@CeO2 Catalyst: Contribution of Oxygen Vacancies in CeO2

“…[1][2][3][4] AlthoughN 2 is very abundant in the atmosphere, accountingf or about 78 %, it is very inert, with ah igh triple-bond energy of 940.95 kJ mol À1 and no permanent dipole;t hus artificially fixing N 2 to NH 3 is extremely challenging. [5][6][7] Currently,t he century-old Haber-Bosch process is still dominant for the production of NH 3 on an industrial scale. [1,2,[4][5][6][7][8] However,t his process needs to consume around1 -3% of the world's annuale nergys upply;3 -5 %o ft he world's natural gas production for H 2 production; ands imultaneously releases massive amounts of CO 2 ,a ccounting for about1 .5 % of all greenhouse gas emissions.…”

“…[5][6][7] Currently,t he century-old Haber-Bosch process is still dominant for the production of NH 3 on an industrial scale. [1,2,[4][5][6][7][8] However,t his process needs to consume around1 -3% of the world's annuale nergys upply;3 -5 %o ft he world's natural gas production for H 2 production; ands imultaneously releases massive amounts of CO 2 ,a ccounting for about1 .5 % of all greenhouse gas emissions. [1,4,5,8,9] Therefore, the development of environmentallyf riendly NH 3 synthesis technologies by utilizing atmospheric N 2 under mild conditions is still in demand from the viewpoints of both energy conservation and environmental protection.…”

“…In recent years, the electrocatalytic N 2 reductionr eaction (NRR)t oN H 3 by using water as the hydrogen source and operating under ambient conditions has exhibited greatp otential as ap romising substitute for the energy-and capital-intensive Haber-Bosch process. [1,[4][5][6][7][8][9] To date, metal-based materials have been the most widelyi nvestigatede lectrocatalysts for the NRR, exhibiting acceptable NH 3 yields andf aradaic efficiencies (FEs) in aqueous electrolytes and significantly improved FEs in ionicliquid electrolytes. [10,11] Recently, severalg roupsu tilized different syntheticm ethodst of abricate noble-metal gold-based materials, such as atomically dispersed Au, [12] flower-like Au, [13] hollowA un anocages, [14] Au-containing alloys, [15] Au nanoparticles/C, [16] Au nanoclusters, [17] amorphous Au, [18] and Au nanorods with high-index faces; [19] these have been experimentally and theoretically provent ob ee lectrochemically active for the NRR.…”

Atomically Dispersed Molybdenum Catalysts for Efficient Ambient Nitrogen Fixation

“…[1][2][3][4] From an energy-saving perspective,g reen N 2 to NH 3 fixation methods are strongly desired because the main industrial process for producing NH 3 -the Haber-Bosch process-requires extremely harsh reaction conditions (400-600 8 8C, 20-40 MPa) and causes pollution and greenhouse gas emissions. [8][9][10][11][12][13][14][15][16][17][18][19][20][21][22][23][24][25][26][27] However,t he efficiency of the NRR suffers from ap arallel hydrogen evolution reaction (HER) in aqueous solutions on traditional NRR electrocatalysts. [8][9][10][11][12][13][14][15][16][17][18][19][20][21][22][23][24][25][26][27] However,t he efficiency of the NRR suffers from ap arallel hydrogen evolution reaction (HER) in aqueous solutions on traditional NRR electrocatalysts.…”

Ten years of carbon‐based metal‐free electrocatalysts

“…33 Few months later (also in 2018), Ndoped porous carbon was also reported to show NRR in 0.1 M KOH electrolyte with an impressive NH 3 production rate of 3.4 × 10 −6 mol/cm 2 /h and Faradic efficiency (FE) of 10.2%. 34 In these cases, the pyridinic and pyrrolic N species were attributed to NRR in acidic medium whereas the moieties with C-vacancy and pyridinic N were found to facilitate efficient NRR in the alkaline electrolyte. DFT calculations revealed the preferable pathway for ammonia synthesis (*N≡N → *NH = NH → *NH 2 = NH 2 → 2NH 3 ) in an alkaline medium, and found that the NRR on pyridinic (0.45 eV) and pyrrolic N (0.56 eV) sites are energetically more favorable than the graphitic N sites.…”