Ammonia Electrosynthesis with High Selectivity under Ambient Conditions via a Li⁺ Incorporation Strategy

Abstract

We report the discovery of a dramatically enhanced N electroreduction reaction (NRR) selectivity under ambient conditions via the Li incorporation into poly(N-ethyl-benzene-1,2,4,5-tetracarboxylic diimide) (PEBCD) as a catalyst. The detailed electrochemical evaluation and density functional theory calculations showed that Li association with the O atoms in the PEBCD matrix can retard the HER process and can facilitate the adsorption of N to afford a high potential scope for the NRR process to proceed in the "[O-Li]·N-H" alternating hydrogenation mode. This atomic-scale incorporation strategy provides new insight into the rational design of NRR catalysts with higher selectivity.

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.…”

Ammonia Synthesis Under Ambient Conditions: Selective Electroreduction of Dinitrogen to Ammonia on Black Phosphorus Nanosheets

“…under ambient conditions.D ensity functional theory calculations reveal that the active orbital and electrons of zigzag and diff-zigzag type edges of FL-BP NSs enable selective electrocatalysis of N 2 to NH 3 via an alternating hydrogenation pathway.T his work proves the feasibility of using an onmetallic simple substance as an itrogen-fixing catalyst and thus opening an ew avenue towardst he development of more efficient metal-free catalysts. [4][5][6] However,o wing to the strong dipole moment of the N N triple bond and the vigorous competing hydrogen evolution reaction (HER), [7][8][9][10][11] the development of highly effective catalysts with sufficient activity and selectivity is essential. [1] At present, the energyintensive Haber-Bosch process is the main artificial synthesis route for ammonia, and this process uses more than 1% of global annual energy consumption and produces carbon dioxide emissions.…”

High‐Performance Electrocatalytic Conversion of N2 to NH3 Using Oxygen‐Vacancy‐Rich TiO2 In Situ Grown on Ti3C2Tx MXene

“…Their general formula is recorded as M n+1 X n T x , where "M" stands for the transition metal element, "X" is C or N or CN, while T x represents the terminal groups of -OH or -F, etc., and n could be 1, 2, or 3. [12,45] Meanwhile, since the marginal titanium atoms on the Ti 3 C 2 T x MXenes surface are thermodynamically metastable, which could act as nucleating sites to enable the generation of relatively stable TiO 2 , thereby a heterojunction structure of TiO 2 nanoparticles (NPs) distributed at the 2D Ti 3 C 2 T x nanosheets (TiO 2 /Ti 3 C 2 T x ) could be facilely formed. [44] Recent studies have revealed the great applicability of the Ti 3 C 2 T x MXene as electrocatalyst in NRR, but there still remains large space for improving both the NH 3 yield and the Faradaic efficiency (FE).…”