Boron-Doped Graphene for Electrocatalytic N2 Reduction

Abstract

Boron-doped graphene with different boron structures was rationally synthesized to enhance the adsorption of N 2 , thus enabling an efficient metal-free electrocatalyst for electrochemical N 2 reduction in aqueous solution at ambient conditions. At a doping level of 6.2%, boron-doped graphene achieved a NH 3 production rate of 9.8 mg$hr À1 $cm À2 and an excellent faradic efficiency (10.8% at À0.5 V versus reversible hydrogen electrode).

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

“…[8,[14][15][16][17][18][19][20][21][22][23] Specifically,b enefiting from the unoccupied and occupied dorbitals of transition metals,t he electron density from N 2 is synergically accepted with appropriate energy and symmetry,a nd then, the transition metal donates electrons to the p*o rbital of NN, strengthening N 2 adsorption and weakening the NNbond. [29] Similar nitrogen reduction activity was also observed on metal-free boron carbide nanosheets. [24] Compared to transition metals,t he weak hydrogen adsorption of nonmetallic elements and their abundant valence electrons should provide am ore ideal nitrogen activation center.…”

“…[25,26] Some recent studies have shown that the use of nonmetallic components as active centers may be an effective way to obtain high selectivity. [29] Similar nitrogen reduction activity was also observed on metal-free boron carbide nanosheets. [29] Similar nitrogen reduction activity was also observed on metal-free boron carbide nanosheets.…”

“…[12][13][14][15] To this end, the search for an electrocatalytic NRR center in recent years has mainly focused on transition-metal-based materials. [27][28][29][30][31] Fore xample, Yu et al reported ah igh NH 3 production rate and faradaic efficiency by using boron-doped graphene as am etal-free NRR catalyst under ambient conditions. [7] It is worthwhile to note that although an unoccupied nonbonding orbital and electron donor site with abundant electron cloud density are prerequisites for aN RR catalyst, the do rbital electrons in transition metals also benefit the formation of metal-hydrogen bonds,w hich will exacerbate the competitive hydrogen evolution reaction and limit the nitrogen reduction selectivity and catalytic efficiency.…”

“…[24] Compared to transition metals,t he weak hydrogen adsorption of nonmetallic elements and their abundant valence electrons should provide am ore ideal nitrogen activation center. [27][28][29][30][31] Fore xample, Yu et al reported ah igh NH 3 production rate and faradaic efficiency by using boron-doped graphene as am etal-free NRR catalyst under ambient conditions. [27][28][29][30][31] Fore xample, Yu et al reported ah igh NH 3 production rate and faradaic efficiency by using boron-doped graphene as am etal-free NRR catalyst under ambient conditions.…”

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.…”