TY - JOUR

T1 - Role of Catalyst in Controlling N2 Reduction Selectivity

T2 - A Unified View of Nitrogenase and Solid Electrodes

AU - Bagger, Alexander

AU - Wan, Hao

AU - Stephens, Ifan E. L.

AU - Rossmeisl, Jan

PY - 2021

Y1 - 2021

N2 - The Haber-Bosch process conventionally reduces N-2 to ammonia at 200 bar and 500 degrees C. Under ambient conditions, i.e., room temperature and ambient pressure, N-2 can be converted into ammonia by the nitrogenase molecule and lithium-containing solid electrodes in nonaqueous media. In this work, we explore the catalyst space for the N-2 reduction reaction under ambient conditions. We describe N-2 reduction on the basis of the *N-2 binding energy versus the *H binding energy; we find that under standard conditions, no catalyst can bind and reduce *N-2 without producing H-2. We show why a selective catalyst for N-2 reduction will also likely be selective for CO2 reduction, but N-2 reduction is intrinsically more challenging than CO2 reduction. Only by modulating the reaction pathway, like nitrogenase, or by tuning chemical potentials, like the Haber-Bosch and the Li-mediated process, N-2 can be reduced.

AB - The Haber-Bosch process conventionally reduces N-2 to ammonia at 200 bar and 500 degrees C. Under ambient conditions, i.e., room temperature and ambient pressure, N-2 can be converted into ammonia by the nitrogenase molecule and lithium-containing solid electrodes in nonaqueous media. In this work, we explore the catalyst space for the N-2 reduction reaction under ambient conditions. We describe N-2 reduction on the basis of the *N-2 binding energy versus the *H binding energy; we find that under standard conditions, no catalyst can bind and reduce *N-2 without producing H-2. We show why a selective catalyst for N-2 reduction will also likely be selective for CO2 reduction, but N-2 reduction is intrinsically more challenging than CO2 reduction. Only by modulating the reaction pathway, like nitrogenase, or by tuning chemical potentials, like the Haber-Bosch and the Li-mediated process, N-2 can be reduced.

KW - classification

KW - N-2 reduction

KW - CO2 reduction

KW - CO reduction

KW - electrochemistry

KW - electrocatalysis

KW - density functional theory

KW - ELECTROCHEMICAL CO2 REDUCTION

KW - EVOLUTION REACTION

KW - AMMONIA-SYNTHESIS

KW - FEMO-COFACTOR

KW - PERSPECTIVE

KW - MECHANISM

KW - PATHWAYS

KW - LIGAND

U2 - 10.1021/acscatal.1c01128

DO - 10.1021/acscatal.1c01128

M3 - Journal article

VL - 11

SP - 6596

EP - 6601

JO - ACS Catalysis

JF - ACS Catalysis

SN - 2155-5435

IS - 11

ER -