NO is a dominant atmosphere pollutant, causing ozone depletion and global warming. Currently, electrochemical reduction of NO has gained increasing attention to remove NO, but its product is worthless N. Here, we propose a direct eight-electron (8) pathway to electrochemically convert NO into NH. As a proof of concept, using density functional theory calculation, an Fe double-atom catalyst (DAC) anchored by N-doped porous graphene (Fe@NG) was screened out to be the most active and selective catalyst for NO electroreduction toward NH via the novel 8 pathway, which benefits from the unique bent NO adsorption configuration. Guided by theoretical prediction, Fe@NG DAC was fabricated experimentally, and it can achieve a high NO-to-NH Faradaic efficiency of 77.8% with a large NH yield rate of 2.9 mg h cm at -0.6 V vs RHE in a neutral electrolyte. Our study offers a feasible strategy to synthesize NH from pollutant NO with simultaneous NO removal.
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http://dx.doi.org/10.1021/acs.nanolett.4c00576 | DOI Listing |
ACS Appl Mater Interfaces
July 2024
State Key Laboratory of Molecular Engineering of Polymers, Department of Macromolecular Science, Fudan University, Shanghai 200438, China.
Direct borohydride fuel cell (DBFC) is considered a promising energy storage device due to its high theoretical cell voltage and energy density. For DBFC, an Au catalyst has been used as an anode for achieving an ideal eight-electron reaction. However, the poor activity of the Au catalyst for borohydride oxidation reaction (BOR) limits its large-scale application because of the weak BH adsorption.
View Article and Find Full Text PDFNano Lett
July 2024
Anhui Province Industrial Generic Technology Research Center for Alumics Materials, School of Physics and Electronic Information, Huaibei Normal University, Huaibei, Anhui 235000, China.
NO is a dominant atmosphere pollutant, causing ozone depletion and global warming. Currently, electrochemical reduction of NO has gained increasing attention to remove NO, but its product is worthless N. Here, we propose a direct eight-electron (8) pathway to electrochemically convert NO into NH.
View Article and Find Full Text PDFInorg Chem
June 2024
School of Materials Science and Engineering, Jiangsu University, Zhenjiang 212013, China.
The efficiency of electrochemical nitrate (NO) reduction to ammonia (NH) still remains a challenge due to the sluggish kinetics of the complex eight-electron reduction process and competitive hydrogen evolution reaction (HER). Herein, we designed new three-dimensional (3D) porous Cu/CuO nanosheet arrays (Cu/CuO NSA) by coupling a template-directed method with electroreduction. Thanks to the 3D porous structure and in-plane heterojunctions, Cu/CuO NSA can provide abundant active sites and a good interfacial effect, obtaining the maximum Faradaic efficiency (FE) of ammonia (88.
View Article and Find Full Text PDFNano Lett
December 2023
Department of Chemistry, Colorado State University, Fort Collins, Colorado 80523, United States.
Nanoparticle syntheses are designed to produce the desired product in high yield but traditionally neglect atom-economy. Here we report that the simple, but significant, change of the solvent from 1-octadecene (1-ODE) to the operationally inert octadecane (ODA) permits an atom-economical synthesis of copper selenophosphate (CuPSe) nanoparticles. This change eliminates the competing selenium (Se) delivery pathways from our first report that required an excess of Se.
View Article and Find Full Text PDFAdv Mater
May 2023
Key Laboratory of Advanced Catalysis, Gansu Province, State Key Laboratory of Applied Organic Chemistry, College of Chemistry and Chemical Engineering, Lanzhou University, Lanzhou, Gansu, 730000, China.
Involving eight electron transfer process and multiple intermediates of nitrate (NO ) reduction reaction leads to a sluggish kinetic and low Faradaic efficiency, therefore, it is essential to get an insight into the reaction mechanism to develop highly efficient electrocatalyst. Herein, a series of reduced-graphene-oxide-supported RuCu alloy catalysts (Ru Cu /rGO) are fabricated and used for the direct reduction of NO to NH . It is found that the Ru Cu /rGO shows the ammonia formation rate of 0.
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