Reaction pathways on N-substituted carbon catalysts during the electrochemical reduction of nitrate to ammonia

Chen, ZhengInstitute of Inorganic Chemistry, RWTH Aachen University, 52056 Aachen, Germany (author)

Electrochemical reduction of nitrate into ammonia is one potential strategy to valorize pollutants needed to close the nitrogen cycle. The understanding of carbonaceous materials as metal-free representatives of electrocatalysts is of high importance to ensure sufficient activity and target selectivity. We report on the role of defects in cellulose-derived nitrogen-doped carbon (NDC) materials, produced by ammonolysis at different temperatures, to obtain efficient electrocatalysts for the nitrate reduction reaction (NO3RR). Carbon catalyst ammonolysis at 800 °C (NDC-800) yields the highest electrochemical performance, exhibiting 73.1% NH4+ selectivity and nearly 100% NO3− reduction efficiency with a prolonged NO3RR time (48 h) at −1.5 V vs. Ag/AgCl in a 0.1 M Na2SO4 electrolyte. We provide support to our findings by undertaking complementary structural analyses with scanning electron microscopy (SEM), transmission electron microscopy (TEM), powder X-ray diffraction (PXRD), X-ray photoelectron spectroscopy (XPS), Raman spectroscopy, low-temperature N2 adsorption, and theoretical studies based on multi-scale/level calculations. Atomistic molecular dynamics simulations based on a reactive force field combined with quantum chemistry (QC) calculations on representative model systems suggest possible realistic scenarios of the material structure and reaction mechanisms of the NO3− reduction routes.

TEKNIK OCH TEKNOLOGIER Nanoteknik hsv//swe
ENGINEERING AND TECHNOLOGY Nano-technology hsv//eng
NATURVETENSKAP Kemi hsv//swe
NATURAL SCIENCES Chemical Sciences hsv//eng
Engineering Science with specialization in Nanotechnology and Functional Materials
Teknisk fysik med inriktning mot nanoteknologi och funktionella material

Chen, JianhongStockholms universitet,Institutionen för material- och miljökemi (MMK),Department of Materials and Environmental Chemistry, Stockholm University, 10691 Stockholm, Sweden(Swepub:su)jich2514 (author)
Barcaro, GiovanniCNR-ICCOM−Institute of Chemistry of Organometallic Compounds, 56124 Pisa, Italy (author)
Budnyak, TetyanaStockholms universitet,Institutionen för material- och miljökemi (MMK),Department of Materials and Environmental Chemistry, Stockholm University, 10691 Stockholm, Sweden(Swepub:su)tebu2966 (author)
Rokicińska, AnnaFaculty of Chemistry, Jagiellonian University, ul. Golebia 24, 30-387 Krakow, Poland (author)
Dronskowski, RichardInstitute of Inorganic Chemistry, RWTH Aachen University, 52056 Aachen, Germany;Hoffmann Institute of Advanced Materials, Shenzhen Polytechnic, 7098 Liuxian Blvd, Shenzhen, China (author)
Budnyk, SerhiyAC2T research GmbH, Viktor-Kaplan-Str. 2c, 2700 Wiener Neustadt, Austria (author)
Kuśtrowski, PiotrFaculty of Chemistry, Jagiellonian University, ul. Golebia 24, 30-387 Krakow, Poland (author)
Monti, SusannaCNR-ICCOM−Institute of Chemistry of Organometallic Compounds, 56124 Pisa, Italy (author)
Slabon, AdamInorganic Chemistry, University of Wuppertal, Gaußstr. 20, 42119 Wuppertal, Germany (author)
Institute of Inorganic Chemistry, RWTH Aachen University, 52056 Aachen, GermanyInstitutionen för material- och miljökemi (MMK) (creator_code:org_t)

In:Catalysis Science & Technology: Royal Society of Chemistry12:11, s. 3582-35932044-47532044-4761

By the author/editor: Chen, Zheng; Chen, Jianhong; Barcaro, Giovann ...; Budnyak, Tetyana; Rokicińska, Anna; Dronskowski, Ric ...; show more...; Budnyk, Serhiy; Kuśtrowski, Piot ...; Monti, Susanna; Slabon, Adam; show less...

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