Tandem Electrocatalytic Reduction of Nitrite to Ammonia on Rhodium–Copper Single Atom Alloys

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(36)

Published: April 23, 2024

Abstract Electrocatalytic reduction of NO 2 − to NH 3 (NO RR) presents a fascinating approach for simultaneously migrating pollutants and producing valuable . In this study, single‐atom Rh‐alloyed copper (CuRh 1 ) is explored as highly active selective catalyst toward the RR. Combined theoretical calculations in situ FTIR/EPR spectroscopic experiments uncover synergistic effect Rh Cu promote RR energetics CuRh through tandem catalysis pathway, which activates preliminary adsorption hydrogenation → *NO *NOOH *NO), while generated on then transferred substrate promotes rate‐determining step *NHO synthesis. As result, equipped flow cell an unprecedented yield rate 2191.6 µmol h −1 cm −2 ‐Faradaic efficiency 98.9% at high current density 322.5 mA , well long‐term stability 100 electrolysis.

Language: Английский

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Electrochemical Co-Production of Ammonia and Biodegradable Polymer Monomer Glycolic Acid via the Co-Electrolysis of Nitrate Wastewater and Waste Plastic

ACS Catalysis, Journal Year: 2023, Volume and Issue: 13(15), P. 10394 - 10404

Published: July 25, 2023

Electrochemical reformation of nitrate wastewater and poly(ethylene terephthalate) (PET) plastic waste into ammonia (NH3) fine chemicals is a sustainable strategy for resource utilization. Herein, co-production system glycolic acid (GA, degradable polymer monomer) constructed by coupling reduction ethylene glycol (EG, in PET hydrolysate) oxidation. Low-crystalline CoOOH (LC-CoOOH/CF) Pd nanothorns (Pd NTs/NF) grown situ on the metal foam substrates are employed as cathode anode, respectively. The high density amorphous regions LC-CoOOH/CF enables enhanced adsorption provides abundant active sites, ultimately leading to an Faradic efficiency (FE) 97.38 ± 1.0% at −0.25 V vs reversible hydrogen electrode (RHE). Meanwhile, unique nanothorn morphology endows NTs/NF with high-curvature tip, triggering tip effect (TE) promote highly selective oxidation EG GA. Furthermore, two-electrode system, NH3 GA operated low energy consumption (onset voltage: 0.5 V), much lower than traditional electrolysis process (1.4 V). This study method utilization co-produce value-added chemicals.

Language: Английский

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Electroreduction of Nitrite to Ammonia Over Ni₁Ru Single‐Atom Alloys

Advanced Functional Materials, Journal Year: 2023, Volume and Issue: 34(3)

Published: Oct. 3, 2023

Abstract Electroreduction of nitrite to ammonia (NO 2 RR) holds great promise for concurrently achieving efficient NH 3 electrosynthesis and wastewater purification. This study first develops Ni 1 Ru single‐atom alloys as an robust NO RR catalyst. Extensive experiments theoretical computations reveal that isolated atoms electronically couple their adjacent render with high thermodynamic stability, boosted − ‐to‐NH hydrogenation energetics suppressed hydrogen evolution. As a result, assembled in flow cell shows exceptional yield rate 37.5 mg h −1 cm −2 ‐Faradaic efficiency 93.9% at current density 312.3 mA , representing one the highest performances ever reported.

Language: Английский

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p-d hybridized In-Co dual sites promote nitrite electroreduction to ammonia at high current density

Nano Energy, Journal Year: 2024, Volume and Issue: 125, P. 109594 - 109594

Published: April 6, 2024

Language: Английский

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P-Block Antimony–Copper Single-Atom Alloys for Selective Nitrite Electroreduction to Ammonia

ACS Nano, Journal Year: 2024, Volume and Issue: 18(20), P. 13141 - 13149

Published: May 8, 2024

Electrocatalytic reduction of NO2– to NH3 (NO2RR) offers an effective method for alleviating pollution and generating valuable NH3. Herein, a p-block single-atom alloy, namely, isolated Sb alloyed in Cu substrate (Sb1Cu), is explored as durable high-current-density NO2RR catalyst. As revealed by the theoretical calculations operando spectroscopic measurements, we demonstrate that Sb1 incorporation can not only hamper competing hydrogen evolution reaction but also optimize d-band center Sb1Cu intermediate adsorption energies boost protonation energetics NO2–-to-NH3 conversion. Consequently, integrated flow cell achieves outstanding yield rate 2529.4 μmol h–1 cm–2 FENH3 95.9% at high current density 424.2 mA cm–2, well durability 100 h electrolysis.

Language: Английский

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Nb1-Zr dual active sites constructed on ZrO2 boost nitrite-to-ammonia electroreduction

Chemical Engineering Journal, Journal Year: 2024, Volume and Issue: 481, P. 148733 - 148733

Published: Jan. 13, 2024

Language: Английский

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Electroreduction of Nitrite to Ammonia over a Cobalt Single-Atom Catalyst

ACS Sustainable Chemistry & Engineering, Journal Year: 2024, Volume and Issue: 12(7), P. 2783 - 2789

Published: Feb. 2, 2024

Electrochemical nitrite-to-ammonia reduction (NO2RR) holds great promise for converting harmful NO2– into valuable NH3. Herein, we develop Co single atoms dispersed on a C3N4 substrate (Co1/C3N4) as an efficient catalyst toward the NO2RR. Experimental and theoretical investigations reveal that single-atom sites can effectively active optimize formation energy of key *NOH intermediate to promote → NH3 energetics. Remarkably, Co1/C3N4 equipped in flow cell delivers exceptional NH3–Faradaic efficiency 97.9% yield rate 1080.3 μmol h–1cm–2 at industrial-level current density 355 mA cm–2, along with long-term durability 100 h electrolysis, showing considerable potential practical electrosynthesis.

Language: Английский

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Controlled Synthesis of Unconventional Phase Alloy Nanobranches for Highly Selective Electrocatalytic Nitrite Reduction to Ammonia

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(26)

Published: April 22, 2024

Abstract The controlled synthesis of metal nanomaterials with unconventional phases is significant importance to develop high‐performance catalysts for various applications. However, it remains challenging modulate the atomic arrangements nanomaterials, especially alloy nanostructures that involve different metals distinct redox potentials. Here we report general one‐pot IrNi, IrRhNi and IrFeNi nanobranches hexagonal close‐packed (hcp) phase. Notably, as‐synthesized hcp IrNi demonstrate excellent catalytic performance towards electrochemical nitrite reduction reaction (NO 2 RR), superior NH 3 Faradaic efficiency yield rate 98.2 % 34.6 mg h −1 cat (75.5 Ir ) at 0 −0.1 V (vs reversible hydrogen electrode), respectively. Ex/in situ characterizations theoretical calculations reveal Ir−Ni interactions within improve electron transfer benefit both activation active generation, leading a stronger trend NO RR by greatly reducing energy barriers rate‐determining step.

Language: Английский

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Recent advances of ammonia synthesis under ambient conditions over metal-organic framework based electrocatalysts

Applied Catalysis B Environment and Energy, Journal Year: 2023, Volume and Issue: 340, P. 123161 - 123161

Published: Aug. 10, 2023

Language: Английский

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Single-atom Co alloyed Ru for electrocatalytic nitrite reduction to ammonia

Nano Research, Journal Year: 2023, Volume and Issue: 17(5), P. 3660 - 3666

Published: Nov. 8, 2023

Language: Английский

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