Fe/Cu diatomic catalysts for electrochemical nitrate reduction to ammonia

Nature Communications, Journal Year: 2023, Volume and Issue: 14(1)

Published: June 19, 2023

Electrochemical conversion of nitrate to ammonia offers an efficient approach reducing pollutants and a potential technology for low-temperature low-pressure synthesis. However, the process is limited by multiple competing reactions NO3- adsorption on cathode surfaces. Here, we report Fe/Cu diatomic catalyst holey nitrogen-doped graphene which exhibits high catalytic activities selectivity production. The enables maximum Faradaic efficiency 92.51% (-0.3 V(RHE)) NH3 yield rate 1.08 mmol h-1 mg-1 (at - 0.5 V(RHE)). Computational theoretical analysis reveals that relatively strong interaction between promotes discharge anions. Nitrogen-oxygen bonds are also shown be weakened due existence hetero-atomic dual sites lowers overall reaction barriers. dual-site hetero-atom strategy in this work provides flexible design further development expands electrocatalytic techniques reduction

Language: Английский

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Alloying of Cu with Ru Enabling the Relay Catalysis for Reduction of Nitrate to Ammonia

Advanced Materials, Journal Year: 2023, Volume and Issue: 35(19)

Published: March 5, 2023

Involving eight electron transfer process and multiple intermediates of nitrate (NO3- ) reduction reaction leads to a sluggish kinetic low Faradaic efficiency, therefore, it is essential get an insight into the mechanism develop highly efficient electrocatalyst. Herein, series reduced-graphene-oxide-supported RuCu alloy catalysts (Rux Cux /rGO) are fabricated used for direct NO3- NH3 . It found that Ru1 Cu10 /rGO shows ammonia formation rate 0.38 mmol cm-2 h-1 (loading 1 mg efficiency 98% under ultralow potential -0.05 V versus Reversible Hydrogen Electode (RHE), which comparable Ru catalyst. The activity can be attributed synergetic effect between Cu sites via relay catalysis, in exclusively NO2- exhibits superior In addition, doping tunes d-band center effectively modulates adsorption energy , promotes This electrocatalysis strategy opens new avenue developing multifunctional catalysts.

Language: Английский

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Elucidating the activity, mechanism and application of selective electrosynthesis of ammonia from nitrate on cobalt phosphide

Energy & Environmental Science, Journal Year: 2021, Volume and Issue: 15(2), P. 760 - 770

Published: Dec. 17, 2021

Cobalt phosphide is an effective electrocatalyst for NO 3 − electroreduction into NH . Phosphorus crucial stabilizing the active phase and optimizing energy barriers, Co 4p orbitals directly participate in nitrate reduction.

Language: Английский

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Electrochemical Nitrate Reduction: Ammonia Synthesis and the Beyond

Advanced Materials, Journal Year: 2023, Volume and Issue: 36(17)

Published: June 9, 2023

Natural nitrogen cycle has been severely disrupted by anthropogenic activities. The overuse of N-containing fertilizers induces the increase nitrate level in surface and ground waters, substantial emission oxides causes heavy air pollution. Nitrogen gas, as main component air, used for mass ammonia production over a century, providing enough nutrition agriculture to support world population increase. In last decade, researchers have made great efforts develop processes under ambient conditions combat intensive energy consumption high carbon associated with Haber-Bosch process. Among different techniques, electrochemical reduction reaction (NO

Language: Английский

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Flower-like open-structured polycrystalline copper with synergistic multi-crystal plane for efficient electrocatalytic reduction of nitrate to ammonia

Nano Energy, Journal Year: 2022, Volume and Issue: 97, P. 107124 - 107124

Published: March 10, 2022

Language: Английский

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Regulating active hydrogen adsorbed on grain boundary defects of nano-nickel for boosting ammonia electrosynthesis from nitrate

Energy & Environmental Science, Journal Year: 2023, Volume and Issue: 16(6), P. 2611 - 2620

Published: Jan. 1, 2023

The grain boundary defect engineered Ni nanoparticles has been explored for boosting selective nitrate electroreduction to ammonia, and its NH 3 generation rate is much higher than those of the reported copper or noble metal-based catalysts.

Language: Английский

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Emerging Applications, Developments, Prospects, and Challenges of Electrochemical Nitrate‐to‐Ammonia Conversion

Advanced Functional Materials, Journal Year: 2023, Volume and Issue: 33(29)

Published: April 23, 2023

Abstract Ammonia is not only an important feedstock for chemical industry but also a carbon‐free energy carrier and safe storage media hydrogen. Due to the advantages compared Haber–Bosch process, electrochemical NO 3 − ‐to‐NH conversion via nitrate reduction reaction (NO RR) received attention. Recently, “green hydrogen” generated from water electrolysis shows promise become future limited by safety of transportation. This review proposes can store renewable electric into NH , which potential solution solving puzzle Moreover, theoretical insights RR electrocatalyst design are discussed. Finally, challenges opportunities in this field elucidated. provides novel perspective accelerates development effective electrocatalysts conversion.

Language: Английский

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Interfacial Reduction Nucleation of Noble Metal Nanodots on Redox-Active Metal–Organic Frameworks for High-Efficiency Electrocatalytic Conversion of Nitrate to Ammonia

Nano Letters, Journal Year: 2022, Volume and Issue: 22(6), P. 2529 - 2537

Published: March 10, 2022

Electrochemically converting nitrate to ammonia is a promising route realize artificial nitrogen recycling. However, developing highly efficient electrocatalysts an ongoing challenge. Herein, we report the construction of stable and redox-active zirconium metal-organic frameworks (Zr-MOFs) based on Zr6 nanoclusters redox-reversible tetrathiafulvalene (TTF) derivatives as inorganic nodes organic linkers, respectively. The Zr-MOF can facilitate in situ reduction noble metal precursors free external reductants uniform nucleation nanodots (NDs) Zr-MOF, achieving preparation M-NDs/Zr-MOF (M = Pd, Ag, or Au). porous with good conductivity mass transfer process. Among catalysts, Pd-NDs/Zr-MOF exhibits highest electrocatalytic activity, delivering NH3 yield 287.31 mmol·h-1·g-1cat. Faradaic efficiency 58.1%. proposed interfacial strategy for anchoring M NDs Zr-MOFs be applied other challenging energy conversion reactions.

Language: Английский

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Microscopic-Level Insights into the Mechanism of Enhanced NH₃ Synthesis in Plasma-Enabled Cascade N₂ Oxidation–Electroreduction System

Journal of the American Chemical Society, Journal Year: 2022, Volume and Issue: 144(23), P. 10193 - 10200

Published: May 19, 2022

Integrated/cascade plasma-enabled N2 oxidation and electrocatalytic NOx– (where x = 2, 3) reduction reaction (pNOR-eNOx–RR) holds great promise for the renewable synthesis of ammonia (NH3). However, corresponding activated effects process plasma toward O2 molecules mechanism eNOx–RR to NH3 are unclear need be further uncovered, which largely limits large-scale deployment this integration technology. Herein, we systematically investigate activation recombination processes molecules, more meaningfully, at a microscopic level is also decoupled using copper (Cu) nanoparticles as representative electrocatalyst. The concentration produced NOx in pNOR system confirmed function length spark discharge well volumetric ratio feeding gas. successive protonation key N-containing intermediates (e.g., −NH2) detected with situ infrared spectroscopy. Besides, Raman spectroscopy reveals dynamic reconstruction Cu during process. nanoparticle-driven pNOR-eNOx–RR can finally achieve high yield rate ∼40 nmol s–1 cm–2 Faradaic efficiency nearly 90%, overperforming benchmarks reported literature. It anticipated that work will stimulate practical development green electrosynthesis directly from air water under ambient conditions.

Language: Английский

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ITO@TiO2 nanoarray: An efficient and robust nitrite reduction reaction electrocatalyst toward NH3 production under ambient conditions

eScience, Journal Year: 2022, Volume and Issue: 2(4), P. 382 - 388

Published: May 6, 2022

Ambient electrochemical nitrite (NO2-) reduction is viewed as an effective and sustainable approach for simultaneously removing NO2- producing ammonia (NH3). However, the complex multi-electron transfer steps involved in reaction (NO2-RR) lead to sluggish kinetics low product selectivity toward NH3, underscoring need NH3 synthesis electrocatalysts with high activity durability. Herein, we report amorphous indium–tin oxide sputtered on a TiO2 nanobelt array Ti plate ([email protected]2/TP) 3D NH3-producing catalyst NO2-. In 0.5 ​M LiClO4 0.1 NO2-, it shows greatly boosted NO2-RR production, excellent selectivity, achieving large yield of 411.3 ​μmol ​h−1 ​cm−2 Faradaic efficiency 82.6%. It also durability continuous electrolysis. A Zn‐NO2- battery [email protected]2/TP cathode offers 23.1 peak power density 1.22 ​mW ​cm−2.

Language: Английский

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