Tailoring Electronic and Morphology Features of Iron‐Doped Ni₂P Nanoflowers for Enhanced Ammonia Electrosynthesis in Solid Electrolyte Reactors

Advanced Energy Materials, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 13, 2025

Abstract Electrochemical nitrate (NO 3 − ) reduction to ammonia (NH presents a promising route for both wastewater treatment and generation but still suffers from sluggish catalytic activity, insufficient mass transfer, the reliance on high‐concentration supporting electrolytes. This work reports an innovative efficient electrosynthesis reactor by integrating self‐assembled iron‐doped Ni 2 P (Fe‐Ni P/NF) nanoflower cathode with solid‐electrolyte (SE). The SE design eliminates need electrolytes, providing highly ion‐conducting pathway enabling direct production of NH NO . Through tailoring electronic surface characteristics Fe‐Ni P/NF, this achieves complete reduction, 96.7% selectivity, 81.8% faradaic efficiency concentration 100 m at current density mA −2 Density functional theory (DFT) calculations reveal that phosphating Fe doping synergistically enhance adsorption increase availability active hydrogen, thus favoring low energy barrier 0.695 eV. Additionally, superhydrophilicity P/NF catalyst promotes transfer facilitating electrolyte access ensuring rapid gas bubble release. study provides sustainable scalable method converting ‐laden into valuable products.

Language: Английский

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Selective Urea Electrosynthesis from Nitrate and CO₂ on Isolated Copper Alloyed Ruthenium

ACS Energy Letters, Journal Year: 2024, Volume and Issue: 9(9), P. 4624 - 4632

Published: Aug. 30, 2024

Urea electrosynthesis by coelectrolysis of NO3– and CO2 (UENC) represents a promising method to enable efficient sustainable urea production. In this work, isolated Cu alloyed Ru (Cu1Ru) is developed as highly active selective UENC catalyst. Combined theoretical computations in situ spectroscopic measurements reveal the synergistic effect Cu1–Ru site Ru–Ru on Cu1Ru promote via tandem catalysis pathway, which drives *NO2/CO2 coupling followed *CO2NO2-to-*CO2NH step. The formed *CO2NH then migrates from adjacent promotes *CO2NH⃗*CO2NH2 → *COOHNH2 steps toward generation. Impressively, achieves high performance flow cell, exhibiting yield rate 21.04 mmol h–1 gcat–1 Faradaic efficiency 51.27% at −0.6 V, outperforming most reported catalysts.

Language: Английский

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Achieving Near 100% Faradaic Efficiency of Electrocatalytic Nitrate Reduction to Ammonia on Symmetry-Broken Medium-Entropy-Alloy Metallene

ACS Catalysis, Journal Year: 2024, Volume and Issue: 14(10), P. 7907 - 7916

Published: May 6, 2024

Electrochemical nitrate reduction (NO3RR) offers an ecofriendly way for ammonia production. However, improving the sluggish kinetics of such a multistep reaction still remains challenging. Herein, asymmetry strategy is proposed to adjust charge distribution active centers on metallene by presenting novel symmetry-broken medium-entropy-alloy (MEA) via heteroatom alloying. Benefiting from maximized exposure well-regulated sites, proof-of-concept PdCuCo MEA delivers near 100% NH3 Faradaic efficiency in both neutral and alkaline electrolytes, along with record-high yield rate over 532.5 mg h–1 mgcat–1. Moreover, it enables 99.7% conversion industrial wastewater level 6200 ppm drinkable water level. Detailed studies further revealed that redistribution induced elemental electronegativity difference metallene, which will weaken N–O bond *NO, thus reducing energy barrier rate-determining step. Meanwhile, competitive HER formation NO2– are also hindered. We believe our this work shed light design efficient NO3RR catalysts more practical

Language: Английский

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Periodic Adjacent Pd‐Fe Pair Sites for Enhanced Nitrate Electroreduction to Ammonia via Accelerating Proton Relay

Advanced Energy Materials, Journal Year: 2024, Volume and Issue: 14(33)

Published: May 29, 2024

Abstract Recently, bimetallic nanoparticles (NPs) are promising for driving nitrate (NO 3 − ) reduction reaction RR) to produce ammonia (NH due their multiple active sites and electron redistribution via strong metal–metal interaction. However, the quantitatively determining atomic configuration of revealing respective roles in NO RR process still challenged. Herein, atomically ordered PdFe L1 2 intermetallic NPs into mesoporous carbon nanofibers (O‐PdFe ‐mCNFs) is reported as an efficient catalyst NH synthesis. Compared face‐centered cubic one, O‐PdFe ‐mCNFs demonstrate a high removal 98.3% within 270 min with large yield rate 1014.2 µmol h −1 cm −2 . The detailed situ theoretical analysis reveals that performance attributed synergetic effect from periodic adjacent Pd‐Fe pair at (110) facet accelerating proton relay, where Fe show preferable stabilization nitrogen−oxygen (*NO) intermediates while Pd serve reservoir *NO hydrogenation. Moreover, d ‐ orbital hybridization tunes ‐band center alloy effectively modulates adsorption energy *NO. This electrocatalyst design offers new avenue developing highly multifunctional catalysts.

Language: Английский

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In-situ exsolution of FeCo nanoparticles over perovskite oxides for efficient electrocatalytic nitrate reduction to ammonia via localized electrons

Applied Catalysis B Environment and Energy, Journal Year: 2024, Volume and Issue: 357, P. 124267 - 124267

Published: June 5, 2024

Language: Английский

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Two-dimensional peak-valley alternating self-supporting electrode accelerating nitrate electrocatalytic reduction: Ammonia synthesis and wastewater treatment

Chemical Engineering Journal, Journal Year: 2024, Volume and Issue: 485, P. 149876 - 149876

Published: Feb. 20, 2024

Language: Английский

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Selective Nitrate Electroreduction to Ammonia on CNT Electrodes with Controllable Interfacial Wettability

Environmental Science & Technology, Journal Year: 2024, Volume and Issue: 58(16), P. 7228 - 7236

Published: March 29, 2024

The development of electrocatalysts that can efficiently reduce nitrate (NO

Language: Английский

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Regioselective Doping into Atomically Aligned Core–Shell Structures for Electrocatalytic Reduction of Nitrate to Ammonia

Advanced Energy Materials, Journal Year: 2024, Volume and Issue: 14(46)

Published: Aug. 26, 2024

Abstract The electrochemical nitrate reduction reaction (NO 3 − RR) presents an environmentally friendly approach for efficient NO pollutant removal and ammonia (NH ) production, compared to the conventional Haber–Bosch approach. While core/shell engineering has demonstrated its potential in enhancing RR performance, significant synthetic challenges limited shell layer modification capabilities impede exploration of high‐performance catalysts. Herein, CuCoO/Co(OH) 2 structure via situ activation is synthesized. catalyst delivers a maximum NH Faradaic efficiency (FE) 94.7% at −0.5 V RHE with excellent durability selectivity over wide range potentials RR, surpassing electrocatalytic performance both undoped core components. outstanding Cu─CoO/Co(OH) ascribed enhanced charge transfer, stabilization key intermediates, regulation hydrogen adsorption Cu‐doped structure. Furthermore, assembled Zn−NO battery device attains peak current density exceeding 32 mA cm −2 yield up 145.4 µmol h −1 . work offers novel strategy sheds light on doping effects synthesis.

Language: Английский

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Rational Design of Dynamic Interface Water Evolution on Turing Electrocatalyst toward the Industrial Hydrogen Production

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(26)

Published: March 29, 2024

Manipulating the structural and kinetic dissociation processes of water at catalyst-electrolyte interface is vital for alkaline hydrogen evolution reactions (HER) industrial current density. This seldom actualized due to intricacies electrochemical reaction interface. Herein, this work introduces a rapid, nonequilibrium cooling technique synthesizing ternary Turing catalysts with short-range ordered structures (denoted as FeNiRu/C). These advanced empower FeNiRu/C exhibit excellent HER performance in 1 m KOH an ultralow overpotential 6.5 166.2 mV 10 1000 mA cm

Language: Английский

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Boron‐Doped Ti₃C₂T_x MXene for Effective and Durable High‐Current‐Density Ammonia Synthesis

Small, Journal Year: 2024, Volume and Issue: 20(45)

Published: July 24, 2024

Abstract Ammonia (NH 3 ) synthesis via the nitrate reduction reaction (NO RR) offers a competitive strategy for nitrogen cycling and carbon neutrality; however, this is hindered by poor NO RR performance under high current density. Herein, it shown that boron‐doped Ti C 2 T x MXene nanosheets can highly efficiently catalyze conversion of RR‐to‐NH at ambient conditions, showing maximal NH Faradic efficiency 91% with peak yield rate 26.2 mgh −1 mg cat. , robust durability over ten consecutive cycles, all them are comparable to best‐reported results exceed those pristine MXene. More importantly, when tested in flow cell, designed catalyst delivers density ‒1000 mA cm −2 low potential ‒1.18 V versus reversible hydrogen electrode maintains selectivity wide range. Besides, Zn–nitrate battery as cathode assembled, which achieves power 5.24 mW 1.15 . Theoretical simulations further demonstrate boron dopants optimize adsorption activation intermediates, reduce potential‐determining step barrier, thus leading an enhanced selectivity.

Language: Английский

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