A Bi‐Co Corridor Construction Effectively Improving the Selectivity of Electrocatalytic Nitrate Reduction toward Ammonia by Nearly 100%

Advanced Materials, Journal Year: 2023, Volume and Issue: 35(48)

Published: Sept. 22, 2023

Improving the selective ammonia production capacity of electrocatalytic nitrate reduction reaction (NO3 RR) at ambient conditions is critical to future development and industrial application electrosynthesis ammonia. However, involves multi-proton electron transfer as well desorption underutilization intermediates, posing a challenge selectivity NO3 RR. Here electrodeposition site Co modulated by depositing Bi bottom catalyst, thus obtaining Co+Bi@Cu NW catalyst with Bi-Co corridor structure. In 50 mm NO3- , exhibits highest Faraday efficiency ≈100% (99.51%), an yield rate 1858.2 µg h-1 cm-2 high repeatability -0.6 V versus reversible hydrogen electrode. Moreover, change NO2- concentration on surface observed in situ reflection absorption imaging intermediates RR process detected electrochemical Raman spectroscopy together verify trapping effect It believed that measure modulating deposition loading element easy-to-implement general method for improving NH3 corresponding scientific research applications.

Language: Английский

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Modulating Metal‐Nitrogen Coupling in Anti‐Perovskite Nitride via Cation Doping for Efficient Reduction of Nitrate to Ammonia

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(38)

Published: Aug. 1, 2023

The complexes of metal center and nitrogen ligands are the most representative systems for catalyzing hydrogenation reactions in small molecule conversion. Developing heterogeneous catalysts with similar active metal-nitrogen functional centers, nevertheless, still remains challenging. In this work, we demonstrate that coupling anti-perovskite Co4 N can be effective modulated by Cu doping to form Co3 CuN, leading strongly promoted process during electrochemical reduction nitrate (NO3- RR) ammonia. combination advanced spectroscopic techniques density theory calculations reveal dopants strengthen Co-N bond upshifted d-band towards Fermi level, promoting adsorption NO3- *H facilitating transition from *NO2 /*NO H/*NOH. Consequently, CuN delivers noticeably better RR activity than pristine N, optimal Faradaic efficiency 97 % ammonia yield 455.3 mmol h-1 cm-2 at -0.3 V vs. RHE. This work provides an strategy developing high-performance catalyst synthesis.

Language: Английский

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Synergistic Effect of Ni/Ni(OH)₂ Core‐Shell Catalyst Boosts Tandem Nitrate Reduction for Ampere‐Level Ammonia Production

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(27)

Published: April 23, 2024

Electrocatalytic reduction of nitrate to ammonia provides a green alternate the Haber-Bosch method, yet it suffers from sluggish kinetics and low yield rate. The follows tandem reaction nitrite subsequent hydrogenation generate ammonia, Faraday efficiency (FE) is limited by competitive hydrogen evolution reaction. Herein, we design heterostructure catalyst remedy above issues, which consists Ni nanosphere core Ni(OH)

Language: Английский

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Critical review in electrocatalytic nitrate reduction to ammonia towards a sustainable nitrogen utilization

Chemical Engineering Journal, Journal Year: 2024, Volume and Issue: 483, P. 148952 - 148952

Published: Jan. 22, 2024

Language: Английский

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Metal Doped Unconventional Phase IrNi Nanobranches: Tunable Electrochemical Nitrate Reduction Performance and Pollutants Upcycling

Environmental Science & Technology, Journal Year: 2024, Volume and Issue: 58(24), P. 10863 - 10873

Published: June 6, 2024

Electrochemical nitrate reduction (NO3RR) provides a new option to abate contamination with low carbon footprint. Restricted by competitive hydrogen evolution, achieving satisfied performance in neutral media is still challenge, especially for the regulation of this multielectron multiproton reaction. Herein, facile element doping adopted tune catalytic behavior IrNi alloy nanobranches an unconventional hexagonal close-packed (hcp) phase toward NO3RR. In particular, obtained hcp IrNiCu favor ammonia production and suppress byproduct formation electrolyte indicated situ differential electrochemical mass spectrometry, high Faradaic efficiency (FE) 85.6% large yield rate 1253 μg cm–2 h–1 at −0.4 −0.6 V (vs reversible electrode (RHE)), respectively. contrast, resultant IrNiCo promote nitrite, peak FE 33.1% −0.1 RHE). Furthermore, hybrid electrolysis cell consisting NO3RR formaldehyde oxidation constructed, which are both catalyzed nanobranches. This electrolyzer exhibits lower overpotential holds potential treat polluted air wastewater simultaneously, shedding light on green chemical based contaminate degradation.

Language: Английский

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Boosting electrochemical oxygen reduction to hydrogen peroxide coupled with organic oxidation

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: July 19, 2024

Abstract The electrochemical oxygen reduction reaction (ORR) to produce hydrogen peroxide (H 2 O ) is appealing due its sustainability. However, efficiency compromised by the competing 4e − ORR pathway. In this work, we report a hierarchical carbon nanosheet array electrode with single-atom Ni catalyst synthesized using organic molecule-intercalated layered double hydroxides as precursors. exhibits excellent 2e performance under alkaline conditions and achieves H yield rates of 0.73 mol g cat −1 h in H-cell 5.48 flow cell, outperforming most reported catalysts. experimental results show that atoms selectively adsorb , while nanosheets generate reactive species, synergistically enhancing production. Furthermore, coupling system integrating ethylene glycol oxidation significantly enhances rate 7.30 producing valuable glycolic acid. Moreover, convert electrolyte containing directly into downstream product sodium perborate reduce separation cost further. Techno-economic analysis validates economic viability system.

Language: Английский

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Balancing dynamic evolution of active sites for urea oxidation in practical scenarios

Energy & Environmental Science, Journal Year: 2023, Volume and Issue: 16(12), P. 6015 - 6025

Published: Jan. 1, 2023

The role of single atomic Ru site for enhanced UOR performance.

Language: Английский

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Promoting Electrocatalytic Hydrogenation of 5-Hydroxymethylfurfural over a Cooperative Ag/SnO₂ Catalyst in a Wide Potential Window

ACS Catalysis, Journal Year: 2023, Volume and Issue: 13(20), P. 13528 - 13539

Published: Oct. 6, 2023

Electrochemical reduction of biomass-derived 5-hydroxymethylfurfural (HMF) to produce 2,5-dihydroxymethylfuran (DHMF) is a promising approach for biomass upgrading. The achievement high activity and Faradaic efficiency (FE) in wide potential window critical mature applications considering the significantly varied voltages supplied by different renewable energies. However, it still challenging due multiple reaction pathways competitive hydrogen evolution reaction. Herein, we synthesized cooperative catalyst supporting Ag nanoparticles (AgNPs) on SnO2 nanosheet arrays, which realizes electrochemical HMF DHMF with FE (>95%) (from −0.62 −1.12 V vs reversible electrode). situ measurements reveal that AgNPs promote water splitting generate reactive (H*) species, effectively react via Langmuir–Hinshelwood mechanism. Moreover, accelerate formation oxygen vacancies under conditions, act as electrophilic sites realize selective adsorption hydrogenation carbonyl bond (C═O) yield DHMF. Finally, designed coupling system simultaneously oxidation 2,5-furandicarboxylic acid, showing lower at same current density than traditional cathodic anodic reaction, an economical manner.

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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Regulating Reconstruction‐Engineered Active Sites for Accelerated Electrocatalytic Conversion of Urea

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(36)

Published: June 14, 2024

Reconstruction-engineered electrocatalysts with enriched high active Ni species for urea oxidation reaction (UOR) have recently become promising candidates energy conversion. However, to inhibit the over-oxidation of brought by valence state Ni, tremendous efforts are devoted obtaining low-value products nitrogen gas avoid toxic nitrite formation, undesirably causing inefficient utilization cycle. Herein, we proposed a mediation engineering strategy significantly boost high-value formation help close loop employment economy. Specifically, platinum-loaded nickel phosphides (Pt-Ni

Language: Английский

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