Modulation of the Lattice Structure of CuFe/Copper Foam Catalysts by Doping with Bi to Improve the Efficiency of Electrocatalytic Ammonia Synthesis DOI

Chaofan Guo,

Suyi Yang,

Liting Wei

et al.

ACS Sustainable Chemistry & Engineering, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 22, 2025

Nitrogen reduction reaction (NRR) offers a sustainable alternative to the energy-intensive Haber–Bosch process for ammonia synthesis under ambient conditions while also mitigating serious global warming impact of fossil fuels. However, competing hydrogen evolution remains significant challenge in NRR systems. In this work, we propose Bi-doped CuFe nanoclusters loaded on 3D copper foams (CFs) as an enhanced N2 electrocatalyst NRR. The catalyst exhibited superior activity compared undoped counterpart, achieving high yield 216.1 μg h–1 cm–2 with Faradaic efficiency 46.8% at −0.4 V vs reversible electrode. Importantly, showed good selectivity minimal N2H4 byproduct generation and excellent stability. Bismuth incorporation induced lattice expansion electronic defects, which turn created structural defects oxygen vacancies. These changes effectively promoted adsorption activation molecules. Comprehensive characterization revealed that Bi doping decreased vacancy density bulk phase but increased surface. This phenomenon expanded spacing, inhibiting H* combination produce H2, surface vacancies regulated strength NxHy intermediates during electrocatalytic process. Density functional theory calculations further confirmed active sites, well subsequent hydrogenation steps, leading lower energy barrier distal pathway NH3 formation. Moreover, Zn–N2 battery assembled Bi–CuFe/CF shows power 14.01 mW cm–2, enables simultaneous production supply, gives it potential field energy. work demonstrates promising approach developing efficient electrocatalysts by structure modulation, contributing transition toward low-carbon economy.

Language: Английский

Highly Conductive Non-Calcined 2D Cu0.3Co0.7 Bimetallic–Organic Framework for Urea Electrolysis in Simulated Seawater DOI

Soheila Sanati,

David B. Cordes, Alexandra M. Z. Slawin

et al.

Inorganic Chemistry, Journal Year: 2024, Volume and Issue: 64(1), P. 510 - 518

Published: Dec. 20, 2024

Global clean energy demands can be effectively addressed using the promising approach of hydrogen generation combined with less consumption. Hydrogen generated, and urea-rich wastewater pollution mitigated in a low-energy manner urea oxidation reaction (UOR). This paper seeks to assemble unique electrocatalyst pristine 2D MOF, [Co(HBTC)(DMF)]n (Co-MUM-3), from 1,3,5-benzenetricarboxylate (BTC) oxidize simulated seawater. Ni foam (NF)-based working electrodes were fabricated by incorporating series heterometallic CuCo-MUM-3 frameworks (Cu0.1Co0.9-MUM-3, Cu0.2Co0.8-MUM-3, Cu0.3Co0.7-MUM-3, Cu0.4Co0.6-MUM-3), after which their application was examined. A very low required overpotential [1.26 V vs reversible electrode (RHE) 1 M KOH + 0.5 NaCl (simulated seawater) 0.33 urea] Tafel slope 112 mV dec–1 could observed for Cu0.3Co0.7-MUM-3 electrocatalyst, ensuring achievement electro-oxidation evolution reactions at corresponding 10 mA cm–2 electrocatalytic current density. relatively lower will evident compared other reported MOFs, outperforming commercial catalyst RuO2 (1.41 cm–2, 131 dec–1) considerable stability significantly high densities minimum 72 h.

Language: Английский

Citations

4
Hierarchical Spin‐Polarized Nanosheet Array for Boosting Ampere‐Level Water Oxidation Under Magnetic Field DOI Open Access
Haifan Li, Quan Quan, Hongliang Dong

et al.

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

Published: Jan. 7, 2025

Abstract The spin‐polarization strategy by manipulating magnetic electrocatalysts can promote the spin‐sensitive oxygen evolution reaction (OER) while developing efficient spin‐polarized materials toward ampere‐level OER is still challenging. Herein, a hierarchical inter‐doped (Ru‐Ni)O x nanosheet array in situ grown on nickel foam designed, which exhibits distinguished overpotential of 286 mV at 1 A cm −2 under 0.4 T field and steady lifespan 200 h ampere current density (i.e., ), outperforming most reported state‐of‐art spin‐selective catalysts alkaline electrolytes Integrating intrinsic interfacial significantly boost catalytic activity for field. Specifically, spin‐aligned Ru sites optimize rate‐determined O─O coupling step to reduce thermodynamic barrier OER. Meanwhile, charge transfer kinetics promoted due accelerating electron via spin pinning ferromagnetic‐antiferromagnetic interface. design structure that integrates strategies provides an additional route catalyst capable serving densities.

Language: Английский

Citations

0
Enhanced activation of peroxymonosulfate by one-step biosynthesis of reduced graphene oxide-supported nano iron sulfide: Effect of physicochemical factors on catalytic activity DOI

Heng Li,

Zhenjun Zhang, Jinfeng Lü

et al.

Colloids and Surfaces A Physicochemical and Engineering Aspects, Journal Year: 2025, Volume and Issue: unknown, P. 136142 - 136142

Published: Jan. 1, 2025

Language: Английский

Citations

0
What Is the Mechanism by which the Introduction of Amorphous SeOx Effectively Promotes Urea‐Assisted Water Electrolysis Performance of Ni(OH)2? DOI Open Access
Qiuyan Chen, Jinwei Chen, Xinran Dong

et al.

Small, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 15, 2025

Nickel hydroxide (Ni(OH)2) is considered to be one of the most promising electrocatalysts for urea oxidation reaction (UOR) under alkaline conditions due its flexible structure, wide composition and abundant 3D electrons. However, slow electrochemical rate, high affinity intermediate *COOH, easy exposure low exponential crystal faces limited metal active sites that seriously hinder further improvement UOR activities. Herein it reported electrocatalyst composed rich oxygen-vacancy (Ov) defects with amorphous SeOx-covered Ni(OH)2 (Ov-SeOx/Ni(OH)2). Surprisingly, at 100 mA cm-2, compared (1.46 V (vs RHE)), Ov-SeOx/Ni(OH)2 has a potential 1.35 V. Meanwhile, catalyst also showed good hydrogen evolution (HER) performance, so used as electrolytic cell assembled by HER bifunctional catalysts only 1.57 could reach cm-2. Density functional theory (DFT) study revealed introduce SeOx optimizes electronic structure central metal, amorphous/crystalline interfaces promote charge-carrier transfer, shift d-band center entail numerous spin-polarized electrons during reaction, which speeds up kinetics.

Language: Английский

Citations

0
Modulation of the Lattice Structure of CuFe/Copper Foam Catalysts by Doping with Bi to Improve the Efficiency of Electrocatalytic Ammonia Synthesis DOI

Chaofan Guo,

Suyi Yang,

Liting Wei

et al.

ACS Sustainable Chemistry & Engineering, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 22, 2025

Nitrogen reduction reaction (NRR) offers a sustainable alternative to the energy-intensive Haber–Bosch process for ammonia synthesis under ambient conditions while also mitigating serious global warming impact of fossil fuels. However, competing hydrogen evolution remains significant challenge in NRR systems. In this work, we propose Bi-doped CuFe nanoclusters loaded on 3D copper foams (CFs) as an enhanced N2 electrocatalyst NRR. The catalyst exhibited superior activity compared undoped counterpart, achieving high yield 216.1 μg h–1 cm–2 with Faradaic efficiency 46.8% at −0.4 V vs reversible electrode. Importantly, showed good selectivity minimal N2H4 byproduct generation and excellent stability. Bismuth incorporation induced lattice expansion electronic defects, which turn created structural defects oxygen vacancies. These changes effectively promoted adsorption activation molecules. Comprehensive characterization revealed that Bi doping decreased vacancy density bulk phase but increased surface. This phenomenon expanded spacing, inhibiting H* combination produce H2, surface vacancies regulated strength NxHy intermediates during electrocatalytic process. Density functional theory calculations further confirmed active sites, well subsequent hydrogenation steps, leading lower energy barrier distal pathway NH3 formation. Moreover, Zn–N2 battery assembled Bi–CuFe/CF shows power 14.01 mW cm–2, enables simultaneous production supply, gives it potential field energy. work demonstrates promising approach developing efficient electrocatalysts by structure modulation, contributing transition toward low-carbon economy.

Language: Английский

Citations

0