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

Mott–Schottky Barrier Enabling High‐Performance Hydrazine‐Assisted Hydrogen Generation at Ampere‐Level Current Densities DOI

Yaping Huang,

Xia Zhang, Linfeng Li

et al.

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: unknown

Published: April 18, 2024

Abstract Local electron density manipulation can optimize the adsorption and desorption nature of catalysts leading to enhanced catalytic activity for water oxidation. Construction a Mott–Schottky barrier allows transition in because their different Fermi levels. Herein, Pt@NiFc‐MOF heterojunction is constructed, which electrons are transferred from NiFc‐MOF Pt as triggered by formed built‐in electric field at interface. The as‐prepared reveals exceptional performance toward hydrazine oxidation reaction (HzOR), hydrogen evolution (HER), overall splitting (OHzS) ampere‐level current densities. advanced configured also be further evidenced concept direct liquid N 2 H 4 /H O fuel cell (Pt@NiFc‐MOF//Pt Net), yielding maximum power 415.2 mW cm ‒2 80°C work stably 190 h 500 mA (at 25°C). One more function clarified well, that it purify hydrazine‐rich wastewater 718 6 ppb (less than U.S. Environmental Protection Agency 10 ppb) 120 min . This represents breakthrough interface engineering metal–organic frameworks (MOFs) industry‐level generation its beyond.

Language: Английский

Citations

34
Design and regulation of defective electrocatalysts DOI
Yiqiong Zhang, Jingjing Liu, Yangfan Xu

et al.

Chemical Society Reviews, Journal Year: 2024, Volume and Issue: unknown

Published: Jan. 1, 2024

This review focuses on the synthesis and characterization of defective electrocatalysts, internal correlation between defects catalytic activity, development application electrocatalysts in various fields.

Language: Английский

Citations

27
Construction of 2D CoFe-MOF derived from LDH electrocatalyst for efficient oxygen and urea evolution DOI

Aojie Yuan,

Jianhao Du,

Yang Zheng

et al.

Journal of Colloid and Interface Science, Journal Year: 2025, Volume and Issue: 684, P. 243 - 250

Published: Jan. 15, 2025

Language: Английский

Citations

5
Enhanced Photocatalytic Efficiency Through Oxygen Vacancy‐Driven Molecular Epitaxial Growth of Metal–Organic Frameworks on BiVO4 DOI Open Access

Yan Xin,

Jian Tian, Xianqiang Xiong

et al.

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

Published: Jan. 19, 2025

Abstract Efficient charge separation at the semiconductor/cocatalyst interface is crucial for high‐performance photoelectrodes, as it directly influences availability of surface charges solar water oxidation. However, establishing strong molecular‐level connections between these interfaces to achieve superior interfacial quality presents significant challenges. This study introduces an innovative electrochemical etching method that generates a high concentration oxygen vacancy sites on BiVO 4 surfaces (Ov‐BiVO ), enabling interactions with oxygen‐rich ligands MIL‐101. reduces formation energy and promotes conformal growth . The Ov‐BiVO /MIL‐101 composite exhibits ideal interface, achieving impressive photocurrent density 5.91 mA cm −2 1.23 V RHE , along excellent stability. high‐performing photoanode enables unbiased tandem device /MIL‐101‐Si cell system, solar‐to‐hydrogen efficiency 4.33%. integration mitigates states enhances internal electric field, facilitating migration photogenerated holes into MIL‐101 overlayer. process activates highly efficient Fe catalytic sites, which effectively adsorb molecules, lowering barrier oxidation improving kinetics. Further studies confirm broad applicability vacancy‐induced molecular epitaxial in various MOFs, offering valuable insights defect engineering optimizing enhancing photocatalytic activity.

Language: Английский

Citations

4
Strong Interfacial Interaction in Polarized Ferroelectric Heterostructured Nanosheets for Highly Efficient and Selective Photocatalytic CO2 Reduction DOI Open Access
Xiao Liu, Yuyin Wang, Wenchao Tian

et al.

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

Published: Jan. 19, 2025

Abstract Heterojunctions are sustainable solutions for the photocatalytic CO 2 reduction reaction (CO RR) by regulating charge separation behavior at interface. However, their efficiency and product selectivity severely hindered inflexible weak built‐in electric field electronic structure of two phases. Herein, ferroelectric‐based heterojunctions between polarized bismuth ferrite (BFO(P)) CdS constructed to enhance interfacial interactions catalytic activity. The intrinsic polarization depending on ferroelectric state causes significant electrostatic potential difference energy‐band bending. This helps overcome unsatisfactory redox that differs from classical mechanism, synergy heterostructure facilitates effective transfer photogenerated charges with an extended lifetime (>20 ns) significantly enhanced photovoltage (1002 times BFO). optimized carrier dynamics allow heterojunction achieve a much higher yield compared state‐of‐the‐art photocatalysts, 85.46 23.47 than those pristine BFO, respectively. Moreover, it maintains impressive 100% together excellent repeatability cycling. work not only sheds light how strong inherent polarity promotes performance photocatalysts but also provides new insights designing efficient RR.

Language: Английский

Citations

4
General Modification Strategy on Amorphous Materials to Boost Catalytic Performance DOI

Binbin Jia,

Gui Liu, Baohong Zhang

et al.

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(44)

Published: May 21, 2024

Abstract Amorphous materials with a high number of unsaturated coordinated dangling bonds exhibits macroscopic homogeneity and isotropy, making it easily modifiable to improve the catalytic properties. At present, several feasible modification strategies for amorphous have been proposed applied multiple fields. This review aims provide comprehensive overview recent research advancements in catalysis. First, general modifying are summarized. Subsequently, potential applications modified electrocatalysis photocatalysis highlighted. Additionally, positive effects various tools on properties elucidated. Finally, summary challenges offer critical perspective further development presented. The primary goal this is systematic understanding how enhance performance stimulate catalysts future.

Language: Английский

Citations

15
Manipulation of Oxidation States on Phase Boundary via Surface Layer Modification for Enhanced Alkaline Hydrogen Electrocatalysis DOI
Huawei Huang, Liangliang Xu, Shouwei Zuo

et al.

Advanced Materials, Journal Year: 2024, Volume and Issue: unknown

Published: July 27, 2024

Abstract In alkaline water electrolysis and anion exchange membrane technologies, the hydrogen evolution reaction (HER) at cathode is significantly constrained by a high energy barrier during dissociation step. This study employs phase engineering strategy to construct heterostructures composed of crystalline Ni 4 W amorphous WO x aiming enhance catalytic performance in HER under conditions. work systematically modulates oxidation states within heterostructure adjust electronic boundary, barriers associated with step, adsorption/desorption properties intermediates process. The optimized catalyst, W/WO ‐2, quasi‐metallic state coordinated low oxygen content , demonstrates exceptional (22 mV@10 mA cm −2 ), outperforming commercial Pt/C (30 ). Furthermore, operando X‐ray absorption spectroscopy analysis theoretical calculations reveal that atoms serve as active sites for nearby facilitated release H 2 . These findings provide valuable insights into designing efficient heterostructured materials conversion.

Language: Английский

Citations

14
Advancing overall water splitting via phase-engineered amorphous/crystalline interface: A novel strategy to accelerate proton-coupled electron transfer DOI
Hui Feng, Yue Han, Yutong Wang

et al.

Journal of Colloid and Interface Science, Journal Year: 2024, Volume and Issue: 667, P. 237 - 248

Published: April 15, 2024

Language: Английский

Citations

12
Promoting Polysulfide Redox Reactions through Electronic Spin Manipulation DOI Creative Commons
Jing Yu, Chen Huang, Oleg Usoltsev

et al.

ACS Nano, Journal Year: 2024, Volume and Issue: 18(29), P. 19268 - 19282

Published: July 9, 2024

Catalytic additives able to accelerate the lithium–sulfur redox reaction are a key component of sulfur cathodes in batteries (LSBs). Their design focuses on optimizing charge distribution within energy spectra, which involves refinement and occupancy electronic density states. Herein, beyond distribution, we explore role spin configuration polysulfide adsorption properties catalytic activity additive. We showcase importance this parameter by generating polarization through defect engineering approach based introduction Co vacancies surface CoSe nanosheets. show change electron state increasing number unpaired electrons with aligned spins. This local rearrangement enhances adsorption, reducing activation Li–S reactions. As result, more uniform nucleation growth Li2S an accelerated liquid–solid conversion LSB obtained. These translate into exhibiting capacities up 1089 mA h g–1 at 1 C 0.017% average capacity loss after 1500 cycles, 5.2 cm–2, 0.16% decay per cycle 200 cycles high loading cells.

Language: Английский

Citations

10
Oxygen Evolution Reaction of Amorphous/Crystalline Composites of NiFe(OH)x/NiFe2O4 DOI
Lu Yao, Xiaofeng Wu, Zhibin Geng

et al.

ACS Nano, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 29, 2025

Orbital structures are strongly correlated with catalytic performance, whereas their regulation strategy is still in pursuit. Herein, the Fe 3d and O 2p orbital hybridization was optimized by controlling content of amorphous NiFe(OH)x (a-NiFe(OH)x), which grown situ on crystalline NiFe2O4 (c-NiFe2O4) using an ultrasonic reduction method. The results electron energy loss spectroscopy (EELS) X-ray absorption spectra (XAS) revealed that Fe-Oa a-NiFe(OH)x effectively strengthened jointing adjacent oxygen (Oc) c-NiFe2O4, further confirmed higher antibonding energies based density functional theory (DFT) calculations. resultant Oa-Fe-Oc at composite interface leads to balanced adsorption desorption energies. Accordingly, optimal strong 3d-O enhanced OER overpotential 150 mV, lower than pristine sample. This work represents a promising approach via introduction phase construct highly efficient catalysts.

Language: Английский

Citations

1