Non-metallic iodine single-atom catalysts with optimized electronic structures for efficient Fenton-like reactions DOI Creative Commons

Junjun Pei,

Jianbin Liu,

Kaixing Fu

et al.

Nature Communications, Journal Year: 2025, Volume and Issue: 16(1)

Published: Jan. 18, 2025

In this study, we introduce a highly effective non-metallic iodine single-atom catalyst (SAC), referred to as I-NC, which is strategically confined within nitrogen-doped carbon (NC) scaffold. This configuration features distinctive C-I coordination that optimizes the electronic structure of nitrogen-adjacent sites. As result, arrangement enhances electron transfer from peroxymonosulfate (PMS) active sites, particularly electron-deficient carbon. followed by deprotonation process generates radical (SO5•-). Subsequently, SO5•- undergoes disproportionation reaction, leading production singlet oxygen (1O2). Furthermore, energy barrier for rate-limiting step generation in I-NC significantly lower at 1.45 eV, compared 1.65 eV NC reduction effectively overcomes kinetic obstacles, thereby facilitating an enhanced 1O2. Consequently, exhibits remarkable catalytic efficiency and unmatched reactivity PMS activation. leads accelerated degradation pollutants, evidenced relatively high observed rate constant (kobs ~ 0.436 min-1) other metallic SACs. study offers valuable insights into rational design SACs, showcasing their promising potential Fenton-like reactions water treatment applications.

Language: Английский

Coupled Surface-Confinement Effect and Pore Engineering in a Single-Fe-Atom Catalyst for Ultrafast Fenton-like Reaction with High-Valent Iron-Oxo Complex Oxidation DOI

Bingkun Huang,

Zelin Wu, Xinhao Wang

et al.

Environmental Science & Technology, Journal Year: 2023, Volume and Issue: 57(41), P. 15667 - 15679

Published: Oct. 6, 2023

The nanoconfinement effect in Fenton-like reactions shows great potential environmental remediation, but the construction of confinement structure and corresponding mechanism are rarely elucidated systematically. Herein, we proposed a novel peroxymonosulfate (PMS) activation system employing single Fe atom supported on mesoporous N-doped carbon (FeSA-MNC, specific surface area = 1520.9 m2/g), which could accelerate catalytic oxidation process via surface-confinement effect. degradation activity confined was remarkably increased by 34.6 times compared to its analogue unconfined system. generation almost 100% high-valent iron-oxo species identified 18O isotope-labeled experiments, quenching tests, probe methods. density functional theory illustrated that narrows gap between d-band center Fermi level atom, strengthens charge transfer rate at reaction interface reduces free energy barrier for PMS activation. exhibited excellent pollutant efficiency, robust resistance coexisting matter, adaptation wide pH range (3.0-11.0) various temperature environments (5-40 °C). Finally, FeSA-MNC/PMS achieve sulfamethoxazole removal without significant performance decline after 10,000-bed volumes. This work provides insights into chemistry guides design superior systems remediation.

Language: Английский

Citations

105
Rational modulation of Fe single-atom electronic structure in a Fe-N2B4 configuration for preferential 1O2 generation in Fenton-like reactions DOI
Yuhan Long, Zhenhua Cao,

Weiran Wu

et al.

Applied Catalysis B Environment and Energy, Journal Year: 2023, Volume and Issue: 344, P. 123643 - 123643

Published: Dec. 21, 2023

Language: Английский

Citations

50
Advancements in Electrocatalytic Nitrogen Reduction: A Comprehensive Review of Single‐Atom Catalysts for Sustainable Ammonia Synthesis DOI
Xianhu Long, Fan Huang,

Zhangnan Yao

et al.

Small, Journal Year: 2024, Volume and Issue: 20(32)

Published: March 22, 2024

Abstract Electrocatalytic nitrogen reduction technology seamlessly aligns with the principles of environmentally friendly chemical production. In this paper, a comprehensive review recent advancements in electrocatalytic NH 3 synthesis utilizing single‐atom catalysts (SACs) is offered. Into research and applications three categories SACs: noble metals (Ru, Au, Rh, Ag), transition (Fe, Mo, Cr, Co, Sn, Y, Nb), nonmetallic (B) context ammonia delved. In‐depth insights into material preparation methods, coordination patterns, characteristics reaction (NRR) are provided. The systematic comparison capabilities various SAC types offers framework for their integration NRR. Additionally, challenges, potential solutions, future prospects incorporating SACs endeavors discussed.

Language: Английский

Citations

26
Long-range interactions driving neighboring Fe–N4 sites in Fenton-like reactions for sustainable water decontamination DOI Creative Commons
Zelin Wu, Zhaokun Xiong,

Bingkun Huang

et al.

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

Published: Sept. 5, 2024

Language: Английский

Citations

26
Atomically Dispersed p‐Block Aluminum‐Based Catalysts for Oxygen Reduction Reaction DOI Open Access
Lei Zhao, Yunkun Dai, Yunlong Zhang

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(20)

Published: March 13, 2024

The main group metals are commonly perceived as catalytically inert in the context of oxygen reduction reactions (ORR) due to delocalized valence orbitals. Regulating local environment and structure metal center coordinated by nitrogen ligands (M-N

Language: Английский

Citations

20
The “4 + 1” strategy fabrication of iron single-atom catalysts with selective high-valent iron-oxo species generation DOI Creative Commons
Chen Liu, Jinglu Li,

Xinxia He

et al.

Proceedings of the National Academy of Sciences, Journal Year: 2024, Volume and Issue: 121(23)

Published: May 30, 2024

Single-atom catalysts (SACs) with atomic dispersion active sites have exhibited huge potentials in peroxymonosulfate (PMS)-based Fenton-like chemistry water purification. However, four-N coordination metal (MN 4 ) moieties often suffer from such problems as low selectivity and narrow workable pH. How to construct SACs a controllable strategy optimized electronic structures is of great challenge. Herein, an innovative (i.e., the “4 + 1” fabrication) was devised precisely modulate first-shell coordinated microenvironment FeN SAC using additional N (SA-FeN 5 ). This leads almost 100% selective formation high-valent iron-oxo [Fe(IV)═O] (steady-state concentration: 2.00 × 10 −8 M) SA-FeN /PMS system. In-depth theoretical calculations unveil that configuration optimizes electron distribution monatomic Fe sites, which thus fosters PMS adsorption reduces energy barrier for Fe(IV)═O generation. then attached polyvinylidene difluoride membrane continuous flow device, showing long-term abatement microcontaminant. work furnishes general effective activation metal-oxo species generation by high N-coordination number regulation SACs, would provide guidance rational design superior environmental

Language: Английский

Citations

19
Atomically dispersed Fe-N5 sites with optimized electronic structure for sustainable wastewater purification via efficient Fenton-like catalysis DOI
Yanan Li, Jia Wei,

Nan Cui

et al.

Applied Catalysis B Environment and Energy, Journal Year: 2024, Volume and Issue: 358, P. 124385 - 124385

Published: July 9, 2024

Language: Английский

Citations

18
Ball-milled pyrite@biochar induced percarbonate activation for sustainable degradation of antibiotic norfloxacin at inherent pH environment DOI

Zhihua Mo,

Chengjian Li,

Yu Zhang

et al.

Separation and Purification Technology, Journal Year: 2024, Volume and Issue: 335, P. 126202 - 126202

Published: Jan. 4, 2024

Language: Английский

Citations

17
The structure-performance relationships in active center size-dependent Fenton-like catalysis: From nanoparticles to single atoms DOI

Bingkun Huang,

Zelin Wu, Hongyu Zhou

et al.

Applied Catalysis B Environment and Energy, Journal Year: 2024, Volume and Issue: 355, P. 124157 - 124157

Published: May 9, 2024

Language: Английский

Citations

17
Synergetic Manipulation Mechanism of Single-Atom M–N4 and M–OH (M = Mn, Fe, Co, Ni) Sites for Ozone Activation: Theoretical Prediction and Experimental Verification DOI

Guangfei Yu,

Jing Wang,

Zhaomeng Xu

et al.

Environmental Science & Technology, Journal Year: 2024, Volume and Issue: 58(21), P. 9393 - 9403

Published: May 15, 2024

Carbon-based single-atom catalysts (SACs) have been gradually introduced in heterogeneous catalytic ozonation (HCO), but the interface mechanism of O3 activation on catalyst surface is still ambiguous, especially effect a hydroxyl group (M–OH) at metal sites. Herein, we combined theoretical calculations with experimental verifications to comprehensively investigate mechanisms series conventional SAC structures N-doped nanocarbon substrates (MN4–NCs, where M = Mn, Fe, Co, Ni). The synergetic manipulation atom and M–OH pathways was paid particular attention. tends directly interact MnN4–NC, FeN4–NC, NiN4–NC catalysts, among which MnN4–NC has best activity for its relatively lower energy barrier (0.62 eV) more active surface-adsorbed oxygen species (Oads). On CoN4–NC catalyst, direct interaction site energetically infeasible, can be activated generate Oads or HO2 from indirect participation results showed that 90.7 82.3% total organic carbon (TOC) removed within 40 min during p-hydroxybenzoic acid respectively. Phosphate quenching, characterization, EPR measurement further supported prediction. This contribution provides fundamental insights into SACs, methods ideals could helpful future studies environmental catalysis.

Language: Английский

Citations

17