JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2025
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IF 9.7
Min Tang,Wu Liu,Jinquan Wan,Shiyu Zuo,Zhiyong Wang,Rui Peng
Fenton-like oxidation is often hampered by high energy barriers, uncontrolled oxidation pathways, and inefficient reactive oxygen species (ROS) utilization. Here, we report an energy-driven confined catalytic nanoreactor that leverages the in-situ confinement energy generated within nanopores to fundamentally regulate degradation thermodynamics. Taking sulfamethoxazole (SMX) as a model contaminant, the confined nanoreactor exhibited a 22.11-fold higher kinetic constant (0.157 min −1 ) and 40 % enhanced mineralization efficiency compared with its non-confined system. The imprinting channel of confined nanoreactor enabled selective adsorption of SMX within the nanochannel, inducing pronounced confinement effects. The resulting confinement energy triggered a low-entropy degradation pathway (ΔS reduced by 3.2 × 10 3 -fold), which broke thermal equilibrium constraints and redirected SMX oxidation along a low-energy-barrier route. The in-situ confinement-induced low-entropy reaction not only accelerated pollutant degradation but also improved ROS conversion efficiency. This study demonstrated a green and sustainable approach to overcome the intrinsic efficiency bottleneck of Fenton-like processes and provide a new perspective on exploiting nanoconfinement effects for environmental remediation.
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高影响因子
WATER AIR AND SOIL POLLUTION
·
2025
·Vol. 237
·期 1
·9
·
IF 3
Liu Yiqing,Hu Hong,Chen Chuanzeng,Xu Linghan
Generally, Fe(II) has an efficiently catalytic activity toward peroxymonosulfate (PMS), but the slow conversion of Fe(III) to Fe(II) and production of iron sludge impede the practical application of Fe(II)/PMS system. In this work, ascorbic acid (AA), a complexing agent and reductant, was introduced to Fe(III)/PMS process to facilitate the Fe(III) reduction. The decoloration of rhodamine B (RhB) was obviously enhanced in Fe(III)/PMS process with the addition of AA. Fe(III)-AA complex was firstly generated in Fe(III)/AA/PMS process via the complexation and then was reduced to Fe(II), which could catalyze PMS to yield oxidative species. Fe(IV), sulfate radical (SO 4 •− ) and hydroxyl radical ( • OH) were the working oxidants for RhB decoloration in this system, and SO 4 •− played a major role. Increasing Fe(III), AA or PMS dosage was beneficial to RhB decoloration, but their excessive concentration would hinder RhB decoloration. The existence of HCO 3 − , SO 4 2− or FA in this system showed an inhibition effect on RhB decoloration, while a facilitation effect was obtained when the high concentration of Cl − was present. This research offers a way to improve PMS activation by Fe(III) and a technology for eliminating the refractory organic pollutants from the contaminated water.
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ENVIRONMENTAL RESEARCH
·
2026
·
IF 8.2
Chengwan Wang,Junchen He,Aoyu Shen,Tong Xie,Ruo Huang,Xian Wu,Yue Yuan,Sheng-Tao Yang
Nitrate (NO 3 - ), a prevalent pollutant in aquatic ecosystems, poses significant ecological and human health risks due to its excessive accumulation, which accelerates eutrophication. In this study, a novel bimetallic material (B-Fe/Cu) was synthesized via high-energy ball milling using micron-sized zero-valent iron (ZVI) and copper salts. When integrated with ultraviolet (UV) light, the UV/B-Fe/Cu system achieved complete conversion (100%) of 10 ppm NO 3 - -N within 120 minutes. Intriguingly, abundant Cu species were found to mediate the efficient redox cycling between Fe 3+ and Fe 2+ , and superoxide radicals (O 2 ·- ) facilitated the redox cycling between Fe 3+ /Fe 2+ and Cu 2+ /Cu + , while the localized micro-acidic microenvironment of B-Fe/Cu enabled the dynamic pH regulation during nitrate reduction. These triple functionalities ensured the full nitrate conversion in UV/B-Fe/Cu system without toxic NO 2 - byproduct formation across a wide pH range of 3.0-11.0. Furthermore, the UV/B-Fe/Cu system demonstrated exceptional operational stability and environmental robustness, retaining >90% reduction efficiency after four consecutive reuse cycles. These insights advance the rational design of iron-based materials for scalable and sustainable water purification technologies.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2026
·
IF 9.6
Saeed Rehman,Tao Chen,Hongjuan Sun,Muddasir Hanif,Tongjiang Peng,Osama Tariq Satti,Aref Alshameri
Phthalate esters (PAEs), widely used as plasticizers, persist as recalcitrant organic pollutants with severe ecological implications. In this study, a dual-step pyrolysis strategy was employed to engineer a Fe-N-RHC@p-MMt composite photocatalyst enriched with high-valent Fe sites, nitrogen dopants, and oxygen vacancies. The tailored hybrid achieved a remarkable 92 ± 1.4% degradation of dimethyl phthalate (DMP) with a pseudo-first-order rate constant of 0.64 min −1 in a peroxydisulfate (PDS)-mediated oxidation system under near-visible light irradiation. Structural and spectroscopic analyses revealed graphitized carbon frameworks with superior conductivity, efficient charge migration, and abundant Fe(IV) = O species formation. Mechanistic analysis reveals that Fe₄N centers regulate interfacial electron transfer, stabilize high-valent Fe(IV) = O species, and drive selective non-radical PDS activation dominated by singlet oxygen ( 1 O₂). Moreover, the generated intermediates exhibited significantly reduced toxicity, mutagenicity, and bioaccumulation risks (although intermediates P1, P3, and P6 showed elevated toxicity), validating the process's environmental compatibility. These results highlight Fe-N-RHC@p-MMt as a safe and efficient catalyst for sustainable remediation of PAE-contaminated water.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2026
·
IF 5.4
Da Teng,Pengxiang Qiu,Yingying Xu,Chunjie Zhu,Xiu Zhang,Leyi Liu,Chen Wei,Yalin Yu,Ningxuan Xue,Xinyu Gai,Yiyang Chen,Siyue He,Guanjie Lin,Fengling Liu,Jiayu Gu,Shuai Zhang,Zhaobing Guo
Ferrate(VI) (Fe(VI)) is a powerful oxidant for wastewater treatment, but its use is hindered by electron transfer limitations. To address this, we designed a NiFe-layered double hydroxide-carbon nanotube (NiFe-LDH-CNT) hybrid photocatalyst. The design is based on the hypothesis that incorporating conductive CNTs can enhance interfacial charge-transfer capability, thereby promote Fe(VI) activation. Under visible light, this catalyst enhances Fe(VI) performance by facilitating the formation of reactive high-valent iron intermediates, accompanied by the generation of reactive oxygen species. Compared with pristine NiFe-LDH, the CNT-integrated composite exhibits improved charge separation and accelerated interfacial electron transport, resulting in enhanced pollutant degradation efficiency. In addition, the catalyst remains stable and effective over time, even in complex water environments. This approach offers a practical way to enhance Fe(VI)-based water treatment processes.
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CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Siyu Zhu,Shaojie Shi,Yuqi Yang,Fengjiao Jiang,Xiaoling Gu,Shaodong Jiang,Hongyun Niu,Yaqi Cai
Polycyclic aromatic hydrocarbons (PAHs) are ubiquitous and highly persistent in soil. Owing to the potential adverse effects of peroxides to soil ecosystems, oxidant-free advanced oxidation process (AOP) is highly demanded for PAHs remediation. We utilize the composites of phosphatized sludge biochars and core/shell Fe 3 P@Fe (PSL-Fe 3 P/Fe) as catalysts to decompose PAHs in soil. In a wide range of soil moisture, pyrene, benzo[ a ]anthracene, benzo[ a ]pyrene, indeno[1,2,3- cd ]pyrene, and dibenzo[ a , h ]anthracene are efficiently degraded by PSL-Fe 3 P/Fe within 6 h. For the first time, we find that reactive oxygen species resulting from internal micro-electrolysis (IME) of biochars (cathode) and Fe 3 P@Fe (anode) are sufficient for PAHs degradation. Strong adsorption, excellent electrical conductivity, high potential difference between Fe 3 P@Fe anode and biochars cathode, and acid-microenvironment provided by P 2 O 5 component trigger the remarkable reactivity of PSL-Fe 3 P/Fe. The environmental-benign PSL-Fe 3 P/Fe can eliminate the phytotoxicity of high-level of PAHs (200 mg/kg), recover soil microbial diversity, and promote the growth of lettuce Lactuca sativa .
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CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 13.2
Zhuojun Wu,Wenwen Gong,Xiao Wang,Yuhan Zhang,Wei Zhou,Shixiong Yi,Hong Yang,Guilong Peng
The selective oxidation of methyl phenyl sulfoxide (PMSO) to methyl phenyl sulfone (PMSO 2 ) is widely used to probe high-valent metal-oxo species in advanced oxidation processes (AOPs). However, its specificity remains uncertain. This study systematically investigates PMSO oxidation by sodium hypochlorite (NaClO), sodium periodate (PI), and peroxymonosulfate (PMS) under acidic (pH = 3.0 ± 0.2), neutral (pH = 7.2 ± 0.2), and alkaline (pH = 9.2 ± 0.2) conditions. Batch experiments and kinetic simulations using Kintecus V6.80 revealed that NaClO exhibited the highest reactivity across all pH values, with second-order rate constants of 125, 25, and 2.15 M −1 s −1 under acidic, neutral, and alkaline conditions, respectively. PI was reactive only in acidic media (7.5 M −1 s −1 ), while PMS showed comparable oxidation rates under acidic and alkaline conditions (1.25 and 1.28 M −1 s −1 ), but negligible activity at neutral pH. H 2 18 O labeling confirmed 18 O incorporation into PMSO 2 even without metal catalysts, supporting oxygen atom transfer (OAT) as the dominant mechanism. These results demonstrate that PMSO oxidation and 18 O labeling are not exclusive indicators of high-valent metal species and should therefore be interpreted with caution. The study underscores the need for more selective and reliable approaches to identify transition-metal-based oxidants in AOPs.
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CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 13.2
Jia Zhao,Heng Zhang,Mengfan Luo,Hongyu Zhou,Zehua Wang,Jialong Yin,Chuanshu He,Peng Zhou,Jing Zhang,Bo Lai
Ferrate (Fe(VI)) activation by Mn(II) has been proven as a powerful technology due to the high catalytic activity of Mn(II) and the generation of multiple intermediates. However, the reactivity and stability of these intermediates greatly differ, thus necessitating the precise regulation of redox pathways towards the generation of the most desirable intermediates. In this study, we utilized ligand engineering to finely tune the redox pathways between Fe(VI) and Mn(II). Mn(II) complexing with ethylenediaminetetraacetic acid (EDTA) and nitrotriacetic acid (NTA) switched the redox pathways from generating Mn(IV) to more robust intermediates and enhanced the decontamination ability of Fe(VI). Ligand-to-metal charge transfer promoted the electron migration from Mn(II) complexes to Fe(VI), generating Fe(V) and Mn(III) intermediates. Then, complexing regulated the transformation of Mn(III) to generate different reactive species. Specifically, Mn(II)-EDTA activated Fe(VI) through Fe(IV)/Fe(V) and Mn(V), whereas the Fe(VI)-Mn(II)-NTA system relied on Mn(VII). Owing to the weaker chelating effect of NTA, unstable Mn(III)-NTA was successively oxidized via Mn(V) to Mn(VII). In contrast, the stronger stability of EDTA suppressed the excessive oxidation of Mn(V)-EDTA, boosting pollutant interception of reactive species. Accordingly, the Fe(VI)-Mn(II)-EDTA process delivered stronger activation and wider applicability, diminishing contaminant toxicity and resisting background interference. This study provides valuable insights into Fe(VI) activation induced by transition metal complexes and serves as a reference for selecting efficient strategies to avoid excessive consumption of oxidative capacity.
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Surfaces and Interfaces
·
2026
·
IF 6
Yu Feng,Wenjing Xie,Ao Qian,Yunxuan Xiao,Peng Liu
Phosphate inhibits As sequestration while redirecting interfacial redox pathways. • Passive phosphatization forms a phosphate-enriched mixed corrosion shell. • Surface-associated ROS contribute to enhanced oxic As(III) oxidation. • Surface Fe(II) retention is associated with an anoxic As(0) fraction up to 32.7%. Surface corrosion layers govern the reactivity of zero-valent iron (ZVI), yet their dynamic reconstruction by co-occurring phosphate and its consequences for arsenic (As) transformation remain poorly understood. In this work, we demonstrate that in situ passive phosphatization restructures the ZVI interface into a phosphate-enriched mixed corrosion shell. This interfacial reconstruction decreased overall As sequestration through competitive phosphate occupancy but promoted distinct As(III) redox pathways depending on oxygen availability. Under oxic conditions, phosphate promoted aqueous As(V) accumulation and increased the XPS-derived near-surface As(V) fraction from 52.1% to 78.1% on the finer ZVI. Oxygen-exposure, scavenger, and probe experiments indicated that this enhancement involved surface-associated reactive oxygen species. Under anoxic conditions, phosphate incorporation increased the near-surface Fe(II) fraction to 70.6% and the As(0) fraction from 6.7% to 32.7%, indicating enhanced interfacial As reduction associated with Fe(II) retention. Spectroscopic and electrochemical analyses further showed altered ZVI corrosion behavior and charge-transfer resistance. These findings establish co-occurring phosphate as an active regulator of ZVI interfacial reactivity rather than merely a competitive inhibitor, revealing a trade-off between As redox transformation and sequestration and highlighting its potential for ZVI-based pretreatment coupled with downstream As capture. Download: Download high-res image (212KB) Download: Download full-size image
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2026
·
IF 5.4
Qing Jin,Kai Ma,Guilong Gao,Xinyu Zhou,Lijie Xu,Ying Zhang,Jiangtao Shi,Lu Gan
In this study, a series of carbon nanofiber (CNF) based one-dimensional catalysts were prepared by pyrolyzing MIL-88B(Fe) anchored PAN/lignin electrospun nanofibers, which were then employed to activate peroxymonosulfate (PMS) for bisphenol A (BPA) degradation. The results indicated that adjusting the lignin content in nanofiber precursor could engineer the crystalline phase of iron compounds in the catalysts, as well as their catalytic activity and stability. Specifically, the precursor with lower lignin content was converted into Fe 3 O 4 loaded CNF (P2L1-Fe-C), whereas Fe 3 C loaded CNF was obtained (P1L1-Fe-C) by increasing lignin content to 50 wt% in the nanofiber precursor. Having multiple Fe valence states within Fe 3 C which facilitated internal electron transfer, P1L1-Fe-C exhibited high catalytic activity with high stability and low iron ion leaching when activating PMS for BPA degradation. P1L1-Fe-C/PMS system could produce more kinds of active species including hydroxyl radical (•OH) and multiple non-radical species like singlet oxygen ( 1 O 2 ), high-valent iron-oxo species, and electron transfer process. Comparatively, P2L1-Fe-C/PMS system was only able to produce •OH and 1 O 2 . The existence of more BPA degradation pathways resulted in enhanced resistance of P1L1-Fe-C/PMS system towards various environmental interferences. This study inspires a new thinking of developing iron based Fenton-like catalyst with tunable crystalline phases through precursor recipe regulation, achieving both high activity and stability. Download: Download high-res image (225KB) Download: Download full-size image
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CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Junren Zhu,Juanjuan Zou,Ting Peng,Xinyi Li,Chaohan Jiang,Shiyang Bai,Wei Ding,Zhenzhen Jiang
HCO 3 − coordination-enabled high-valent cobalt-oxo pathway absent without HCO 3 − • Quantitative Co(IV) contribution elevation from 2.5% to 28% with bicarbonate • Oxidation pathway switch from radical to non-radical regime by bicarbonate • CoCO 3 SO 3 2− complex identified as kinetically competent intermediate • Efficient performance across real waters with Co dosage below discharge limit Bicarbonate, a ubiquitous constituent of natural waters, is typically regarded as a radical scavenger in sulfate-radical-based advanced oxidation processes (SR-AOPs); however, its coordinative interaction with the catalytic metal center and the consequent modulation of oxidative pathways remain poorly understood. In this work, the role of HCO 3 − in the Co(II)-catalyzed activation of calcium sulfite (CaSO 3 ) was systematically investigated. HCO 3 − species is identified to coordinate with Co(II) to assemble a ternary Co(II) − HCO 3 − −S(IV) complex that facilitates the rate-limiting Co(II)-to-Co(III) oxidation, while the subsequent Co(III) − HCO 3 − complexation prevents Co(III) precipitation and sustains the catalytic cycle. Critically, this coordination is a prerequisite for Co(IV) generation: by depressing the Co(IV)/Co(II) redox potential, it unlocks the otherwise forbidden oxygen-atom transfer pathway, yielding a non-radical oxidant entirely absent without HCO 3 − . Together with 1 O 2 , this HCO 3 − -exclusive Co(IV) pathway operates in parallel with the SO 4 •− radical pathway, redirecting the dominant oxidation mechanism from a radical-driven regime toward a non-radical-driven regime, accompanied by a pronounced reduction in apparent activation energy (37.46 kJ mol −1 ). This system functions effectively across a wide pH, exhibits high tolerance to common anionic interferents, and achieves efficient performance across multiple authentic water matrices. In short, this work establishes HCO 3 − as a coordination-directed switch that sustains the catalytic cycle while uniquely gating access to the Co(IV) oxidation pathway, offering a ligand-engineering strategy for tuning reactive species speciation in S(IV)-based AOPs. The HCO 3 − enhanced- and altered- CaSO3 activation by Co(II). Download: Download high-res image (301KB) Download: Download full-size image
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2026
·
IF 9.6
Xiaobo Feng,Boding Zhang,Tong Wu,Hao Jin,Deju Yuan,Anjia Deng,Dong Liu,Likun Pan,Tianjun Ni
Co Fe dual single-atom sites tailor electronic structure to boost PMS activation. • 97.7% ± 2.6% tetracycline removal in 15 min ( k = 0.22 min −1 ), outperforming single-atom catalysts. • Fixed-bed reactor sustains ∼95% tetracycline removal for 120 h with lower ecotoxicity. Single-atom catalysts (SACs) for peroxymonosulfate (PMS) activation are often constrained by the limited electronic tunability of isolated mono-metal centers, which weakens oxidant adsorption and interfacial charge transfer. Herein, we overcome this limitation by constructing a Co Fe dual single-atom catalyst anchored on a nitrogen-doped carbon aerogel (Co–Fe/NCNA) for visible-light-assisted tetracycline degradation. Spectroscopic and synchrotron analyses confirm that atomically dispersed Co N 3 and Fe N 4 sites coexist within a hierarchically porous three-dimensional carbon framework, ensuring high active-site accessibility and rapid mass transport. The Co–Fe/NCNA system achieves 97.7% ± 2.6% tetracycline (TC) removal within 15 min ( k = 0.22 min −1 ), dramatically outperforming single-metal and metal-free analogues. Density functional theory calculations indicate that the coupled Co Fe sites reconstruct the local electronic structure, elevate the d-band center, strengthen PMS adsorption, and reduce the activation barrier for PMS conversion to 0.30 eV. The TC degradation proceeds through a cooperative radical/nonradical oxidation network, in which h + -mediated oxidation acts as the primary apparent pathway, while 1 O 2 , ·O 2 − , ·OH, SO 4 · − , and possible high-valent metal-oxo-like species contribute synergistically or serve as auxiliary pathways. Notably, a fixed-bed continuous-flow reactor sustains ∼95% tetracycline removal over 120 h, and outstanding activity is retained under natural sunlight. This work establishes electronic structure engineering of dual single-atom sites as a powerful strategy to boost visible-light-driven PMS activation for sustainable water remediation. Under visible-light irradiation, the Co Fe dual single-atom sites regulate the local electronic structure, optimize the d-band center, and promote photogenerated charge separation and interfacial electron transfer, thereby enabling efficient peroxymonosulfate (PMS) activation. Through the synergistic cooperation of electron-mediated PMS reduction, hole-mediated PMS oxidation, and Co/Fe self-cycling, radical and non-radical reactive species are generated to construct an integrated oxidation network, which drives the efficient degradation and mineralization of tetracycline. Download: Download high-res image (401KB) Download: Download full-size image
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危险品化学品经营许可证（带存储）