Journal of Environmental Chemical Engineering
·
2026
·Vol. 14
·期 5
·124526
·
IF 7.5
You Zhou,Zhiquan Yang,Siyuan Di,Huarong Yu,Fangshu Qu
Addressing antibiotic water pollution through novel and effective strategies has become a critical endeavor. Increasing studies have shown that peroxymonosulfate (PMS) can be activated to generate singlet oxygen ( 1 O 2 ) by incorporating transition metals into carbon-based materials. Hollow carbon nanocages (HCNs) have proven to be a promising material for advancing energy conversion and battery technologies. However, studies based on HCNs in the field of Fenton-like reactions are scarce. In this study, the Fenton-like activity of HCNs-based catalysts were enhanced via confinement effect coupled with asymmetric Si coordination configuration. The hollow architecture endowed the catalyst with accelerated mass transport and markedly elevated utilization efficiency of active species. Co-HCNs delivered exceptional catalytic performance, accomplishing 99% tetracycline (TC) degradation within 40 min with a 67% mineralization rate, combined with robust anti-interference capacity in real-world water matrices. Density Functional theory (DFT) calculations indicated that the carbon-dense layer boosts the generation of 1 O 2 , in contrast to the cobalt core, which predominantly induced radical-mediated pathways. Integrated experimental analyses further confirmed that the degradation process is dominated by 1 O 2 , with other radicals playing synergistic contributions. Ecotoxicity evaluation verified the environmental compatibility of this process. This work further reveals an "oxidant-derived, dual-channel-driven 1 O 2 supply mechanism." This mechanism enhances the instantaneous supply capacity of 1 O 2 in the system and provides a clearer catalytic rationale for the selective oxidation of pollutants and stable purification in complex water matrices.
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PROCESS SAFETY AND ENVIRONMENTAL PROTECTION
·
2026
·
IF 7.9
Fangchong Han,Bin Zhang,Jie Liu,Lijun Niu,Jun Ke
In this work, a carbon and cobalt co-doped carbon nitride (Co 0.04 -CCN 0.25 ) catalyst was synthesized for superior generation of singlet oxygen ( 1 O 2 ) via peroxymonosulfate (PMS) activation. The findings indicate that carbon self-doping not only reduces the interfacial charge transfer resistance but also constructs efficient electron transfer channels between g-C 3 N 4 support and cobalt active sites. This directional electron transfer increases the electron density of cobalt species, which can accelerate the Co(II)/Co(III) redox cycle. As a result, the optimized Co 0.04 -CCN 0.25 catalyst achieves 100% of bisphenol A (BPA) degradation within 6 min under ambient conditions. Mechanistic investigations reveal that the singlet oxygen is the dominant reactive oxygen species (ROS) at the Co active site in the Co 0.04 -CCN 0.25 , which presents a desirable and recyclable redox pair of Co(II)/Co(III). Furthermore, the modified catalyst exhibits excellent pH tolerance over a broad range and strong anti-interference ability against co-existing anions and humic acid in aqueous solutions. Liquid chromatography-mass spectrometry (LC-MS) analysis and ecotoxicity assessment further demonstrate that the toxicities of BPA degradation intermediates are significantly reduced during the oxidation process. Therefore, this study provides a promising and practical strategy for designing high-efficient C 3 N 4 -based catalyst of PMS activation. Download: Download high-res image (175KB) Download: Download full-size image
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CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Zening Pan,Yudie Fu,Jiayu Wu,Aihua Xu,Xiuying Liu,Shuaiqi Zhao,Xiaoxia Li
Vacancy electronic quality, not quantity, governs catalytic performance. • Co-doping and quenching construct asymmetric Co–Ov–Mo motifs, transforming inert deep traps into active shallow donors. • CMO-Q activates PMS through a dual non-radical pathway. The electronic structure characteristics of oxygen vacancies (O v ) - rather than their quantity - are the fundamental factors determining peroxymonosulfate (PMS) activation. This study proposes a strategy of cobalt doping and controllable quenching to precisely construct two types of O v configurations with distinct electronic properties in MoO 3 : the symmetrical Mo–O v –Mo coordination structure in MoO 3 -Q and the asymmetrical Co–O v –Mo coordination structure in CMO-Q. Comprehensive multimodal characterizations confirm that although MoO 3 -Q has the highest O v concentration (39.78%) and the strongest EPR signal, the significantly broadened tail feature in its valence band XPS spectrum clearly indicates that the vacancies exist in the form of deep-level trap states, making it difficult for the captured charges to participate in subsequent interfacial reactions, thus presenting electronic inertness. In contrast, cobalt doping plays a directional anchoring role in the lattice, guiding the vacancies to preferentially form in the Co-adjacent coordination environment. The constructed asymmetrical Co–O v –Mo structure induces an internal polarization electric field due to the difference in electronegativity between Co 2+ and Mo 6+ , forming a shallow donor state with electron-donating function, thereby endowing the vacancies with intrinsic electronic activity. The electrochemical tests quantitatively reveal the essential differences in interfacial charge transfer kinetics between the two: CMO-Q exhibits the largest open-circuit potential shift (0.59 V ) and the smallest peak potential difference (ΔE = 0.13 V ), while MoO 3 -Q shows the smallest shift (0.47 V ) and the largest ΔE (0.26 V ). Further normalization by the electrochemically active surface area (ECSA) highlights the intrinsic activity difference: the k obs /C dl of CMO-Q reaches 6.18 min −1 ·cm 2 ·mF −1 , which is ten times higher than that of MoO 3 -Q (0.62 min −1 ·cm 2 ·mF −1 ). This work establishes vacancy quality over quantity as the design principle for high-performance catalysts.
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CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Zhimo Fang,Zhou Zhou,Xiaomeng Li,Dongyang Li,Bin Hu,Haoyu Wang,Lin Zhang,Qin Dai,Kai Li,Yao Kong,Shiguan Yang,Qiang Lu
Superexchange-mediated dual-acceptor sites enable spatial charge separation. • Synergistic single-atom and vacancy engineering creates multifunctional sites. • Cu SA -TO-O V delivered excellent corresponding turnover frequencies of 177.52 h −1 . • The photo-Fenton system exhibited wide pH adaptability and anti-interference. Synchronously and efficiently utilizing photogenerated electrons and holes remains a significant challenge in Fenton-like reaction. Herein, the Cu single-atom (Cu SA ) and oxygen vacancy (O V ) co-modified TiO 2 nanoflake-like catalyst is successfully synthesized. O V modulate the electronic coupling interaction, which is proposed to trigger superexchange -mediated electron transfer from Cu 3 d x 2 − y 2 to Ti 3 d xy via O 2 p y orbitals. Specifically, Cu SA serves as the hole-accepting site for 1 O 2 generation, while O V and Ti 3+ functions as the electron-accepting site for •OH production and contaminant adsorption. The substrate enrichment effect and the free radical/non-radical coupling interaction significantly enhances photo-Fenton catalytic performance, achieving superior sulfanilamide removal efficiency across a broad pH range (3–11) and a high turnover frequency of of 177.52 h −1 . This work not only highlights the potential of active site engineering in designing photo-Fenton catalysts but also advances the development of efficient and sustainable water purification solutions.
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ACS ES&T Water
·
2026
·
IF 4.5
Zhan Qihong,Rao Zepeng,Xiao Xin,Chen Baoliang
Micronanobubbles
(MNBs) offer enhanced interfacial area and distinct
interfacial physicochemical properties, but the mechanistic role of
interfacial charge in governing ozone-derived reactive oxygen species
(ROS) remains inadequately understood. Herein, the pH-dependent interfacial
charge characteristics of ozone micronanobubbles (O 3 -MNBs)
were systematically examined to elucidate their influence on sulfamethoxazole
(SMX) degradation. O 3 -MNBs increased the apparent degradation
rate by approximately 4-fold relative to macrobubbles, with initial
enhancement driven by facilitated ozone dissolution and subsequent
acceleration governed by interfacial reaction processes. ζ potential
measurements and ROS probe analyses demonstrated that solution pH
modulates MNB interfacial charge, thereby regulating pollutant interfacial
enrichment and shifting ROS dominance. Acidic conditions promoted
hydroxyl radical ( • OH) formation through interfacial
instability, whereas neutral and alkaline conditions favored the generation
of superoxide radicals (O 2 •– )
and singlet oxygen ( 1 O 2 ). Quadrupole time-of-flight
mass spectrometry (Q-TOF-MS) further confirmed that these distinct
ROS regimes correspond to divergent SMX transformation pathways. The
findings establish interfacial charge regulation as a critical determinant
of reaction selectivity in O 3 -MNB systems and provide mechanistic
guidance for optimizing MNB-assisted ozonation in advanced water treatment.
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JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY
·
2026
·Vol. 74
·期 31
·24501-24512
·
IF 6.7
Xie Sikui,He Yu-Cai
Lignocellulosic biomass, which consists primarily of
cellulose,
hemicellulose, and lignin, is a promising renewable feedstock for
producing high-value biobased amines. In this study, an integrated
chemobiocatalytic strategy was developed to synthesize furfurylamine
from corncob using a newly formulated deep eutectic solvent, [Bet][FA][LA],
that provides both catalytic and solubilizing functions. Under optimized
conditions, corncob was efficiently converted into furfural, which
was subsequently aminated by recombinant Escherichia coli BM-AlaDH coexpressing an ω-transaminase
and alanine dehydrogenase. The whole-cell catalyst enabled in situ
regeneration of L -alanine, thereby reducing amine-donor
requirements and improving biocatalytic efficiency. Integration of
[Bet][FA][LA]-mediated chemocatalysis with whole-cell biocatalysis
converted corncob into furfurylamine in [Bet][FA][LA]. The biocatalytic
amination system could convert biomass-derived 5-hydroxymethylfurfural
(320 mM) and vanillin (20 mM) into the corresponding amines in yields
of 95.4% and 91.0%, respectively. This work establishes a sustainable
route for converting lignocellulose-derived aldehydes into value-added
biobased amines and advances the comprehensive valorization of lignocellulosic
biomass.
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WATER AIR AND SOIL POLLUTION
·
2026
·Vol. 237
·期 20
·1139
·
IF 3.5
Liu Runjie,Chen Li,Zhang Yun,Wu Jingtao,Wang Longfei,Yang Yingchun
In this study, sulfur surface-modified manganese ferrite (MnFe 2 O 4 ) with enriched oxygen vacancies was synthesized using a metal-organic complex precursor strategy for periodate activation toward tetracycline degradation. The optimized catalyst achieved 97% tetracycline removal within 30 min. Sulfur surface modification enhanced oxygen vacancy formation, reduced charge transfer resistance, and promoted interfacial electron transfer. Mechanistic analyses revealed that periodate activation proceeded via an electron-transfer-mediated pathway, in which iodate radicals (IO 3 · ) played the dominant role, while superoxide radicals (O 2 ·− ), hydroxyl radicals ( · OH), singlet oxygen ( 1 O 2 ), and sulfate radicals (SO 4 ·− ) contributed secondarily. Iodine species (I 2 , I 3 − , and HOI) were observed below detection limits under the tested conditions, and periodate was ultimately converted to iodate. These findings demonstrate that sulfur surface modification is an effective strategy for improving ferrite-catalyzed periodate activation and provide insight into more environmentally safer advanced oxidation processes for antibiotic-contaminated water treatment.
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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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CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Yongxue Chen,Xiaodong Lu,Jianping Ge
PC coatings with structural colors are fabricated by embedding method through cooperative DSDV process. • Different from traditional strategies, the embedding method adopts a new “coating before assembly” strategy. • Conformal PC coatings are prepared on 33 substrates, including boards, fabrics, inorganics, metals, plastics, and rubbers. • The embedding method works for the polystyrene-arylate, alkyd, polyurethane, and polyvinyl alcohol-based PC coatings. Colloidal photonic crystal (PC) coating has wide application in automotive manufacturing, textile dyeing, packaging and printing, cosmetics and personal care, and anti-counterfeiting materials. However, the traditional methods based on strategies of “coating after assembly” and “coating along with assembly” show poor compatibility with the substrates and polymer components. Here, a new method based on the embedding of colloidal crystals into the precoated polymer layer was developed to prepare durable PC coatings with bright and uniform structural colors. This embedding method pioneers a new synthetic strategy, which is “coating before assembly”. The coating formation is proved to follow the DSDV mechanism, which refers to the cooperative “polymer dissolution”, “liquid photonic crystal (LPC) sinking”, “polymer diffusion”, and “solvent volatilization” processes. The embedding method successfully produces conformal SiO 2 /(PS-PMMA) PC coatings with fine surface features on 33 substrates, including fibrous boards, fabrics, inorganics, metals, plastics, and rubbers, and it also works for the fabrication of alkyd resin, polyurethane, and polyvinyl alcohol-based PC coatings, which will accelerate its practical implementation in various scenarios. An embedding method following the “Coating before Assembly” strategy is developed to prepare durable PC coatings with bright and uniform structural colors. This method yields conformal coatings on diverse substrates, including fibrous boards, fabrics, inorganic materials, metals, plastics, and rubbers. Additionally, it is applicable to coatings based on acrylic resin, alkyd resin, polyurethane, and polyvinyl alcohol. Download: Download high-res image (100KB) Download: Download full-size image
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CHEMICAL PAPERS
·
2026
·
IF 2.7
Zhu Li,Gao Xizi,Zhang Lijuan,Zhang Jun,Guo Sheng
Advanced oxidation processes (AOPs) based on persulfate (PS) have been widely applied in environmental remediation owing to their ability to generate strong oxidizing reactive species. However, the traditional homogeneous and heterogeneous PS activation systems are prone to cause secondary pollution problems such as the leaching of toxic metals or the formation of sludge. To overcome these technical bottlenecks, this study constructed a ternary catalyst-free system coupling mechanical stirring (MA), ultrasonic irradiation (US), and PS, aiming to efficiently degrade organic contaminants in water bodies. In the proposed MA/US/PS system, peroxymonosulfate (PMS) demonstrates a significantly higher removal rate of Rhodamine B (RhB) than those of sodium persulfate (PDS), ammonium persulfate (PNS), and hydrogen peroxide (H 2 O 2 ) under the same conditions, which could be associated with the asymmetry structure of PMS, potentially facilitating its activation. Moreover, the MA/US/PMS system maintains stable catalytic activity over a broad pH range (3.09–10.52) and demonstrates excellent degradation efficiency in the presence of various coexisting anions and in actual water matrices. The effects of key operational parameters such as PMS dosage, agitation speed, ultrasonic power, and temperature on the degradation efficiency is comprehensively investigated. By combining radical quenching tests and electron paramagnetic resonance (EPR) techniques, the dominant reactive species responsible for RhB removal are identified. This work proposes an efficient, green, and catalyst-free activation strategy for PMS, which holds great potential for the advanced treatment of actual wastewater.
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CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Jin Qian,Xiaoting Hao,Duo Li,Chengshuai Lu,Lulu Chen,Wenjia Han,Zhuqing Liu
High mechanical strength (41.5 MPa) and self-healing efficiency (119%) achieved via DA dynamic covalent bonds and BC reinforcement. • BC-dispersed MWCNTs enable high sensitivity (GF = 10.15) and stable sensing over 0–130% strain. • The flexible electronic skin enables real-time monitoring of joint motions and ECG/EMG signals. Conventional waterborne polyurethane (WPU)-based flexible sensors often exhibit insufficient strength, limited self-healing capacity, and unstable cyclic performance. Herein, a self-healing WPU/bacterial cellulose (BC) composite matrix was fabricated by combining BC nanofiber reinforcement with thermally reversible Diels-Alder (DA) dynamic covalent bonds. Multi-walled carbon nanotubes (MWCNTs) were incorporated as the conductive phase. BC nanofibers interweave with WPU chains to provide topological confinement, while interfacial hydrogen bonding and physical entanglement anchor the polymer chains. At a BC loading of only 5‰, the composite achieved a tensile strength of 41.5 MPa and an elongation at break of 674%. The reversible DA bonds mitigate the trade-off between mechanical strength and self-healing, yielding a self-healing efficiency of 119% after thermal treatment, together with good thermal stability and recyclability. BC also suppresses MWCNT agglomeration and promotes the formation of stable conductive networks. The resulting films exhibited a gauge factor (GF) of 10.15, a stable sensing response over a strain range of 0–130%, and the ability to detect human motion, electromyographic, and electrocardiographic signals. These multifunctional composite films combine mechanical robustness, self-healing performance, and reliable sensing behaviour, indicating their potential for wearable electronics and physiological monitoring. Download: Download high-res image (146KB) Download: Download full-size image
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2026
·
IF 9.1
Liuqing Yang,Zhuoting Xiong,Haowen Zou,Bin Zhao,WingKei Ho,Dingze Lu
Improving the efficiency of nitric oxide (NO) removal while reducing the formation of toxic nitrogen dioxide (NO 2 ) is a challenge. Nonetheless, it remains uncertain regarding the distinct roles of carbon versus nitrogen vacancies in graphitic carbon nitride (g-C 3 N 4 ) in governing the oxidation pathway. In this study, g-C 3 N 4 enriched with carbon or nitrogen vacancies, along with the corresponding polyvinylidene fluoride (PVDF)-supported composite films, are prepared. The adsorptions and anchoring of NO and its intermediates are significantly enhanced by the carbon vacancies. Despite a high free energy barrier of the conversion from nitrite to nitrate, the strong anchoring suppresses the release of gaseous NO 2 . The formation of Nitrogen vacancies gives rise to polarization of the spin, leading to a significant negative displacement of the potential of the conduction band and increased carrier lifetime along with a considerable decrease in the barrier for the conversion of nitrite to nitrate. This mechanism leads to enhanced reaction flux that will improve deep oxidation. The incorporation of these materials into the PVDF film greatly enhances performance and provides reusability. This work elucidates the distinct mechanisms by which carbon and nitrogen vacancies regulate NO oxidation, providing a theoretical basis for designing efficient and selective air purification materials.
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