JOURNAL OF MEMBRANE SCIENCE
·
2026
·
IF 8.8
Yu Gao,Yugang Zhou,Shuaicai Wang,Tao Zhang,Ruina Zhang,Yanshuo Li,Wei Fang
The treatment of heavy metal-contaminated wastewater remains a critical challenge due to the coexistence of multiple metal ions and the lack of efficient recovery strategies. Herein, we report an H-type electrochemical membrane reactor that enables the sequential recovery of Pb 2+ and Zn 2+ from multicomponent wastewater while simultaneously driving chlor-alkali electrolysis. The system operates in a two-electrode configuration with a polysulfone-ZrO 2 composite membrane, which prevents cross-contamination between the compartments and stabilizes the local pH environment. In a solution containing 0.01 M Pb 2+ and 0.01 M Zn 2+ , Pb 2+ is preferentially reduced and deposited as fluffy lead with 99.3% recovery efficiency after 10 h of galvanostatic electrolysis at 10 mA cm −2 . When most of Pb 2+ is depleted, the hydrogen evolution reaction becomes dominant, raising the pH and inducing the precipitation of Zn 2+ as Zn(OH) 2 with 99.8% recovery efficiency, which is subsequently converted to ZnO. The membrane improves Pb 2+ /Zn 2+ recovery efficiencies and reduces energy consumption compared with the membrane-free system. The anode produces Cl 2 with Faradaic efficiency >95%, and the cathode generates H 2 (with Faradaic efficiency: from 1.6% at 1 h to 99.2% at 10 h) and NaOH. This integrated strategy offers a sustainable pathway for the stepwise recovery of metal resources from complex wastewater while co-generating valuable chemicals.
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TALANTA
·
2026
·
IF 6.7
Zifeng Wang,Cong Dai
The dual-channel fluorescent sensing of hydroxyl radicals (·OH) is of great importance for environment and life. Organic cage for fluorescence sensing suffers from short excitation/emission wavelength and poor water solubility, while the application of carbon quantum dots is also hindered by the time-consuming preparation in high pressure and temperature conditions. Herein, we report a red emitted carbon dots derived from cationic organic cage for dual-channel fluorescent sensing of ·OH. The abundant flexible methylene within the cationic organic cage leads to remarkable collapse of intrinsic cavity. The ring-opening of imidazole structure occurs via redox reaction at acidic condition, resulting in the simple formation of carbon dots with the emission at 640 nm. Under acidic conditions, the ·OH generated via Fenton reaction exhibits strong affinity toward the prepared carbon dots. The mild oxidation at pH 1 significantly enhances the fluorescence, whereas the severe oxidative degradation at pH 6 leads to obvious fluorescence quenching. Based on the mutual verification of dual signals, a dual-channel fluorescent sensing method is established for ·OH in environmental samples and biological fluids. The sensing at pH 6 and 1 respectively achieves the linearity range of 1-50 and 5-50 μM, the limit of detection of 7.3 and 11.8 nM, and the relative standard deviation of 0.76% and 0.83% for 10 replicate analysis. The proposed method gives the recoveries of spiked ·OH ranged from 97.3% to 103.4% in real samples, demonstrating excellent accuracy and reliability. This study underscores the promising application potential of organic cage and carbon dots in fluorescent sensing. Furthermore, combined with Fenton reaction, the proposed dual-channel sensing platform can also be utilized to the detection of hazardous substances or biomarkers capable of H 2 O 2 generation.
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JOURNAL OF HAZARDOUS MATERIALS
·
2026
·
IF 10.6
Lan Li,Hui Chen,Yuheng Chen,Baiyang Chen
Singlet oxygen ( 1 O 2 ) is a key reactive species in environmental, chemical, and biological systems. For decades, furfuryl alcohol (FFA) has been used as a probe for quantifying 1 O 2 based on the assumption that it reacts selectively with 1 O 2 but is inert toward other oxidants. However, we demonstrate that this assumption is fundamentally flawed in the chlorine-hydrogen peroxide (H 2 O 2 ) system-one of the most common contexts for 1 O 2 generation. Results demonstrate that chlorine alone can degrade FFA significantly, implying that previous studies may have systematically overestimated 1 O 2 yields. Specifically, raising pH facilitated the decay of chlorine but hindered FFA degradation, suggesting that 1 O 2 formation is unfavorable under alkaline conditions. Increasing the dosage of chlorine enhanced FFA degradation, but decreased the relative contribution of 1 O 2 to FFA degradation. More strangely, increasing the FFA dosage unexpectedly reduced the kinetics of FFA degradation, implying that the concentration of 1 O 2 was not constant under fixed chlorine-H 2 O 2 condition. Maintaining low dissolved oxygen enhanced FFA decay, suggesting that superoxide is not an intermediate for 1 O 2 formation. Furthermore, pyranone was not formed during FFA degradation processes, invalidating it as a characteristic product. These evidences together challenge the accountability regarding FFA selectivity, pyranone formation, and 1 O 2 formation mechanisms before using FFA for 1 O 2 quantification in chlorine-involved systems.
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ENVIRONMENTAL RESEARCH
·
2026
·
IF 8.2
Suzhou Xu,Xinyu Wang,Zhiwei Yang,Yueqi Pan,Kecheng Wen,Xiaoning Guan,Xianchun Chen,Jing Zhang
Regulating the electronic structure of Fe active sites is an effective strategy to enhance peroxymonosulfate (PMS)-triggered high-valent iron-oxo (Fe IV =O) systems for environmental remediation. In this study, we designed the emerging two-dimensional Mo 4 / 3 B 2 MBene with ordered metal vacancies as ideal anchoring sites for Fe Ⅲ to boost PMS activation and regulate Fe IV =O generation. The Mo 4 / 3 B 2 MBene/Fe Ⅲ /PMS system exhibits outstanding catalytic performance: the pseudo-first-order rate constant ( k obs ) of bisphenol A (BPA) degradation is 200-fold higher than that of the pristine Fe Ⅲ /PMS system, and over 90% of BPA can be removed within 5 min. PMSO probe experiments and density functional theory (DFT) calculations confirm that surface-anchored Fe Ⅲ acts as the active center to activate PMS via direct electron transfer for Fe IV =O formation, and verify the critical role of ordered metal vacancies. Quenching experiments and electron paramagnetic resonance (EPR) spectroscopy reveal that sulfate radicals and hydroxyl radicals serve as supplementary reactive oxygen species in the Mo 4 / 3 B 2 MBene/Fe Ⅲ /PMS system. This work provides a new Fe site design strategy to promote Fe IV =O generation for water purification.
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ANALYTICAL CHEMISTRY
·
2026
·Vol. 98
·期 30
·22473-22483
·
IF 7.3
Xia Jianing,Guo Jian,Gao Min,Mei Bingbao,Li Zhen,Dai Weilin,Zhao Hongbin,Yu Le,Ye Daixin
Intelligence and bionics are key directions for next-generation
sensors, yet achieving dynamic adaptability remains challenging. Inspired
by natural enzymes like chymotrypsin, this work synthesizes a N-doped
graphyne-based composite nanozyme (Se-2NGY) featuring selenium (Se)-single
atoms and cluster sites. Biologically active Se-single atoms act as
the primary catalytic center, while nearby clusters reduce the energy
and stabilize the configuration by inducing the formation of hydrogen
bonds with H 2 O molecules. This synergistic architecture
delivers excellent peroxidase (POD)-like activity. Density functional
theory calculations confirm the clusters’ role in modulating
the p -band center and reducing the energy barrier.
A key innovation is that the POD-like activity can be finely tuned
by UV-light exposure. In-situ characterizations reveal that photoexcitation
converts Se 0 to Se δ+ , generating more
hydroxyl radicals and enhancing catalytic performance. Leveraging
this unique photoresponsive activity, we develop a proof-of-concept,
intelligent colorimetric sensor for water quality monitoring, specifically
targeting thiosulfate detection. By simply adjusting light intensity,
the sensor’s detection range and sensitivity can be dynamically
and rapidly modulated─analogous to an artificial iris─enabling
flexible adaptation to environmental samples with vastly different
pollutant concentrations. This work provides a high-performance nanozyme
design strategy and pioneers a pathway toward light-controllable,
intelligent sensing systems for real-world environmental monitoring.
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Nature Communications
·
2026
·
IF 18.1
Zhang Chunyu,Sun Haozhe,Liu Xiang,Kong Kejian,Zhou Tiancong,Wang Xi,Duan Haohong
Electrochemical C–S bond construction represents an attractive route to produce valuable organosulfur compounds, yet current approaches suffer from low reaction efficiency and rely on sulfites (SO 3 2− ) as the sulfur source. Here we report a paired electrolysis for hydroxymethanesulfonate synthesis from widespread industrial-waste sulfides (HS − ). Specifically, HS − is oxidized to SO 3 2− by in-situ generated H 2 O 2 at cathode, and methanol is oxidized to formaldehyde at anode, with following C–S coupling to form hydroxymethanesulfonate. By matching HS − concentration with current density and strengthening convective mass transfer between intermediates, we achieve efficient hydroxymethanesulfonate production with Faradaic efficiency of 102.8% and productivity of 282 μmol h −1 in a membrane-free H-cell under optimized conditions (50 mA cm −2 , 0.05 M HS − , stirring in anodic chamber). By constructing a flow reactor, this paired electrolysis enables conversion of HS − -contaminated wastewater (from <10 ppm to 3000 ppm) with Faradaic efficiencies exceeding 100%, while tolerating coexisting anions and heavy metals in real effluents. It also converts waste H 2 S gas with >87% conversion and >74% hydroxymethanesulfonate selectivity over 102 hours of stable operation, demonstrating more cost-effective economics to both industrial and previous electrochemical methods.
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MOLECULES
·
2026
·Vol. 31
·期 14
·2407
·
IF 5.1
Junxiong Zhao,Juanping Zhang,Shengchao Xu,Leilei Wang,Xiaochen Li,Yiping Chen,Yan Yang,Guangming Xu
To address the potential ecological risks and environmental persistence of organosilicon-fluorine viscosity reducers in conventional silicone-fluoride drilling fluid systems, this work designs and synthesizes a non-organosilicon-fluorine, high-temperature, comb-shaped zwitterionic polymer viscosity reducer, AD-XSJ. The viscosity reducer is prepared via aqueous free-radical polymerization of acrylic acid (AA), acrylamide (AM), 2-acrylamido-2-methylpropane sulfonic acid (AMPS), and dimethyl diallyl ammonium chloride (DADMAC), and it exhibits low molecular weight, uniform molecular weight distribution, and excellent thermal stability. Analyses by FT-IR, thermogravimetry, particle size, zeta potential measurements and Electrostatic potential (ESP) demonstrate that AD-XSJ dismantles the bentonite network structure through the synergistic combination of hydrogen-bonding adsorption and electrostatic repulsion, releasing trapped free water and thereby substantially reducing viscosity and gel strength. Compared with conventional organosilicon-fluorine viscosity reducers, AD-XSJ exhibits superior viscosity reduction capability under high-solid, high-temperature, and high-salinity calcium-contamination conditions, achieving viscosity reduction rates of 33.3% and 50.0% in fluids contaminated with 10.0% NaCl and 1.0% CaCl2, respectively. In field applications under conditions of high bentonite content and calcium contamination, the viscosity reduction rates reach 57.7% and 62.5%, accompanied by markedly improved rheological properties and an average borehole enlargement rate of only 5.7%, indicating effective shale inhibition and anti-sloughing performance. Integrating efficient viscosity reduction, dispersion stabilization, and inhibition capabilities, this viscosity reducer can replace traditional organosilicon-fluorine products, reduce potential hazards to aquatic ecosystems at the source, and holds considerable promise for engineering and environmentally conscious deployment.
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JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY
·
2026
·
IF 4.4
Tingyang Ming,Miao Hu,Wei Zhu
Non-equilibrium adsorption contributes to post-illumination TC removal. • Bi 2 WO 6 /Ni(OH) 2 shows enhanced adsorption and photocatalytic kinetics. • Charge storage is unlikely to dominate the dark-stage behavior. • Acid extraction reveals adsorption-related surface retention of TC. • Light-off timing supports adsorption relaxation after photocatalysis. The photocatalytic removal of antibiotic pollutants has been widely investigated for water purification, where continued pollutant decay after light irradiation (“dark-stage removal”) represents an intriguing post-illumination phenomenon in photocatalytic systems. Although charge storage provides an important explanation for post-illumination activity, adsorption relaxation after light-off may also contribute to dark-stage removal. In this work, a Ni(OH) 2 -modified Bi 2 WO 6 system was employed as a representative model to investigate non-equilibrium adsorption in photocatalytic dark-stage tetracycline removal. The photocatalytic performance under visible light was first evaluated to establish a high-activity reaction system. Subsequently, a combination of acid extraction, solution–surface distribution analysis, and charge probing experiments was used to clarify the contributions of adsorption redistribution and charge storage. The results demonstrate that charge storage is negligible and unlikely to dominate the dark-stage behavior in the Bi 2 WO 6 /Ni(OH) 2 system. Instead, the apparent dark-stage removal is primarily governed by a non-equilibrium adsorption process, arising from the imbalance between rapid photocatalytic consumption and adsorption–desorption dynamics during illumination. After light-off, the system gradually relaxes toward equilibrium, leading to continued redistribution of tetracycline from the solution to the catalyst surface. This work reveals a photocatalysis-induced non-equilibrium adsorption pathway for dark-stage removal, providing a complementary perspective for understanding post-illumination behavior in photocatalytic systems. Download: Download high-res image (181KB) Download: Download full-size image
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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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LANGMUIR
·
2026
·Vol. 42
·期 29
·21195-21206
·
IF 4.4
Liu Qixin,Zhu Manyu,Li Shanshan,Zhang Yuqi,Li Zihao,Wang Yiran,Wu Lie,Ishibashi Takaaki,Jiang Xiue
Accurately understanding the water structure around multiple
groups
and their synergistic effect at electrified interfaces has been challenging
due to the complexity of the interface. The interfacial chiral symmetry-breaking
effect leads to differences in the spatial distribution of functional
groups and the consequent water structure, thereby providing a possibility
for the accurate analysis of molecular group-associated water. On
the basis of this model and combined with surface-enhanced infrared
absorption spectroscopy and ab initio molecular dynamics simulation,
we have systematically investigated the precise water structure around
carboxyl and amino groups, including the influence of carboxyl groups
on tetrahedrally coordinated water, the effect of amino groups in
tightening the surrounding water organization, and their synergy in
directing the first-layer water toward the surface. The presence of
methyl groups can enhance the interaction between amino groups and
water due to their electron-donating function. Furthermore, we revealed
a ligand-induced enhancement in the hydrogen evolution reaction at
the single group level. Our research provides a new methodology for
obtaining comprehensive insights into the impact of each functional
group, how they synergize to regulate the water structure and proton
reduction in complex systems, and their contribution to proton-coupled
electron-transfer reactions.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2026
·
IF 9.6
Yaqi Cui,Ruilin Lou,Zulpya Mahmut,Fangyu Shi,Jiaqi Zhou,Yaqi Zhu,Zhenzhou Wang,Yifan Chen,Lin Xu,Lin Wang,Biao Dong
Heterojunction structure MOSF NCs serve as an “electron reservoir”. • MOSF NCs transport electrons into bacteria via the surface Fe 3+ /Fe 2+ cycle. • Electronic attack on the CoQ-mediated respiratory chain of bacteria. • This study built a real-time fluorescence system for bacterial ETC interference. Although the phenomenon of current flow between bacteria and nanomaterials has long been observed, the direction of electron flow and specific interaction sites remain unclear. To address this, we designed a molybdenum (Mo) - based heterojunction electron reservoir (MOSF nanocrystals), enabling rapid Mo 6+ /Mo 4+ cycling, and introduced Fe as a mediator to shuttle electrons into bacteria through surface Fe 3+ /Fe 2+ redox. Upon contact with bacteria, MOSF nanocrystals (NCs) have the potential to block the coenzyme Q (CoQ)-mediated electron transport chain (ETC), causing energy depletion and bacterial death. This study also pioneers the development of a real-time fluorescent detection system to monitor electronic interference with bacterial ETC. This system can track how electrons in MOSF NCs inhibit bacterial deoxyribonucleic acid (DNA) replication, which is attributed to the inhibition of adenosine triphosphate (ATP) synthesis. By integrating transcriptomic and biochemical analysis techniques, we deduced at the atomic level that the antibacterial effect likely stems from the disruption of CoQ on the bacterial cell membrane, which in turn blocks the bacterial ETC. This study proposes an effective antibacterial nanoenzyme and a novel detection system, and provides an in-depth exploration of electron interference at the molecular level, advancing the development of bioenergetic therapeutics. We designed a strategy utilizing a Mo-based heterojunction as an electron reservoir (MOSF NCs), enabling rapid electron transfer between Mo 6+ in MoO₃ and Mo 4+ in MoS₂. Additionally, we introduced iron as an electron transfer mediator between the nanomaterials and the bacteria, thereby regulating the electron flow between them and ultimately achieving the goal of bacterial inactivation. Concurrently, this study pioneered the development of a real-time fluorescent detection system for monitoring electronic interference with the bacterial ETC. This system enables direct visualization of how electrons from MOSF NCs inhibit bacterial DNA replication, a process attributed to the suppression of ATP synthesis. Download: Download high-res image (182KB) Download: Download full-size image
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INORGANIC CHEMISTRY
·
2026
·Vol. 65
·期 31
·18314-18324
·
IF 4.6
Zhu Lingfeng,Chen Hao,Liu Xinyue,Shen Quanyi,Yang Suyu,Pu ZeRui,Liu Lizhong,Wu Huifang
Stable
fluorescent sulfur quantum dots (SQDs) were generated directly
through a one-step process via S 2– -mediated regulation
(SMR) of residual polysulfides present in analytical-grade sodium
thiosulfate, eliminating the need for the conventional acid-induced
formation of elemental sulfur from sodium thiosulfate. During this
process, S 2– not only hydrolyzes to produce OH – , which promotes the cleavage of sulfur chains in the
residual polysulfides, but also rapidly captures the generated elemental
sulfur and converts it into abundant polysulfides. These polysulfide
intermediates subsequently undergo nucleation and structural reorganization,
ultimately yielding highly stable SQDs enriched with surface negative
charges. Steady-state and transient fluorescence spectroscopy reveals
that the SQDs produced via SMR (denoted as S 2– -SQDs)
exhibit a quantum yield of 11.13% and a fluorescence lifetime of 9.24
ns, together with significantly enhanced long-term photostability
compared with SQDs prepared under alkaline regulation alone. Furthermore,
the S 2– -SQDs enable rapid and selective fluorescence
sensing of bilirubin, with a detection limit as low as 0.23 μM.
This work provides new mechanistic insights into the fabrication of
stable sulfur-based quantum emitters. More importantly, it highlights
the often-overlooked role of residual sulfur species in commercial
reagents and underscores their substantial contribution to the formation
and luminescence behavior of SQDs.
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