Journal of Materials Chemistry A
·
2015
·Vol. 3
·期 25
·13308-13316
·
IF 7.443
Bin Yang,Lei Yu,Huijun Yan,Yanbo Sun,Qi Liu,Jingyuan Liu,Dalei Song,Songxia Hu,Yi Yuan,Lianhe Liu,Jun Wang
Pseudocapacitor electrode materials, such as transition metal oxides/sulfides, have been extensively investigated and shown to have fast energy storage properties, but their low rate performance and poor cycle stability are serious problems in practical applications. We present here a design for the architecture of these electrode materials with the aim of improving the rate performance and cycle stability of pseudocapacitors by using an interface ion-exchange method. Precursor materials obtained by a hydrothermal reaction were soaked in aqueous NaHS solution to synthesize the urchin-like core–shell structure of NiCo2(CO3)1.5(OH)3@NiCo2S4. Such core–shell nanostructure electrode materials can make full use of both components with synergistic effects. Excellent results were obtained with a capacitance of 956.4 F g−1 at a current density of 4 A g−1 in the three-electrode system and an actual energy density of 32.3 W h kg−1 and power density of 1835 W kg−1 in the asymmetrical supercapacitor.
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ACS Sustainable Chemistry & Engineering
·
2026
·
IF 7.6
Lin Zhang,Shihang Jin,Shuo Liu,Qiusheng Fu,Xiaoran Shi,Xian Zhang,Zhizhou Yang,Sheng Gao
The introduction of dynamic covalent bonds imparts reprocessability to the thermosets. However, achieving reprocessing in conventional thermosets, which lack dynamic bonds in their cross-linked networks, remains a significant challenge. Herein, we propose a strategy to fabricate silicon-containing resin-based covalent adaptable networks (CANs) from fully cured phenolic resin and silicone resin via the hybrid exchange reaction between phenolic hydroxyl groups (Ph–OH) and siloxane (Si–O–Si) bonds. This hybrid exchange reaction was validated by the degradation of the silicone resin by phenolic compounds. Subsequently, silicon-containing resin-based CANs were prepared from the two fully cured resins by utilizing this reaction. The resulting CANs demonstrate exceptional mechanical and thermal properties, including a tensile strength reaching up to 25.7 MPa, a glass transition temperature (Tg) exceeding 400 °C, and thermal decomposition temperatures (Td5 and Td10) of 410 and 452 °C, respectively, under a nitrogen atmosphere, along with a high char yield (Yc) of 63.7% at 800 °C. Moreover, the materials demonstrate excellent reprocessability, retaining 91.4% and 87.5% of their original tensile strength after the first and second recycling cycles, respectively, while maintaining a Tg consistently above 400 °C throughout. The silicon-containing resin-based CANs presented here offer a promising new strategy for overcoming the reprocessing challenges associated with traditional thermosets.
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INORGANIC CHEMISTRY
·
2026
·
IF 4.6
Yingying Fang,Guangliang Liu,Ying Wang,Ligang Hu,Yong Liang,Yongguang Yin,Yong Cai,Guibin Jiang
Mercury (Hg) biogeochemical cycling involves redox transformations between Hg(0) and Hg(II), likely via a mercurous Hg(I) intermediate. Despite previously thought metastable, Hg(I) was found to exist stably in natural waters; yet, the redox behavior governing Hg(I) occurrence remains elusively studied. Here, we simulated an environmental Eh gradient (0.219–0.600 V, vs SHE) using noninterfering 1,4-benzoquinone and 1,4-hydroquinone as redox mediators, and demonstrate that Hg(I) redox transformations are strongly Eh-dependent. Hg(I) was stable at 0.302–0.339 V, contrasting significant oxidation (19–98%) at 0.369–0.600 V or reduction (81%) at 0.219–0.255 V. Speciation analysis and thermodynamic calculations confirm that varying proton level alters Hg(II) species abundance (HgHPO4, HgPO4–, and Hg(OH)2), driving this Eh-dependence. Specifically, HgHPO4/HgPO4– exhibits lower reduction potentials (to Hg(I), as Hg2(OH)2) than Hg(OH)2. Consequently, Hg(I) is subject to oxidation to HgHPO4/HgPO4– at 0.369–0.440 V (pH 6.0), while Hg(OH)2 preferentially undergoes stepwise reduction to Hg(I) and Hg(0) at 0.236–0.308 V (pH 7.5). Additionally, externally forced Hg(0) removal processes, e.g., purging used in conventional Hg(0) analysis, significantly affect Hg(I) transformations and enhance Hg reduction under reducing conditions, whereas natural degassing has negligible effects. This work provides valuable parameters for Hg redox thermodynamics and important implications for predicting Hg(I) occurrence in aquatic environments.
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LANGMUIR
·
2026
·
IF 4.4
Li Daiqiang,Liu Yang,Zhang Runduo,Di Zhaoying,Guo Xiaonan
The fabrication of highly uniform and dispersed catalysts
is achievable
through atomic layer deposition (ALD). However, the application of
this method in porous materials is largely restricted by the size
compatibility between the host and the guest molecules. In this study,
we coupled ALD with different Cu-based catalysts to develop an interfacial
engineering strategy for the selective catalytic oxidation of ammonia
(NH 3 –SCO). Using Cu(hfac) 2 as the precursor,
it was demonstrated that the pore structure served as a critical steric
gatekeeper. Unhindered mass transfer pathway was observed in mesoporous
Al-SBA-15, which successfully accommodated the large precursors. This
led to a high copper loading of 1.58 wt % along with high interfacial
dispersion. On the contrary, the narrow pores of microporous zeolites
caused significant pore-mouth blockage and external accumulation because
of the size exclusion effect. Therefore, superior intrinsic catalytic
activity was found in the Cu-Al-SBA-15, realizing complete NH 3 conversion at 350 ° C combined with excellent N 2 selectivity. Comprehensive characterizations indicated that a large
proportion (75.64%) of active mononuclear [Cu(OH)] + species
was stabilized by the abundant mesopores and numerous anchoring sites.
These findings provide fundamental information regarding the size-exclusion
mechanisms in ALD, suggesting a potential material design to precisely
control metal–support interfaces for catalysis.
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CHEMICAL ENGINEERING SCIENCE
·
2026
·
IF 5.1
Kao Chen,Huailiang Li,Jingyi Chen,Annan Wang,Weiwei Zhu
Highly recoverable and stable heterogeneous catalysts are critical for peroxymonosulfate (PMS)-based advanced oxidation processes (AOPs). This work addresses the difficult separation and metal leaching issues of conventional powdered metal–organic frameworks (MOFs) by constructing a self-supporting Co-MOF@chitosan (Co-MOF@CS) composite membrane. Through in situ reconstruction during PMS activation, the low-crystallinity Co-MOF precursor transforms into an amorphous CoO(OH) nanolayer on the membrane surface. The reconstructed active phase anchors firmly on the porous CS substrate, thereby enabling efficient PMS activation by facilitating rapid electron transfer and providing abundant surface active sites. The Co-MOF@CS membrane exhibited excellent catalytic performance, degrading > 96% of the methylene blue (MB) and ∼70% of sulfadiazine (SDZ) after five consecutive cycles. Notably, the degradation efficiency increased slightly after multiple cycles due to continuous exposure of CoO(OH) active sites. The Co species effectively anchored onto the CS matrix through strong coordination, contributing to extremely low cobalt leaching (0.05 to 0.06 mg/L) and outstanding long-term reusability. Radical quenching and electron paramagnetic resonance (EPR) analyses revealed superoxide radicals (O 2 •− ) and singlet oxygen ( 1 O 2 ) as the dominant reactive species. This work elucidates the dynamic self-activation of low-crystallinity Co-MOFs in AOPs while providing a green and sustainable solution to secondary pollution caused by powdered nanocatalysts during water treatment.
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Journal of Environmental Sciences
·
2025
·
IF 6.3
Yinan Zhang,Bingyi Wang,Wenhui Sun,Lilai Shen,Zhiquan Liu,Binhao Wang,Jiafeng Ding,Yu Han,Hangjun Zhang
Emerging pollutants such as polystyrene-nanoplastics (PS-NPs) and polybrominated diphenyl ethers (PBDEs) are a threat to human health and ecological safety. However, NP-mediated PBDE exposure and toxicity remain poorly understood. Herein, male frogs ( Pelophylax nigromaculatus ) were exposed to 2,2′,4,4′-tetrabromodiphenyl ether (BDE-47) and 6-hydroxy-2,2′,4,4′-tetrabromodiphenyl ether (6-OH-BDE-47) alone or in combination with PS-NPs for 30 days to explore the carrier toxicity effect and mechanism of co-exposure. Transcriptome data verified that both BDE-47 and 6-OH-BDE-47 could mediate the steroid hormone synthesis signaling pathway to induce reproductive toxicity. The presence of PS-NPs increased the bioconcentration of BDE-47 and 6-OH-BDE-47 by 54.36 % and 51.49 %, respectively, and aggravate the damage of the testes. To investigate the mechanism underlying the disrupted steroidogenesis, changes in hormones of the hypothalamic-pituitary-gonadal (HPG) axis and gene expression involved in synthesis and transformation of sex hormones were assessed. AR, StAR, CYP11A1 and HSD3B1 were all downregulated, while mRNA expression levels of CYP19A1 and ESR1 were upregulated, accompanied by a decrease in testosterone and an increase in oestradiol. The results demonstrated that PS-NPs can exacerbate the estrogen-like effects of BDE-47 and 6-OH-BDE-47 in male frogs, highlighting the potential risks posed by these pollutants in aquatic ecosystems.
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ANALYTICAL AND BIOANALYTICAL CHEMISTRY
·
2025
·
IF 3.8
Yu Luyao,Liu Meichen,Niu Ziyi,Zhang Jiarui,Deng Yue,Zhou Xinyue,You Jiansong,Xue Hongyu,Yin Lei,Shi Meiyun
Monodisperse polyethylene glycol (PEG) derivatives offer significant advantages over conventional polydisperse PEGs for biomedical applications due to their precisely defined molecular structures. This study establishes an eco-efficient, selective, and sensitive analytical assay integrating microscale solid-phase extraction (μ-SPE) with ultra-performance liquid chromatography tandem mass spectrometry (UPLC-MS/MS) to investigate the cellular uptake of HO-PEG 8 -OH polymers in MCF-7 cells. The method achieved greater than 91% recovery from 20 μL lysates using M-PEG 6 -OH as the internal standard, with validated linearity (10–1000 ng/mL, R > 0.997), accuracy (relative error < ± 7.49%), and precision (RSD < 7.50%). The novelty of the assay is the harmonization of analytical performance with green analytical chemistry principles. The validated method provides a robust platform for studying monodisperse PEG derivatives while addressing growing demands for sustainable analytical technologies. Green analytical chemistry metric assessments confirmed the environmental sustainability of the method. Cellular pharmacokinetic analysis revealed time-/concentration-dependent uptake kinetics of HO-PEG 8 -OH polymers in MCF-7 cells, showing 3.2-fold accumulation between 0.5 and 48 h exposure. These findings offer important insights for PEG-based drug delivery system optimization and establish a new standard for environmentally conscious bioanalytical method development. Graphical
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JOURNAL OF CATALYSIS
·
2025
·
IF 6.5
Zhen Zhang,Quanxiao Dong,Yingqi Cui,Dan Wu,Armin Rezayan,Tianliang Lu,Renfeng Nie,Xiaoqin Si,Jianshe Wang,Chunbao Xu,Yongsheng Zhang
Catalytic oxidative depolymerization of lignin is an important strategy for producing valuable oxygen-functionalized monoaromatic compounds. However, this process is less efficient over heterogeneous catalysts due to the slow rate-determining step of selective oxidation of secondary alcohol (C α -OH to C α =O) in β-O-4 lignin linkages. Herein, a facile and efficient Ru(OH) x /C catalyst was developed for the oxidative depolymerization of lignin model compounds and real lignin in aqueous phase using molecular oxygen as oxidant. Extensive characterizations revealed that molecular oxygen abstracts electrons from the conductive carbon matrix to generate superoxide radicals (•O 2 – ), which are subsequently converted to hydroperoxide radicals (HOO•) in the presence of water. The C α -OH in the β-O-4 linkages first reacts with Ru-OH to form a Ru-O-C(H)- metal alkoxide intermediate, which then undergoes β-H elimination with the help of HOO• to generate H 2 O 2 and surface Ru-O-C•- species. Hydrolysis of Ru-O-C•- leads to the generation of C α =O products and the regeneration of Ru-OH sites. Different from the traditional Ru(OH) x -catalyzed alcohol dehydration mechanism in which Ru abstracts β-H to form Ru-H, in this case, the β-H in the Ru-alkoxide intermediate is eliminated by the hydroperoxide radicals rather than Ru, avoiding the formation of inert Ru-H species, thereby accelerating the dehydrogenation of C α -OH to C α =O. Electrochemical measurements further confirmed the charge transfer from Ru(OH) x to carbon during alcohol oxidation, demonstrating that electron donation by alcohol occurs on Ru(OH) x , while electron abstraction by O 2 occurs on the carbon. The free-radical-involved β-H elimination reaction pathway endows Ru(OH) x /C with superior catalytic oxidation activity in the aqueous phase compared with traditional metal oxides supported Ru(OH) x (e.g. SiO 2 , Al 2 O 3 , TiO 2 ), and provides a fundamental basis for the rational design of aqueous phase oxidation catalysts.
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FOOD CHEMISTRY
·
2026
·
IF 10.4
Qijun He,Wei Hu,Zhihao Yi,Bin Du,Yuan He,Jianjie Xu
Early and portable detection of foodborne pathogens is a key challenge for food safety, as conventional methods suffer from insufficient sensitivity and cumbersome operation. Herein, inspired by cellular compartmentalization, we designed the composite nanozyme MIL-88(Fe)@Pt@COF-B(OH) 2 (MPC-B(OH) 2 ) and constructed a dual-mode biosensing platform with Escherichia coli ( E. coli ) as the model. In this design, a catalytic MIL-88(Fe)@Pt core was encapsulated by a boronic acid-functionalized COF shell, which mimicked a cell membrane to provide specific recognition while optimizing the local microenvironment to enhance peroxidase-like activity, as clarified by density functional theory calculations. Meanwhile, its porous COF layer improved electrochemical performance. This sensor achieved detection limits of 2 and 3 CFU/mL for colorimetric/electrochemical modes, and 7 CFU/mL for on-site detection via a smartphone platform. With excellent selectivity, stability and reliability in real samples, this work provided a new strategy for biomimetic nanozyme design and a practical platform for on-site food safety monitoring.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Fuguang Liu,Zhonghan Feng,Xinyue Zhang,Liang Cui,Jingquan Liu
The creation of inexpensive, high-performance catalysts to reduce the overpotential of the oxygen evolution reaction (OER) process is critical for the electrolysis of water for hydrogen production. Therefore, we applied a one-step hydrothermal method using cation exchange reaction (CER) to prepare Fe-doped and interfacial Ru nanoclusters co-engineered Ni(OH) 2 nanosheets directly grafted on Ni foam (Ru@Fe-Ni(OH) 2 /NF) for OER process. Results of electrochemical tests reveal that Ru@Fe-Ni(OH) 2 /NF has excellent OER activity, and its overpotential (η) is only 266.4 mV when the current density is 50 mA cm −2 in 1 M KOH solution, even lower than that of commercial OER catalyst RuO 2 (355 mV). The Tafel slope also decreases from 133.8 mV dec −1 for pristine Ni(OH) 2 /NF material to 24.1 mV dec −1 for Ru@Fe-Ni(OH) 2 /NF, indicating the higher charge transfer rates and fastest kinetics for water oxidation. At an overpotential of 300 mV the optimal turnover frequency (TOF) of 0.062 s −1 for Ru@Fe-Ni(OH) 2 /NF is achieved compared to that of Ni(OH) 2 /NF (0.014 s −1 , NN), demonstrating the fast reaction kinetics of the as-prepared electrocatcalyst. After 24 h stability test, the catalytic activity of Ru@Fe-Ni(OH) 2 /NF was only attenuated by 2 %, showing excellent OER stability and durability. Our results show that we have successfully developed an efficient OER catalyst for green and efficient electrocatalytic hydrolysis to produce H 2 and O 2 , providing a promising method for clean H 2 production.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Ziwei Gao,Tao Zhang,Md. Nahid Pervez,Guojuan Qu,Wei Jin,Yaping Zhao
Materials combing catalytic and adsorption dual active sites are very important for arsenite (As(III)) due to its high mobility in water. Therefore, in this study, a bifunctional walnut-like Co-doped La(OH) 3 composites (Co-La) with independent catalytic sites and post-formed adsorption sites were synthesized via a simple hydrothermal method. Nearly 100% As(III) removal can be achieved in Co-La and peroxymonosulfate interaction systems (Co-La/PMS) within 10 min at the molar ratio of PMS to As(III) of 1.2. The results indicate that the combined Co-La adsorption system demonstrated superior performance compared to the Co-La adsorption alone. Precisely, the maximum removal capacity of the system was measured at 243.90 mg·g −1 , and the pseudo-first-order kinetic rate constant ( k 1 ) was determined to be 1.0771 min −1 . These values were significantly greater than those observed for Co-La adsorption alone. Notably, the kinetic rate constant was 239 times faster, and the removal capacity was 4.6 times higher in the combined system. The fast kinetics of As(III) elimination can be elucidated by the production of reactive oxygen species (ROS) such as S O 4 · - , •OH, O 2 · - and 1 O 2 , which expedite the conversion of As(III) into arsenate (As(V) in this particular system. Meanwhile, the increase in adsorption capacity is ascribed to the fact that PMS can drive La(OH) 3 of Co-La to transform into transition states La 2 SO 4 (OH) 4 , thus generating a new exchangeable adsorption site for As(V). A fixed membrane reactor assembled with Co-La was utilized to achieve a near-complete removal of As(III) within 3 min. The Co-La/PMS systems demonstrate exceptional effectiveness in eliminating arsenic from water across diverse real-water metrics, offering a unique perspective and technological progress in purifying water contaminated with arsenic.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Guanhan Chen,Hongjie Wang,Wenyi Dong,Wenhui Ding,Feifei Wang,Zilong Zhao,Yuxiong Huang
Cobalt oxide (Co 3 O 4 ) activated peroxymonosulfate (PMS) system was extensively studied due to its excellent catalytic performance. However, the relatively high cobalt (Co 2+ ) leaching (up to 2 mg/L) would pose high ecotoxicological risks. Herein, we identified the existence of Co(OH) 2 on the surface of Co 3 O 4 were the major source of Co 2+ leaching in the Co 3 O 4 activated PMS system. Furthermore, the Co 2+ leaching was effectively suppressed by converting Co(OH) 2 to Co 3 O 4 via pyrolysis treatment. In addition, reduced graphene oxide (rGO) was engaged to enhance the degradation performance of antibiotics in the Co 3 O 4 activated PMS system. The oxygen functionalities of rGO would catalyze PMS to generate sulfate radicals (SO 4 − ) and trigger the non-radical pathway of singlet oxygen ( 1 O 2 ). We have achieved outstanding catalytic performance for carbamazepine (CAZ) degradation with low Co 2+ leaching, as CAZ (5 mg/L) could be completely degraded in 30 min. Combining experimental investigation and theoretical calculation, we also revealed the degradation pathways and mechanisms that CAZ would be oxidized and detoxified by 1 O 2 and SO 4 − . We have provided a simple approach to inhibit the Co 2+ leaching and enhance the catalytic performance of Co 3 O 4 activated PMS system for the effective control of antibiotics.
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