ENVIRONMENTAL POLLUTION
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2024
·
IF 7.6
Siyi Pan,Pingxiao Wu,Leiye Sun,Meiqing Chen,Bo Li,Tianming Wang,Zhongbo Shang,Jiangmin Fang,Nengwu Zhu,Zhi Dang
Green rust (GR), as a vital intermediate product during the formation of various iron oxides, exists with organic matters and metals contaminants in natural environments. Understanding the effects of these natural factors on the transformation process of GR into iron oxides and the environmental behaviors of heavy metals and organic matters during process are critical for environmental quality management, but the fundamental identification of the interaction mechanisms between them and GR is still challenging. In this study, the transformation mechanisms of Co-bearing green rust (GR-Co) synthesized by co-precipitation, and the redistribution behaviors of Co(II) in an environment containing oxalic acid (OA) and citric acid (CA) were clarified. The findings indicated that OA promoted the Fe(II) dissolution and the transformation of GR-Co to goethite, while CA decreased the Fe(II) dissolution and the proportion of non-extractable Co. Furthermore, in the presence of CA, the transformation products of GR-Co were ferrihydrite, magnetite, lepidocrocite and goethite instead of only lepidocrocite and goethite. Meanwhile, CA prohibited ferrihydrite from transforming into more highly crystalline iron minerals. The finding of this study improves the understanding of the interaction mechanisms between GR-Co and organic matter, and the environmental geochemical behaviors of Co and organic carbon during the transformation processes in nature.
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INORGANIC CHEMISTRY COMMUNICATIONS
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2025
·
IF 5.4
Yilei Sun,Yao Liu,Zeda Meng,Won-Chun Oh
Different concentrations of N-doped modified Zn-based metal-organic frameworks (xN-Zn-MOFs) were prepared by a solvothermal method, as well as the successful synthesis of 0N-Zn-MOFs as well as 1N-Zn-MOFs and 2N-Zn-MOFs catalytic materials. The experimental results suggested that 2N-Zn-MOF displayed the maximum specific surface area and pore size among the three materials. The catalytic material stability and CO 2 reduction reaction (CO 2 RR) activity were investigated by linear sweep voltammetry (LSV), cyclic voltammetry (CV), electrochemical impedance spectroscopy (EIS), and chronocurrent tests (I-T). The corresponding Faraday efficiency (FE) was calculated in conjunction with product analysis. Among the three catalytic materials, 2N-Zn-MOF had the optimal catalytic reduction performance with a maximum current density of 20 mA-cm −2 ; Its charge transfer resistance was 7.84 Ω. It was stably tested at a potential of −0.45 V (vs. RHE) for 12 h in the IT test, and its reduction products were methane (CH 4 ) and carbon monoxide (CO), with a maximum total Faraday efficiency of 30.64 %.
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JOURNAL OF APPLIED POLYMER SCIENCE
·
2025
·
IF 2.8
Yuanpeng Cai,Danyang Li,Yufei Ling,Huihui Jiang,Hui Liu
A novel triple-responsive composite hydrogel, p(NIPAM-co-MAA-co-SPMA), was designed and synthesized via free radical polymerization, incorporating N-isopropylacrylamide (NIPAM) for temperature responsiveness, methacrylic acid (MAA) for pH sensitivity, and spiropyran methacrylate (SPMA) for light responsiveness. This study aimed to develop a novel stimuli-responsive sustained release drug delivery system. The composition and structure of the hydrogel were characterized by nuclear magnetic resonance spectroscopy (NMR), Fourier transform infrared spectroscopy (FTIR), X-ray photoelectron spectroscopy (XPS), and scanning electron microscopy (SEM). Doxorubicin (DOX) was used as a model drug to evaluate loading and release behavior. The hydrogel achieved a drug loading content (DLC) of 25.7% and a drug loading efficiency (DLE) of 74.3% and enabled controlled release with approximately 89% cumulative DOX release within 6 h under combined thermal, acidic, and ultra-violet light stimuli. Cytotoxicity assays and cellular uptake studies confirmed the excellent biocompatibility of the hydrogel and its efficacy in suppressing cancer cell growth. These results highlight the potential of p(NIPAM-co-MAA-co-SPMA) as an intelligent platform for on-demand targeted anticancer therapy.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2021
·
IF 19.503
Sijin Zuo,Shengcai Zhu,Jiaying Wang,Weiping Liu,Juan Wang
A N/O-codoped carbon-based catalyst (N/O-C-8) designed with dual reaction sites (pyridinic N and carbonyl group) was fabricated in this work, for persulfate based advanced oxidation reaction. The pyridinic N served as the adsorption site for target molecule, via series of high resolution XPS analysis and DFT calculation. Meanwhile, the carbonyl group functioned as the persulfate activation site, to generate oxidative 1 O 2 . Engineering and isolating the two reaction sites on catalyst surface can greatly shorten the migration distance from 1 O 2 to target organic molecule, resulting in good catalytic removal efficiency. As demonstrated, during a 4-hour continuous flow experiment, our catalyst showed stable and efficient removal of tetracycline, with a flow rate of 4 mL/min. The study provides keen insights into the design of effective non-metal based catalysts for practical water remediation.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2025
·
IF 9
Shuai Li,Yimei Zhang
Enhancing the energy efficiency of hydrogen evolution reaction (HER) represents a significant yet challenging goal. One promising approach to achieve this is developing catalysts with high activity and robust stability to couple HER with Fenton reaction. Herein, mesoporous nanosheet arrays (MNA) with featuring a mean pore size of 25 nm, was fabricated via a hydroxide precursor annealing strategy. The produced Co-P MNA 25 and Fe-Co-P MNA 25 are applied in HER and Fenton reaction, respectively. Compared to the MNA 12 synthesized by traditional method of self-growth and solid-phase phosphorization, the MNA 25 exhibited remarkable enhancement in performance, including a 49 % reduction in HER overpotential at 10 mA cm −2 , a 41 % increase in pseudo-first-order degradation kinetics of methylene blue in Fenton reaction, along with superior stability. In addition, the MNA 25 based flow reactor, which couples the two reaction and features a fastener-free design, demands just a minimal voltage of 1.61 V to drive, demonstrating impressive energy efficiency (81.56 % for HER and 2.77 g kWh −1 for Fenton) and application potential. More importantly, numerical simulations reveals that the larger pore size in MNA not only facilitated faster electrolyte diffusion, but also enhanced its impact buffer performance, thereby improving its catalytic activity and stability. Our work unveils the mechanism of mesopore size on the electrochemical performance of catalysts at the theoretical level, which offers a promising avenue for enhancing the energy efficiency of HER.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2020
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IF 16.683
Xianghai Song,Xin Li,Xinyu Zhang,Yuanfeng Wu,Changchang Ma,Pengwei Huo,Yongsheng Yan
Photocatalytic reduction of CO 2 to hydrocarbon fuels is an ultimate and utmost strategy to resolve the ever-increasing environmental problems and energy crisis. Our study aimed to develop a specific type of photocatalysts with increasing light utilization efficiency, reducing electron-hole recombination rate and enhancing photocatalytic activity by integrating unique donor-acceptor systems into the polymeric network of graphitic carbon nitride (g-CN). The results of the characterization showed that C and O are successfully integrated into the framework of g-CN. The O-containing and C-containing section of the as-prepared catalysts (OCCNx) play the role of donor and acceptor, respectively. The donor-acceptor systems of OCCN x offer an extra electron transfer transition mode, which dramatically extends the optical absorption range, and narrows down the bandgap of g-CN from 2.74 to 2.03 eV. Also, the donor-acceptor systems significantly improve the delocalized ability of the photoinduced charge carriers, which efficiently prolongs the lifetime of the charge carriers and reduces the electron-hole recombination rate, as all of these are all beneficial for boosting the photocatalytic activity of the catalysts. Experimental results show that OCCN 0.25 displays the best photocatalytic CO 2 reduction performance with a CO production rate of 34.97 μmol g −1 in 4 h, which is 4.3-fold higher than that obtained in the case of bulk g-CN. Moreover, the reaction is performed in water without any co-catalyst and sacrificial agent, which makes it a green and environmentally friendly reaction. Results obtained from DFT simulation agree well with the empirical results, and a possible reaction mechanism is suggested based on these calculations.
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APPLIED CATALYSIS A-GENERAL
·
2023
·
IF 5.5
Shanhai Zhao,Chunhe Li,Kuankuan Ren,Zebo Fang,Ping Fang,Yanyan Zhu,Pengfei Fang
Photothermal catalytic CO 2 reduction is an attractive way to alleviate the current energy crisis, but it is important to prepare catalysts with efficient catalytic capacity. In this work, Prussian blue analogs were firstly prepared, and then calcined to obtain porous transition metal (Ni, Co, Fe) oxides (TMOs). The metal composition of catalysts has great influences on their structures and catalytic properties. Among them, NCF-TMO catalyst shows excellent photothermal catalytic performance, and can produce 2.9 mmol g -1 h -1 CO and 1.6 mmol g -1 h -1 mmol CH 4 at low CO 2 and H 2 concentrations. For the NCF-TMO, its superior catalytic performance mainly benefitted from two reasons: (1) The construction of heterojunction between NiO, Co 3 O 4 and Fe 2 O 3 , which promotes the efficient dynamic processes of charge carriers; (2) The formation of abundant surface reactive active sites facilitates the efficient conversion of CO 2 molecules. This study offers a bright direction for the resource utilization of CO 2 .
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Journal of Materials Chemistry A
·
2017
·Vol. 5
·期 22
·11163-11170
·
IF 8.867
Lifeng Hang,Yiqiang Sun,Dandan Men,Shengwen Liu,Qian Zhao,Weiping Cai,Yue Li
Hierarchical micro/nanostructured C doped Co/Co3O4 hollow spheres were prepared by two-step treatment (annealing at 600 °C in an Ar atmosphere and then at 250 °C in air) of PS@Co(OH)2 core–shell structures templated from PS microspheres without any modification. In 1 M KOH, such hollow nanospheres showed an overpotential of 352 mV at a benchmark oxygen evolution reaction (OER) current density of 10 mA cm−2, which was lower than that of RuO2 (364 mV), Co3O4 hollow nanospheres (410 mV) and C-Co/Co3O4 nanoparticles (462 mV). Importantly, the C-Co/Co3O4 hollow spheres exhibited a small onset potential (1.49 V) due to their more active sites, higher electrical conductivity, larger specific surface area, and excellent electron and ion diffusion permeability. This work provides a strategy to design and fabricate earth-abundant, low-cost electrocatalysts for water splitting in practical applications.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2025
·
IF 9
Qing Xu,Jianyi Lu,Zhiyong Zhou,Yujia Jin
Synthesis of zeolite from industrial wastes has become an important environmental protection strategy. This study explored the synthesis of nano-sized NaX and NaY zeolites from coal/rice husk co-combustion ash (co-ash) using alkali-melting-hydrothermal synthesis and seed guiding methods, followed by modification with Li + and K + exchange. NaY zeolite, synthesized at a SiO 2 /Al 2 O 3 ratio of 5 and crystallization temperature of 100 °C, exhibited the most complete crystal structure and optimal CO 2 adsorption capacity. The specific surface area (SSA) of NaX and NaY zeolites (583.0 m 2 /g and 790.1 m 2 /g, respectively) are comparable to those of commercial zeolites, emphasizing their structural parity, and demonstrating their potential as effective CO 2 adsorbents. NaY demonstrated a CO 2 adsorption capacity of 5.31 mmol/g at 298.15 K and 1 bar, competitive with other conventionally synthesized and commercial zeolites. Cation exchange had a minimal impact on CO 2 adsorption of NaY, with LiX improving capacity by 11.65 % compared to NaX, while LiY showed only a 2.94 % increase. K + exchange negatively affected both zeolites. Kinetic and thermodynamic analyses, using the proposed first-order (PFO) and Langmuir-Freundlich models, indicated that CO 2 adsorption is a rapid physisorption process with thermal effects ranging from 22 to 41 kJ/mol. Both zeolites exhibited excellent CO 2 /N 2 selectivity and regeneration stability, with the loss of adsorption capacity retaining only 10.57 % and 9.63 % for NaX and NaY after fifteen cycles. This highlights their potential as efficient CO 2 adsorbents.
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Materials Chemistry Frontiers
·
2017
·Vol. 1
·期 10
·2065-2077
·
IF 0
Fu Yang,Bangbang Wang,Hang Su,Shijian Zhou,Yan Kong
Surface defective or heterojunction sites of catalysts generally afford remarkable catalytic activity thanks to their high-surface-energy. Regularly-generating multiple defective sites on the surface of a catalyst is exceedingly promising in many reactions. In this study, we report an unexpected Co/Fe–Co planar hybrid composite nanosheet with serried surface defects including surface biphasic junction sites or defective holes. A facile thermal-induced process was applied to trigger the generation of defective sites on planar Co/Fe–Co hydroxides. Through a controlled thermal process, massive serried CoO nanocrystals were in situ dissolved out of the surface of cobalt hydroxide, while defective surface holes were formed on the Fe-doped Co(OH)2 nanosheets under a prolonged thermal procedure. The morphology and microscale structure of the resulting Co/Fe–Co hybrid 2-dimensional (2D) composites were systematically examined by virtue of various characterization techniques. As expected, the obtained surface defective Co/Fe–Co planar composites showed obviously enhanced catalytic activity in the Fenton-like reaction. Based on a catalytic study, we proved that the CoO nanocrystals densely-distributed on thinlayer Co(OH)2. Uniformly-introduced Fe heteroatoms in the inter-structure of Co(OH)2, along with the formed surface defective holes on Fe–Co hybrid composites, are synergistically responsible for increased catalytic removal efficiency of MB in the presence of peroxomonosulfate.
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WATER RESEARCH
·
2025
·
IF 12.4
Kexin Yin,Yufeng Tang,Zisen Li,Han Zhao,Xing Xu,Qian Li,Qinyan Yue,Yue Gao,Baoyu Gao
Understanding and controlling the structure-activity relationship of single atom catalysts (SACs) is crucial for optimizing their catalytic performance. This study investigated the influence of montmorillonite (MT) as a support material on the microstructure of SACs, and how these influences modulate the catalytic performance and mechanism of peroxymonosulfate (PMS) activation. The enrichment effect within the MT interlayer space significantly enhanced the interaction between organic pollutant molecules, PMS, and active sites, thereby improving adsorption capacity and mass transfer efficiency. This enhancement increased the likelihood of subsequent peroxide bond cleavage, enabling the system to exhibit a greater capacity to generate high-valent Co (IV)-oxo and free radicals (SO 4 •− and • OH), leading to a higher removal efficiency of sulfamethoxazole (SMX). The introduction of MT altered the pathway of SMX removal, and the CoSAC@MT/PMS system predominantly degraded SMX into intermediate products with lower molecular weights and negligible fluorescence signals. Additionally, the incorporation of MT significantly boosted the yield of SACs synthesized via traditional pyrolysis methods, offering a novel strategy to reduce preparation costs and achieve large-scale synthesis.
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MICROCHIMICA ACTA
·
2022
·Vol. 189
·期 9
·1-11
·
IF 6.408
Sun Wenying,Wang Nan,Zhou Xiaobin,Sheng Yuxuan,Su Xingguang
A Co, N co-doped porous carbon-based nanozyme (Co–N-C nanozyme) has been fabricated. Taking advantages of the excellent oxidase catalytic activity and significant stability of Co–N-C nanozyme, we propose a fluorescence and colorimetric system based on Co–N-C nanozyme and red-emitting carbon quantum dots (RCDs) for butyrylcholinesterase (BChE) sensing. As the chromogenic substrate 3,3′,5,5′-tetramethylbenzidine (TMB) was catalyzed and oxidized by Co–N-C nanozyme, the generated oxTMB had a new absorption peak at 652 nm, which resulted in the significant quenching of the fluorescence of the carbon quantum dots at 610 nm. Under the catalysis of BChE, thiocholine was generated from the hydrolysis of S-butyrylthiocholine iodide (BTCh), and the as-generated thiocholine effectively inhibited the oxidation of TMB catalyzed by Co–N-C nanozyme, leading to a decrease of the absorption of oxTMB at 652 nm and effective fluorescence recovery of RCDs. By measuring the absorbance of produced oxTMB at 652 nm and the fluorescence of RCDs at 610 nm, the fluorescence and colorimetric system both exhibited an outstanding linear response to the activity of BChE in the range 0.5 to 40 U L −1 , with a detection limit of 0.16 U L −1 and 0.21 U L −1 , respectively. Furthermore, this established dual-channel biosensing strategy has been successfully applied to the determination of BChE in human serum samples. The present work has effectively expanded the development and application of nanozyme in biosensing. Graphical abstract
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