SEPARATION AND PURIFICATION TECHNOLOGY
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2026
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IF 9.1
Chen Liu,Huanxuan Li,Chen Xu,Zijie Shi,Xueheng Wei,Zhitong Yao,Shaodan Xu,Jingang Huang,Mingzhi Huang
The increasing complexity and concentration of refractory organic pollutants in industrial wastewater necessitate the development of efficient and stable advanced oxidation processes (AOPs). Herein, metal–organic framework (MOF)-derived Co₃Fe₇@CN carbon composites were successfully fabricated and evaluated as peroxymonosulfate (PMS) activators for the degradation of oxytetracycline (OTC). Among the as-prepared catalysts, Co₃Fe₇@CN-1 exhibited superior catalytic performance, achieving 90% OTC removal within 10 min with an apparent rate constant ( k obs ) of 0.158 min −1 , which represents a 1.7- and 1.5-fold enhancements over Co₃Fe₇@CN-2 and Co₃Fe₇@CN-3, respectively. The outstanding activity of Co₃Fe₇@CN-1 is primarily attributed to its favorable pore structure and pronounced adsorption–catalysis synergy. Specifically, Co₃Fe₇@CN-1 and Co₃Fe₇@CN-3 achieved 23% and 21% of OTC removal via adsorption, respectively, whereas the dense structure of Co₃Fe₇@CN-2 significantly impeded pollutant uptake (<5%). Mechanistic investigations revealed that PMS activation is driven by the synergistic redox cycling of Co (Co 0 /Co(II)/Co(III)) and Fe (Fe 0 /Fe(II)/Fe(III)) species. Electrons transferred from zero-valent and low-valent metals promote O O bond cleavage in PMS, triggering the generation of SO₄• − and •OH radicals. Crucially, the Fe species acts as an electron reservoir to accelerate the reduction of Co(III) to Co(II), thereby effectively circumventing the rate-limiting step of the Co redox cycle. Simultaneously, high-valent Fe(III)/Co(III) species interact with PMS to form high-valent metal-oxo intermediates ( Fe(IV) O and Co(IV) O), which serve as the predominant reactive species responsible for OTC degradation. The coexistence of radical and non-radical pathways ensures efficient OTC degradation. This work establishes a controllable strategy for constructing MOF-derived carbon catalysts and elucidates the structure–activity relationship between pore architectures and redox centers.
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Journal of Materials Chemistry A
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2026
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IF 9.5
Qing Cheng,Yuqi Zhang,Yingying Cao,Long Liu,Yanqiang Zhang
The novel ionic liquid-H2O2 propellants are urgently to solve the intrinsic ignition problem for achieving the aerospace applications. We addressed this issue by tuning the d-band center to adjust the catalyst's adsorption strength for IL/H2O2 toward the optimal value, thus enhancing catalytic activities for the efficient decomposition of H2O2 to generate reactive oxygen species. Herein, the regulation of the d-band center of Cu(I) in Cu(I)-MOF catalyst by precise ligand engineering design was studied. Remarkably, The Cu-S3 coordination of Cu-SH' shifts its d-band center closer to the Fermi level, promoting the adsorption of [BMIM]N(CN)2 and H2O2. Cu-SH' enables efficient H2O2 activation and robust •OH and 1 O2 generation to trigger the rapid self-ignition of [BMIM]N(CN)2-H2O2 propellant. The resulted tid as low as 18.4 ms is nearly 34% lower than that of homogeneous catalyst [FcCH2N(CH3)3]2[Cu2I4]. This work provides fundamental insights into the design of efficient ligand-based combustion catalysts for the higher performance of rockets and spacecrafts.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
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IF 24.319
Menglu Xu,Yibing Zhang,Huaqin Yin,Jinnan Wang,Aimin Li,Philippe François-Xavier Corvini
Co-ZFO@Mn-CN with 1 O 2 and O 2 •− as main reactive oxygen species was synthesized for catalytic ozonation , which could efficiently degrade organic pollutants . EPR and XPS analysis indicated that lattice doping of Co induced formation of abundant of OVs, which could provide localized electrons for O 3 activation with the generation of HO 2 • /O 2 •− . 1 O 2 and H 2 O 2 were produced by the recombination of HO 2 • /O 2 •− . DFT calculation demonstrated that H 2 O 2 was deprotonated to generate HOO − , which preferred to form HOO-Mn-N X bonds with Co-ZFO@Mn-CN. Under the attack of O 3 , HOO-Mn-N X bonds were broken with the generation of HO 2 • and HO 3 • /O 3 •− , not only accelerating 1 O 2 production for organics degradation but also avoiding Mn(Ⅱ) sites oxidation . Combining advantages of OVs and HOO-Mn-N X , Co-ZFO@Mn-CN achieved 70–100% mineralization for different organic pollutants . Thus, this work provided a simple and efficient way for enhancing the utilization of O 3 by the synergistic effect of OVs and HOO-Mn-N X bonds, also improving ROS transformation.
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BIOELECTROCHEMISTRY
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2023
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IF 5
Mengjiao Zhu,Yu Liu,Meiyue Wang,Tao Liu,Zhenyu Chu,Wanqin Jin
Owing to the high mortality and strong infection ability of COVID-19, the early rapid diagnosis is essential to reduce the risk of severe symptoms and the loss of lung function. In clinic, the commonly used detection methods, including the computed tomography (CT) and reverse transcription-polymerase chain reaction (RT-PCR), are often time-consuming with bulky instruments, which normally require more than one hour to report the results. To shorten the analytical period for testing the COVID-19 virus (SARS-CoV-2), we proposed an ultrafast and ultrasensitive DNA sensors to achieve an accurate determination of the DNA sequence by the RNA reverse transcription (rtDNA) of the SARS-CoV-2. A nanocubic architecture of the MnFe@Pt crystals was constructed to integrate both electrocatalysis and conductivity to greatly improve the biosensing performance. After the immobilization of a specific capture and report DNA on above nanocomposite, the rtDNA can be rapidly caught to the DNA sensor to form a double-helix structure, thus generating the current signal change. Within only 10 min, the as-prepared DNA sensors exhibited ultralow detection limit (1 × 10 −20 M) and wide linear detection range, together with an outstanding selectivity among various interfering substances.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2021
·
IF 19.503
Heng Fei,Junxia Shao,Hua Li,Najun Li,Dongyun Chen,Qingfeng Xu,Jinghui He,Jianmei Lu
g-C 3 N 4 (CN), which shows enormous potential for photocatalysis, has long been studied, but still exhibits an unsatisfactory degradation rate. Herein, dual cocatalysts, Br and ultrafine RhO x nanoparticles, were constructed on ultrathin CN for synergetic photocatalysis. Ultrathin CN increased the exciton separation efficiency, while cocatalysts Br and RhO x can accelerated electron and hole transfer simultaneously, maximizing the photocatalytic degradation performance of CN. This CN-Br 0.12 /2%RhO x degraded 10 ppm bisphenol A (BPA) in 9 min, which represents the fastest degradation rate reported to date. This excellent performance was also demonstrated by a larger photocurrent response, higher separation efficiency, and faster transfer rate for electron–hole pairs than CN. This work obtained an enhanced electron–hole separation efficiency and migration rate by combing ultrathin CN with dual-channel cocatalysts, leading to the best photocatalytic degradation performance reported for CN.
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
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2021
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IF 4.098
Ling-Juan Yan,Chen Jiang,Ai-Ying Ye,Qiong He,Cheng Yao
Hydrazine plays an important role in chemistry, pharmaceuticals, agriculture and aerospace. However, it is not to be underestimated and has been identified as harmful to the human body. Therefore, it is significant and urgent to develop the detection of hydrazine in vivo and in vitro. Here, the probe TAN was synthesized by using benzothiazole derivatives as the fluorophore and 2,3-diaminomaleonitrile as the identified group to detect hydrazine. The presence of hydrazine resulted in a colorimetric and ratiometric fluorescence response of the probe based on the formation of hydrazone. The detection limit of TAN was 0.31 µM for hydrazine. In addition, the probe TAN was successfully used to visualize hydrazine in living HepG-2 cells and mouse with low cytotoxicity and excellent biocompatibility.
研究领域:
分析化学
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生物医学工程
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毒理学
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2021
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IF 8.128
Jingrong Zhai,Qiaoling Kang,Qiuyue Liu,Dawei Lai,Qingyi Lu,Feng Gao
Three-dimensional (3D) network structure of metal–organic framework (MOF) can accommodate outstanding electrocatalysis performances, but always collapse during the conversion to active materials or applications process. How to maintain the 3D network when producing active species is of great importance for full application of MOF. Herein, a new MOF material, In[Co(CN) 6 ] (In-Co PBA) nanocubes, are firstly synthesized. Through a controlled low-temperature deligandation process, the In-Co PBA nanocubes are transformed to a novel In 2 O 3 @In-Co PBA quasi-MOF nanocubes, which basically retain the 3D porous structure of PBA but with in situ generated In 2 O 3 nanoparticles inside. When used as CO 2 RR electrocatalyst , such a novel cubic composite structure exhibits excellent performances with faradaic efficiency of 85% for formate at a potential of −0.96 V and with current density of 31.5 mA·cm −2 at −1.32 V, surpassing most of the reported indium-based catalysts. The excellent performance can be attributed to the special composite structure, which provides not only active sites by In 2 O 3 nanoparticles to catalyze CO 2 RR, but also the 3D porous framework by quasi-MOF to accelerate gaseous exchange and electrolyte permeation and prevent the electrode choking. This work offers a new strategy for the design of post-transition metal catalysts and the structure design of quasi-MOF.
研究领域:
材料科学
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电化学
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Journal of Environmental Chemical Engineering
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2022
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IF 7.968
Jiliang Ma,Junqiang Zhang,Dongnv Jin,Shuangquan Yao,Runcang Sun
Synchronous photocatalytic water splitting and the reforming of a biomass-derived feedstock to generate hydrogen and high-value-added chemicals make full utilization of the biomass-water-splitting redox reaction; however, limited successes in this regard have been reported. Herein, incompletely polymerized graphitic carbon nitride co-doped with zinc/oxygen atoms (Zn 2 /O@IP- g -CN) was prepared via a step-by-step low-temperature calcination process with the assistance of melamine and zinc phthalocyanine, which successfully resulted in simultaneous photocatalytic water splitting and the reforming of biomass-derived monosaccharides to produce hydrogen (11436.7 μmol g −1 h −1 ) and lactic acid (92.6 %), respectively. Zn 2 /O@IP- g -CN exhibits a fast separation/migration rate and low resistance compared to those of pure CN, resulting in Zn 2 /O@IP- g -CN showing enhanced photocatalytic activity. The hydrogen release rate of 86.8 % and lactic acid yield of 89.0 % were retained compared to initial values when Zn 2 /O@IP- g -CN was reused in 5 th cycles. Poisoning experiments indicated that 1 O 2 , ·O 2 - , ·OH, and h + were all beneficial for lactic acid production.
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ELECTROCHIMICA ACTA
·
2022
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IF 7.336
Dengfeng Yu,Bo Yang,Huimin Liang,Gongyuan Zhao,Hong Zhang,Yuanlin Wang,Ye Sun,Miao Yu
Constructing hollow-structured materials is an efficient route to address the volume expansion of anode and enhance ion diffusion for sodium-ion battery (SIB). Superior to the single-walled products, multi-walled hollow-structured anode materials possess more storage sites, enhanced robustness, and higher volumetric capacity; nevertheless, synthesis of the multi-walled hollow structure often requires harsh synthesis conditionand complicated etching process. Herein, we report fabrication of Co 0.85 Se double-walled hollow cages coated by a nitrogen-doped carbon layer (Co 0.85 Se@CN) as high-performance anode materials for SIB. Using ZIF-67 as precursor, a facile ion exchange strategy is employed with no aid of high temperature treatment and complex etching process. The resultant Co 0.85 Se@CN exhibit distinct double-walled hollow structure with abundant lacunas on the walls, which increases the accessible area, shortens the ion transport path and most importantly provides appropriate buffer space against volume expansion. Moreover, the C protective layer on both sides of the inner- and outer-walls further benefits high conductivity, chemical stability, and robustness during charge/discharge process. As a result, the Co 0.85 Se@CN anode deliver a high reversible capacity of 402 mAh g –1 at 50 mA g –1 and 316 mAh g –1 at 100 mA g –1 after 100 cycles for SIB.
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Journal of Materials Chemistry C
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2020
·Vol. 8
·期 37
·12984-12992
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IF 7.059
Awais Siddique Saleemi,Muhammad Hafeez,Aqsa Munawar,Naeem Akhtar,Waseem Abbas,Muhammad Ehsan Mazhar,Zahid Shafiq,Anthony P. Davis,Shern-Long Lee
Arsenic(III) poisoning may lead to neurological disorders, heart diseases or carcinogenic effects due to long-term exposure. The presence of arsenic in drinking water is a widespread problem and presents an important analytical challenge. Among the methods for As(III) monitoring, electrochemical analysis offers fast response, low detection limits and high sensitivity. Here we report a novel system, which achieves exceptional performance without use of expensive noble metals by exploiting a metal oxide rich in oxygen vacancies (OVs). Novel OV-rich spinel ZnFe2O4 microspheres (ZF-Ms) were synthesized and applied to electrochemical monitoring of As(III) in underground drinking water by square wave anodic stripping voltammetry (SWASV) in acetate buffer (pH 6.0). To boost sensing capability, the surface of ZF-Ms was further wrapped with carbon and nitrogen rich nanodots (CNs) and modified with benzimidazolium-1-acetate ionic liquid (IL). The designed CN-wrapped IL-modified ZF-Ms (CN@ZF-Ms-IL) sensor offered an ultra-low detection limit of 0.0006 ppb (based on the 3σ method), high sensitivity (41.08 μA ppb−1) and a wide linear range (∼1–60 ppb) including the World Health Organization (WHO)'s desirable range (10 ppb). To the best of our knowledge, the system outperforms most alternatives based on noble metal electrodes and almost all those based on the reported metal-free electrochemical sensors. A possible sensing mechanism is proposed and supported with experimental evidence. Additionally, the system has been successfully applied to monitor arsenic-contaminated real ground drinking water collected from a flood-affected area, Muzaffargarh, Punjab, Pakistan.
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ENVIRONMENTAL RESEARCH
·
2024
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IF 7.7
Yaxuan Liu,Chen Yu,Huixia Lu,linan Liu,Jingchun Tang
Photocatalytic property of nano Ag is weak and its enhancement is important to enlarge its application. Herein, a novel strategy of constructing silver g-C 3 N 4 biochar composite (Ag-CN@BC) as photocatalyst is developed and its photocatalytic degradation of bisphenol A (BPA) coupled with peroxydisulfate (PDS) oxidation process is characterized. Characterization result showed that silver was evenly embedded into the g-C 3 N 4 structure of the nitrogen atoms format, impeding agglomeration of Ag by distributing stably on biochar. In optimum condition, BPA of 10 mg/L could be degraded completely at pH of 9.0 with a 0.5 g/L photocatalyst, 2 mM PDS in Ag-CN@BC-2 (Ag/melamine molar ratio of 0.5)/PDS system (99.2%, k = 4.601 h −1 ). Ag-CN@BC shows superior mineralization ratio in degrading BPA to CO₂ and H₂O via active radical way, including holes ( h ⁺), superoxide radicals (•O 2 ⁻ ), sulfate radicals (SO 4 • ⁻ ), and hydroxyl radicals (•OH). Proper amount of silver can be dispersed effectively by gC 3 N 4 , which is responsible for improving the visible-light absorbing capability and accelerate charge transfer during activation of PDS for BPA degradation, while biochar as carrier in the composite is supposed to enhance the photoelectric degradation of BPA by reducing the band gap and increasing the photocurrent of Ag-CN@BC catalyst. Ag-CN@BC exhibits excellent catalyst stability and photocatalytic activity for treatment of toxic organic contaminants in the environment.
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ACS Applied Materials & Interfaces
·
2025
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IF 8.2
Lei Zhao,Zilong Zhang,Tianyuan Zhang,Xiang Wang,Huanjun Peng,Jingdong Peng
The Fenton reaction in advanced oxidation processes is an ideal pathway for the generation of highly reactive hydroxyl radicals (•OH). However, its application in organic wastewater treatment is limited due to the requirement for acidic pH conditions and the additional introduction of H2O2 and Fe2+. In this study, FeOOH–CN/Ni(OH)2 composites were constructed as photocatalysis-self-Fenton catalysts by the amorphous FeOOH, which was uniformly anchored onto the surface of pure g-C3N4 (carbon nitride (CN)), and Ni(OH)2 was assembled on top. In this process, FeOOH–CN/Ni(OH)2 achieved self-sufficiency in H2O2 production while enabling efficient degradation of tetracycline hydrochloride (TCH) over a wide pH range, with a degradation ratio of up to 98.82%, and a first-order reaction rate constant (k) was determined to be 0.04925 min–1, representing a 10.15 times enhancement compared to the pristine CN. A reasonable S-scheme heterojunction charge migration mechanism was demonstrated based on valence-band X-ray photoelectron spectroscopy (VB-XPS), atomic force microscopy (AFM) equipped with a Kelvin probe force microscope, and density functional theory (DFT) theoretical calculations. Furthermore, degradation experiments demonstrated that the catalyst possesses remarkable degradation efficiency for other contaminants as well. On one hand, this significant improvement can be attributed to the formation of an S-scheme heterojunction between Ni(OH)2 and CN, which not only increased the specific surface area of the composite but also remarkably enhanced the separation and transfer efficiency of photogenerated charges. On the other hand, the synergistic effect between Ni and Fe effectively facilitated the activation of H2O2 and promoted the cycling of Fe3+/Fe2+. This study provided an efficient visible-light-driven photocatalysis-self-Fenton system, offering novel perspectives for enhancing Fenton-based processes and advancing the application of Fenton reactions in the treatment of organic wastewater.
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