Sustainable Materials and Technologies
·
2026
·
IF 9.7
Qian Wang,Qiuchen Wang,Xuelin Zhang,Yuheng Zhang,Xinyue Chi,Weijian Yuan,Dianpeng Qi,Jianfeng Wu
Selective aerobic oxidation of thioethers to sulfoxides over efficient visible-light photocatalysts is an essential yet highly challenging transformation in catalytic oxidation chemistry. Herein, we introduce an asymmetric perylene diimide–based π-conjugated polymer (BCPDI) with intrinsic polarization that enhances charge transport and tunes the local microenvironment to efficiently regulate reactive oxygen species(ROS) generation for efficient thioether oxidation. DFT calculations show that symmetry breaking separates frontier orbitals and creates an internal electrostatic potential gradient, thereby accelerating charge carrier transport and driving O 2 reduction to generate superoxide radicals (·O 2 − ), whereas symmetric analogs produce only singlet oxygen ( 1 O 2 ) via energy transfer. Driven by the synergistic effect of electron and energy transfer pathways, BCPDI achieved over 99% conversion and selectivity for thioether oxidation under ambient conditions, outperforming most recently reported materials. In addition, BCPDI also exhibits a superior catalytic activity for thioether oxidation (e.g., aromatic thioethers, aliphatic sulfide, and Mustard Gas sulfide). This study provides a new approach for the design of catalysts for photocatalytic aerobic oxidation of thioethers and deepens the understanding of thioether activation mechanisms mediated by photogenerated charge carriers and reactive oxygen species.
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Materials
·
2023
·Vol. 16
·期 2
·684
·
IF 3.4
Yunxin Yang,Cong Wang,Hua Zhang,Jiancai Qian,Song Yang,Huiyun Liao,Xuehui Sun,Yipeng Wang,Peijian Sun,Yunzhen Jia,Junwei Guo,Huaiyuan Zhu,Cong Nie
Removal of 1,3-butadiene from cigarette smoke plays an important role in human health and environmental protection. Herein, a series of UiO-66 X% containing different ratios of the -NH2group was synthesized via the solvothermal method by using terephthalic acid (H2BDC) and 2-aminoterephthalic acid (NH2-BDC) as ligands. Using GO as support, a series of UiO-66-NH2/GO Y% were prepared by controlling the ratio of UiO-66-NH2and GO. The effects of -NH2and GO contents on the structure and composition of MOFs were investigated. Finally, the different -NH2contents of UiO-66 X% and the different GO contents of UiO-66-NH2/GO Y% were applied in 1,3-butadiene removal from cigarette smoke. The results showed that UiO-66 X% with the higher contents of -NH2showed a higher rate of 1,3-butadiene removal, and UiO-66-NH2/GO Y% with the GO contents of 5% showed the highest removal rate of about 33.85%, which was 25.54% higher than that of activated carbon. In addition, the saturation capacity of the adsorbent materials for 1,3-butadiene was as high as 210.01–239.54 mg/g, showing great potential in reducing harmful components in cigarette smoke and environmental protection.Keywords:UiO-66;UiO-66-NH2/GO;1,3-butadiene removal;cigarette smoke
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
·
2022
·
IF 4.831
Kunming Sun,Tinghui Deng,Jing Sun,Shuo Gao,Huwei Liu,Shuyun Zhu,Xian-En Zhao
Artemisinin (ART) is a type of frontline drug to treat drug-resistant falciparum malaria. Simple, accurate and selective determination of ART is significant to monitor its clinical pharmaceutical efficacy. Herein, a new ratiometric fluorescence method has been designed for the determination of ART with Zn-MOF as fluorescence reference and hemin as catalyst, respectively. Zn-MOF possesses intrinsic fluorescence at 443 nm owing to 2-aminoterephthalic acid ligand. When o -phenylenediamine (OPD) is mixed with hemin, a weak fluorescent signal at 570 nm ascribed to oxidized product of OPD (oxOPD) is observed. In the presence of ART, hemin can catalyze ART to break its peroxide bridge and release a large number of reactive oxygen species, which effectively oxidize OPD into luminescent oxOPD. Therefore, the fluorescence at 570 nm is enhanced significantly while the fluorescence of Zn-MOF remains basically unchanged. Thus, a ratiometric fluorescence sensing platform has been constructed for the detection of ART. This method exhibits wider linear range (0.15 μM-150 μM) with detection limit of 50 nM. This novel and selective method has been used to detect ART in compound naphthoquinone phosphate tablets.
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ACS Omega
·
2023
·
IF 4.1
Qiyue Zhang,Aori Qileng,Jiale Li,Yiran Cao,Weipeng Liu,Yingju Liu
Organic dyes can produce harmful effects on the water environment, such as affecting the growth of aquatic organisms, reducing the transparency of water bodies, and causing eutrophication of water bodies, so it is necessary to mitigate the hazards of organic dyes. In this study, a metal–organic framework [NH2-MIL-101(Fe)] was synthesized by the solvothermal method as a carrier for the in situ uniform deposition of AgCl nanoparticles on its surface, which was successfully used for both adsorption and degradation of Congo red. Adsorption results showed that the adsorption kinetics conformed to the proposed secondary adsorption kinetics equation with a maximum adsorption capacity of 248.4 mg·g–1. Furthermore, the degradation results indicated that with the aid of sodium borohydride as a reducing agent, the degradation of Congo red followed pseudo-first-order kinetics with a degradation rate of 0.077 min–1, and the complete degradation of Congo red was finished within 18 min. Therefore, AgCl/NH2-MIL-101(Fe) may find a potential application in the removal of dyes from wastewater.
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
·
2023
·
IF 4.4
Donglian Deng,Jingyuan Xu,Tingting Li,Dongdong Tan,Yibing Ji,Ruijun Li
This work designed a fluorometric/colorimetric dual-mode sensor for detecting 2,6-dipicolinic acid (DPA) based on the blue emission property and peroxidase-like activity of Fe-MIL-88NH 2 . The fluorescence of Fe-MIL-88NH 2 was obviously turned off by Cu 2+ , but DPA was able to bring it back because it has a strong chelate bond with Cu 2+ . Fe-MIL-88NH 2 also displayed high peroxidase-like activity, which accelerated the oxidation of 3,3′,5,5′-tetramethylbenzidine (TMB) to the blue oxidation product (oxTMB) when H 2 O 2 was present. When DPA was added, it efficiently inhibited the peroxidase-like activity of Fe-MIL-88NH 2 , causing less oxTMB and less absorbance at 652 nm. The fluorescence recovery of Fe-MIL-88NH 2 and the change in absorbance at 652 nm were used as analytical signals for dual-mode detection of DPA. The linear responses in the range of 10–60 μM and 60–160 μM were achieved for the fluorometric mode, and the limit of detection (LOD) was 1.46 μM. The respective values of linear range and LOD for the colorimetric mode were 5–25 μM and 3.00 μM, respectively. In summary, the dual-mode testing strategy successfully detected DPA in aqueous environmental samples, suggesting great potential in disease prevention and environmental analysis.
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JOURNAL OF POWER SOURCES
·
2022
·
IF 9.794
Xiang Li,Jianwei He,Yucong Liao,Shaoshan Zhu,Yayun Tang,Hanyang Li,Ning Lv,Yuexin Xu,Yadong Wang
Herein, a conjugate carbonyl polyimide (MF-PI) and nano-silicon composite (MF-PI/Si) is designed and synthesized through a simple one-pot method to confront rapid capacity fading and complicated electrode material preparation in silicon-based electrodes for lithium ion battery . This composite can be directly used to prepare electrode without the need of further adding of binding materials. In this composite, MF-PI acts as binder for powder electrode, active reversible lithiation material, buffering media to alleviate volume change of silicon particles, and coating shell to avoid the direct contact between silicon particles and electrolyte. These functions from MF-PI collectively assigned the MF-PI/Si composite anode material a relative high specific capacity and excellent cycling stability. The electrode prepared by this as-synthesized MF-PI/Si shows preferable electrochemical interface and surface area, further enhancing the electrode kinetics and then electrochemical performance. The improved ionic and electronic conductivity compared to other binder materials also contributes the excellent performance.
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MICROCHEMICAL JOURNAL
·
2022
·
IF 5.304
Zhiwen Gan,Tian Zhang,Xuanxuan An,Qin Tan,Shujun Zhen,Yongmei Hu,Xiaoli Hu
Many nanozymes have been synthesized, though, it is still necessary to rationally synthesize multifunctional nanozymes for diverse applications. Herein, we fabricate three fluorescent nanozymes with peroxidase- and laccase-like activities under moderate conditions. Three nanozymes, NH 2 BDC/CuFe/ATP (NPs-1), NH 2 BDC/CuFe/ADP (NPs-2), NH 2 BDC/CuFe/AMP (NPs-3), are constructed based on three adenosine phosphates coordinated transition metal ions (Cu 2+ and Fe 3+ ) and adsorbing fluorescent amino terephthalic acid (NH 2 -BDC). They exhibit different laccase-like activity, which may result from the difference in steric configurations of nanozymes. Among them, NPs-1 possesses high peroxidase-mimicking activity and stability. Interestingly, o-phenylenediamine (OPD) is oxidized to 2,3-diaminophenazine (DAP) by ·OH which NPs-1 catalyzes H 2 O 2 to produce. The fluorescence of NPs-1 ( λ em = 445 nm) is effectively reduced based on the inner filter effect between DAP and NPs-1, which recovers after adding AA. Based on stable fluorescence and high peroxidase-like activity of NPs-1, a system for determining H 2 O 2 and AA is established in linear ranges of 2.0–200.0 and 4.0–300.0 μmol L −1 with limits of detection of 1.82 and 2.92 μmol L −1 . The fluorescent probe shows a good performance in detecting AA in real samples. Furthermore, NPs-1 is applied in smartphone-based detection of AA by measuring its intrinsic fluorescence. This work provides a facile strategy for the design of multi-functional nanozymes.
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JOURNAL OF HAZARDOUS MATERIALS
·
2020
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IF 9.038
Chunhua Li,Xiaoshuo Zhang,Simin Wen,Rui Xiang,Yong Han,Wenzhi Tang,Tianli Yue,Zhonghong Li
The increasing misgivings of environmental pollution derived from antibiotic residues make it imperative to explore a bifunctional platform for synchronous monitoring and removal of antibiotics. Herein, zeolite imidazolate framework-8 (ZIF-8) is anchored on two-dimensional (2D) amino-functionalized Al-metal organic framework (NH 2 -MIL-53(Al)) nanoplates to construct a dual metal–organic frameworks smart platform (ZIF-8/NH 2 -MIL-53(Al)) for simultaneous capture and fluorescence sensing of tetracyclines (TCs). ZIF-8 nanoparticles anchored on 2D nanoplates having a smaller size and a larger specific surface area boost the adsorption capabilities (561, 533, 526 and 578 mg g −1 for doxycycline (DOX), tetracycline (TET), oxytetracycline (OTC) and chlortetracycline (CTC), respectively). Notably, the pyridine N of ZIF-8 cooperated with the abundant NH 2 on the surface of NH 2 -MIL-53(Al) exhibits high affinity toward TCs, remarkably enhancing the sensitivity by facilitating the photo-induced electron transfer and the inner-filter effect. The LOD s (1.2 μg L −1 for TET, DOX, OTC and 2.2 μg L −1 for CTC, respectively) are at least 10-fold lower than those of NH 2 -MIL-53(Al) and are comparable or superior to those of reported sensors. The dual metal–organic frameworks smart platform presents satisfactory reliabilities and accuracies for detecting TCs in real samples, which anticipates new routes to develop integrated systems for simultaneous capture and detection of organic pollutants.
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JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
·
2023
·
IF 6.1
Jianhao Liang,Jinxia Fu,Hongwei Lin,Junyue Chen,Shiyu Peng,Yuyue Sun,Yongjun Xu,Shimin Kang
Valorization for the recycling of polyethylene terephthalate (PET) wastes has garnered significant attention. An innovative one-step approach, devoid of catalysts and solvent, was developed for the ammonolysis of PET to terephthalamide (TP) at mild temperatures (40–120 °C). The study extensively explored and discussed the impacts of key process parameters such as temperature, reaction time, material ratio, stirring speed, and various PET-containing materials. The reaction conditions were further optimized via Response Surface Methodology. The results demonstrated proposed ammonolysis technique facilitates the straightforward recovery of high TP yield (>90 mol%) and purity (>95 %), establishing an effective avenue for TP production through PET waste valorization.
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APPLIED CATALYSIS A-GENERAL
·
2023
·
IF 5.5
Huifang Feng,Yitong Sun,Qiaozhen Xu,Hong Liu
Developing efficient photocatalyst to promote the conversion of CO 2 into value-added chemicals remains challenging. Here, novel NH 2 -MIL-101(Fe)@Bi 2 MoO 6 S-scheme heterojunctions were fabricated via a solvothermal method, in which Bi 2 MoO 6 (BMO) nanoparticles uniformly growing on the NH 2 -MIL-101(Fe) (NM101) octahedrons with intimate contact interface. The resultant heterojunctions revealed significantly enhanced activity for CO 2 photoreduction. The optimal performance was achieved when the content of BMO was 10 wt%, and the formation rate of CO reached 67.0 μmol·g −1 ·h −1 under visible light illumination (with apparent quantum efficiency of 0.09 % at 450 nm), which was 3.2-fold of individual NM101. The boosting activity benefited from the formation of S-scheme heterojunction at the NM101 @BMO interfaces, which facilitated the separation of photoinduced electron-hole pairs with strong redox ability at the interface. This S-scheme charge transfer mechanism was further validated by the in-situ XPS and fluorescence probe molecular experiment. Besides, the intermediates and preliminary mechanism of photoreaction were unraveled based on in-situ DRIFTS analysis. This work provides some novel insights for designing efficient S-scheme photocatalysts for CO 2 photoreduction.
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Catalysts
·
2023
·Vol. 13
·期 7
·1073
·
IF 3.9
Kaiwen Yuan,Bo Gong,Chundong Peng,Yanmei Feng,Yingmo Hu,Kai Chen,Daimei Chen,Derek Hao
Cr(VI) is a common heavy metal pollutants present in the aquatic environment, which possess toxic and carcinogenic properties. In this study, a solvothermal reaction was used to prepare porphyrin (TCPP)-modified UiO-66-NH2(UNT). The UNT integrated adsorption and photocatalytics in the application for dealing with Cr(VI). The photocatalytic reduction activities of UNT for Cr(VI) were investigated under visible light illumination. We found that the TCPP doping amount of 15 mg UNT (15-UNT) had a 10 times higher reduction rate of Cr(VI) than pristine UiO-66-NH2. The optimal 15-UNT photocatalyst demonstrated the highest photocatalytic activity, and Cr(VI) was completely removed within 80 min. In addition, the introduction of porphyrin not only enhanced the absorption of light but also enabled the transport of photogenerated electrons from porphyrin to UiO-66-NH2, which promoted the separation of charge carriers. Furthermore, the effects of factors such as porphyrin content, pH and light source on the photocatalytic reduction performances of UNT were also explored. Overall, this work presented a possible relationship between the crystal structures and the performance of UNT.Keywords:photocatalytic reduction;porphyrin;UiO-66-NH2;hexavalent chromium
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ELECTROCHIMICA ACTA
·
2023
·
IF 6.6
Qiuyitong Zhang,Yuexin Xu,Ning Lv,Hanyang Li,Zijie Wei,Tian Tian,Yadong Wang,Haolin Tang
A simplified and greener procedure for in-situ obtaining polyimide anode materials for lithium-ion battery electrodes is developed. The combined polyimide material synthesis and electrode preparation reduces the number of processing steps and treatment duration and decreases the energy required for heat treatment, solvent evaporation , and organic solvent use. More importantly, polymerization in situ on the electrode surface render the polyimide particles a sea urchin-like structure, leading to fast electrochemical kinetics, and significant improvement in discharge capacity and cycling performance compared with materials obtained using traditional procedures. Specific capacities of 1870 mAh g − 1 and 2277 mAh g − 1 at 30 °C and 60 °C, respectively, are obtained. A capacity of 1774 mAh g − 1 is retained after 500 cycles at high current density of 1000 mA g − 1 at 60 °C. This new preparation process not only simplifies the preparation process and makes it greener, but also significantly improves the battery performance, providing new possibilities for the preparation of high-performance low-cost lithium-ion battery electrodes.
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