ACS Sustainable Chemistry & Engineering
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2022
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IF 9.224
Peng Zhu,Weizi Zhang,Qinfang Li,Haian Xia
Photocatalytic oxidation of 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA) is an environmental friendly way to convert platform molecules into high-value chemicals. Here, Au/ZnO catalysts with different oxygen vacancies were fabricated by the deposition precipitation method and were used for the photocatalytic oxidation of HMF to FDCA under visible light irradiation. All of the Au/ZnO catalysts showed excellent photocatalytic oxidation selectivity to FDCA greater than 90% under mild conditions. The Au/ZnODP-H catalyst treated by H2 afforded the highest HMF conversion and the selectivities of FDCA up to 96.9%. The localized surface plasmon resonance effect of Au nanoparticles, oxygen vacancy, and the existence of the Schottky barrier enhance the separation and transfer efficiency of photogenerated electron–hole pairs of the catalyst, so as to enhance its photocatalytic activity. The active species trapping experiment and electron spin resonance analysis showed that •O2– and h+ were the active species responsible for the oxidation reaction. The recycle experiment also proved that the catalyst has good stability. This work provides a new strategy for the design of photocatalysts for converting biomass into high-value chemicals.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
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IF 24.319
Bing Wang,Zhuo Li,HaiXia Ma,JianBo Zhang,LinYu Jiao,Hong Hao,EnZhou Liu,Long Xu,Chen Wang,Bo Zhou,XiaoXun Ma
Achieving efficient photocatalytic oxidation of antibiotics represents a key challenge, which can be overcome by developing dynamic attachment strategies between supramolecular and semiconducting catalysts. Herein, we utilize hydrogen bonding and van der Waals forces to dynamically connect self-assembled SubPc-1 dimers and Ag 3 PO 4 semiconductor catalysts for photocatalytic oxidation of antibiotics, which is systematically demonstrated by spectroscopic measurements and theoretical calculations. The degradation efficiency of SubPc-1/Ag 3 PO 4 supramolecular nanoarrays for tetracycline and oxytetracycline is 93.54% and 94.9% under 30 min visible light irradiation, respectively. The superior activity and excellent stability of supramolecular arrays are demonstrated to be more attributed to the dynamic hydrogen bonding and van der Waals connection between SubPc-1 and Ag 3 PO 4 . This work reveals a potential for preparing specific S -scheme heterojunction photocatalysts based on dynamic attachment supramolecular and semiconductor catalysts.
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高影响因子
ACS ES&T Engineering
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2022
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IF 0
Jinxing Zhang,Jie Sun,Hongying Zhao,Guohua Zhao
A traditional Fenton reaction suffers the limitation of acidic conditions, impeding its practical application for environmental remediation. Selective reduction of oxygen with sustainable photoelectrochemical (PEC) technology was first proposed to enlarge the practicable pH range of 7–11. A novel photoelectrode with single-atom copper anchored on oxygen vacancy anatase (Cu-SA/TiO2–x) was designed for the efficient production of hydroxyl radicals (HO•) in an alkaline solution. The in situ-formed O–Cu on the electrode surface promoted the decomposition of electrogenerated H2O2 into HO•. The optimal accumulated concentration of HO• was 276.23 μmol·L–1 during PEC reduction of O2 at pH = 9. The removal of sulfamethoxazole was up to 96.3% in 10 min with the Cu-SA/TiO2–x electrode with an apparent kinetic constant (kobs) of 0.311 min–1. The energy consumption, recycling capacity, and electrolyte effect were evaluated in detail from the perspective of actual application. Furthermore, the high removal of chemical oxygen demand (69.1–93.9%) and the efficient removal of total nitrogen (25.1–87.7%) in five real water samples were almost uninfluenced by water quality. This work not only proposed a strategy of HO• production in the alkaline environment but also provided guidance for developing sustainable and efficient technologies, especially for decentralized water treatment.
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JOURNAL OF HAZARDOUS MATERIALS
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2022
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IF 14.224
Jing Liao,Yuke Wu,Xueshan Chen,Huimin Yu,Yao Lin,Ke Huang,Jinyi Zhang,Chengbin Zheng
Hexavalent chromium (Cr(VI)), a confirmed human respiratory carcinogen, has attracted widespread attention due to its high toxicity and mobility in natural water systems. However, the developed catalytic colorimetric probes for Cr(VI) detection remain challenging, such as various species of Cr(VI) coexisting in water or acid buffer, the obvious interference from oxidizing ions at acidic pH, the synthesis of complex materials, and the consumption of hydrogen peroxide. In this work, a phenomenon of UV light-triggered chromate to produce singlet oxygen under neutral pH was found. An environmentally-friendly method based on the rapid oxidation of chromogenic substrates was thus developed for the highly specific and accurate detection of Cr(VI). Cr(VI) serves as both the active center and the target of this system, which ensures the rapidity, simplicity, and environmental protection of the proposed colorimetric strategy. Importantly, the neutral catalytic condition ensures that the predominant species CrO 4 2- can be accurately quantified and avoids the interference of oxidizing ions. Subsequently, a portable analytical system integrating an array of LED lamps, a miniature color reading device, and a developed smartphone-based program was successfully developed to accomplish high-throughput and on-site analysis of Cr(VI) in natural water. The proposed method provides a rapid screening and water quality assessment tool for the faster, more cost-effective, and accurate detection of Cr(VI) in the water system.
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Journal of Materials Chemistry C
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2022
·Vol. 10
·期 36
·13014-13024
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IF 8.067
Xinnan Ma,Jiacong Wu,Juan Han,Lei Wang,Chunmei Li,Yun Wang
Ingenious design of electron transport channels is crucial to improving the electron utilization efficiency in novel photo-enzyme coupled catalyst systems. Herein, carbon nanotubes (CNT) were used as a bridge between CN and HRP for the electron transformation in the HRP/CNT/CN photo-enzyme system for the first time, which improved the separation efficiency of photogenerated charge carriers due to its unique advantage. Besides, the steric hindrance of CNT can effectively limit the damage of superoxide radicals toward HRP and increase the service life of HRP, which effects the enhancement of stability for HRP. Thus, the desired high-efficiency and stable degradation of the target BPA in water was achieved. These findings may provide a new idea for the design of a photo-enzyme coupled system with an oriented electron transport channel in a controllable manner.
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Polymers
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2022
·Vol. 14
·期 14
·2959
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IF 4.967
Jun Wang,Xiaocui Wen,Shaojun Jiang,Tao Chen
Inappropriate disposal of leaching residues from the lead-zinc tailings recovery process may result in environmental pollution. Its recycling and reuse remain a prevalent topic in environmental science and technology. It was roasted to prepare leaching residues-based materials (TLRS) in this work, and the TLRS were creatively used as the catalyst to active sodium persulfate (PS) to degrade organic pollutants. Degradation of tetracycline using the TLRS–PS system was evaluated, and the treating parameters were optimized. Roasting resulted in the exposure of active sites on TLRS surface, in which transition metals can donate electrons to PS to form SO4·−. SO4·−can further react with OH−to form ·OH. Formation of these radicals was confirmed by both quenching experiments and EPR analysis. Under optimized conditions, 85% of the TC can be degraded in 3.0 h, and ~50% of degraded TC was mineralized to CO2and H2O. The performance of TLRS barely changed after four reuses, suggesting the chemical stability of TLRS. The presence of dissolved substance in the water matrix could weaken the performance of the TLRS–PS system. A mechanism of TC degradation was proposed based on the experimental results and literature. These preliminary results provide us new insight on the reuse of lead-zinc flotation tailings.Keywords:leaching residues;tetracycline;persulfate activation;oxidative degradation;solid waste
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高影响因子
Journal of Environmental Chemical Engineering
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2022
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IF 7.968
Hangjun Zhang,Bingzhi Yu,Xizi Li,Yan Li,Yuchi Zhong,Jiafeng Ding
Harmful algal blooms caused by cyanobacteria in drinking water have posed serious threats to destroy aquatic ecosystems , and the toxins they produce are harmful to human and animal health. Herein, the feasibility of removing Microcystis aeruginosa ( M. aeruginos ) and microcystin-LR ( MC-LR ) by free radicals produced by simple-atomic iron-doped g-C 3 N 4 (Fe-g-C 3 N 4 )-activated peroxydisulfate (PDS) was studied. Pristine g-C 3 N 4 and three kinds of Fe-g-C 3 N 4 with different compositions were successfully synthesized and characterized. When the initial algae density was 2.5 × 10 6 cells·mL −1 , approximately 96.25 % of M. aeruginosa cells were inactivated with 2.0 g·L −1 Fe-g-C 3 N 4 and 4.0 mM PDS under the conditions of pH 7.0, and MC-LR could also be effectively degraded. The activated system can effectively remove M. aeruginosa, and MC-LR was evaluated for its morphological characteristics, cell membrane integrity and microcystin degradation. In addition to the widely recognized reaction species (SO 4 • − and • OH), singlet oxygen ( 1 O 2 ) was another predominant radical for destroying the cell structure and removing MC-LR . The materials can be well recycled, and a possible removal mechanism was proposed. This work shows that the Fe-g-C 3 N 4 -activated PDS system is an environmentally friendly and efficient technology for algae removal and algal toxin reduction.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Yanan Zhang,Zhenli Zhang,Hongjing Han,Mei Zhang,Haiying Wang,Hua Song,Yanguang Chen
NaP zeolite was successfully synthesized via ultrasonic-assisted hydrothermal synthesis. The approaches for Cu or Fe doping were screened. Additionally, the oxidation process of methylene blue (MB) and methyl violet-6B (MV-6B) by the doped NaP ultra zeolites was surveyed. NaP ultra zeolite exhibited higher crystallinity (94.99%), while the crystallization temperature and duration decreased from 120 °C to 90 °C and from 8 h to 4 h with the n (SiO 2 )/ n (Al 2 O 3 ) increasing from 2.0 to 4.0, compared to the hydrothermal synthesis. At the ultrasonic power intensity of 30% and the density of 60 mL/W, the conversion rates of Si and Al rosed from 66.46% to 84.68% and from 73.75% to 95.25%, respectively. Comparatively, the complexation approach demonstrated superior findings in the crystallinity (Fe-NaP ultra : 92.37% and Cu-NaP ultra : 94.14%) at the n (Fe(NO 3 ) 3 ): n (Al 2 O 3 ) ratio of 1:4 and the n (Cu(NO 3 ) 2 ): n (Al 2 O 3 ) ratio of 1:6. The ultrasonic resulted in the smaller crystal sizes for Fe-NaP ultra (1.90 μm) and Cu-NaP ultra (1.80 μm). Cu-NaP ultra displayed better oxidation performance in the elimination of MB (93.22%) and MV-6B (98.71%) via the HO at the condition of pH = 5.0, 30 min, 2.5 g/L, 50 mg/L, and 25 °C. Through the combined action of adsorption and Fenton-like oxidation, the rapid enrichment of organic dyes by the zeolite was realized, and the dyes were removed efficiently. Cu-NaP ultra was capable of retaining good removal performance throughout four cycles, suggesting that it is a promising catalyst for Fenton-like oxidation reactions and may help to pave the way for the removal of organic dyes.
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Molecular Catalysis
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2022
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IF 5.089
Tao Chen,Dongxin Pan,Jie Zhu,Menglin Xie,Ting Li,Yu Zhou,Jun Wang
Direct benzene hydroxylation with dioxygen (O 2 ) is among the most promising alternative pathways for green phenol production, but efficient catalysis systems usually involve metal species or other additives such as sacrificial agents. In this work, we designed a carbon catalyst from the hydrothermal treatment of biomass-derived sucrose and constructed a metal-/additive free heterogeneous catalytic system for benzene hydroxylation to phenol with O 2 . The champion carbon sample gave a high phenol yield of 13.4%. The catalyst was facilely recovered and reused without apparent deactivation. There abundant oxygen functional groups such as phenolic and quinone carbonyl groups served as the active sites and polyfuran units accelerated the O 2 adsorption and activation. The synergistic effect of these surficial organic groups is conducive to the formation of reactive oxygen species, hydroxyl radicals, which effectively oxidized the benzene to phenol.
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高影响因子
NEW JOURNAL OF CHEMISTRY
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2022
·Vol. 46
·期 36
·17223-17234
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IF 3.925
Dajie Zhang,Jiabao Sun,Qiang Li,Haocheng Song,Dongsheng Xia
Biochar emerged as a promising material due to its high efficiency and tunable physicochemical properties. In order to improve the economic applicability of biochar catalysts, we attempted to apply formed Cu-doped deactivated magnetic loofah biochar (Cu-Fe-LBC) as a peroxymonosulfate (PMS) activator to remove tetracycline (TC). The catalyst exhibited high activation of PMS and high stability with the TC removal of 97.6%. The chemical composition and groups on the catalyst surface confirmed the presence of copper ions on the biochar by complexation with COO–. Analysis of quenching experiments and electron paramagnetic resonance indicated the significance of HO˙ and 1O2 in TC degradation. The catalytic system had high catalytic efficiency with a wide pH range and coexisting anions. The possible degradation mechanism was proposed. Moreover, the research provides an insight into the PMS activation by reusing waste biochar catalysts.
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CHEMOSPHERE
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2022
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IF 8.943
Mengen Dang,Dandan Chen,Ping Lu,Guiling Xu
Poplar wood (PW) hydrochar modified by iron (Fe@HC) was prepared greenly by one-step hydrothermal method. The adsorption and degradation performance of DDT was investigated in a heterogeneous advanced oxidation system (Fe@HC/PMS) formed by Fe@HC collaborated with peroxymonosulfate (PMS). The effects of Fe@HC dosage, PMS dosage and DDT initial concentration were quantitatively analyzed. The results showed that DDT removal efficiency can reach to 88.62% in 240 min under optimal conditions (4 g/L Fe@HC, 10 mM PMS, 0.5 mg/L DDT, 5.5 pH 0 ) in Fe@HC/PMS system. Furthermore, Fe@HC/PMS system exhibited high degradation rate and TOC removal efficiency for the removal of various organic contaminants . The influence mechanisms of Fe@HC/PMS system on DDT adsorption and degradation were proposed based on electron paramagnetic resonance (EPR) testing analysis and radical quenching experiments. Based on the mechanism analysis, the influence of Fe@HC/PMS on DDT removal efficiency can be concluded in the order: Active substance indirect degradation (60.95%) > Fe@HC direct degradation (10.13%) > Fe@HC adsorption (17.54%). Among active substance indirect degradation, SO 4 •− , • OH, O 2 •− and 1 O 2 occupied 27.56%, 15.74%, 5.33% and 12.32%, respectively. Moreover, DDT degradation intermediates were detected by a gas chromatography-mass spectrometer (GC-MS) to predict DDT degradation pathways. This study provided a green progress for the reuse of biomass resources and a new way for the enhanced degradation of DDT.
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Jingwen Huang,Chendong Puyang,Yawen Wang,Jiawen Zhang,He Guo
This paper aims to investigate hydroxylamine activated by discharge plasma for tetracycline degradation in water. Results indicated that hydroxylamine can be activated by discharge plasma successfully, and promoted tetracycline degradation. The degradation efficiency of tetracycline by discharge plasma could improve from 70.7% to 90.0% with 0.25 mmol/L hydroxylamine. The energy efficiency (G50) could enhance from 2.28 g/kWh to 3.18 g/kWh, respectively. Synergetic effect could be generated between discharge plasma and hydroxylamine. Ozone and electrons produced by plasma can interact with hydroxylamine to produce more •OH. Capture agent experiment and ESR technique verified that •OH, O 2 • - , 1 O 2 and electrons all participated in tetracycline degradation in plasma/hydroxylamine system. The degradation process was investigated thoroughly based on three dimensional fluorescence , LC-MS and DFT analysis, and two main pathways were proposed. Enhancing applied voltage was beneficial to the degradation of tetracycline. Higher degradation efficiency of tetracycline was obtained at lower initial concentration. Compared with acidic condition, alkaline condition was conducive to the decomposition of tetracycline. The addition of hydroxylamine in plasma system promoted the mineralization of tetracycline. Overall, the plasma/hydroxylamine method can be considered as a preferable potential option for the reduction of tetracycline in water.
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