CHEMOSPHERE
·
2022
·
IF 8.943
Wanying Xie,Wei Song,Ji Li,Xiaolei Zhang,Wenyi Dong,Feiyun Sun
Modifying PVDF membrane by blending hydrophilic nano TiO 2 has been highly concerning, but its practical application is not well investigated. In this study, PVDF-TiO 2 membrane was employed in two modes to treat micro-polluted raw water for the first time, direct membrane filtration and pre-oxidation assists membrane filtration. At two filtration modes, the PVDF-TiO 2 membrane had comparable rejection capability to the unmodified PVDF membrane, as the removal of permanganate index (COD Mn ) was 0.26–0.72 mg/L, UV 254 was 0.0070–0.0618 cm −1 , turbidity was 1.60–4.49 NTU, and the total number of colonies was 360–23,780 CFU/mL. As for raw water treatment , using Fe 2+ /sodium dithionite (DTN)/O 2 system as the pre-oxidation process to assist the filtration of the PVDF-TiO 2 membrane was feasible. After optimization, the applicable conditions of the Fe 2+ /DTN/O 2 process were DTN dosage at 100 mg/L and a C Fe / C DTN of 1:4. As a result, the effluent qualities of the PVDF-TiO 2 membrane significantly improved. It was investigated that atrazine (ATZ), COD Mn , UV 254, and turbidity reduced, which was realized by the synergic effects of the pre-oxidation by free radicals and flocculation by iron. Pre-oxidation of the Fe 2+ /DTN/O 2 process could also enhance the permeability of the PVDF-TiO 2 membrane from 53.6 to 58.0 L/(m 2 ·h), nearly two times the PVDF membrane. Besides, the practical fouling of the PVDF-TiO 2 membrane was stably alleviated by the reduced R t , R re, and R ir , mainly due to constraining the internal pore fouling effectively.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Yuancheng Qin,Zhenhua Jiang,Yue Guo,Muhammad Asim Mushtaq,Zhen Shen,Wanjun Du,Cailing Ni,Geng Luo,Yu Ji,Zhiqi Zhang,Yonggui Deng,Arshad Hussain,Lasharl Najeeb Ur Rehman,Xingke Cai,Panagiotis Tsiakaras,Jie Zhao
Porous organic polymers (POPs) have emerged as functional materials in photocatalytic degradation of tetracycline (TC) antibiotics but still did not get enough attention on the degradation mechanism and “structure-performance” relationship. It is of great scientific concern to explore the photo-degradation capability of POPs for TC antibiotics under visible light and to reveal their “structure-performance” relationship at the molecular level. Herein, we have constructed a novel benzotriazole-based POP by polymerizing benzotriazole-based structure with melamine. The photo-degradation test results indicate that the POP with benzotriazole-based structure presents an excellent photocatalytic performance with a high TC removal efficiency of 92.12 % and good recyclability. The corresponding pseudo-first-order reaction kinetic constant of benzotriazole-based POP is 6.8 times that of benzene-based one. Such excellent performance of benzotriazole-based POP can be attributed to the physical/chemical property contributions of benzotriazole-based structure to POP, e.g. , the narrow energy bandwidth (2.48 eV) for producing more photo-generated electrons/holes, the small charge transfer resistance for circumventing recombination of photo-generated electrons/holes, and the large number of O 2 − radicals converted from high-activated O 2 that produced by the interactions between photocatalyst and O 2 under visible light irradiation. This strategy of introducing the benzotriazole-based structure into POP opens new avenues to develop next-generation advanced photocatalysts for removing TC antibiotics from wastewater.
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ENVIRONMENTAL RESEARCH
·
2022
·
IF 8.431
Yong Cheng,Han-Qing Zhao,Aqiang Ding,Fei Chen,Jun Liu,Dazhi Fang,Chenglong Li,Yongkui Huang,Peili Lu
The widespread application of quaternary ammonium compounds (QAC) has posed a serious hazard to the environment and human being, and high concentration of Cl − in QAC wastewater may further increase the difficulty of pollutants elimination . In this study, such a QAC wastewater under high salinity conditions was chosen as the target, the prepared Ti/(Ru x Ir y )O 2 anode exhibited favorable catalytic performance for the oxidation and mineralization of QAC under high salinity conditions. Increasing the Ru/Ir ratio of Ti-based electrode coating also slightly promoted the inner catalytic capacity. The combination of electron paramagnetic resonance (EPR) and quenching experiments indicates that 1 O 2 served as a main reactive specie in the Ti/(Ru x Ir y )O 2 electrooxidation system. The increase of pH could decrease the removal efficiency of QAC for the reduced 1 O 2 yield, and the rise of Cl − concentration could favor the QAC oxidation, and Cl − was a better electrolyte to promote the oxidation of organic contaminants when compared to Na 2 SO 4 or Na 2 CO 3 . Additionally, the conversion pathway of the model pollutant was tentatively investigated, the results demonstrated that there were almost no halogenated final products residual by electrocatalytic oxidation with Ti/(Ru x Ir y )O 2 anode. This study not only elucidate the reaction mechanism of Ti/(Ru x Ir y )O 2 anode electrocatalytic oxidation of high salinity QAC wastewater, but also may provide an efficacious and eco-friendly method for the treatment of high salinity QAC wastewater.
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ACS Applied Energy Materials
·
2022
·
IF 6.959
Jie-wen Liu,Jian Zhang,Ming-jie Xu,Chuan-jin Tian,Xiao-jun Zeng,Chang-an Wang
Developing highly active and reliable Pt-based catalysts is a major challenge for the widespread commercialization of proton-exchange membrane fuel cells. Herein, we have designed Pt3Co@C hollow sphere catalysts by the template method, in which PtCo alloy nanoparticles of approximately 3 nm diameter are anchored in a porous shell of nitrogen-doped carbon hollow spheres. Due to the confinement effect of the porous carbon shell, PtCo alloy nanoparticles possess excellent resistance to sintering, maintaining 2–3 nm size after calcination at 800 °C. Also, Pt3Co@C hollow sphere catalysts exhibit superior catalytic activity and stability in the oxygen reduction reaction, achieving 3.6 times the mass activity of the corresponding commercial Pt/C catalyst. Such catalysts with a mass activity retention rate of 87% after accelerated durability testing and no significant decay in activity after 10,000 potential cycles. Meanwhile, Pt3Co@C catalysts exhibit extremely high catalytic activity and surprising durability for the hydrogen evolution reaction process over the entire pH range. We believe that this methodology provides an insight into the preparation of high-performance electrocatalysts.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2021
·
IF 9.028
Liying Wu,Zhiqiang Sun,Yufei Zhen,Shishu Zhu,Chen Yang,Jing Lu,Yu Tian,Dan Zhong,Jun Ma
Ubiquitous oxygen vacancies (Vo) existing in metallic compounds can activate peroxymonosulfate (PMS) for water treatment. However, under environmental conditions, especially oxygenated surroundings, the interactions between Vo and PMS as well as the organics degradation mechanism are still ambiguous. In this study, we provide a novel insight into the PMS activation mechanism over Vo-containing Fe–Co layered double hydroxide (LDH). Experimental results show that Vo/PMS is capable of selective degradation of organics via a single-electron-transfer nonradical pathway. Moreover, O2 is firstly demonstrated as the most critical trigger in this system. Mechanistic studies reveal that, with abundant electrons confined in the vacant electron orbitals of Vo, O2 is thermodynamically enabled to capture electrons from Vo to form O2•– under the imprinting effect and start the activation process. Simultaneously, Vo becomes electron-deficient and withdraws the electrons from organics to sustain the electrostatic balance and achieve organics degradation (32% for Bisphenol A without PMS). Different from conventional PMS activation, under the collaboration of kinetics and thermodynamics, PMS is endowed with the ability to donate electrons to Vo as a reductant other than an oxidant to form 1O2. In this case, 1O2 and O2•– act as the indispensable intermediate species to accelerate the circulation of O2 (as high as 14.3 mg/L) in the micro area around Vo, and promote this nano-confinement electron-recycling process with 67% improvement of Bisphenol A degradation. This study provides a brand-new perspective for the nonradical mechanism of PMS activation over Vo-containing metallic compounds in natural environments.
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Journal of Materials Chemistry A
·
2021
·Vol. 9
·期 42
·24056-24063
·
IF 12.732
Yanfang Chen,Xuemei Yan,Jixiang Xu,Lei Wang
H2O2 has a wide range of uses as an oxidant and is also utilized as a high density and environmentally friendly fuel. In this study, crystalline g-C3N4 was modified with K+, Ni and N-doped carbon by thermal-polymerization of Ni2+-anchored and polyvinyl pyrrolidone-encapsulated melamine-cyanuric acid supramolecules, followed by re-calcination in a KCl–LiCl mixture. The obtained strip-like g-C3N4 nanocrystals exhibited high charge separation efficiency and good light absorption capability. Density-functional theory calculations confirmed that the orbital hybridization of Ni–N atoms enabled the formation of charge-transfer channels, which can capture electrons, achieve enhanced oxygen adsorption and reduction via a two-electron pathway. Under the synergistic effects of K+, Ni and N-doped carbon dopants and crystallinity, the obtained sample exhibited high photocatalytic H2O2 yields of 79.6 μM in O2-saturated pure water, which was 10-fold higher than the yield using pristine g-C3N4. This work provides a novel design for production of highly efficient photocatalysts for H2O2 production.
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Nanoscale
·
2021
·Vol. 13
·期 16
·7774-7782
·
IF 7.79
Gangyong Li,Guangming Ren,Wei (Alex) Wang,Zongqian Hu
Carbonaceous materials are promising electrode materials for enzymatic biofuel cells (EBFCs) due to their excellent electrical conductivity, chemical and physical stability and biocompatibility. Design and preparation of carbon materials with a hollow structure and a rough surface are of great significance for immobilization of enzymes both inside and outside the carbon materials for EBFC applications. We report herein the synthesis of novel carbonaceous materials consisting of bamboo-shaped hollow N-doped carbon nanotubes (N-CNTs) and C3N4 nanosheets (denoted as N-CNTs@C3N4) as electrode materials for dual-capture of enzymes in glucose/O2 EBFCs. The combination of one-dimensional N-CNTs with an open structure and two-dimensional C3N4 nanosheets forms a three-dimensional crosslinking network that significantly enhances the immobilization of enzymes, electrode stability, and mass transfer of substrates, thus boosting the EBFC performance. As a result, EBFCs equipped with N-CNTs@C3N4 can generate a high open circuit potential of 0.93 V and output a maximum power density of 0.57 mW cm−2 at 0.47 V. Additionally, the as-fabricated glucose/O2 EBFCs are capable of directly harvesting energy from various soft drinks, which indicates the promising applications of the N-CNTs@C3N4 nanocomposite as an electrode material for EBFCs.
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IET Nanobiotechnology
·
2020
·Vol. 14
·期 5
·347-356
·
IF 1.859
Mei Yang,Qingyuan Gui,Jinlei Ma,Lei Qi,Bijun Bao,Yida Huang
In this study, Gd 2 O 2 S:Ln 3+ (Ln 3+ = Yb 3+ , Er 3+ ) upconversion nanotubes (UCNTs) were synthesised by using Gd(OH) 3 :Ln 3+ (Ln 3+ = Yb 3+ , Er 3+ ) nanotubes as the template. The luminescent and biological properties of Gd 2 O 2 S:Ln 3+ (Ln 3+ = Yb 3+ , Er 3+ ) UCNTs, along with photodynamic therapy (PDT) applications of the Gd 2 O 2 S:8%Yb 3+ , 2%Er 3+ UCNT–Ce6 (chlorin e6) nanocomposites, were systematically studied. The resultant UCNTs showed excellent biocompatibility with human retinal pigment cells (ARPE-19) even after a prolonged incubation time of 72 h, and could be used as luminescent probes. Microscopic imaging revealed that the UCNTs existed mainly in cytoplasm. PDT studies on the Gd 2 O 2 S:8%Yb 3+ , 2%Er 3+ UCNT–Ce6 nanocomposites indicate that the growth of the tumour (cell) could be inhibited dramatically when it was injected (incubated) with Gd 2 O 2 S:8%Yb 3+ , 2%Er 3+ UCNT–Ce6 nanocomposites under the irradiation of 980 nm laser.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2022
·
IF 5.518
Linfeng Peng,Hang Yin,Lu Zou,Faquan Yu
As a promising energy storage technology, Li-CO 2 /O 2 batteries not only deliver ultrahigh discharge capacity but also capture and convert CO 2 into renewable energy. The exploration into the deposition and decomposition kinetics of discharge product (Li 2 CO 3 ) is urgent for the high thermodynamic stability. Herein, the influence of current density on the essential characteristics of Li 2 CO 3 has been explored. The results show that the Li 2 CO 3 with poor crystallinity and elliptical disk morphology can be obtained at medium current density, corresponding to the excellent electrochemical performance including ultrahigh capacity of 5800 mA h/g, lower discharge-charge gap of 1.15 V, and long-term cycle life of 80 cycles. In addition, the morphology and crystallinity of Li 2 CO 3 are tailored by the relative energy barriers for electron migration and O 2 - generation. At a medium current density (500 mA/g), the accelerated electron migration can realize the nucleation rate equivalent to growth one of Li 2 CO 3 . At this time, Li 2 CO 3 will uniformly deposit on the cathode surface, forming elliptical disk morphology with poor crystallinity. Obviously, this work provides new sights for promoting the development of Li-CO 2 /O 2 battery through rational design of catalysts to accelerate the deposition and decomposition processes of Li 2 CO 3 .
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JOURNAL OF PHYSICS D-APPLIED PHYSICS
·
2024
·Vol. 57
·期 43
·435204
·
IF 3.1
Pengyu Zhao,Yikang Jia,Sihong Ma,Rui Zhang,Kaiyu Li,Tianyi Song,Jianbao Zheng,Jingyao Zhang,Li Guo,Dingxin Liu,Xiaohua Wang,Mingzhe Rong
Methicillin-resistant Staphylococcus aureus (MRSA) presents a significant threat due to the multiple resistance to antibiotics, leading to severe and challenging-to-treat infections. Plasma-activated saline (PAS) prepared by plasma gases, could efficiently inactivate various pathogenic bacteria including both sensitive and antibiotic-resistant bacteria. In this study, the PAS was prepared by plasma gases with different ratios of N2 and O2 activated by gliding arc discharge. First, the gaseous reactive species in the plasma gases were compared, revealing that the highest levels of NOx including NO2 and N2O5 were generated in the gases with the N2/O2 ratios of 4:6, 5:5, and 6:4. Subsequently, the PAS prepared by the two plasma-activated gases at the N2/O2 ratios of 5:5 and 6:4 exhibited the strongest inactivation effects on both planktic MRSA and biofilms. Furthermore, the aqueous reactive species in the PAS exhibited varied change trends with the increasing N2/O2 ratios. Additionally, ultraviolet spectroscopy combined with the probe of N, N-diethyl-p-phenylenediamine was applied for the detection of O2NOO− in the PAS, and the levels of O2NOO− in the PAS were positively correlated with the inactivation effects. Moreover, the PAS induced varying levels of nitration modification on the soluble proteins in MRSA cells, which were related to the intensities of O2NOO− in the PAS. This study regulated the reactive species in the PAS through gas composition and explored the inactivation mechanism of the PAS, providing a new strategy to promote the preparation efficiency of plasma-activated solutions for biomedical applications.
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Catalysis Science & Technology
·
2024
·
IF 4.4
Pengken Li,Hui Zhao,Rong Ji,Wenwen Chi,Xinyu Sun,Yuming Dong,Yongfa Zhu
A one-step two-electron oxygen reduction pathway is crucial for the stable and efficient photosynthesis of hydrogen peroxide. However, the lower oxygen adsorption and activation capacity significantly restrict the ability of the one-step two-electron oxygen reduction pathway. In this work, a covalent organic framework containing a diacetylene unit (COF-Tfp-BDDA) as an efficient oxygen reduction active site was designed for the photosynthesis of hydrogen peroxide. This work demonstrates that the introduction of the diacetylene unit efficiently improved the oxygen adsorption and activation capacity of the COF. Additionally, the introduction of a diacetylene unit effectively promoted charge separation. COF-Tfp-BDDA exhibited a superior rate of H2O2 preparation (880 μmol g−1 h−1) under visible light irradiation from pure water and oxygen, better than most COF-based photocatalysts. The catalyst exhibited a stable hydrogen peroxide photosynthesis efficiency above 100 hours in cycling experiments. Based on the experimental and DFT calculation results, the introduction of a diacetylene unit not only enhances the adsorption and activation of oxygen but also alters the reduction pathway of oxygen, leading to effective charge separation. These factors contribute to the efficient photosynthesis of hydrogen peroxide in pure water. This work provides a novel idea regarding the application of COFs in the field of solar energy conversion.
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高影响因子
SOLID STATE IONICS
·
2016
·
IF 2.38
Cheng-Dong Li,Jin Xu,Ji-Sheng Xia,Wei Liu,Xin Xiong,Zhu-An Zheng
The FeF 3 -coated Li[Li 0.2 Mn 0.54 Ni 0.13 Co 0.13 ]O 2 cathode materials were synthesized via a wet chemical process followed by a solid state reaction . The physical properties of the as-prepared samples were conducted using X-ray diffraction, scanning electron microscopy, and transmission electron microscopy . The results indicated that the surface of cathode particles was covered by FeF 3 film (about 5–15 nm thick). Compared with the bare cathode, the FeF 3 -coated Li[Li 0.2 Mn 0.54 Ni 0.13 Co 0.13 ]O 2 one delivered the higher coulombic efficiency, better rate capability, longer cycle life, and better structure stability. A high capacity retention of 95% (190 mAh g − 1 ) after 100 cycles at 0.5 C rate was obtained for the FeF 3 -coated Li[Li 0.2 Mn 0.54 Ni 0.13 Co 0.13 ]O 2 cathode. Besides, the results from cyclic voltammetry and electrochemical impedance spectra revealed that the noteworthy enhanced electrochemical properties of the surface-modified sample were due to the presence of FeF 3 coating layer , which suppressed the side reaction between the Li[Li 0.2 Mn 0.54 Ni 0.13 Co 0.13 ]O 2 particles with electrolyte and further stabilized the Li[Li 0.2 Mn 0.54 Ni 0.13 Co 0.13 ]O 2 structure with cycling.
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危险品化学品经营许可证（带存储）