APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Binbin Tan,Jing Wang,Yao Deng,Huidi Zhang,Jiang Wang,Zhihao Zhang,Wenlei Wang
The key to enhancing the activation efficiency of peroxydisulfate (PDS) lies in facilitating the adsorption of PDS and accelerating the rate of electron transfer at the interface. In this work, the oxygen vacancy (Ovs) concentration of ultrathin Bi 4 Ti 3 O 12 (BTO) was controlled in situ by high-energy electron beam bombardment. BTO V -300 exhibited a significant activation effect on PDS. The degradation rate constant ( k obs ) for the removal of ciprofloxacin (CIP) was measured to be 0.2080 min −1 under visible light irradiation, which was 3.71 times greater than that of the original BTO. Density functional theory calculations uncovered the principal role of oxygen vacancies as active sites for PDS activation. Introducing OVs significantly boosted the adsorption energy of PDS on BTO and lengthened the O O bond of PDS. This study represents the potential mechanism behind the activation of PDS by BTO V and provides valuable insights for enhancing the photoactivation efficiency of PDS.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Jintong Lan,Lijun Qiu,Xi Cai,Yang Lin,Bo Xie,Hongqi Shi,Lizhi Zhang,Xiao Liu
Trichloroethylene (TCE) with trace concentrations is often detected in soils and groundwater, posing potential damages to public health. The elimination of TCE can be achieved through reductive dechlorination using zero-valent iron (ZVI). However, ZVI usually suffers from the presence of passive iron (hydro)oxides layer and low electron transfer rate, thus leading to the unsatisfactory reactivity. Herein, we fabricated oxalated ZVI (Ox-ZVI bm ) by mechanical ball-milling of micro-scale ZVI and H 2 C 2 O 4 ·2H 2 O to modify the ZVI surface composition. To be specific, the modification of the iron oxide shell by oxalic acid facilitated the generation of unsaturated coordination Fe(II), enhancing TCE adsorption. Furthermore, the formed FeC 2 O 4 on the iron oxide shell improved electron transfer efficiency, contributing to the enhanced TCE reductive dechlorination. Impressively, the rate of TCE degradation by Ox-ZVI bm was 10-fold higher than that of ZVI bm without oxalate modification. Moreover, Ox-ZVI bm samples were filled in a laboratory Permeable Reactive Barriers (PRB) column to treat actual underground wastewater containing TCE pollutants. The effluent concentration of TCE maintained steadily below 0.21 mg/L for over 10 days, complying with the National Groundwater Class IV standard (GBT 14848–2017). This marks a significant step toward practical groundwater treatment.
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GREEN CHEMISTRY
·
2023
·Vol. 25
·期 17
·6717-6727
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IF 9.8
Xi Luo,Jiahui Zhan,Qingqing Mei,Shicheng Zhang
Polystyrene plastic is a widely used artificial material, but there is still no efficient, economic or environmentally friendly recycling method for waste polystyrene plastic, which has caused serious environmental pollution and a waste of resources. Herein, the method of nitric acid oxidative upgrade is used to convert polystyrene plastic into a high-value chemical raw material, benzoic acid. The yield can reach nearly 90% at 180 °C within 3 h, and the purity of the product is more than 95%. In this process, nitric acid is decomposed by heat to generate nitrogen dioxide and oxygen, which react with the carbon-centered radicals formed at weak sites on the long chain of polystyrene and further generate peroxy radicals and hydroxyl radicals. The formation of oxygen-containing functional groups promoted the fracture of the C–C bond and eventually formed benzoic acid. In addition, this method also has good treatment effects on real-life polystyrene plastic products. This research provides a new method for the recycling and high-value utilization of waste polystyrene plastics. The intrinsic material value of polymers can be maintained by recycling functional chemicals through oxidative upgrade.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Dingyuan Zheng,Zehuai Li,Wenrui Yao,Yuning Wang,Ce Sun,Haiyan Tan,Yanhua Zhang
Wood has garnered renewed interest due to its capacity to reduce carbon emissions when replacing non-renewable materials. Wood modification is often necessary because achieving optimal performance solely from the wood itself is challenging. Strategies for wood modification fall short of being genuinely sustainable and eco-friendly. In this context, a catalyst-free esterification method mediated by maleic anhydride (MA) is introduced for modifying wood. Notably, this approach aligns with principles of recycling, reuse, and reduction. A comprehensive comparison of MA-mediated wood esterification versus TEMPO-mediated wood oxidization highlights the effectiveness and superiorities of the MA esterification approach. Delignified wood esterified by MA (MA-DW) exhibits higher charge content (2.42 ± 0.24 vs. 0.53 ± 0.08 mmol/g), superior mass gain (18.4 ± 2.6 wt% vs. −15.92 ± 3.5 wt%), efficient recycling capability of the reaction medium (MA could be recycled five times, while TEMPO cannot be recycled), and integrity of the final products (retaining intact geometry vs. complete disintegration) compared to TEMPO-oxidized delignified wood (TEMPO-DW). Moreover, the MA-DW platform can serve in energy storage applications as an electrode or in sewage remediation applications as a catalyst. The esterification method mediated by MA provides an eco-friendly pathway for modifying wood, serving as a platform for creating diverse materials, potentially offering innovative concepts and insights for wood modification research.
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ACS Applied Polymer Materials
·
2023
·
IF 5
Kangjie Wu,Xiao Chen,Xuran Xu,Chao Yu,Chuanxiang Chen
Multifunctional strain sensors simultaneously satisfy all the requirements including flexibility, stretchability, biocompatibility, and high responsibility to external stimuli, which are always in high demand for wearable electronics. In this work, we introduced modified bacterial cellulose nanofibers (BCNF) as double-network hydrogel-reinforced substrates to prepare an MXene-based strain sensor (MPCB). The well-percolated BCNF play an important role in reinforcing the polymer skeleton and inducing the continuous MXene–MXene conductive paths. Consequently, the electrical conductivity was significantly improved and excellent mechanical properties were retained (with the elongation at break over 500%). The prepared hydrogel can act as a wearable sensor for human motion detection, including swallowing movements, finger bending, and wrist bending. It also exhibits promising applications with multiple characteristics, i.e., ideal EMI, adjustable flexibility, self-healing, and self-adhesive performance. Our work provides a simple and practical strategy for a generation of wearable electronic sensor devices.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Qian Li,Jiahui Zhang,Jiayu Zhou,Wang Xu,Zhuowei Cheng,Piet N.L. Lens,Jianmeng Chen,Dongzhi Chen
The effective and economic treatment of chlorobenzenes has become one of the most intractable issues in the field of air pollution control. Herein, a visible-light photocatalysis coupled with biodegradation (VPCB) system was developed by integrating an innovative visible-light responsive TiO 2 /oxygenous groups decorated g-C 3 N 4 (TiO 2 /OCN) with polyurethane carriers immobilized with Ralstonia sp. XZW-1 for chlorobenzene removal. Performance tests showed that light intensity, preparation of the MICs, catalyst dosage and composition of the TiO 2 /OCN cast significant influence on chlorobenzene removal efficiency, with the degradation efficiency, mineralization and dechlorination ratios of VPCB achieving 100%, 35.5%, and 99.4% under the optimal conditions, respectively, outcompeting the sum of visible-light photocatalytic system and biodegradation protocols. Cycling tests further demonstrated the excellent stability of VPCB. Mechanism analysis found that increased reactive sites, improved visible-light harvesting, accelerated charge transfer and separation, and the resulting abundant active species jointly contributed to the enhanced photocatalytic activity of TiO 2 /OCN. Photogenerated holes were most significant active species for chlorobenzene removal, followed by OH and O 2 − radicals. The carriers could effectively protect microorganisms from light illumination and strong oxidizing species, allowing the further microbial metabolism of chlorobenzene photocatalytic oxidation intermediates with good biodegradability, not only greatly promoting the microbial growth and activity, but further enhancing chlorobenzene photocatalytic degradation. Plausible synergistic mechanism for chlorobenzene degradation between photocatalysis and biodegradation was also revealed. Furthermore, the VPCB system constructed presented wide applicability towards various pollutants, and its performance was found closely related with the hydrophobicity of pollutants. This work provided insight into the design and application of the VPCB system for the efficient and economic treatment of refractory pollutants.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2023
·
IF 8.2
Xiaomeng Li,Lei Jiang,Manqing Yan,Hong Bi,Qiyang Wang
To meet the requirements of eco-friendly and sustainability in the 21st century, hydrogels based on biopolymer with conductivity and stretchable property have attained increasing attention for strain sensor. However, the as-prepared of hydrogel sensor with excellent mechanical property and high strain sensitivity is still a challenge. In this study, chitin nanofiber (ChNF) reinforced composite hydrogels of PACF are fabricated via a facile one-pot method. The obtained PACF composite hydrogel exhibits good transparency (80.6 % at 800 nm)and excellent mechanical properties (tensile strength, 261.2 kPa; tensile strain as high as 550.3 %). Moreover, the composite hydrogels also demonstrate excellent anti-compression performance. The composite hydrogels own good conductivity (1.20 S/m) and strain sensitivity. Most importantly, the hydrogel can be assembled as a strain/pressure sensor for detecting large-scale and small-scale human motion. Therefore, flexible conductive hydrogel strain sensors will have broad application prospects in artificial intelligence, electronic skin, and personal health.
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CHINESE CHEMICAL LETTERS
·
2023
·
IF 9.1
Han-Qing Zhao,Peili Lu,Fei Chen,Chen-Xuan Li,Rui Yan,Yang Mu
Sulfide oxidation under aerobic conditions can produce active oxygen for the transformation of organic pollutants in aquatic environments. However, the catalytic performance of transition metal-supported carbon material on this process is poor understood. This study found that Co-loaded carbon nanotubes (CNTs) was able to realize the efficient aerobic transformation of antibiotic ciprofloxacin (CIP) by sulfide, with the pseudo -first order reaction rate constant improved from 0.013 h −1 without catalyst to 0.44–0.71 h −1 with 100 mg/L Co-loaded CNTs. Singlet oxygen ( 1 O 2 ) was the main active specie playing key roles in the process of CIP aerobic transformation with presence of Co-loaded CNTs. Mechanism studies indicated that the excellent electron transfer ability of Co-loaded CNTs might play an important role to promote the electron transfer and facilitate the formation of intermediate H 2 O 2 and 1 O 2 . Additionally, the Co-loaded CNTs/sulfide system effectively reduced the acute toxicity of organic pollutant, and Co-loaded CNTs showed remarkable cycling stability and negligible leaching. This study gives a better understanding for the Co-loaded CNTs mediated aerobic antibiotics transformation by sulfide, and provide a reference for the application of Co-loaded carbon materials on organics aerobic transformation by sulfide.
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CELLULOSE
·
2023
·Vol. 30
·期 11
·7095-7111
·
IF 5.7
Fu Danning,Yang Rendang,Wang Ruibin,Wang Yang,Li Zhihan
Recently, ionic conductive organohydrogels (ICOs) have received widespread attention in wearable electronics. However, it remains challenging to combine reliable ionic conduction with good mechanical strength well, especially under extreme conditions. Herein, a novel ICO is produced by assembling polyvinyl alcohol with functionalized cellulose nanofibrils (CNFs) via a DMSO/H 2 O sol–gel process. A comprehensive study of the quaternized and carboxylated CNFs on ICOs is made. It is found that embedding of the latter can help ICOs to present excellent mechanical properties (tensile/compressive stress of 2.10/7.61 MPa), freezing tolerance (− 78 °C), and the highest electrical conductivity (3.23 S·m −1 ). Since all the primary alcohol carbons in the carboxylated CNFs have been thoroughly carboxylated, it is undoubted that their intermolecular attraction is sharply decreased to increase the counterion Na + attraction, thus providing more hopping sites to enhance the ion transfer. Moreover, benefiting from these advantages, a human-interactive sensor based on the novel ICO is constructed to discern multiple human motions, including finger bending, wrist flexing, elbow bending, and walking. Overall, a facile yet versatile strategy is introduced that is expected to shed light on fabricating ICOs with all-around performance applicable in wearable electronics.
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CELLULOSE
·
2023
·Vol. 30
·期 10
·6507-6521
·
IF 5.7
Fan Lingling,Zheng Wenfeng,Yang Yuan,Sun Yan,Peng Songlin,Xu Jie,Yin Guangfu
Bacterial cellulose (BC)/polypyrrole (PPy) nanofibrous composites have been extensively studied in supercapacitors owing to their large specific surface area and excellent tensile strength. However, the inferior cycling stability due to structural pulverization of PPy impedes their potential applications. Herein, nanofibrous composite membranes of MXene, PPy and oxidized BC (TOBC) were prepared for flexible supercapacitor electrodes. The C6 primary hydroxyl groups of BC nanofibers were oxidized into aldehyde or carboxyl groups. Due to the enhanced interaction of TOBC with PPy and MXene, the TOBC nanofibers were horizontally wrapped on the MXene nanosheets and PPy was homogeneously deposited on the TOBC nanofibers. The flexible solid-state supercapacitors fabricated with the MXene@TOBC@PPy (TMP) electrodes achieved an areal specific capacitance of 928.9 mF cm −2 at 0.7 mA cm −2 and a capacitance retention of 85.5% after 5000 cycles. Therefore, the TMP electrodes could be a promising electrode material for flexible supercapacitors.
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Environmental Science-Nano
·
2023
·Vol. 10
·期 7
·1897-1906
·
IF 7.3
Yang Yang,Junmin Peng,Huilin Tao,Zhou Yang,Yidong Hou,Wei Lin,Jinshui Zhang
The development of efficient catalysts is of great significance in the photocatalytic ozonation process for organic wastewater treatment. However, the effect of exposed facets and surface defects of the catalyst on the photocatalytic ozonation performance is less covered. Herein, ZnO nanocomposites with different preferentially exposed crystal facets (ZnO-rod and ZnO-disk) were synthesized and used for photocatalytic ozonation of phenol. The characterization and density functional theory calculation results demonstrated that the exposed {0001} facets and oxygen vacancies promoted the separation and transfer of photogenerated charges as well as improved the adsorption and activation of ozone molecules on the catalyst surface. Consequently, the TOC removal rate in the UV-O3/ZnO-disk process (62.4%) was much higher than those in the UV-O3/ZnO-rod process (41.3%) and the UV-O3 process (15%). Moreover, the experimental results of the identification and quenching of active species illustrated that ˙OH was more likely to be produced in the UV-O3/ZnO-disk process, while 1O2 was more likely to be formed over ZnO-rod. A large amount of ˙OH with a stronger oxidation capability than 1O2 contributed to the superiority of ZnO-disk over ZnO-rod in organic pollutant removal. This work demonstrates that the engineering of crystal facets and surface defects provides an effective strategy for constructing efficient catalysts for the photocatalytic ozonation process.
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ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Qihang Wang,Lifen Hu,Hongyang Ma,Shyam Venkateswaran,Benjamin S. Hsiao
A nanofibrous composite reverse osmosis (RO) membrane with a polyamide barrier layer containing interfacial water channels was fabricated on an electrospun nanofibrous substrate via an interfacial polymerization process. The RO membrane was employed for desalination of brackish water and exhibited enhanced permeation flux as well as rejection ratio. Nanocellulose was prepared by sequential oxidations of 2,2,6,6-tetramethylpiperidine-1-oxyl (TEMPO) and sodium periodate systems and surface grafting with different alkyl groups including octyl, decanyl, dodecanyl, tetradecanyl, cetyl, and octadecanyl groups. The chemical structure of the modified nanocellulose was verified subsequently by Fourier transform infrared (FTIR), thermal gravimetric analysis (TGA), and solid NMR measurements. Two monomers, trimesoyl chloride (TMC) and m-phenylenediamine (MPD), were employed to prepare a cross-linked polyamide matrix, i.e., the barrier layer of the RO membrane, which integrated with the alkyl groups-grafted nanocellulose to build up interfacial water channels via interfacial polymerization. The top and cross-sectional morphologies of the composite barrier layer were observed by means of scanning electron microscopy (SEM), atomic force microscopy (AFM), and transmission electron microscopy (TEM) to verify the integration structure of the nanofibrous composite containing water channels. The aggregation and distribution of water molecules in the nanofibrous composite RO membrane verified the existence of water channels, demonstrated by molecular dynamics (MD) simulations. The desalination performance of the nanofibrous composite RO membrane was conducted and compared with that of commercially available RO membranes in the processing of brackish water, where 3 times higher permeation flux and 99.1% rejection ratio against NaCl were accomplished. This indicated that the engineering of interfacial water channels in the barrier layer could substantially increase the permeation flux of the nanofibrous composite membrane while retaining the high rejection ratio as well, i.e., to break through the trade-off between permeation flux and rejection ratio. Antifouling properties, chlorine resistance, and long-term desalination performance were also demonstrated to evaluate the potential applications of the nanofibrous composite RO membrane; remarkable durability and robustness were achieved in addition to 3 times higher permeation flux and a higher rejection ratio against commercial RO membranes in brackish water desalination.
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