Journal of Environmental Chemical Engineering
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2023
·
IF 7.7
Jun Chen,Shangqing Xia,Xiaohong Yang,Xue Li,Zhaoming Chen,Zihui Song,Yutong Wang,Zongsheng Zhan,Jie Jin,Dongliang Shao
New technology is required for the effective disinfection of pathogenic bacteria in water. A novel type of activator material (Fe-Mg-Mt-SS) was prepared using bimetallic iron-magnesium (Fe-Mg), montmorillonite (Mt), and sewage sludge carbon (SS) and applied it for disinfection. The specific surface area of Fe-Mg-Mt-SS was 115.72 m 2 /g, and the spatial structure of Fe-Mg-Mt-SS was orderly and layered. Mt played a role in frame support, and Fe-Mg was integrated into the structure in an orderly manner. Fe-Mg-Mt-SS effectively activated persulfate (PS) to disinfect Escherichia coli ( E. coli ) in water, with a disinfection rate of 7.00 lg of E. coli within 80 min in the PS/Fe-Mg-Mt-SS system, and the high disinfection rate was stable under different pH and elevated temperatures. Fe-Mg-Mt-SS showed broad spectrum disinfectant efficiency against other bacteria ( Staphylococcus aureus, Pseudomonas aeruginosa, and Bacillus subtilis ). Fe-Mg-Mt-SS activated PS killed E. coli mainly by producing hydroxyl and oxygen radicals, which damaged the E. coli cell membrane. Bimetallic activation with Fe and Mg synergistically activated PS, graphitised SS had more orderly spatial and laminar structures, and Mt improved the thermal stability and layer spacing of Fe-Mg-Mt-SS, which facilitated better metal insertion and improved its activation properties. The preparation of Fe-Mg-Mt-SS and activation of PS provide a new technology for the disinfection of pathogenic bacteria in water.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Kexia Jin,Da Zhang,Binqiang Pan,Khak Ho Lim,Tiffany Abitbol,Wen-Jun Wang,Xuan Yang
With nano-dimension, high aspect ratio, and high mechanical properties, cellulose nanofibrils (CNFs) are emerging sustainable nanomaterials with potential applications in films and composites. However, their preparation often involves a series of chemical treatments such as delignification, bleaching and harsh chemical pretreatments, and treats lignin as waste. Herein, we report a sustainable method to prepare high-quality lignin-containing cellulose nanofibrils (LCNFs) from bamboo chips, using a one-step maleic anhydride esterification treatment without any toxic organic solvent or catalyst. The resultant LCNFs have high lignin content (24%), high surface charge (2.25 mmol/g), fine diameter (∼2.5 nm), and high aspect ratio (>400). These superior properties can be translated into the corresponding nanopaper films with high optical transmittance (85% at 600 nm), UV shielding (<10% transmittance at 200–350 nm), hydrophobicity (water contact angle 75°), thermal stability (maximal weight loss temperature at 338 °C), and mechanical properties. Importantly, such films show the best reported tensile strength (290 MPa) among all the LCNF films, and it still outperforms conventional CNF films after 5 rounds of recycling. Furthermore, as sustainable nanofillers, such LCNFs can be directly incorporated into a hydrophobic polyester matrix, and significantly enhances the UV shielding and mechanical properties of the final nanocomposites. Altogether, with eco-friendly production and multiple functions, these LCNFs are a new class of nanocelluloses with high industrial relevance.
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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
Shaowei Wang,Xiaoyue Jin,Yiying Yue,Changtong Mei,Xinwu Xu,Qinglin Wu,Huining Xiao,Jingquan Han
High-performance electronics based on transition-metal carbides/nitrides (MXene) have attracted extensive attention due to their two-dimensional structure, modifiable surface chemistry and excellent conductivity. However, because of the weak interconnections between adjacent nanosheets, the construction of robust and flexible macroscopic MXene-based films for wearable electronics remains a challenge. Herein, mechanically tough, highly electroconductive and multi-photoresponsive films (TTM-Al) with a hierarchical nacre-like structure composed of tannic acid-modified 2,2,6,6-tetramethylpiperidin-1-yloxy-oxidized cellulose nanofibers (TA@TOCNs) and MXene are developed via sequentially bridged hydrogen and ionic bonds. TA@TOCNs with abundant phenolic hydroxyl groups as the intercalation layer can enhance the hydrogen bonding interactions with adjacent MXene nanosheets and improve the dispersibility, film-forming ability, mechanical toughness, as well as the in-plane orientation of MXene nanosheets, which can facilitate the construction of well-aligned “brick and mortar” structure. The ionic bonds induced by aluminum ions and oxygen-containing groups in TA@TOCNs and MXene can not only strengthen the interlocking ability and mechanical toughness of TTM-Al, but also promote the electron transfer and heat conduction between MXene nanosheets. Benefiting from the synergism of sequentially bridged hydrogen and ionic bonds, the optimized ultra-thin TTM-Al (∼40 μm) integrates high mechanical strength (∼118.56 MPa), toughness (∼6.84 MJ m −3 ), electroconductivity (∼5587 S m −1 ), photoelectric response (photosensitivity ∼ 3050%) and fast photothermal conversion capability (saturation temperature up to 181.6 °C in only 20 s) under near-infrared irradiation. The patternable and flexible devices based on polydimethylsiloxane encapsulated TTM-Al demonstrate the tunable photoelectric/photothermal dual response, enhanced mechanical and waterproof properties, delivering an alternative construction strategy for next-generation multifunctional photoresponsive wearable devices.
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Nano Today
·
2023
·
IF 17.4
Jianan Yin,Guohe Huang,Huining Xiao,Ning Chen,Chunjiang An,Tzu-Chiao Chao,Renfei Feng,Stuart Read
Treating water resources contaminated by pathogenic microorganisms and heavy metals is a great challenge because of the difficulties in developing efficient strategies for water treatment. Traditional adsorbent materials have the drawbacks of high cost, low adsorption efficiency, secondary pollution creation, and a lack of adaptability in removing a wide variety of pollutants. In this study, inspired by the hierarchical fibrous structure and antibacterial property of the natural silkworm cocoon, we developed a guanidine-functionalized sericin/nanocellulose aerogel (GSNA) with a biomimetic skeletal architecture, which holds great promise for achieving hybrid water disinfection and heavy metal removal. The nanocellulose (CNC) fibers integrated into a robust building block with an interconnected structure and mechanical stability. The grafted polyhexamethylene biguanide (PHMB) endows the biomimetic aerogel with exceptional bactericidal activity (7 log reduction against Escherichia coli within 30 min). Benefiting from the abundant surface functional groups on sericin and CNC-PHMB, the obtained aerogel also exhibits superior heavy metal adsorption capacity (571.5 mg/g for Cu). These compelling merits enable the aerogel to disinfect water and remove heavy metal ions simultaneously as a membrane filter . The synthesized GSNA can be a promising candidate for water disinfection and purification because of its facile preparation, cost-effectiveness, and environmentally friendly characteristics.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
·
IF 22.1
Linlin Sun,Xiaoshuo Liu,Yibing Feng,Xunlei Ding,Jigang Wang,Nan Jiang,Shanjiang Wang
A special two-layer coordination configuration anchored single-atom La (SALa) catalyst is synthesized to realize the effective separation of electrons in space and efficient active sites for the activation of O 2 to produce more active species. The special SALa microenvironment is obtained by a novel and facile reduction method that avoids the formation of rare earth oxides and the concentration of loaded SALa (10.34 wt%) exceeds that in most previous studies. The photodegradation test results show that antibiotics are almost completely removed within 30 min by SALa/CN. The first-order kinetic constant of SALa/CN (0.10661 min −1 ) is approximately 9.81 times higher than that of 3DA-CN (0.01087 min −1 ). SALa can be considered as a bridge to transfer electrons and •O 2 − , 1 O 2 and h + are the main active species to degrade tetracycline into some pollution-free small molecules. This work provides an efficient rare earth single-atom catalyst activity strategy possessing certain potential in practical applications.
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CHEMICAL ENGINEERING JOURNAL
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2023
·
IF 15.1
Yunning Chen,Zhengkai Wu,Renquan Guan,Xueying Cheng,Qingkun Shang,Yingnan Sun
Improving the efficiency of photogenerated charge separation and transport is the primary goal of designing and constructing efficient composite photocatalysts. The matching of energy bands and the formation of chemical bond between the two components are very conducive to the separation and transmission of photogenerated charges. Herein, three perylene diimide derivatives (PDIs) are synthesized by introducing sulfonic acid group (PDI-SA) and benzenesulfonic acid (PDI-BSA) respectively into the amide bond and further chlorine bay-substituting (Cl-PDI-BSA). The good water solubility of Cl-PDI-BSA ensures its forms a stable chemical bond with TiO 2 through the sulfonic acid group in the single molecular state, coupled with the matching of energy band structure, TiO 2 @Cl-PDI-BSA exhibited excellent performance upon visible light photocatalytic degradation to phenol and trenbolone acetate (TBA). It can remove 100% of phenol in 15 min and 100% trenbolone acetate (TBA) in 30 min, which is 14.3 times that of TiO 2 . Combining to DFT calculation, Kelvin probe force microscope and EPR analysis prove that bay chlorine substitution has a greater impact on the energy band structure and electron cloud distribution of PDIs than N-sulfonation, thereby seriously affecting the transport of photogenerated carriers with TiO 2 .
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ACS Nano
·
2023
·
IF 17.1
Lei Zhang,Siheng Wang,Zhuomin Wang,Zeyu Liu,Xu Xu,He Liu,Dan Wang,Ziqi Tian
Hydrogels with strong yet reversible mechanical and adhesive properties fabricated in a facile and friendly manner are important for engineering and intelligent electronics applications but are challenging to create and control. Existing approaches for preparing hydrogels involve complicated pretreatments and produce hydrogels that suffer from limited skin applicability. Copolymerized hydrogels are expected to present an intriguing target in this field by means of thermoresponsive features, while the perceived intrinsic flaws of brittleness, easy fracture, and weak adhesion enervate the development prospects. Herein, we report a hydrogel with strong yet reversible mechanical and adhesive properties using cellulose nanofibrils to simultaneously address multiple dilemmas inspired by a temperature-mediated phase separation strategy. This strategy applies temperature-driven formation and dissociation of hydrogen bonds between common copolymers and cellulose nanofibrils to trigger the onset and termination of phase separation for dynamically reversible on-demand properties. The resulting hydrogel exhibits up to 96.0% (117.2 J/m2 vs 4.8 J/m2 for interfacial toughness) and 85.7% (0.02 MPa vs 0.14 MPa for mechanical stiffness) adhesive and mechanical tunability when worked on skin, respectively. Our strategy offers a promising, simple, and efficient way to directly achieve robust adhesion performance in one step using common copolymers and biomass resources, with implications that could go beyond strong yet adhesive hydrogels.
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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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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2023
·
IF 9.9
Yiqing Li,Manqin Fu,Xiaoxia Zhang,Chun He,Dingsheng Chen,Ya Xiong,Liqing Guo,Shuanghong Tian
Highly reactive nanoclusters of metal oxides are extremely difficult to be synthesized due to their thermodynamic instability. For the first time, CuO x nanoclusters supported on anatase TiO 2 nanotubes (NT) with many defects as anchoring sites were successfully prepared. Although the copper loading reached as high as 2.5 %, the size of CuO x nanoclusters in the sample of 2.5 %CuO x /NT were mainly around 1.0 nm. The aggregation of copper species during the calcination process was undoubtedly hampered by the anchoring effects of the abundant defects in NT support. Due to the highly exposed undercoordinated atoms of CuO x nanoclusters, the mixed valences of copper, and the strong interface interaction between CuO x nanoclusters and NT support, 2.5 %CuO x /NT-catalyzed ozonation showed the highest pseudo-first-order reaction rate constant of 8.5 × 10 −2 min −1 , 2.2 and 4.0 times that of NT-catalyzed ozonation and ozonation alone, respectively. Finally, the catalytic mechanism was revealed by both experiments and density functional theory calculations (DFT). The results demonstrated that the undercoordinated Cu in CuO x /NT could highly promote the adsorption of ozone with a high adsorption energy of −125.16 eV and the adsorbed ozone was activated immediately, tending to dissociate into a O 2 molecule and a surface O atom. Thus, abundant reactive oxygen species , e.g., hydroxyl radical (·OH), superoxide radical (·O 2 – ) and singlet oxygen ( 1 O 2 ), could be generated via chain reactions. Especially, ·OH mainly contributed to the removal of ibuprofen pollutants. This work sheds a light on the design and preparation of highly reactive nanoclusters of metal oxide catalysts for catalytic ozonation of refractory organic pollutants .
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Journal of Materials Chemistry A
·
2023
·Vol. 11
·期 34
·18323-18335
·
IF 11.9
Rui Cheng,Ying Wu,Bin Wang,Jinsong Zeng,Jinpeng Li,Jun Xu,Wenhua Gao,Kefu Chen
To shield significantly serious radiation pollution and reduce fire disasters, fire-retardant MXene-based electromagnetic interference (EMI) shielding nanocomposites featuring superb mechanical properties are highly desired, but remain a major challenge to prepare. Here, we propose a Janus structural engineering strategy to manufacture all-natural cellulose nanofiber (CNF)/montmorillonite (MMT)-supported MXene papers (CMMPs) using a sequential deposition followed by hot-pressing. Inspired by natural nacre, MMT nanosheets are incorporated into CNFs to construct a substrate layer with a “brick-mortar” layered structure that serves to provide mechanical properties, while the independent MXene layer ensures electrical conductivity. The resultant CMMPs exhibit extraordinary mechanical performances involving a mechanical strength of 272.7 MPa and Young's modulus of 10.8 GPa, high electrical conductivity, and a superb EMI shielding effectiveness of 56.1 dB and EMI SE/t of 19 140.8 dB cm−1. Moreover, the designed CMMPs possess impressive flame-retardant and electro-/photothermal heating features, demonstrating their reliability, safety, and versatility. Therefore, such high-performance CMMPs developed by a facile and sustainable preparation strategy possess substantial application prospects in EMI shielding, thermal management, and fire protection.
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Biochar
·
2023
·Vol. 5
·期 1
·1-15
·
IF 12.7
Miao Xiaozeng,Chen Xiliang,Wu Wenhao,Lin Daohui,Yang Kun
Nonradical oxidation based on peroxydisulfate (PDS) activation has attracted increasing attention for selective degradation of organic pollutants. Herein, topological defects were introduced into biochar (BC) via removing N atoms in N-doped BC (NBC) in an attempt to improve the nonradical catalytic performance. Compared to the pristine BC and NBC, the introduction of topological defects could achieve up to 36.6- and 8.7-times catalytic activity enhancement, respectively. More importantly, it was found that the catalytic activity was dominated by topological defects, which was verified by the significant positive correlation between the pseudo-first-order rate constants and the content of topological defects. Theoretical calculations suggested that topological defects enhanced the electron-donating ability of BC by reducing the energy gap, which made the electrons transfer to PDS molecules more easily. As a result, holes were generated after the carbon defects lost electrons, and induced a nonradical oxidation process. Benefiting from the merits of nonradical oxidation, the developed BC/PDS system showed superior performance in removing electron-rich contaminants in the presence of inorganic anions and in the actual environments. This study not only provides a potential avenue for designing efficient biochar-based catalysts, but also advances the mechanism understanding of nonradical oxidation process induced by carbon defects. Graphical Abstract
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