Energy & Environmental Materials
·
2022
·Vol. 6
·期 6
·e12454
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IF 13.443
Guoqiang Zhou,Xiao Wang,Ting Wan,Chaozheng Liu,Weimin Chen,Shaohua Jiang,Jingquan Han,Youguo Yan,Meichun Li,Changtong Mei
The titanium carbide nanosheets (MXene) hold great potential for fabricating high-performance electronics due to their two-dimensional layered structure, high electrical conductivity, and versatile surface chemistry. However, assembling the small MXene nanosheets into flexible macroscopic films for wearable electronics still remains a challenge. Herein, we report the hierarchical assembling of MXene nanosheets and cellulose nanofibers into high-performance composite films via an electrostatic self-assembly strategy induced by polyethyleneimine. Benefited from the nacre-like microstructure of MXene “bricks” and cellulose nanofibers “mortars” interlocked by polyethyleneimine via hydrogen bonding and electrostatic interaction, composite films possess integrated superior flexibility, high tensile strength, and stable electrical conductivity, which are advantageous for wearable electronic applications. To provide a proof-of-concept design, a symmetric quasi-solid-state supercapacitor with the as-prepared composite film as electrode is fabricated, which exhibits a specific capacitance of 93.9 mF cm −2 at a current density of 0.1 mA cm −2 and almost constant capacitive behavior under different bending states. In addition, the composite film possesses capacities of electrothermal conversion and complete degradation in a hydrogen peroxide solution. These results demonstrate that the electrostatically self-assembled composite films hold great promise in the development of highly flexible, mechanically robust, and environmentally friendly energy storage and conversion devices.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2022
·
IF 11.357
Honglong Zhang,Zhenyu Shi,Jun Ma,Fuyi Cui,Jing Zhang,Timothy J. Strathmann
In this study, a representative redox mediator, 2,2,6,6-tetramethylpiperidine-N-oxyl (TEMPO), and its para-substituted derivatives (TEMPOs: 4-hydroxyl-TEMPO, 4-acetylamino-TEMPO, and 4-amino-TEMPO) significantly accelerated the abatement of trace organic contaminants (TrOCs, i.e., bisphenol-A (BPA), phenol, amines, and phenylbutazone) by Mn(VII) over a wide pH range of 4.0–9.0. The addition of substituents at para to the > N–O• moiety significantly influenced the degradation kinetics of TrOCs by changing the reduction potentials of TEMPOs and the corresponding oxoammonium cations (TEMPOs+); a linear relationship was observed between the substituents’ para Hammett sigma constants and the reduction potentials of TEMPOs and TEMPOs+. Pseudo-first-order reaction rate constants (kobs, min–1) of TrOC degradation by Mn(VII)/TEMPOs were also affected by the pKa of the TrOCs. Generally, the highest kobs values for individual TrOCs were observed at pH near the pKa even for TEMPOs+ with relatively pH-invariant reduction potentials. Overall, TrOC abatement kinetics were related to a combination of reactive species (Mn(VII), in situ formed MnO2, and TEMPOs+). For BPA, the relative contributions (R) of reactive species ranked as R(TEMPOs+) > R(Mn(VII)) > R(in situ formed MnO2) at pH 4.0–8.0, whereas R(Mn(VII)) > R(TEMPOs+) at pH 9.0 mainly owing to a change in BPA speciation as the pH approached the pKa1 value for BPA. The results of this study are useful for the development of heterogeneous TEMPO-based redox mediators and future applications of TEMPO-mediated oxidation systems for accelerated abatement of TrOCs in water.
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Molecular Catalysis
·
2022
·
IF 5.089
Jie Xu,Jiusheng Shi,Jingyu Wang,Lihui Zhang,Yujie Wang
Depolymerizing lignin to prepare aromatic high-value chemicals is beneficial to solve the problem of energy shortage and waste of resources. However, cleavage of lignin C C bonds still faces greater challenges due to the recalcitrance of C C bonds in lignin. Photocatalysis is considered to be a promising way to break lignin C C bonds under mild conditions. Here, the micellar aqueous medium (SDS) composed of sodium lauryl sulfonate and water was prepared. 1, 2-Diphenylethanol (lignin model compound, Dpol) and dioxanesolv poplar lignin can be well dispersed in SDS-8 (mass fraction of 0.08% for sodium lauryl sulfate). Photocatalyst g-C 3 N 4 can efficiently break the lignin C C bonds in SDS-8 and very high photocatalytic efficiency can be obtained. A small amount of acetic acid can further improve photocatalytic efficiency. The main products produced by photocatalytic breaking lignin C C bonds are benzaldehyde and benzoic acid. The mechanism of photocatalytic cleavage of lignin C C bonds mainly follows a photogenerated electron-hole coupled redox mechanism. Thereinto, the hydrogen provided by SDS-8 has powerfully promoted photocatalytic efficiency. Our work provides a new direction for photocatalytic cleavage of lignin C C bonds into aromatic high-value chemicals.
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CATALYSIS LETTERS
·
2022
·Vol. 153
·期 4
·1109-1119
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IF 2.936
Ren Yanrong,Pu Hongzheng,Zeng Hanlu,Deng Chaofang,Yin Fengling,Wu Ya,Yang Dingfeng,Li Yuanyuan
Modulating the band edge position of a photocatalyst is important in photocatalysis. In this study, a more positive valence band position was realized by doping Sb in Li 2 SnO 3 . The downshifted valence band position was mainly attributed to the relatively low Sb energy level resulting from its higher electronegativity. Such band structure modification resulted in a stronger photo-oxidative capability for photogenerated holes (h + ), leading to an enhanced photodegradation rate toward tetracycline (TC) solution. For Li 2 Sn 0.9 Sb 0.1 O 3 , the efficiency reached 74% within 30 min, which was approximately 2.5 times that of Li 2 SnO 3 . Radical trapping experiments showed that h + played the dominant role in the photodegradation process. Finally, the photodegradation pathway was analyzed using liquid chromatography–mass spectrometry (LC–MS). These results might provide important insight for designing photocatalysts with high efficiency through band structure modification. Graphical Abstract
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ACS Sustainable Chemistry & Engineering
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2022
·
IF 9.224
Jiansu Ran,Ruixue YangCheng,Yuntong Cui,Jianjian Wang
Selective and efficient low-temperature hydrodeoxygenation (HDO) of lignin derivatives in water for the production of valuable biofuel and chemicals is still challenging. Herein, we reported biomass carbon-supported ultrafine Pd nanoparticles as highly active and stable catalysts for low-temperature HDO of vanillin (a typical lignin-derived compound) to 2-methoxy-4-methylphenol (MMP). We found that the abundant carboxyl groups on the resultant catalyst greatly accelerated the conversion of the generated intermediate (vanillyl alcohol, VAL), and then, the synergistic catalysis between carboxyl groups and Pd nanoparticles promoted the efficient production MMP through a free-radical pathway. Other lignin derivatives with different functional groups were also efficiently converted to the corresponding products over the prepared catalyst. This work may provide a new idea for designing a biomass-derived catalyst for efficient transformation of various lignin derivatives to produce value-added biofuels and chemicals.
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Chemistry-An Asian Journal
·
2022
·Vol. 17
·期 15
·e202200309
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IF 4.839
Haoran Zhang,Yachong Liu,Rong Jin,Sanyang Han,Qianqian Su
Graphical A novel excitation energy lock-in approach is developed to boost ultraviolet upconversion emission in a new class of multilayer core-shell nanoparticles with a gadolinium-rich core domain and optically inert NaYF 4 interlayer. These UV-emitting upconversion nanoparticles are promising for NIR-responsive reactive oxygen species generation. Multiphoton upconversion that can convert near-infrared irradiation into ultraviolet emission offers many unique opportunities for photocatalysis and phototherapy. However, the high-lying excited states of lanthanide emitters are often quenched by the interior lattice defects and deleterious interactions among different lanthanides, resulting in weak ultraviolet emission. Here, we describe a novel excitation energy lock-in approach to boost ultraviolet upconversion emission in a new class of multilayer core-shell nanoparticles with a gadolinium-rich core domain. Remarkably, we observe more than 70-fold enhancements in Gd 3+ emission from the designed nanoparticles compared with the conventional nanoparticles. Our mechanistic investigation reveals that the combination of energy migration over the core domain and optically inert NaYF 4 interlayer can effectively confine the excitation energy and thus lead to intense multiphoton ultraviolet emission in upconversion nanostructures. We further achieve a 35.6% increase in photocatalytic reactivity and 26.5% in reactive oxygen species production yield in ZnO-coated upconversion nanocomposites under 808-nm excitation. This study provides a new insight to energy transfer mechanism in lanthanide-doped nanoparticles and offers an exciting avenue for exploring novel near-infrared photocatalysts.
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JOURNAL OF HAZARDOUS MATERIALS
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2022
·
IF 14.224
Yang Liu,Fenxian Cun,Dongqi Tian,Peng Zhou,Yue Yuan,Zhaokun Xiong,Chuanshu He,Ye Du,Zhicheng Pan,Bo Lai
Sodium bismuthate dihydrate (NaBiO 3 .2 H 2 O, NBH) nanosheets were successfully prepared in this study using the persulfate oil bath oxidation method. Benefited from the unique layered structure of NBH, the Fe(III) as a variable valence metal ion was explored for enhancing NBH activation of peroxymonosulfate (PMS) to degrade levofloxacin (LVF) in the visible-light catalytic system. Based on results of the reactive oxygen species (ROS) quenching experiments and electron paramagnetic resonance (EPR) analysis, singlet oxygen ( 1 O 2 ) and superoxide radical (O 2 ·- ) were identified as the main ROS. The morphology, chemical structure, and optical properties of NBH were analyzed using various characterization methods. It was confirmed that Fe(III) embedded in the NBH via the ion exchange with Na, resulting in lattice oxygen vacancies on the surface of the NBH, after the formation of oxygen defect sites, reacts with PMS in the solution to produce active oxygen species with oxidizing efficiency. This study expands the technological application of NBH in the catalytic oxidation of variable valence metals, which are essential for the removal of fluoroquinolone antibiotics.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Sheng-Nan Zhuo,Hong-Yu Ren,Guang-Li Cao,Guo-Jun Xie,De-Feng Xing,Nan-Qi Ren,Bing-Feng Liu
In this study, an encapsulated nanoscale zero-valent iron biochar (BC-Fe 0 ) derived from waste lignocellulose rice straw (RS) was synthesized. BC-Fe 0 has excellent properties, including long-term stability, a large specific surface area, many micropore structures, active defects active and oxygen-containing groups. The material was first used to activate persulfate (PDS), showing a highly efficient catalysis for acetaminophen (ACT) degradation. The removal efficiency of ACT within 20 min reached 100%, and the degradation rate constant ( k obs ) reached 0.37475 min −1 at the ACT concentration of 10 mg/L, BC-Fe 0 of 0.5 g/L, temperature of 298 K. EPR demonstrated that ·OH, SO 4 −· , ·O 2 − and 1 O 2 occurred during the reaction process, and ·O 2 − , 1 O 2 and electron transfer played major roles in PDS/BC-Fe 0 system. Fe 0 nanoparticles promoted the activation of PDS to generate ·O 2 − , which induced a series of other reactive oxygen species (ROS) to attack ACT. C = O might also contribute to the production of 1 O 2 . In addition, graphitic carbon, C–O, defects and micropores on BC-Fe 0 together created a rich electron environment, which is conducive to the redox reaction between ACT and ROS. Satisfyingly, BC-Fe 0 not only had a high catalytic activation capacity, but also exhibited a desirable durability and recyclability. The development of BC-Fe 0 catalysts and the study of PDS activation for organic pollutant degradation are significant to biomass conversion and advanced oxidation processes in environmental remediation.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2022
·
IF 9.136
Aihua Qiao,Renliang Huang,Anastasia Penkova,Wei Qi,Zhimin He,Rongxin Su
Nanocellulose-based aerogels have gradually attracted attention in the field of oil/water separation owing to their light weight, excellent absorption properties, and environmental-friendliness. Herein, we report a facile and easily scalable method for fabricating superhydrophobic, elastic and anisotropic cellulose nanofiber (CNF) aerogels. Directional freeze-drying, soaking in polydimethylsiloxane (PDMS) solution and heat treatment were applied to obtain anisotropic and aligned CNF-PDMS aerogel sheets and blocks with superhydrophobicity and high elasticity. The CNF-PDMS aerogel sheets could realize continuous oil/water separation by filtration with a flux up to 2800 L·m −2 ·h −1 and a separation efficiency of 99.9%. The CNF-PDMS aerogel blocks could separate the oil/water mixture by the absorption–extrusion, and could also be applied in real-time continuous oil/water separation by vacuum suction with a flux as high as 145 L·h −1 ·g −1 and a separation efficiency of 99.9%. Overall, our anisotropic CNF-PDMS aerogels are the promising materials for low-cost rapid oil/water separation in multiple separation pathways.
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Biomaterials Advances
·
2022
·
IF 0
Tianshu Chu,Chun Dai,Xiang Li,Lei Gao,Hongyan Yin,Jianjun Ge
Following vein grafting, the vein must adapt to arterial hemodynamics, which can lead to intimal hyperplasia (IH) and restenosis. Moreover, endothelial-to-mesenchymal transition (EndMT) components are highly associated with IH. Therefore, in this study, we aimed to design an extravascular film loaded with rapamycin (extravascular rapamycin film [ERF]) to limit vein graft stenosis. The film exhibited stable physicochemical properties as well as in vivo and in vitro biocompatibility. In vivo , the film inhibited the EndMT by activating the autophagy pathway. Moreover, rapamycin enhanced this biological effect. Collectively, these findings highlighted the applicability of ERF as a new therapeutic target for preventing vein graft restenosis.
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FOOD HYDROCOLLOIDS
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2022
·
IF 11.504
Chan Lei,Yunxiao Xie,Yilan Wu,Yan Li,Bin Li,Ying Pei,Shilin Liu
The stabilization of food-grade water in water (W/W) emulsions, as a potential candidate for encapsulating water-soluble functional components, remain a significant challenge in food science research. The main purpose of the work was to find a suitable particle for the preparation of the novel W/W emulsion. This system was composed of two immiscible water-soluble biopolymers (dextran and maltodextrin), and stabilized by using bacterial cellulose (BC) nanofibrils. The BC-stabilized W/W emulsions were successfully fabricated with the 20 wt% dextran (DEX) and the 10 wt% maltodextrin (MAL). There was no significant change in the droplet size of the emulsion with increasing BC surface charge from 0.41 mmol/g to 1.41 mmol/g dry cellulose. Meanwhile, the apparent viscosity, storage modulus ( G′ ) and loss modulus ( G″ ) of the emulsions were decreased with increasing BC surface charge. The stabilization mechanism of the W/W emulsion was due to the formation of viscoelastic network structure by BC nanofibrils. When the BC content increased from 0.04 wt% to 0.16 wt%, the emulsion droplet size was decreased from 3.78 ± 0.79 μm to 2.01 ± 0.40 μm. Furthermore, the obtained W/W emulsion did not demulsify within 7 d, it had better stability than that of the reported W/W emulsion. Moreover, the BC-stabilized emulsion was insensitive to the change of ionic strength concentration (0–200 mM) and pH (3–11). In brief, it was the first report to use BC nanofibrils to stabilize the W/W emulsion, which enriched the type of W/W emulsion.
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CARBOHYDRATE POLYMERS
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2022
·
IF 10.723
Wei Fan,Jiaqi Li,Lihong Wei,Yan Xu
Carboxylated cellulose nanocrystals prepared by TEMPO-mediated oxidation exhibit a distinct ability to form nematic order, however, their ability to form chiral nematic films remains relatively unexplored. In this study, bleached cotton pulp hydrolyzed with hydrochloric acid and oxidized by TEMPO-mediated oxidation produce carboxylated cellulose nanocrystals with different aspect ratios 33.1, 32.8, 30.9, 29.0 and 28.9, and surface charge densities 0.16, 0.56, 1.00, 1.25, and 1.42 e·nm −2 . By tuning the aspect ratio and surface charge density, the optimal carboxylated cellulose nanocrystals producing left-handed chiral nematic films by evaporation-induced self-assembly are obtained. The left-handed chiral nematic films enable selective reflection of left-handed circularly polarized light with the peak wavelength tunable from the visible to the near-infrared regime by modifying the characteristics of nanorods and suspensions. Such carboxylated cellulose nanocrystal films transform spontaneous luminescence to right-handed circularly polarized luminescence with the peak luminescence dissymmetry factor of −0.51.
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