Frontiers of Chemical Science and Engineering

ISSN 2095-0179

ISSN 2095-0187(Online)

CN 11-5981/TQ

邮发代号 80-969

2019 Impact Factor: 3.552

   优先出版

合作单位

全文下载排行
一年内发表文章 | 两年内 | 三年内 | 全部 | 最近1个月下载排行 | 最近1年下载排行

当前位置: 一年内发表文章
Please wait a minute...
选择: 合并摘要 显示/隐藏图片
Lignin-derived dual-function red light carbon dots for hypochlorite detection and anti-counterfeiting
Yixuan Chang, Fanwei Kong, Zihao Zhu, Ziai Wang, Chunxia Chen, Xiaobai Li, Hongwei Ma
Frontiers of Chemical Science and Engineering    2023, 17 (7): 966-975.   https://doi.org/10.1007/s11705-022-2244-1
摘要   HTML   PDF (6361KB)

The efficient utilization of natural lignin, which is the main by-product of the cellulose industry, is crucial for enhancing its economic value, alleviating the environmental burden, and improving ecological security. By taking advantage of the large sp2 hybrid domain of lignin and introducing amino functional groups, new lignin-derived carbon dots (SPN-CDs) with red fluorescence were successfully synthesized. Compared with green and blue fluorescent materials, red SPN-CDs have desirable anti-interference properties of short-wave background and exhibit superior luminescence stability. The SPN-CDs obtained exhibited sensitive and distinctive visible color with fluorescence-dual responses toward hypochlorite. Considering this feature, a portable, low-cost, and sensitive fluorescence sensing paper with a low limit of detection of 0.249 μmol∙L–1 was fabricated using the SPN-CDs for hypochlorite detection. Furthermore, a new type of visible-light and fluorescence dual-channel information encryption platform was constructed. Low-concentration hypochlorite can be employed as an accessible and efficient information encryption/decryption stimulus, as well as an information “eraser”, facilitating a safe and diversified transmission and convenient decryption of information. This work opens new avenues for high-value-added applications of lignin-based fluorescent materials.

图表 | 参考文献 | 补充材料 | 相关文章 | 多维度评价
Direct pyrolysis to convert biomass to versatile 3D carbon nanotubes/mesoporous carbon architecture: conversion mechanism and electrochemical performance
Chenxi Xu, Shunli Li, Zhaohui Hou, Liming Yang, Wenbin Fu, Fujia Wang, Yafei Kuang, Haihui Zhou, Liang Chen
Frontiers of Chemical Science and Engineering    2023, 17 (6): 679-690.   https://doi.org/10.1007/s11705-022-2266-8
摘要   HTML   PDF (3661KB)

The massive conversion of resourceful biomass to carbon nanomaterials not only opens a new avenue to effective and economical disposal of biomass, but provides a possibility to produce highly valued functionalized carbon-based electrodes for energy storage and conversion systems. In this work, biomass is applied to a facile and scalable one-step pyrolysis method to prepare three-dimensional (3D) carbon nanotubes/mesoporous carbon architecture, which uses transition metal inorganic salts and melamine as initial precursors. The role of each employed component is investigated, and the electrochemical performance of the attained product is explored. Each component and precise regulation of their dosage is proven to be the key to successful conversion of biomass to the desired carbon nanomaterials. Owing to the unique 3D architecture and integration of individual merits of carbon nanotubes and mesoporous carbon, the as-synthesized carbon nanotubes/mesoporous carbon hybrid exhibits versatile application toward lithium-ion batteries and Zn-air batteries. Apparently, a significant guidance on effective conversion of biomass to functionalized carbon nanomaterials can be shown by this work.

图表 | 参考文献 | 补充材料 | 相关文章 | 多维度评价
Electrocatalytic reduction of NO to NH3 in ionic liquids by P-doped TiO2 nanotubes
Shangcong Zhang, Qian Liu, Xinyue Tang, Zhiming Zhou, Tieyan Fan, Yingmin You, Qingcheng Zhang, Shusheng Zhang, Jun Luo, Xijun Liu
Frontiers of Chemical Science and Engineering    2023, 17 (6): 726-734.   https://doi.org/10.1007/s11705-022-2274-8
摘要   HTML   PDF (3692KB)

Designing advanced and cost-effective electrocatalytic system for nitric oxide (NO) reduction reaction (NORR) is vital for sustainable NH3 production and NO removal, yet it is a challenging task. Herein, it is shown that phosphorus (P)-doped titania (TiO2) nanotubes can be adopted as highly efficient catalyst for NORR. The catalyst demonstrates impressive performance in ionic liquid (IL)-based electrolyte with a remarkable high Faradaic efficiency of 89% and NH3 yield rate of 425 μg·h−1·mgcat.−1, being close to the best-reported results. Noteworthy, the obtained performance metrics are significantly larger than those for N2 reduction reaction. It also shows good durability with negligible activity decay even after 10 cycles. Theoretical simulations reveal that the introduction of P dopants tunes the electronic structure of Ti active sites, thereby enhancing the NO adsorption and facilitating the desorption of *NH3. Moreover, the utilization of IL further suppresses the competitive hydrogen evolution reaction. This study highlights the advantage of the catalyst−electrolyte engineering strategy for producing NH3 at a high efficiency and rate.

图表 | 参考文献 | 补充材料 | 相关文章 | 多维度评价
Multiple input self-organizing-map ResNet model for optimization of petroleum refinery conversion units
Jiannan Zhu, Vladimir Mahalec, Chen Fan, Minglei Yang, Feng Qian
Frontiers of Chemical Science and Engineering    2023, 17 (6): 759-771.   https://doi.org/10.1007/s11705-022-2269-5
摘要   HTML   PDF (4284KB)

This work introduces a deep-learning network, i.e., multi-input self-organizing-map ResNet (MISR), for modeling refining units comprised of two reactors and a separation train. The model is comprised of self-organizing-map and the neural network parts. The self-organizing-map part maps the input data into multiple two-dimensional planes and sends them to the neural network part. In the neural network part, residual blocks enhance the convergence and accuracy, ensuring that the structure will not be overfitted easily. Development of the MISR model of hydrocracking unit also benefits from the utilization of prior knowledge of the importance of the input variables for predicting properties of the products. The results show that the proposed MISR structure predicts more accurately the product yields and properties than the previously introduced self-organizing-map convolutional neural network model, thus leading to more accurate optimization of the hydrocracker operation. Moreover, the MISR model has smoother error convergence than the previous model. Optimal operating conditions have been determined via multi-round-particle-swarm and differential evolution algorithms. Numerical experiments show that the MISR model is suitable for modeling nonlinear conversion units which are often encountered in refining and petrochemical plants.

图表 | 参考文献 | 补充材料 | 相关文章 | 多维度评价
Latest advances in ionic liquids promoted synthesis and application of advanced biomass materials
Ting He, Jipeng Yan, Wenzhe Xiao, Jian Sun
Frontiers of Chemical Science and Engineering    2023, 17 (7): 798-816.   https://doi.org/10.1007/s11705-023-2316-x
摘要   HTML   PDF (4351KB)

The utilization of sustainable resources provides a path to relieving the problem of dependence on fossil resources. In this context, biomass materials have become a feasible substitute for petroleum-based materials. The development of biomass materials is booming and advanced biomass materials with various functional properties are used in many fields including medicine, electrochemistry, and environmental science. In recent years, ionic liquids have been widely used in biomass pretreatments and processing owing to their “green” characteristics and adjustable physicochemical properties. Thus, the effects of ionic liquids in biomass materials generation require further study. This review summarizes the multiple roles of ionic liquids in promoting the synthesis and application of advanced biomass materials as solvents, structural components, and modifiers. Finally, a prospective approach is proposed for producing additional higher-quality possibilities between ionic liquids and advanced biomass materials.

图表 | 参考文献 | 相关文章 | 多维度评价
Highly selective and green recovery of lithium ions from lithium iron phosphate powders with ozone
Ruiqi Li, Kang Li, Wei Wang, Fan Zhang, Shichao Tian, Zhongqi Ren, Zhiyong Zhou
Frontiers of Chemical Science and Engineering    2023, 17 (6): 749-758.   https://doi.org/10.1007/s11705-022-2261-0
摘要   HTML   PDF (2572KB)

Since lithium iron phosphate cathode material does not contain high-value metals other than lithium, it is therefore necessary to strike a balance between recovery efficiency and economic benefits in the recycling of waste lithium iron phosphate cathode materials. Here, we describe a selective recovery process that can achieve economically efficient recovery and an acceptable lithium leaching yield. Adjusting the acid concentration and amount of oxidant enables selective recovery of lithium ions. Iron is retained in the leaching residue as iron phosphate, which is easy to recycle. The effects of factors such as acid concentration, acid dosage, amount of oxidant, and reaction temperature on the leaching of lithium and iron are comprehensively explored, and the mechanism of selective leaching is clarified. This process greatly reduces the cost of processing equipment and chemicals. This increases the potential industrial use of this process and enables the green and efficient recycling of waste lithium iron phosphate cathode materials in the future.

图表 | 参考文献 | 补充材料 | 相关文章 | 多维度评价
Synthesis of porous carbon from orange peel waste for effective volatile organic compounds adsorption: role of typical components
Qiaoyan Zhou, Huan Liu, Yipeng Wang, Kangxin Xiao, Guangyan Yang, Hong Yao
Frontiers of Chemical Science and Engineering    2023, 17 (7): 942-953.   https://doi.org/10.1007/s11705-022-2264-x
摘要   HTML   PDF (7255KB)

Volatile organic compounds have posed a serious threat to the environment and human health, which require urgent and effective removal. In recent years, the preparation of porous carbon from biomass waste for volatile organic compounds adsorption has attracted increasing attention as a very cost-effective and promising technology. In this study, porous carbon was synthesized from orange peel by urea-assisted hydrothermal carbonization and KOH activation. The role of typical components (cellulose, hemicellulose, and lignin) in pore development and volatile organic compounds adsorption was investigated. Among the three components, hemicellulose was the major contributor to high porosity and abundant micropores in porous carbon. Higher hemicellulose content led to more abundant –COOR, amine-N, and pyrrolic/pyridonic-N in the derived hydrochar, which were favorable for porosity formation during activation. In this case, the toluene adsorption capacity of the porous carbon improved from 382.8 to 485.3 mg·g–1. Unlike hemicellulose, cellulose reduced the >C=O, amine-N, and pyrrolic/pyridonic-N content of the hydrochar, which caused porosity deterioration and worse toluene adsorption performance. Lignin bestowed the hydrochar with slightly increased –COOR, pyrrolic/pyridonic-N, and graphitic-N, and reduced >C=O, resulting in comparatively poor porosity and more abundant micropores. In general, the obtained porous carbon possessed abundant micropores and high specific surface area, with the highest up to 2882 m2·g–1. This study can provide guidance for selecting suitable biomass waste to synthesize porous carbon with better porosity for efficient volatile organic compounds adsorption.

图表 | 参考文献 | 相关文章 | 多维度评价
Fabrication of recyclable Fe3+ chelated aminated polypropylene fiber for efficient clean-up of phosphate wastewater
Shangyuan Zhao, Fangjia Wang, Rui Zhou, Peisen Liu, Qizhong Xiong, Weifeng Zhang, Chaochun Zhang, Gang Xu, Xinxin Ye, Hongjian Gao
Frontiers of Chemical Science and Engineering    2023, 17 (7): 840-852.   https://doi.org/10.1007/s11705-022-2253-0
摘要   HTML   PDF (3671KB)

Herein, a Fe3+-loaded aminated polypropylene fiber has been reported as an efficient phosphate adsorbent. The remarkable phosphate removal ability of the fiber is due to Fe3+ immobilization, and it demonstrates a maximum adsorption capacity of 33.94 mg·P·g–1. Adsorption experiments showed that the fiber is applicable over a wide pH range from 2 to 9. Furthermore, the adsorption kinetics and isotherm data were consistent with the pseudo-second-order and Langmuir adsorption models, respectively. The adsorption equilibrium of the fiber for phosphate was reached within 60 min, indicating an efficient monolayer chemisorption process. Moreover, the adsorbent maintained prominent phosphate removal in the presence of competitive ions such as NO3 and Cl, exhibiting high selectivity. More importantly, the fiber demonstrated excellent reusability (5 times) and low adsorption limit below 0.02 mg·P·g–1. In addition, the phosphate removal efficiency of the fiber can exceed 99% under continuous flow conditions. The adsorption mechanism was studied by X-ray photoelectron spectroscopy, showing that the adsorption of phosphate on the fiber mainly depended on the chemical adsorption of the modified Fe3+. Overall, this study proves that the fiber possesses many advantages for phosphate removal, including high adsorption efficiency, lower treatment limit, good recyclability, and environmental friendliness.

图表 | 参考文献 | 补充材料 | 相关文章 | 多维度评价
Immobilization of laccase on organic–inorganic nanocomposites and its application in the removal of phenolic pollutants
Wei Zhang, Runtang Liu, Xu Yang, Binbin Nian, Yi Hu
Frontiers of Chemical Science and Engineering    2023, 17 (7): 867-879.   https://doi.org/10.1007/s11705-022-2277-5
摘要   HTML   PDF (3838KB)

Polydopamine-functionalized nanosilica was synthesized using an inexpensive and easily obtainable raw material, mild reaction conditions, and simple operation. Subsequently, a flexible spacer arm was introduced by using dialdehyde starch as a cross-linking agent to bind with laccase. A high loading amount (77.8 mg∙g‒1) and activity retention (75.5%) could be achieved under the optimum immobilization conditions. Thermodynamic parameters showed that the immobilized laccase had a lower thermal deactivation rate constant and longer half-life. The enhancement of thermodynamic parameters indicated that the immobilized laccase had better thermal stability than free laccase. The residual activity of immobilized laccase remained at about 50.0% after 30 days, which was 4.0 times that of free laccase. Immobilized laccase demonstrated excellent removal of phenolic pollutants (2,4-dichlorophenol, bisphenol A, phenol, and 4-chlorophenol) and perfect reusability with 70% removal efficiency retention for 2,4-dichlorophenol after seven cycles. These results suggested that immobilized laccase possessed great reusability, improved thermal stability, and excellent storage stability. Organic–inorganic nanomaterials have a good application prospect for laccase immobilization, and the immobilized laccase of this work may provide a practical application for the removal of phenolic pollutants.

图表 | 参考文献 | 补充材料 | 相关文章 | 多维度评价
Anthocyanins/chitosan films doped by nano zinc oxide for active and intelligent packaging: comparison of anthocyanins source from purple tomato or black wolfberry
Yana Li, Zenghui Li, Yuwen Wang, Liangbo Sun, Houchang Pei
Frontiers of Chemical Science and Engineering    2023, 17 (6): 704-715.   https://doi.org/10.1007/s11705-022-2270-z
摘要   HTML   PDF (4473KB)

The multifunctional films was prepared by blending chitosan and nano-ZnO with purple tomato anthocyanins or black wolfberry anthocyanins. The properties of films functioned by anthocyanins source and nano-ZnO content were studied. It was found purple tomato anthocyanins showed more significant color change against pH than black wolfberry anthocyanins. The nano-ZnO were widely dispersed in matrix and enhanced the compatibility of anthocyanins with chitosan. However, the anthocyanins source influenced the properties of the films more slightly than nano-ZnO addition. The tensile strength, antioxidant and antibacterial effects of the chitosan films dramatically increased after cooperated by nano-ZnO and anthocyanins, which also enhanced with increase of nano-ZnO content, whereas the elongation at break of the composite films decreased. Especially, the anthocyanin and nano-ZnO promoted the antibacterial activity of films synergistically. Composite films made from black wolfberry anthocyanins exhibited higher mechanical performance than those made from purple tomato anthocyanins but weaker antibacterial effects. The purple tomato anthocyanins/chitosan and nano-ZnO/purple tomato anthocyanins/chitosan films effectively reflected pork spoilage, changing their colors from dark green to brown, indicating the potential for applications in active and intelligent food packaging.

图表 | 参考文献 | 相关文章 | 多维度评价
Effect of noble metal nanoparticle size on C–N bond cleavage performance in hydrodenitrogenation: a study of active sites
Yi-Fan Xue, Jie Feng, Yun-Cai Song, Wen-Ying Li
Frontiers of Chemical Science and Engineering    2023, 17 (12): 1986-2000.   https://doi.org/10.1007/s11705-023-2337-5
摘要   HTML   PDF (6649KB)

Breakage of the C–N bond is a structure sensitive process, and the catalyst size significantly affects its activity. On the active metal nanoparticle scale, the role of catalyst size in C–N bond cleavage has not been clearly elucidated. So, Ru catalysts with variable nanoparticle sizes were obtained by modulating the reduction temperature, and the catalytic activity was evaluated using 1,2,3,4-tetrahydroquinoline and o-propylaniline with different C–N bond hybridization patterns as reactants. Results showed a 13 times higher reaction rate for sp3-hybridized C–N bond cleavage than sp2-hybridized C–N bond cleavage, while the reaction rate tended to increase first and then decrease as the catalyst nanoparticle size increased. Different concentrations of terrace, step, and corner sites were found in different sizes of Ru nanoparticles. The relationship between catalytic site variation and C–N bond cleavage activity was further investigated by calculating the turnover frequency values for each site. This analysis indicates that the variation of different sites on the catalyst is the intrinsic factor of the size dependence of C–N bond cleavage activity, and the step atoms are the active sites for the C–N bond cleavage. When Ru nanoparticles are smaller than 1.9 nm, they have a strong adsorption effect on the reactants, which will affect the catalytic performance of the Ru catalyst. Furthermore, these findings were also confirmed on other metallic Pd/Pt catalysts. The role of step sites in C–N bond cleavage was proposed using the density function theory calculations. The reactants have stronger adsorption energies on the step atoms, and step atoms have d-band center nearer to the Fermi level. In this case, the interaction with the reactant is stronger, which is beneficial for activating the C–N bond of the reactant.

图表 | 参考文献 | 补充材料 | 相关文章 | 多维度评价
Dialdehyde cellulose nanocrystal cross-linked chitosan foam with high adsorption capacity for removal of acid red 134
Xiuzhi Tian, Rui Yang, Chuanyin Xiong, Haibo Deng, Yonghao Ni, Xue Jiang
Frontiers of Chemical Science and Engineering    2023, 17 (7): 853-866.   https://doi.org/10.1007/s11705-022-2256-x
摘要   HTML   PDF (6178KB)

The discharge of large amounts of dye-containing wastewater seriously threats the environment. Adsorbents have been adopted to remove these dyes present in the wastewater. However, the high adsorption capacity, predominant pH-responsibility, and excellent recyclability are three challenges to the development of efficient adsorbents. The poly(acryloxyethyl trimethylammonium chloride)-graft-dialdehyde cellulose nanocrystals were synthesized in our work. Subsequently, the cationic dialdehyde cellulose nanocrystal cross-linked chitosan nanocomposite foam was fabricated via freeze-drying of the hydrogel. Under the optimal ratio of the cationic dialdehyde cellulose nanocrystal/chitosan (w/w) of 12/100, the resultant foam (Foam-12) possesses excellent absorption properties, such as high porosity, high content of active sites, strong acid resistance, and high amorphous region. Then, Foam-12 was applied as an eco-friendly adsorbent to remove acid red 134 (a representative of anionic dyes) from aqueous solutions. The maximum dye adsorption capacity of 1238.1 mg∙g‒1 is achieved under the conditions of 20 mg∙L‒1 adsorbents, 100 mg∙L‒1 dye, pH 3.5, 24 h, and 25 °C. The dominant adsorption mechanism for the anionic dye adsorption is electrostatic attraction, and Foam-12 can effectively adsorb acid red 134 at pH 2.5–5.5 and be desorbed at pH 8. Its easy recovery and good reusability are verified by the repeated acid adsorption–alkaline desorption experiments.

图表 | 参考文献 | 补充材料 | 相关文章 | 多维度评价
Enzyme@bismuth-ellagic acid: a versatile platform for enzyme immobilization with enhanced acid-base stability
Junyang Xu, Guanhua Liu, Ying He, Liya Zhou, Li Ma, Yunting Liu, Xiaobing Zheng, Jing Gao, Yanjun Jiang
Frontiers of Chemical Science and Engineering    2023, 17 (6): 784-794.   https://doi.org/10.1007/s11705-022-2278-4
摘要   HTML   PDF (4610KB)

In situ encapsulation is an effective way to synthesize enzyme@metal–organic framework biocatalysts; however, it is limited by the conditions of metal–organic framework synthesis and its acid-base stability. Herein, a biocatalytic platform with improved acid-base stability was constructed via a one-pot method using bismuth-ellagic acid as the carrier. Bismuth-ellagic acid is a green phenol-based metal–organic framework whose organic precursor is extracted from natural plants. After encapsulation, the stability, especially the acid-base stability, of amyloglucosidases@bismuth-ellagic acid was enhanced, which remained stable over a wide pH range (2–12) and achieved multiple recycling. By selecting a suitable buffer, bismuth-ellagic acid can encapsulate different types of enzymes and enable interactions between the encapsulated enzymes and cofactors, as well as between multiple enzymes. The green precursor, simple and convenient preparation process provided a versatile strategy for enzymes encapsulation.

图表 | 参考文献 | 补充材料 | 相关文章 | 多维度评价
Enhanced activation of persulfate using mesoporous silica spheres augmented Cu–Al bimetallic oxide particles for bisphenol A degradation
Fulong Wang, Liang Sun, Ziyu Zhang, Fengkai Yang, Jinlong Yang, Weijian Liu
Frontiers of Chemical Science and Engineering    2023, 17 (10): 1581-1592.   https://doi.org/10.1007/s11705-023-2327-7
摘要   HTML   PDF (5558KB)

Herein, Cu–Al bimetallic oxide was synthesized and mixed with mesoporous silica spheres via a simple hydrothermal method. The prepared sample was then analyzed and employed to activate potassium peroxydisulfate for bisphenol A removal. Based on the results of X-ray diffraction, scanning electron microscopy, and energy dispersion spectroscopy, Cu–Al bimetallic oxide was determined as CuO-Al2O3, and mesoporous silica spheres were found around the these particles. At 30 min, a bisphenol A degradation level of 90% was achieved, and it remained at over 60% after five consecutive cycles, indicating the catalyst’s superior capacity and stability. In terms of removal performance, the radical pathway (including SO4•‒, OH •, and O2•‒) and singlet oxygen (1O2) played minor roles, while electron migration between bisphenol A, potassium peroxydisulfate, and the catalyst played a dominant role. The introduction of Al2O3 promoted the formation of surface oxygen vacancies, which improved ligand complex formation between potassium peroxydisulfate and the catalyst, thereby facilitating electron migration. Furthermore, mesoporous silica spheres augment not only enhanced bisphenol A adsorption but also alleviated Cu leaching. Overall, this work is expected to provide significant support for the rational development of catalysts with high catalytic activity for persulfate activation via surface electron migration.

图表 | 参考文献 | 补充材料 | 相关文章 | 多维度评价
Catalytic conversion of biomass-derived compounds to various amino acids: status and perspectives
Benjing Xu, Jinhang Dai, Ziting Du, Fukun Li, Huan Liu, Xingxing Gu, Xingmin Wang, Ning Li, Jun Zhao
Frontiers of Chemical Science and Engineering    2023, 17 (7): 817-829.   https://doi.org/10.1007/s11705-022-2254-z
摘要   HTML   PDF (3996KB)

Amino acids are important nitrogen-containing chemicals that have a variety of applications. Currently, fermentation is the widely employed method to produce amino acids; however, the products are mostly limited to natural amino acids in the L-configuration. Catalytic synthesis is an alternative approach for the synthesis of amino acids with different types and configurations, where the use of renewable biomass-based feedstocks is highly attractive. To date, several lignocellulose and triacylglycerol-derived intermediates, typically α-keto acids and α-hydroxyl acids, have been transformed into amino acids via the amination reaction in the presence of additional nitrogen sources (i.e., NH3·H2O). Making full use of inherent nitrogen in biomass (i.e., chitin and protein) to produce amino acids avoids the use of extra nitrogen sources and meets the requirements of green chemistry, which is attracting increasing attention. In this review, we summarize different chemical-catalytic systems for the transformation of biomass to amino acids. An outlook on the challenges and opportunities for more effective production of amino acids from biomass by catalytic methods is provided.

图表 | 参考文献 | 相关文章 | 多维度评价
Overoxidized poly(3,4-ethylenedioxythiophene)-overoxidized polypyrrole composite films with enhanced electrocatalytic ability for rutin and luteolin determination
Rongqian Meng, Jianke Tang, Hong Yang, Lijun Guo, Yongbo Song, Qiaoling Li, Yulan Niu
Frontiers of Chemical Science and Engineering    2023, 17 (6): 735-748.   https://doi.org/10.1007/s11705-022-2262-z
摘要   HTML   PDF (4749KB)

In this study, a simple and effective method was proposed to improve the electrocatalytic ability of overoxidized poly(3,4-ethylenedioxythiophene)-overoxidized polypyrrole composite films modified on glassy carbon electrode for rutin and luteolin determination. The composite electrode was prepared by cyclic voltammetry copolymerization with LiClO4-water as the supporting electrolyte. The peak current of rutin and luteolin on the composite electrode gradually decreased or even disappeared with the increase in the positive potential limit. After incubation in NaOH–ethanol solution with a volume ratio of 1:1, the composite electrodes prepared at positive potential limit greater than 1.5 V exhibited enhanced differential pulse voltammetry peak currents, reduced charge transfer resistance, larger effective specific surface area and higher electron transfer rate constant. The composite electrode prepared in the potential range of 0–1.7 V showed optimal electrocatalytic performance. The X-ray photoelectron spectroscopy results indicated that the content of –SO2/–SO and –C=N– groups in the composite film increased significantly after incubation. Further, the Raman spectra and Fourier transform infrared spectra revealed that the thiophene ring structure changed from benzene-type to quinone-type, and the quinone-type pyrrole ring was formed. The electrocatalytic mechanism of the composite film was proposed based on the experimental results and further verified by Density Functional Theory calculation.

图表 | 参考文献 | 补充材料 | 相关文章 | 多维度评价
Easily-manufactured paper-based materials with high porosity for adsorption/separation applications in complex wastewater
Shan Jiang, Jianfeng Xi, Hongqi Dai, Huining Xiao, Weibing Wu
Frontiers of Chemical Science and Engineering    2023, 17 (7): 830-839.   https://doi.org/10.1007/s11705-022-2267-7
摘要   HTML   PDF (2229KB)

A multi-functional porous paper-based material was prepared from grass pulp by simple pore-forming and green cross-linking method. As a pore-forming agent, calcium citrate increased the porosity of the paper-based material from 30% to 69% while retaining the mechanical strength. The covalent cross-linking of citric acid between cellulose fibers improved both the wet strength and adsorption capacity. In addition, owing to the introduction of high-content carboxyl groups as well as the construction of hierarchical micro-nano structure, the underwater oil contact angle was up to 165°. The separation efficiency of the emulsified oil was 99.3%, and the water flux was up to 2020 L·m–2·h–1. The theoretical maximum adsorption capacities of cadmium ion, lead ion and methylene blue reached 136, 229 and 128.9 mg·g–1, respectively. The continuous purification of complex wastewater can be achieved by using paper-based materials combined with filtration technology. This work provides a simple, low cost and environmental approach for the treatment of complex wastewater containing insoluble oil, organic dyes, and heavy metal ions.

图表 | 参考文献 | 补充材料 | 相关文章 | 多维度评价
Reconstruction of Cu–ZnO catalyst by organic acid and deactivation mechanism in liquid-phase hydrogenation of dimethyl succinate to 1,4-butanediol
Fan Sun, Huijiang Huang, Wei Liu, Lu Wang, Yan Xu, Yujun Zhao
Frontiers of Chemical Science and Engineering    2023, 17 (9): 1311-1319.   https://doi.org/10.1007/s11705-022-2281-9
摘要   HTML   PDF (4801KB)

A reconstructed Cu–ZnO catalyst with improved stability was fabricated by organic acid treatment method for the liquid-phase hydrogenation of dimethyl succinate to 1,4-butanediol. According to the characterization results of the fresh Cu–ZnO and reconstructed Cu–ZnO, three different forms of ZnO were suggested to be presented on the catalysts: ZnO having strong interaction with Cu species, ZnO that weakly interacted with Cu species and isolated ZnO. The first form of ZnO was believed to be beneficial to the formation of efficient active site Cu+, while the latter two forms of ZnO took the main responsibility for the deactivation of Cu–ZnO catalysts in the liquid-phase hydrogenation of diesters. The reconstruction of the Cu–ZnO catalyst by the organic acid treatment method resulted in a new Cu–ZnO catalyst with more Cu+ and less ZnO species that leads to deactivation. Furthermore, the deactivation mechanism of Cu–ZnO catalysts in liquid-phase diester hydrogenation in continuous flow system was proposed: the deposition of the polyesters on the catalysts via transesterification catalyzed by weakly interacted ZnO and isolated ZnO leads to the deactivation. These results provided meaningful instructions for designing highly efficient Cu–Zn catalysts for similar ester hydrogenation systems.

图表 | 参考文献 | 补充材料 | 相关文章 | 多维度评价
Triboelectric nanogenerators: the beginning of blue dream
Wanli Wang, Dongfang Yang, Xiaoran Yan, Licheng Wang, Han Hu, Kai Wang
Frontiers of Chemical Science and Engineering    2023, 17 (6): 635-678.   https://doi.org/10.1007/s11705-022-2271-y
摘要   HTML   PDF (17707KB)

Wave energy is inexhaustible renewable energy. Making full use of the huge ocean wave energy resources is the dream of mankind for hundreds of years. Nowadays, the utilization of water wave energy is mainly absorbed and transformed by electromagnetic generators (EMGs) in the form of mechanical energy. However, waves usually have low frequency and uncertainty, which means low power generation efficiency for EMGs. Fortunately, in this slow current and random direction wave case, the triboelectric nanogenerator (TENG) has a relatively stable output power, which is suitable for collecting blue energy. This article summarizes the main research results of TENG in harvesting blue energy. Firstly, based on Maxwell’s displacement current, the basic principle of the nanogenerator is expounded. Then, four working modes and three applications of TENG are introduced, especially the application of TENG in blue energy. TENG currently used in blue energy harvesting is divided into four categories and discussed in detail. After TENG harvests water wave energy, it is meaningless if it cannot be used. Therefore, the modular storage of TENG energy is discussed. The output power of a single TENG unit is relatively low, which cannot meet the demand for high power. Thus, the networking strategy of large-scale TENG is further introduced. TENG’s energy comes from water waves, and each TENG’s output has great randomness, which is very unfavorable for the energy storage after large-scale TENG integration. On this basis, this paper discusses the power management methods of TENG. In addition, in order to further prove its economic and environmental advantages, the economic benefits of TENG are also evaluated. Finally, the development potential of TENG in the field of blue energy and some problems that need to be solved urgently are briefly summarized.

图表 | 参考文献 | 相关文章 | 多维度评价
Piezocatalytic performance of Fe2O3−Bi2MoO6 catalyst for dye degradation
Lili Cheng, Xiaoyao Yu, Danyao Huang, Hao Wang, Ying Wu
Frontiers of Chemical Science and Engineering    2023, 17 (6): 716-725.   https://doi.org/10.1007/s11705-022-2265-9
摘要   HTML   PDF (4465KB)

A Fe2O3−Bi2MoO6 heterojunction was synthesized via a hydrothermal method. Scanning electron microscopy, transmission electron microscopy, energy-dispersive X-ray, powder X-ray diffraction, Fourier transform infrared spectroscopy and ultra-violet−visible near-infrared spectrometry were performed to measure the structures, morphologies and optical properties of the as-prepared samples. The various factors that affected the piezocatalytic property of composite catalyst were studied. The highest rhodamine B degradation rate of 96.6% was attained on the 3% Fe2O3−Bi2MoO6 composite catalyst under 60 min of ultrasonic vibration. The good piezocatalytic activity was ascribed to the formation of a hierarchical flower-shaped microsphere structure and the heterostructure between Fe2O3 and Bi2MoO6, which effectively separated the ultrasound-induced electron–hole pairs and suppressed their recombination. Furthermore, a potential piezoelectric catalytic dye degradation mechanism of the Fe2O3−Bi2MoO6 catalyst was proposed based on the band potential and quenching effect of radical scavengers. The results demonstrated the potential of using Fe2O3−Bi2MoO6 nanocomposites in piezocatalytic applications.

图表 | 参考文献 | 补充材料 | 相关文章 | 多维度评价
Cu-doped Bi/Bi2WO6 catalysts for efficient N2 fixation by photocatalysis
Xiaojing Li, Chunran Zhao, Junfeng Wang, Jiayu Zhang, Ying Wu, Yiming He
Frontiers of Chemical Science and Engineering    2023, 17 (10): 1412-1422.   https://doi.org/10.1007/s11705-023-2312-1
摘要   HTML   PDF (6231KB)

In this paper, Cu-doped Bi2WO6 was synthesized via a solvothermal method and applied it in photocatalytic N2 immobilization. Characterization results showed the presence of a small amount of metallic Bi in the photocatalyst, indicating that the synthesized photocatalyst is actually Bi/Cu-Bi2WO6 composite. The doped Cu had a valence state of +2 and most likely substituted the position of Bi3+. The introduced Cu did not affect the metallic Bi content, but mainly influenced the energy band structure of Bi2WO6. The band gap was slightly narrowed, the conduction band was elevated, and the work function was reduced. The reduced work function improved the transfer and separation of charge carriers, which mainly caused the increased photoactivity. The optimized NH3 generation rates of Bi/Cu-Bi2WO6 reached 624 and 243 μmol·L–1·g–1·h–1 under simulated solar and visible light, and these values were approximately 2.8 and 5.9 times higher those of Bi/Bi2WO6, respectively. This research provides a method for improving the photocatalytic N2 fixation and may provide more information on the design and preparation of heteroatom-doped semiconductor photocatalysts for N2-to-NH3 conversion.

图表 | 参考文献 | 补充材料 | 相关文章 | 多维度评价
ZnFe2O4/BiVO4 Z-scheme heterojunction for efficient visible-light photocatalytic degradation of ciprofloxacin
Beibei Wang, Kejiang Qian, Weiping Yang, Wenjing An, Lan-Lan Lou, Shuangxi Liu, Kai Yu
Frontiers of Chemical Science and Engineering    2023, 17 (11): 1728-1740.   https://doi.org/10.1007/s11705-023-2322-z
摘要   HTML   PDF (5217KB)

A novel Z-scheme ZnFe2O4/BiVO4 heterojunction photocatalyst was successfully synthesized using a convenient solvothermal method and applied in the visible light photocatalytic degradation of ciprofloxacin, which is a typical antibiotic contaminant in wastewater. The heterostructure of as-synthesized catalysts was confirmed using X-ray diffraction, scanning electron microscopy, transmission electron microscopy and X-ray photoelectron spectroscopy characterizations. Compared with the single-phase counterparts, ZnFe2O4/BiVO4 demonstrated considerably enhanced photogenerated charge separation efficiencies because of the Z-scheme transfer mechanism of electrons between the composite photocatalysts. Consequently, the 30% ZnFe2O4/BiVO4 catalyst afforded a degradation rate of up to 97% of 20 mg/L ciprofloxacin under 30 min of visible light irradiation with a total organic carbon removal rate of 50%, which is an excellent activity compared with ever reported BiVO4-based catalysts. In addition, the liquid chromatography-mass spectrometry and quantitative structure-activity relationships model analyses demonstrated that the toxicity of the intermediates was lower than that of the parent ciprofloxacin. Moreover, the as-synthesized ZnFe2O4/BiVO4 heterojunctions were quite stable and could be reused at least four times. This study thus provides a promising Z-scheme heterojunction photocatalyst for the efficient removal and detoxication of antibiotic pollutants from wastewater.

图表 | 参考文献 | 补充材料 | 相关文章 | 多维度评价
Anti-biofouling strategies for implantable biosensors of continuous glucose monitoring systems
Yan Zheng, Dunyun Shi, Zheng Wang
Frontiers of Chemical Science and Engineering    2023, 17 (12): 1866-1878.   https://doi.org/10.1007/s11705-023-2340-x
摘要   HTML   PDF (4420KB)

Continuous glucose monitoring (CGM) systems play an increasingly vital role in the glycemic control of patients with diabetes mellitus. However, the immune responses triggered by the implantation of poorly biocompatible sensors have a significant impact on the accuracy and lifetime of CGM systems. In this review, research efforts over the past few years to mitigate the immune responses by enhancing the anti-biofouling ability of sensors are summarized. This review divided these works into active immune engaging strategy and passive immune escape strategy based on their respective mechanisms. In each strategy, the various biocompatible layers on the biosensor surface, such as drug-releasing membranes, hydrogels, hydrophilic membranes, anti-biofouling membranes based on zwitterionic polymers, and bio-mimicking membranes, are described in detail. This review, therefore, provides researchers working on implantable biosensors for CGM systems with vital information, which is likely to aid in the research and development of novel CGM systems with profound anti-biofouling properties.

图表 | 参考文献 | 相关文章 | 多维度评价
Nanosilver anchored alginate/poly(acrylic acid/acrylamide) double-network hydrogel composites for efficient catalytic degradation of organic dyes
Fan Zhang, Ce Gao, Shang-Ru Zhai, Qing-Da An
Frontiers of Chemical Science and Engineering    2023, 17 (7): 893-905.   https://doi.org/10.1007/s11705-022-2290-8
摘要   HTML   PDF (8854KB)

A novel alginate/poly(acrylic acid/acrylamide) double-network hydrogel composite with silver nanoparticles was successfully fabricated using the sol–gel method. The presence of carboxyl and amide groups in the network structure provided abundant active sites for complexing silver ions, facilitating the in situ reduction and confinement of silver nanoparticles. In batch experiments, the optimal silver loading was 20%, and 5 mmol·L–1 of p-nitrophenol was completely degraded in 113 s with a rate constant value of 4.057 × 10−2 s–1. In the tap water system and simulated seawater system, the degradation time of p-nitrophenol at the same concentration was 261 and 276 s, respectively, with a conversion rate above 99%. In the fixed-bed experiment, the conversion rate remained above 74% after 3 h at a flowing rate of 7 mL·min–1. After 8 cycling tests, the conversion rate remained at 98.7%. Moreover, the catalyst exhibited outstanding performance in the degradation experiment of four typical organic dyes.

图表 | 参考文献 | 补充材料 | 相关文章 | 多维度评价
Effect of different acid anions on highly efficient Ce-based catalysts for selective catalytic reduction of NO with NH3
De Fang, Guanlin Huang, Jingyi Yang, Shengxing Pan, Caihong Lv, Da Li
Frontiers of Chemical Science and Engineering    2023, 17 (10): 1399-1411.   https://doi.org/10.1007/s11705-023-2345-5
摘要   HTML   PDF (5298KB)

Three kinds of Ce-based catalysts (CePO4, CeVO4, Ce2(SO4)3) were synthesized and used for the selective catalytic reduction (SCR) of NO by NH3. NH3-SCR performances were conducted in the temperature range of 80 to 400 °C. The catalytic efficiencies of the three catalysts are as follow: CePO4 > CeVO4 > Ce2(SO4)3, which is in agreement with their abilities of NH3 adsorption capacities. The highest NO conversion rate of CePO4 could reach about 95%, and the catalyst had more than 90% NO conversion rate between 260 and 320 °C. The effect of PO43–, VO43– and SO42– on NH3-SCR performances of Ce-based catalysts was systematically investigated by the X-ray photoelectron spectroscopy analysis, NH3 temperature programmed desorption, H2 temperature programmed reduction and field emission scanning electron microscopy tests. The key factors that can enhance the SCR are the existence of Ce4+, large NH3 adsorption capacity, high and early H2 consumptions, and suitable microstructures for gas adsorption. Finally, CePO4 and CeVO4 catalysts also exhibited relatively strong tolerance of SO2, and the upward trend about 8% was detected due to the sulfation enhancement by SO2 for Ce2(SO4)3.

图表 | 参考文献 | 相关文章 | 多维度评价
NO hydrogenation to NH3 over FeCu/TiO2 catalyst with improved activity
Dan Cui, Yanqin Li, Keke Pan, Jinbao Liu, Qiang Wang, Minmin Liu, Peng Cao, Jianming Dan, Bin Dai, Feng Yu
Frontiers of Chemical Science and Engineering    2023, 17 (12): 1973-1985.   https://doi.org/10.1007/s11705-023-2364-2
摘要   HTML   PDF (6686KB)

Ammonia is crucial in industry and agriculture, but its production is hindered by environmental concerns and energy-intensive processes. Hence, developing an efficient and environmentally friendly catalyst is imperative. In this study, we employed a straightforward and efficient impregnation technique to create various Cu-doped catalysts. Notably, the optimized 10Fe-8Cu/TiO2 catalyst exhibited exceptional catalytic performance in converting NO to NH3, achieving an NO conversion rate exceeding 80% and an NH3 selectivity exceeding 98% at atmospheric pressure and 350 °C. We employed in situ diffuse reflectance Fourier transform infrared spectroscopy and conducted density functional theory calculations to investigate the intermediates and subsequent adsorption. Our findings unequivocally demonstrate that Cu doping enhances the rate-limiting hydrogenation step and lowers the energy barrier for NH3 desorption, thereby resulting in improved NO conversion and enhanced selectivity toward ammonia. This study presents a pioneering approach toward energy-efficient ammonia synthesis and recycling of nitrogen sources.

图表 | 参考文献 | 相关文章 | 多维度评价
Dual cross-linked MXene/cellulose nanofiber/nickel alginate film with improved mechanical properties and electromagnetic interference shielding performance
Pengcheng Deng, Shiyi Feng, Canhui Lu, Zehang Zhou
Frontiers of Chemical Science and Engineering    2023, 17 (10): 1460-1469.   https://doi.org/10.1007/s11705-023-2335-7
摘要   HTML   PDF (6420KB)

Electromagnetic interference pollution has raised urgent demand for the development of electromagnetic interference shielding materials. Transition metal carbides (MXenes) with excellent conductivity have shown great potential in electromagnetic interference (EMI) shielding materials, while the poor mechanical strength, flexibility, and structural stability greatly limit their further applications. Here, cellulose nanofibers and sodium alginate are incorporated with MXene nanosheets as flexible matrices to construct strong and flexible mussel-like layered MXene/Cellulose nanofiber/Sodium Alginate composite films, and nickel ions are further introduced to induce metal coordination crosslinking of alginate units. Benefited from the dual-crosslinked network structure of hydrogen bonding and metal coordination, the tensile strength, Young’s modulus, and toughness of the MXene/cellulose nanofiber/nickel alginate composite film are significantly increased. After subsequent reduction by ascorbic acid, excess nickel ions are reduced to nickel nanoparticles and uniformly dispersed within the highly conductive composite film, which further improved its hysteresis loss effect toward the incident electromagnetic waves. Consequently, the MXene/cellulose nanofiber/nickel alginate-Ni composite film presents a considerably enhanced electromagnetic interference shielding effectiveness (47.17 dB) at a very low thickness of 29 μm. This study proposes a feasible dual-crosslinking and subsequent reduction strategy to synergistically enhance the mechanical properties and electromagnetic interference shielding performance of MXene-based composite materials.

图表 | 参考文献 | 补充材料 | 相关文章 | 多维度评价
Cuprous oxide/copper oxide interpenetrated into ordered mesoporous cellulose-based carbon aerogels for efficient photocatalytic degradation of methylene blue
Rui Cui, Dongnv Jin, Gaojie Jiao, Zhendong Liu, Jiliang Ma, Runcang Sun
Frontiers of Chemical Science and Engineering    2023, 17 (7): 918-929.   https://doi.org/10.1007/s11705-023-2305-0
摘要   HTML   PDF (5224KB)

The casual discharge of dyes from industrial settings has seriously polluted global water systems. Owing to the abundance of biomass resources, preparing photocatalysts for photocatalytic degradation of dyes is significant; however, it still remains challenging. In this work, a cuprous oxide/copper oxide composite was interpenetrated onto carbon nanosheets of cellulose-based flexible carbon aerogels (Cu2O/CuO@CAx) via a simple freeze-drying-calcination method. The introduction of the carbon aerogel effectively prevents the aggregation of the cuprous oxide/copper oxide composite. In addition, Cu2O/CuO@CA0.2 has a larger specific surface area, stronger charge transfer capacity, and lower recombination rate of photogenerated carriers than copper oxide. Moreover, Cu2O/CuO@CA0.2 exhibited high photocatalytic activity in decomposing methylene blue, with a degradation rate reaching up to 99.09% in 60 min. The active oxidation species in the photocatalytic degradation process were systematically investigated by electron spin resonance characterization and poisoning experiments, among which singlet oxygen played a major role. In conclusion, this work provides an effective method for preparing photocatalysts using biomass resources in combination with different metal oxides. It also promotes the development of photocatalytic degradation of dyes.

图表 | 参考文献 | 补充材料 | 相关文章 | 多维度评价
On the monolayer dispersion behavior of Co3O4 on HZSM-5 support: designing applicable catalysts for selective catalytic reduction of nitrogen oxides by ammonia
Yufeng Yang, Lihong Zhang, Tao Song, Yixing Huang, Xianglan Xu, Junwei Xu, Xiuzhong Fang, Qing Wang, Haiming Liu, Xiang Wang
Frontiers of Chemical Science and Engineering    2023, 17 (11): 1741-1754.   https://doi.org/10.1007/s11705-023-2332-x
摘要   HTML   PDF (6953KB)

Based on monolayer dispersion theory, Co3O4/ZSM-5 catalysts with different loadings have been prepared for selective catalytic reduction of nitrogen oxides by ammonia. Co3O4 can spontaneously disperse on HZSM-5 support with a monolayer dispersion threshold of 0.061 mmol 100 m–2, equaling to a weight percentage around 4.5%. It has been revealed that the quantities of surface active oxygen (O2) and acid sites are crucial for the reaction, which can adsorb and activate NOx and NH3 reactants effectively. Below the monolayer dispersion threshold, Co3O4 is finely dispersed as sub-monolayers or monolayers and in an amorphous state, which is favorable to generate the two kinds of active sites, hence promoting the performance of ammonia selective catalytic reduction of nitrogen oxide. However, the formation of crystalline Co3O4 above the capacity is harmful to the reaction performance. 4% Co3O4/ZSM-5, the catalyst close to the monolayer dispersion capacity, possesses the most abundant active O2 species and acidic sites, thereby demonstrating the best reaction performance in all the samples. It is proposed the optimal Co3O4/ZSM-5 catalyst can be prepared by loading the capacity amount of Co3O4 onto HZSM-5 support.

图表 | 参考文献 | 补充材料 | 相关文章 | 多维度评价
Investigation of the roles of lignin in biomass-based hydrogel for efficient desalination
Qizhao Shao, Lan Sun, Xinzhou Wu, Dafeng Zheng
Frontiers of Chemical Science and Engineering    2023, 17 (7): 954-965.   https://doi.org/10.1007/s11705-023-2311-2
摘要   HTML   PDF (5596KB)

The shortage of freshwater has become a global challenge, and solar-driven interfacial evaporation for desalination is a promising way to alleviate the crisis. To develop highly efficient and environmentally friendly photothermal evaporator, the hydroxyethyl cellulose (HEC)/alkaline lignin (AL)/graphene oxide (GO) hydrogels (CLGs) with remarkable evaporative performance were successfully fabricated by a facile sol–gel method using biomass residues. The influence of AL content on the physicochemical properties of the evaporator was investigated. The increasing content of AL improves the mechanical properties, saturated water content and crosslink density of the hydrogels. The designed materials exhibit outstanding thermal insulation capacity (the thermal conductivity of less than 0.05 W·m–1·K–1) and high light absorption capacity of more than 97%. The solar evaporation efficiency and water evaporation rate of the HEC/64 wt % of AL/GO hydrogels (CLG4) achieve 92.1% and 2.55 kg·m–2·h–1 under 1 sun, respectively. The salt resistance test results reveal that the evaporation rate of the CLG4 can still reach 2.44 kg·m–2·h–1 in 3.5 wt % NaCl solution. The solar evaporation rate of the CLG4 can maintain in the range of 2.45–2.59 kg·m–2·h–1 in five cycles. This low-cost lignin-based photothermal evaporator offers a sustainable strategy for desalination.

图表 | 参考文献 | 补充材料 | 相关文章 | 多维度评价