Nature Communications
·
2021
·Vol. 12
·期 1
·1-11
·
IF 14.919
Wang Jinling,Dai Xingchao,Wang Hualin,Liu Honglai,Rabeah Jabor,Brückner Angelika,Shi Feng,Gong Ming,Yang Xuejing
Diminishing fossil fuel resources and calls for sustainability are driving the urgent need for efficient valorization of renewable resources with high atom efficiency. Inspired from the natural goethite mineral with Mn paragenesis, we develop cost-effective MnO 2 /goethite catalysts for the efficient valorization of dihydroxyacetone, an important biomass-based platform molecule, into value-added glycolic acid and formic acid with 83.2% and 93.4% yields. The DHA substrates first undergo C−C cleavage to selectively form glycolic acid and hydroxymethyl (·CH 2 OH) radicals, which are further oxidized into formic acid. The kinetic and isotopic labeling experiments reveal that the catalase-like activity of MnO 2 turns the oxidative radicals into oxygen, which then switches towards a hydroxymethyl peroxide (HMOO) pathway for formic acid generation and prevents formic acid over-oxidation. This nature-inspired catalyst design not only significantly improves the carbon efficiency to 86.6%, but also enhances the oxygen atom utilization efficiency from 11.2% to 46.6%, indicating a promising biomass valorization process.
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高影响因子
CELLULOSE
·
2021
·Vol. 29
·期 2
·941-952
·
IF 5.044
Hu Tao,Hu Xiaoli,Tang Cheng,Liu Dan
This paper describes the synthesis of a novel chelating material derived from cellulose, and its heavy metal ion adsorption properties from aqueous solution. The first section of this paper reports the chemical grafting of cellulose, that amino acetic acid groups were grafted onto the cellulose by in situ synthesis, a novel yet unreported modified cellulose derivative N,N-(dicarboxymethylaminoethyl, carboxymethyl)aminoethylamine carboxymethyl cellulose amide was synthesized. This obtained adsorbent was characterized by elemental analysis, infrared spectroscopy (IR) and Solid State Nuclear Magnetic Resonance (SSNMR) 13 C NMR spectroscopy. In the second section, the adsorption of Cu 2+ and Pb 2+ from single metal ion aqueous solutions onto this adsorbent were evaluated and analyzed by the Freundlich and Langmuir models. Further more, adsorption capacity for Ba 2+ , Mg 2+ , Mn 2+ , Co 2+ , Zn 2+ , Pb 2+ , Ni 2+ and Cu 2+ , and the competitive adsorption of this adsorbent between ions were also evaluated by ICP spectroscopy. The results indicated that this modified cellulose exhibited adsorption properties similar to those of EDTA, and showed good adsorption capacity for a wide range of metal ions.
Graphical abstract
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CELLULOSE
·
2021
·Vol. 29
·期 1
·223-232
·
IF 5.044
Huang Wei,Li Hongqiang,Lai Xuejun,Chen Zhonghua,Zheng Longzhu,Zhong Yu,Zeng Xingrong
With the increasing importance of electronic devices in modern industry, considerable efforts have been devoted to solving the problem that the electronic devices fail to work normally in a cold environment. Herein, we designed and fabricated a graphene wrapped wood-based phase change composite with electro-thermal conversion and energy storage capabilities by delignification of natural wood, coverage and reduction of graphene oxide (GO), impregnation of 1-tetradecanol (TD) and package of epoxy resin. The phase change composite exhibited large latent heat of fusion (218.5 J/g), excellent shape stability with high TD packing content of 88.4% and favorable reliability even after 50 heating–cooling cycles. More importantly, the Joule heat conversed by the rGO layer under voltage was able to quickly transfer to the surrounded TD, leading to the increase of the overall temperature of the composite and the efficient storage of energy. The findings conceivably stand out a sustainable strategy to fabricate an electrically driven wood-based phase change composite for preheating and heat preservation of electronics.
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JOURNAL OF SOILS AND SEDIMENTS
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2021
·Vol. 22
·期 3
·797-808
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IF 3.308
Ma Li,Yao Lei,Li Yuhong
Purpose Bioremediation experiments of polycyclic aromatic hydrocarbon (PAHs) using ryegrass ( Lolium perenne ), a turfgrass in urban landscapes, were carried out aiming to explore the ryegrass-assisted degradation in an actual PAH-contaminated urban soil and the phytotransformation pathways of PAHs within plants. Methods Dynamics of plant-assisted degradation of 15 PAHs in pot soils were recorded over 100-day cultivation, and at the end, the accumulation of PAHs in ryegrass was investigated. Ryegrass with phenanthrene exposure was cultured hydroponically to investigate the phytotransformation intermediates using gas chromatography–mass spectrometry and ultra-performance liquid chromatography coupled to high-resolution mass spectrometry. Results Overall, dissipation of PAHs in soils exhibited an initial fast and subsequent slow degradation pattern. Eventually, on average, 55.7% and 47.1% of \(\sum {PAHs}\) were removed in the planted and unplanted soils, respectively, with the high-molecular-weight PAHs highly eliminated particularly. Plant growth resulted in 4.8–11.1% more \(\sum {PAHs}\) removed from soil compared to the plant-free controls. The PAHs all exhibited the bioconcentration and translocation factors below 1. The mass balance calculation showed that plant uptake accounted for < 1% of the dissipation increase while plant-promoted microbial biodegradation made the dominant contribution. A total of 7 metabolites were tentatively identified based on which possible transformation pathways were proposed. Conclusion The results indicated that ryegrass may act as a metabolic sink for aqueous PAHs while microbes play a dominant role in soil PAH dissipation via biodegradation. The results may pave the path for a scientific, safe, and effective implementation of landscape configuration to ameliorate urban soil pollution.
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Journal of Central South University
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2021
·Vol. 28
·期 9
·2701-2710
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IF 1.716
Zhang Du-chao,Liu Ruo-lin,Wang Hao,Liu Wei-feng,Yang Tian-zu,Chen Lin
To recover zinc from electric arc furnace (EAF) dust, a process of primary normal pressure leaching and secondary alkaline pressure leaching is proposed. First, under the alkaline pressure leaching system, the experiment of pure zinc ferrite being reduced by iron powder was carried out. Under the optimal reduction conditions (i.e., temperature of 260 °C, NaOH concentration of 6 mol/L, liquid-to-solid ratio of 50 mL/g, and a 5-fold excess of iron powder), 89% of zinc was extracted. The iron in the reduced residue exists as a magnetite phase. Subsequently, the normal pressure leaching experiment was carried out with EAF dust as raw material, and 66% zinc was leached. The main phase of zinc in normal leaching residue was determined to be zinc ferrite. Then, the normal leaching residue was reduced by iron powder under the alkaline pressure leaching system, and 66.5% of zinc was extracted. After the two-stage leaching process, the leaching rate of zinc in EAF dust can achieve 88.7%. The alkaline pressure leaching solution can be returned as the normal pressure leaching solution, and the magnetite in the alkaline pressure leaching residue can be recovered by magnetic separation.
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APPLIED BIOCHEMISTRY AND BIOTECHNOLOGY
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2021
·Vol. 194
·期 3
·1290-1302
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IF 2.926
Ji Yingrui,Xu Long,Xu Qingqing,Liu Xuan,Lin Sen,Liao Sentai,Wang Weifei,Lan Dongming
More and more industries demand environmental friendliness. Silkworm pupae oil (SPO), extracted from the desilked silkworm pupae, can serve as a promising substrate alternative to use in plasticization. This study aimed to prepare epoxidized silkworm pupae oil (ESPO) and investigate their effects on the thermal stability and plasticization of polyvinyl chloride (PVC) films. A chemo-enzymatic method of ESPO was developed in the presence of Lipase SMG1-F278N and H 2 O 2 in natural deep eutectic solvents (DESs). Lipase SMG1-F278N could initiate the epoxidation reaction effectively at room temperature with a negligible loss of activities 10 batches. A maximum oxirane value of 6.94% was obtained. The formation of oxirane ring in ESPO was confirmed by FTIR and 13 C NMR spectra. Moreover, ESPO showed a better thermal stability and lower freezing point than epoxidized soybean oil (ESO). It was demonstrated that ESPO had a good frost resistance. In addition, ESPO showed a significantly improved plasticizing effect on flexible polyvinyl chloride (PVC). Compared with ESO, ESPO could increase the tensile elongation at break effectively. A significantly lower migration rate of plasticizer was observed in PVC plasticized with ESPO.
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Biomass Conversion and Biorefinery
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2021
·Vol. 13
·期 14
·12581-12590
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IF 4.987
Liu Ruixia,Ding Tingting,Deng Pingping,Yan Xiaofan,Xiong Fuquan,Chen Jienan,Wu Zhiping
In order to improve the reaction activity of lignin and increase its utilization rate. Lignin extracted from poplar wood powder by deep eutectic solvent was degraded with hydrogen peroxide (H 2 O 2 ) and sodium hydroxide (NaOH) to obtain degraded deep eutectic solvent lignin (DES-lignin). The structures of DES-lignin and degraded DES-lignin were characterized by gel permeation chromatography (GPC), elemental analysis (EA), Fourier transform infrared spectroscopy (FT-IR), two-dimensional nuclear magnetic resonance spectroscopy (2D-HSQC NMR), and thermogravimetric analysis (TGA). The results indicated that the phenolic hydroxyl group of degraded DES-lignin increased by 39.62% and M w and M n decreased by 49.12% and 47.83%, respectively. C content decreased by 1.13%. The relative strength and S/G increased by 25.76% and 13.5%, respectively. The polymerization degree, β-O-4 linkages, and β-β linkages were decreased by 10.82%, 4.8%, and 4.2%, respectively. The residual residue increased by 8.3% at 800 °C. It showed that degraded DES-lignin had the advantages of strong activity, more reaction sites, narrow molecular weight distribution, less condensation structure, and thermal stability, which was more conducive to the high-value utilization of lignin.
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Journal of Bionic Engineering
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2021
·Vol. 19
·期 1
·188-196
·
IF 2.682
Wang Qiaoying,Cai Jiali,Xu Zihan,Huang Shihui,Zhou Ruiping,Wang Zhiyong
Chemotherapy is still a kind of important strategy for cancer treatment, but lacking effective delivery system limits the therapeutic outcome. Owing to the excellent biocompatibility, albumin has been employed as drug vehicle; however, it has to face complicated synthesis procedures and still needs an effective technology for the drug delivery evaluation. In this study, a facile method was utilized to prepare a protein-based theranostic system through the self-assembly of albumins with small molecules and drugs; furthermore, the paramagnetic divalent manganese ions were conjugated on the surface of the nanocomposite through a coordination bond and carried out the magnetic resonance imaging. This nanosystem with a stable structure exhibited about 80 nanometer size and 7.7 [Mn] mM -1 S -1 T 1 relaxivity; moreover, the pH-sensitive drug releasing property and the imaging function empower it with theranostic cancer therapy. Moreover, the nanocomposites effectively entered into the cancer cells and showed superior antitumor ability; and these treated cells exhibited significant T 1 signal. These results suggested that the albumin-based nanosystem is a novel chemotherapy drug delivery vehicle and a promising candidate for magnetic resonance imaging.
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ADVANCES IN ATMOSPHERIC SCIENCES
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2021
·Vol. 38
·期 7
·1238-1251
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IF 3.158
Zhang Hailiang,Xu Yongfu,Jia Long,Xu Min
Acetaldehyde is one of the important VOC species of O 3 precursors in the atmospheric environment. The influences of relative humidity (RH) and initial VOC/NO x ratio ( R CN ) on the formation of O 3 are studied in smog chamber experiments, and the MCM v3.3.1 mechanism of acetaldehyde is modified based on the experimental results. In low-RH conditions (RH = 11.6%±1.1%), the O 3 concentration at 6 h increases first and then decreases with the increase of R CN , and the R CN at the inflection point of O 3 concentrations is 3.2. In high-RH experiments (RH = 78.8%±1.0%), variation of the O 3 concentration at 6 h with R CN is similar to that in low-RH experiments, but the R CN at the inflection point is 2.8. RH has no significant effect on the O 3 concentrations under low R CN (< 3), whereas it has a negative effect under high R CN (> 3). Compared with the experimental results, original MCM v3.3.1 greatly underestimates the O 3 concentrations. Addition of both the photolysis process of peroxyacetyl nitrate and the photolysis process of HNO 3 on the reactor surface into the original MCM can reduce the difference between the simulated O 3 concentrations and the experimental results at 6 h from 24%−35% and 17%−49% to 6%−26% and 10%−42% under low- and high-RH conditions, respectively. The maximum incremental reactivity (MIR) of acetaldehyde simulated with the modified MCM is 4.0 ppb ppb −1 without considering the effect of other VOCs.
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ADVANCES IN ATMOSPHERIC SCIENCES
·
2021
·Vol. 38
·期 7
·1252-1263
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IF 3.158
Wang Yu,Zhao Jie,Liu Huihui,Li Yuan,Dong Wenbo,Wu Yanlin
Iron and oxalic acids are widely distributed in the atmosphere and easily form ferric oxalate complex (Fe(III)-Ox). The tropospheric aqueous-phase could provide a medium to enable the photo-Fenton reaction with Fe(III)-Ox under solar irradiation. Although the photolysis mechanisms of Fe(III)-Ox have been investigated extensively, information about the oxidation of volatile organic compounds (VOC), specifically the potential for Secondary Organic Aerosol (SOA) formation in the Fe(III)-Ox system, is lacking. In this study, a ubiquitous VOC methacrolein (MACR) is chosen as a model VOC, and the oxidation of MACR with Fe(III)-Ox is investigated under typical atmospheric water conditions. The effects of oxalate concentration, Fe(III) concentration, MACR concentration, and pH on the oxidation of MACR are studied in detail. Results show that the oxidation rate of MACR greatly accelerates in the presence of oxalate when compared with only Fe(III). The oxidation rate of MACR also accelerates with increasing concentration of oxalate. The effect of Fe(III) is found to be more complicated. The oxidation rate of MACR first increases and then decreases with increasing Fe(III) concentration. The oxidation rate of MACR increases monotonically with decreasing pH in the common atmospheric water pH range or with decreasing MACR concentration. The production of ferrous and hydrogen peroxide, pH, and aqueous absorbance are monitored throughout the reaction process. The quenching experiments verify that · OH and \(O_2^{\bar .}\) are both responsible for the oxidation of MACR. MACR is found to rapidly oxidize into small organic acids with higher boiling points and oligomers with higher molecular weight, which contributes to the yield of SOA. These results suggest that Fe(III)-Ox plays an important role in atmospheric oxidation.
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高影响因子
CELLULOSE
·
2021
·Vol. 28
·期 11
·6953-6966
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IF 5.044
Liu Yingying,Fan Qing,Huo Ying,Li Mei,Liu Hongbin,Li Bin
Intelligent hydrogels with multifunctions including biocompatibility, good mechanical property, photothermal property, sustained drug delivery ability, and antibacterial property are urgently needed in the biomaterial fields. Herein, mesoporous polydopamine (MPDA) nanoparticles were wrapped by polyethyleneimine-modified cellulose nanocrystals (PCNC) and then physically crosslinked in cellulose nanofibrils (CNFs) hydrogel, obtaining a novel MPDA@PCNC/CNFs composite hydrogel with a double packing structure for controlled drug release. Tetracycline hydrochloride (TH) was selected as the drug model and it was loaded on MPDA nanoparticles. PCNC was warped outside surface of MPDA nanoparticle, which was used to prolong drug release time and reinforce the mechanical strength of MPDA@PCNC/CNFs composite hydrogel. Results presented that the mechanical strength of MPDA@PCNC/CNFs composite hydrogel was 3.5 times stronger than that of pure CNFs hydrogel. Burst release was reduced and drug delivery time of MPDA@PCNC/CNFs composite hydrogel was 3 times and 1.25 times longer than that of CNFs hydrogel and polydopamine/CNFs composite hydrogel, respectively. The drug delivery behavior of the MPDA@PCNC/CNFs composite hydrogel could be controlled by near infrared (NIR) light irradiation and acidic pH condition. Korsmeyer-Peppas model could be used to describe the drug delivery kinetics of the MPDA@PCNC/CNFs composite hydrogel. Fick’s diffusion was the main drug delivery mechanism. Moreover, MPDA@PCNC/CNFs composite hydrogel was found to have good biocompatibility. The as-fabricated composite hydrogel with a double encapsulation structure and unique pH and NIR responsiveness can be applied as a promising drug release carrier, and it may also has potential applications in the fields of physical and chemical therapies.
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ANALYTICAL AND BIOANALYTICAL CHEMISTRY
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2021
·Vol. 413
·期 16
·4267-4275
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IF 4.157
Wang Pengxiang,Wang Tianlin,Wang Xinke,Zhao Minyang,Zhou Xiao,Wang Shuo,Liu Yaqing
In our investigation, a smartphone-integrated ratiometric fluorescent sensing system with lanthanide-based infinite coordination polymers (Ce-GMP-DPA@Tb-DPA) as signal probe has been successfully constructed for sensitive and portable detection of water in organic solvents. The Ce-GMP-DPA presents blue luminescence which is suppressed once the Tb-DPA is integrated to form the complex of Ce-GMP-DPA@Tb-DPA. Due to the energy transfer from Ce to Tb, the as-formed Ce-GMP-DPA@Tb-DPA exhibits green fluorescence of Tb-DPA. The presence of water can decompose the Tb-DPA, which blocks energy transfer from Ce to Tb, resulting in the decrease of green emission of Tb-DPA and the recovery of blue emission of Ce-GMP-DPA. Therefore, a ratiometric fluorescence assay is established for quantitative water detection within a wide linear range from 0.2 to 90.0% in ethanol. The limit of detection (LOD) reaches as low as 0.16% in ethanol, 0.62% in THF, and 0.0076% in acetonitrile, respectively. Furthermore, a smartphone installed with Color Picker APP as signal reader and analyzer is designed to integrate with the detection assay. With white spirit as real sample, water can be on-site detected with high accuracy (RSD < 2.81%). The developed platform presents great potential for portable water detection in practical application with merits of low cost, easy carry, and simple operation.
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