ACS Catalysis
·
2023
·
IF 12.9
Yanfen Fang,Dengyu Ying,Huibin Niu,Yan Xu,Shaobin Wang,Ran Duan,Huaiyong Zhu,Chaoyuan Deng,Chuncheng Chen,Yingping Huang
Although metal-rich biochar (M-BC) is widely used in soil remediation and pollution control, the activation mechanism of molecular oxygen (O2) by M-BC still needs to be clarified due to the low metal loading. In this study, we enhanced the manganese content of low-temperature manganese-rich biochar (Mn-BC) by treating it with hydrogen peroxide (H2O2), resulting in the formation of MnBC-Hx (where x represents the volume of H2O2 used in mL). MnBC-H5 was particularly effective in activating O2, leading to the successful degradation of phenol and dyes. Characterizations showed that the MnII in the outer layer of MnC2O4·2H2O nanoparticles evenly dispersed over Mn-BC was oxidized to MnIII by H2O2. This process was accompanied by the removal of coordinated H2O, resulting in the formation of MnIIIC2O4 on MnBC-H5. Under visible light irradiation, MnIII can bind to O2 to form MnIIIOOH species, which facilitates the transfer of charges and generates superoxide radicals (·O2–) that effectively degrade organics. Notably, MnIII of MnBC-H5 remains stable after the organic degradation reaction. This study will not only provide a theoretical basis for developing environmentally friendly biochar-based catalysts but also promote the study of the environmental effects of biochar.
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BIOCHEMICAL PHARMACOLOGY
·
2023
·
IF 5.8
Lujun Yin,Yingjie Wang,Shiliang Xiang,Kaizhong Xu,Bo Wang,Ai-Qun Jia
Burkholderia cenocepacia is an opportunistic respiratory pathogen of particular relevance to patients with cystic fibrosis (CF), primarily regulating its biological functions and virulence factors through two quorum sensing (QS) systems (CepI/R and CciI/R). The highly persistent incidence of multidrug resistant Burkholderia cenocepacia poses a global threat to public health. In this study, we investigated the effects of tyramine , one biogenic amine , on the QS systems of Burkholderia cenocepacia . Genetic and biochemical analyses revealed that tyramine inhibited the production of N -hexanoyl-homoserine (AHL) signaling molecules (C8-HSL and C6-HSL) by blocking the CepI/R and CciI/R systems. As a result, the inhibition of QS systems leads to reduced production of various virulence factors, such as biofilm formation, extracellular polysaccharides , lipase , and swarming motility. Notably, as a potential quorum sensing inhibitor, tyramine exhibits low toxicity in vivo in Galleria mellonella larvae and is well characterized by Lipinski’s five rules. It also shows high gastrointestinal absorption and the ability to cross the blood–brain barrier according to SwissADME database and ProTox-II server. Additionally, tyramine was found to enhance the efficacy of tetracycline in reducing the infectivity of Burkholderia cenocepacia in Galleria mellonella larvae infection model. Therefore, tyramine could be a promising candidate for combination therapy with traditional antimicrobials to improve their effectiveness against Burkholderia cenocepacia .
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Analytical Methods
·
2023
·Vol. 15
·期 45
·6286-6293
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IF 3.1
Yali Yang,Yan Li,Zelong Long,Lingling Han,Kaijun Quan,Jia Chen,Xiuhui Liu,Hongdeng Qiu
A novel C4-modified bipyridinium stationary phase (Sil-DPC4) was prepared and characterized by elemental analysis (EA) and Fourier transform infrared spectrometry (FT-IR) and further investigated for multi-mode liquid chromatography. The chromatographic performances of Sil-DPC4 were evaluated by reversed-phase chromatography using polycyclic aromatic hydrocarbons (PAHs), phenylamines and phenols, hydrophilic interaction chromatography using nucleosides and nucleobases, and ion exchange chromatography using inorganic ions and organic ions. The effects of the acetonitrile content, salt concentration and pH value of the mobile phase on the retention of Sil-DPC4 were also investigated. Sil-DPC4 showed multiple retention mechanisms including π–π, hydrophobic and electrostatic interactions for PAHs, phenylamines and phenols compared with a dipyridine modified silica stationary phase (Sil-DP) and C18 in RPLC, faster separation for nucleosides and nucleobases compared with Sil-DP, and higher hydrophilicity than HILIC in HILIC, and stronger retention and better separation ability for inorganic ions and organic ions in comparison to Sil-DP in IEC. Besides, Sil-DPC4 was used successfully to detect iodide in artificial seawater and had the potential to analyze radionuclide iodine-131 in seawater. In conclusion, multiple retention mechanisms of Sil-DPC4 could make it have potential applications in complex samples.
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PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
·
2023
·Vol. 120
·期 43
·e2311585120
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IF 11.1
Chao-Hai Gu,Song Wang,Ai-Yong Zhang,Chang Liu,Jun Jiang,Han-Qing Yu
Single-atom Fenton-like catalysis has attracted significant attention, yet the quest for controllable synthesis of single-atom catalysts (SACs) with modulation of electron configuration is driven by the current disadvantages of poor activity, low selectivity, narrow pH range, and ambiguous structure–performance relationship. Herein, we devised an innovative strategy, the slow-release synthesis, to fabricate superior Cu SACs by facilitating the dynamic equilibrium between metal precursor supply and anchoring site formation. In this strategy, the dynamics of anchoring site formation, metal precursor release, and their binding reaction kinetics were regulated. Bolstered by harmoniously aligned dynamics, the selective and specific monatomic binding reactions were ensured to refine controllable SACs synthesis with well-defined structure–reactivity relationship. A copious quantity of monatomic dispersed metal became deposited on the C3N4/montmorillonite (MMT) interface and surface with accessible exposure due to the convenient mass transfer within ordered MMT. The slow-release effect facilitated the generation of targeted high-quality sites by equilibrating the supply and demand of the metal precursor and anchoring site and improved the utilization ratio of metal precursors. An excellent Fenton-like reactivity for contaminant degradation was achieved by the Cu1/C3N4/MMT with diminished toxic Cu liberation. Also, the selective ·OH-mediated reaction mechanism was elucidated. Our findings provide a strategy for regulating the intractable anchoring events and optimizing the microenvironment of the monatomic metal center to synthesize superior SACs.
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Nature Communications
·
2023
·Vol. 14
·期 1
·1-12
·
IF 16.6
Jung Sinyeong,Cheung Wai-Lung,Li Si-jie,Wang Min,Li Wansi,Wang Cangyu,Song Xiaoge,Wei Guodan,Song Qinghua,Chen Season Si,Cai Wanqing,Ng Maggie,Tang Wai Kit,Tang Man-Chung
The realization of operationally stable blue organic light-emitting diodes is a challenging issue across the field. While device optimization has been a focus to effectively prolong device lifetime, strategies based on molecular engineering of chemical structures, particularly at the subatomic level, remains little. Herein, we explore the effect of targeted deuteration on donor and/or acceptor units of thermally activated delayed fluorescence emitters and investigate the structure-property relationship between intrinsic molecular stability, based on isotopic effect, and device operational stability. We show that the deuteration of the acceptor unit is critical to enhance the photostability of thermally activated delayed fluorescence compounds and hence device lifetime in addition to that of the donor units, which is commonly neglected due to the limited availability and synthetic complexity of deuterated acceptors. Based on these isotopic analogues, we observe a gradual increase in the device operational stability and achieve the long-lifetime time to 90% of the initial luminance of 23.4 h at the luminance of 1000 cd m −2 for thermally activated delayed fluorescence-sensitized organic light-emitting diodes. We anticipate our strategic deuteration approach provides insights and demonstrates the importance on structural modification materials at a subatomic level towards prolonging the device operational stability.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2023
·
IF 4.2
Lei Yuan,Leihao Zhang,Guilin Li,Shaojuan Zeng,Qizhou Xue,Chongyang Jiang,Xiangping Zhang
Electric-driven reduction of CO2 to high value-added chemicals is considered to be one of the most promising methods for CO2 utilization. In this work, a novel aprotic electrolyte consisting of phenoxy-nitrile bifunctional ionic liquid ([TBP][p-CN-PhO]) and acetonitrile was designed for CO2 electroreduction to oxalate, which shows the maximum Faradaic efficiency (FE) of 84.9% at −2.6 V. Importantly, a high oxalate formation rate of 233.7 μmol·cm–2·h–1 and oxalate FE of 73.9% were simultaneously achieved to break the trade-off effect at −2.8 V in the bifunctional ionic liquid electrolyte, which is also one of the state-of-the-art performances for CO2 electroreduction to oxalate. The significant performance of CO2 electroreduction was attributed to the strong interaction energies of phenoxy and nitrile groups with CO2 molecules in the bifunctional ionic liquid, which greatly facilitates CO2 activation to form CO2– radicals by a new bulk-phase pathway and then dimerizes into C2O42– at a lower energy barrier.
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FUEL
·
2023
·
IF 7.4
Lixia Li,Zhechao Huang,Fenghao Shu,Ying Gao,Jinxing Long
Novel techniques for upgrading heavy lignin bio-oil, the phenolic oligomer from lignin depolymerization, are of great significance for achieving better utilization efficiency of carbon element in lignin. In this study, we proposed an efficient approach for producing high-quality oxygen-containing fuel from the renewable lignin bio-oil via the C-O bond cleavage and the subsequent hydrogenation over the Cu and Ni supported on alkaline MgO . Noticeably, the optimized Cu 6 Ni 20 /MgO resulted in inspiring yields of ethylbenzene (88.6%) and cyclohexanol (98.3%) from lignin dimers, and a colorless fuel with a high-heating value of 31.4 MJ kg −1 from the realistic lignin bio-oil. The results of catalyst characterization also unveiled that introducing Cu species reduced the formation of NiMgO x solid solution, which increased the content of Ni 0 and consequently promoted the performance of upgrading lignin bio-oil. Furthermore, the recondensation of phenolic oligomers could be effectively restrained by the alkaline MgO. In addition, a plausible mechanism was proposed. Therefore, this work opens a promising avenue to designing efficient strategies for utilizing the heavy components from lignin depolymerization.
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APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Yuhui Zhang,Fei Liu,Li Zhong,Zhaoji Dong,Chuchu Chen,Zhaoyang Xu
Tetracycline antibiotics are currently detected in most water sources. The presence of such pollutants in the environment is becoming increasingly common, and addressing this contamination is a significant challenge due to its potential threat to human health and ecosystem stability. This study successfully prepared cellulose nanofiber/titanium dioxide/chitosan (CNF/TiO 2 /CS) aerogels by directional freeze-drying technique for photocatalytic degradation of tetracycline-contaminated wastewater. The CNF/TiO 2 /CS aerogel photocatalysts have a three-dimensional mesh structure with a large specific surface area, which provides many active sites for the highly efficient photocatalytic degradation of tetracyclines. The CNF/TiO 2 /CS aerogel showed 99.5% tetracycline removal efficiency within 180 min. Free radical scavenging experiments investigated the adsorption and photodegradation mechanism of tetracycline by CNF/TiO 2 /CS aerogel. The critical participation of •O 2 - and h + in the decomposition of tetracycline was verified, which provided experimental support for the photocatalytic reaction mechanism. In addition, the CNF/TiO 2 /CS aerogel has high stability and recyclability for photocatalytic degradation, which can be recycled 7 times, and the recycling process is environmentally friendly. An in-depth analysis of the intermediate degradation products using liquid chromatography-mass spectrometry (LC-MS) revealed two efficient photocatalytic degradation pathways. These findings strongly confirm the extensive potential of photocatalytically active aerogels for wastewater treatment.
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RENEWABLE ENERGY
·
2023
·
IF 8.7
Zhipeng Tian,Xiaoxin Chen,Tao Liu,Junyao Wang,Chao Wang,Riyang Shu,Jianping Liu,Ying Chen
Selective hydrodeoxygenation (HDO) of phenolic compounds derived from the pyrolysis lignin-oil to desired products is a promising route in the high-value utilization of biomass-derived products. As high as 99.99% guaiacol conversion and 96.70% cyclohexanol selectivity are obtained over optimized Co/1 K–Al 2 O 3 catalyst, which are better than those Co-based catalyst reported in previous studies. Highly dispersed Co particles provide more metal active sites and better chemisorption of guaiacol molecules, which promotes HDO activity. Importantly, with the increase amount of K species doped in Al 2 O 3 support, the total amount of acid sites on catalyst decreases and the strong acid site disappear, which inhibits unwanted conversion of cyclohexanol to the byproduct cyclohexane. It can be found that with proper amount of acid sites and strength, the selectivity of cyclohexanol can be maximized during selective HDO reaction of guaiacol. The kinetic study also shows that the activation energy from cyclohexanol to cyclohexane increases from 62.08 kJ/mol over Co/Al 2 O 3 catalyst to 86.11 kJ/mol over Co/1 K–Al 2 O 3 catalyst, implying that the reaction barrier improves, which hinders further removal of hydroxyl group on cyclohexanol. Besides, selective HDO reactions using other typical phenols as substrates over Co/1 K–Al 2 O 3 catalyst were performed and good alkyl cyclohexanols selectivities are observed.
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Horticulturae
·
2023
·Vol. 9
·期 9
·1019
·
IF 3.1
Yuan Zhang,Mina Nan,Huali Xue
Radix Astragali(RA) is the root ofAstragalus membranaceusvar. mongholicus (Bunge) P.K. Hsiao. In order to determine targeted and effective methods for treating mold infections in fresh RA, pathogenic fungi were isolated and identified using morphology and molecular biology techniques, and factors affecting the growth of the pathogenic fungi, such as temperature, pH, light, and carbon and nitrogen sources, were analyzed. Changes in the main active ingredients of RA, such as carbohydrates, flavonoids, and saponins, were detected before and after infection with pathogenic fungi. The results showed thatPenicillium polonicum,Trichothecium roseum, andFusarium equisetiwere the main pathogens causing postharvest disease in fresh RA. The optimum growth temperature for the three pathogens was 25 °C;P. polonicumwas able to grow at an alkaline pH of 8–9, whileT. roseumandF. equisetigrew better and had higher levels of sporulation under acidic conditions with pH values of 5–6. Different carbon and nitrogen sources had different effects on mycelium growth and sporulation. Darkness was favorable for the growth and sporulation of the three pathogens. Compared with healthy RA, the total carbohydrate, flavonoid, and saponin contents of the RA samples infected with the three fungi decreased. This study provides a theoretical basis for the scientific and precise control of RA postharvest disease during storage by targeting different pathogens and their growth conditions.Keywords:Radix Astragali;postharvest disease;identification;biological characteristics;active ingredients
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ChemSusChem
·
2023
·
IF 8.4
Xiangchen Kong,Chao Liu,Hongyun Zeng,Yuyang Fan,Huiyan Zhang,Rui Xiao
Graphical Depolymerization of Kraft lignin to value-added monomers can significantly enhance the profitability of lignocellulosic biorefinery. In this work, the efficient transformation of highly condensed Kraft lignin to valuable aromatic monomers through stepwise alcoholysis and zeolite-catalyzed methylene linkage cleavage is disclosed. Lignin is an aromatic polymer that constitutes over 30 wt% of lignocellulosic biomass and is the most important source of renewable aromatics in nature. The global paper industry generates more than 70 million tons of Kraft lignin annually. Depolymerization of Kraft lignin to value-added monomers can significantly enhance the profitability of biorefinery. However, the method is impeded by the severe condensation of Kraft lignin during the pulping process, which forms robust C−C bonds and results in low monomer yields. In this study, we present a stepwise approach for producing valuable aromatic monomers from Kraft lignin through the cleavage of both C−O and C−C bonds. The approach initiated with complete cleavage of C−O bonds between lignin units within Kraft lignin through alcoholysis in isopropanol, resulting in a monomer yield of 8.9 %. Subsequently, the selective cleavage of methylene linkages present in the residual dimers and oligomers was achieved with commercial MCM-41 zeolite in the same pot, proceeding with an additional monomer yield of 4.0 %, thereby increasing the total monomer yield by 45 %. This work provides an avenue for increasing the depolymerization efficiency of Kraft lignin.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2023
·
IF 4.2
Zheng Huang,Jianna Bao,Xianming Zhang,Wenxing Chen
The incorporation of ionic groups (sodium sulfonate group) in cationic dyeable polyesters (CDPs) leads to alterations in melt flow behaviors and corresponding effects on the conventional production process compared with poly(ethylene terephthalate) (PET). In this study, a range of CDPs were synthesized with a wide range of sodium-5-sulfo-bis(hydroxyethyl)-isophthalate (SIPE) contents, and their structures, properties, and rheological behaviors were comprehensively investigated. The thermal stability of CDPs decreased, while the glass transition temperature initially decreased and then increased with an increase in SIPE content. Several rheological tests were performed, and the time–temperature superposition principle was utilized to give an in-depth analysis of ionic aggregations and internal structures of CDPs. A more complex rheological behavior of CDPs was observed due to the ionic aggregation effects aroused from the strong polarity of sodium sulfonate groups. Based on temperature scans, small amounts of SIPE would act as a plasticizer, reducing the complex viscosity (η*) of CDPs. As the SIPE content increased, the η* of CDPs increased, and the linear viscoelastic interval became narrower, indicative of the formation of ionic aggregates, and this structure was also verified by the results obtained from extensional rheology. Time–temperature superposition began to fail when the SIPE concentration rose further, confirming that ionic aggregation clusters emerged. This work may shed light on the understanding of design and structure–property relationships of PET ionomers.
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