JOURNAL OF MOLECULAR STRUCTURE
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2023
·
IF 3.8
Xiaochen Han,Chongyang Guo,Yugao Wang,Gang Liu,Jun Shen
Furan-2,5-dicarboxylic acid (FDCA) is an important biomass-derived diacid, and it is the most promising substitute for terephthalic acid. The common method of FDCA usually involves 5-hydroxymethylfurfural oxidation. Edible fructose is often used as the feedstock of 5-hydroxymethylfurfural, and the oxidation step would generate undesirable impurities. Herein, FDCA was novelty synthesized by carboxylation of formate and 2-furoic acid (FA) derived from unedible-biomass. This route is potentially advantageous because it is simple to operate and does not require any additional additives. The reaction mechanism has been elucidated by density functional theory (DFT) calculations. In the carboxylation process, the C(sp 2 )-H bond of formate (HCOOM) undergoes cleavage, generating the carbon dioxide radical anion (CO 2 •− ). Subsequently, CO 2 •− attacks the C 5 of FA, forming the C C bond and ultimately yielding FDCA. The conversion of HCOOM to CO 2 •− is an effective way to achieve carboxylation reaction. The rate-determining step of the carboxylation reaction is the cleavage of the C(sp 2 )-H bond of HCOO − with activation barrier of 159.11 kJ⋅mol −1 . The investigation would provide a new strategy for the mechanism of carboxylation reactions, and hold the potential to establish pathways for FDCA production.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2023
·
IF 8.2
Xin Pan,Pei Liu,Ye-jun Zhang,Hao-kuang Zhang,Hao Wei,Jing-yi Jiang,Hui-Yan,Er-xin Shang,Wei-wen Li,Yiwei Wang,Jin-ao Duan
Carboxymethyl chitosan and resistant starch exhibit good performance in diabetes regulation. We prepared carboxymethyl chitosan - resistant starch complex. Test the properties of composite resistant starch by using X-ray diffraction, water contact angle, infrared spectroscopy, and scanning electron microscopy, interactions with intestinal microbiota and mouse experiments were also conducted. The results indicated that the composite resistant starch had a good effect on promoting the proliferation of probiotics on Bifidobacterium and a significant inhibitory effect on Escherichia coli than resistant starch ( P < 0.05). After administration, the water intake and weight of diabetic mice were significantly reduced. The blood glucose of diabetic mice was also reduced, and oral glucose tolerance showed that the glucose degradation rates of composite resistant starch were significantly improved compared to model mice. Cholesterol, triglycerides, high-density lipoprotein and low-density lipoprotein were significantly lower than those in the diabetes group ( P < 0.05). The diversity of the gut microbiota was also proven.
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ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Shuang Yang,Yinan Lao,Wenjin Yu,Zhenyu Tang,Haoqing Guo,Ganghong Liu,Bo Qu,Lixin Xiao,Zhijian Chen
Tin-based perovskites comprise one of the preferred nontoxic alternatives to Pb-based perovskites due to their desirable optoelectronic properties. However, there remains a crucial stability problem due to the property of Sn2+ oxidation. In this study, we reported stable tin-based perovskite nanocrystals (NCs) using stannous acetate as the Sn2+ source because of its stronger Sn–O bonding. To prevent the oxidation of Sn2+, a thin layer of CsBr coverage was formed in situ; tin-based perovskite NCs, CsxSnBrx+2@CsBr (1 < x < 4), show a high photoluminescence quantum yield (PLQY) of 78.2% and high stability. The measured lifetime of PLQY decrease to half of the initial value is ∼1287 h under ambient conditions and ∼2200 h under a nitrogen atmosphere, respectively. Furthermore, the as-fabricated light-emitting diodes based on CsxSnBrx+2@CsBr NCs as the emitting layer exhibit a maximum luminescence of 16 cd/m2 and an external quantum efficiency of 0.035% with peaks at 451 and 615 nm, corresponding to the emissions of CsBr and CsxSnBrx+2, respectively. This work provided a new way to obtain stable Sn-based perovskite NCs and exhibited their potential for application in white light-emitting diodes (LEDs).
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CHEMISTRY-A EUROPEAN JOURNAL
·
2023
·Vol. 29
·期 59
·e202302132
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IF 4.3
Jun-Tao Shi,Xian-Hui Chen,Yuan-Yuan Peng,Gui-Ping Wang,Guang-Yan Du,Quan Li
Graphical A novel mechanically bonded amphiphile (MBA)-bistable [2]rotaxane H2 was designed and prepared. In both the solution and aggregated states, H2 demonstrated pH-responsive emissions due to the presence of a distance-dependent photoinduced electron transfer (PET) process. Moreover, the morphology of H2 aggregates can be tuned from nanospheres to vesicles due to the pH-controlled shuttling motion-induced alternation of H2 amphiphilicity. Advanced Organic Chemical Materials Co-constructed Mechanically bonded amphiphiles (MBAs), also known as mechanically interlocked molecules (MIMs), have emerged as an important kind of functional building block for the construction of artificial molecular machines and soft materials. Herein, a novel MBA, i. e., bistable [2]rotaxane H2 was designed and synthesized. In the solution state, H2 demonstrated pH and metal ion-responsive emissions due to the presence of a distance-dependent photoinduced electron transfer (PET) process and the fluorescence resonance energy transfer (FRET) process, respectively. Importantly, the amphiphilic feature of H2 has endowed it with unique self-assembly capability, and nanospheres were obtained in a mixed H 2 O/CH 3 CN solvent. Moreover, the morphology of H2 aggregates can be tuned from nanospheres to vesicles due to the pH-controlled shuttling motion-induced alternation of H2 amphiphilicity. Interestingly, larger spheres with novel pearl-chain-like structures from H2 were observed after adding stoichiometric Zn 2+ . In particular, H2 shows pH-responsive emissions in its aggregation state, allowing the visualization of the shuttling movement by just naked eyes. It is assumed that the well-designed [2]rotaxane, and particularly the proposed concept of MBA shown here, will further enrich the families of MIMs, offering prospects for synthesizing more MIMs with novel assembly capabilities and bottom-up building dynamic smart materials with unprecedented functions.
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CELLULAR AND MOLECULAR LIFE SCIENCES
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2023
·Vol. 80
·期 8
·1-18
·
IF 8
Cao Xuwen,Xie Yusu,Yang Hanwen,Sun Peiqi,Xue Beining,Garcia L. Rene,Zhang Liusuo
Dietary intake and nutrient composition regulate animal growth and development; however, the underlying mechanisms remain elusive. Our previous study has shown that either the mammalian deafness homolog gene tmc-1 or its downstream acetylcholine receptor gene eat-2 attenuates Caenorhabditis elegans development in a chemically defined food CeMM ( C. elegans maintenance medium) environment, but the underpinning mechanisms are not well-understood. Here, we found that, in CeMM food environment, for both eat-2 and tmc-1 fast-growing mutants, several fatty acid synthesis and elongation genes were highly expressed, while many fatty acid β-oxidation genes were repressed. Accordingly, dietary supplementation of individual fatty acids, such as monomethyl branch chain fatty acid C17ISO, palmitic acid and stearic acid significantly promoted wild-type animal development on CeMM, and mutations in either C17ISO synthesis gene elo-5 or elo-6 slowed the rapid growth of eat-2 mutant. Tissue-specific rescue experiments showed that elo-6 promoted animal development mainly in the intestine. Furthermore, transcriptome and metabolome analyses revealed that elo-6 /C17ISO regulation of C. elegans development may be correlated with up-regulating expression of cuticle synthetic and hedgehog signaling genes, as well as promoting biosynthesis of amino acids, amino acid derivatives and vitamins. Correspondingly, we found that amino acid derivative S-adenosylmethionine and its upstream metabolite methionine sulfoxide significantly promoted C. elegans development on CeMM. This study demonstrated that C17ISO, palmitic acid, stearic acid, S-adenosylmethionine and methionine sulfoxide inhibited or bypassed the TMC-1 and EAT-2-mediated attenuation of development via metabolic remodeling, and allowed the animals to adapt to the new nutritional niche.
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BIOPROCESS AND BIOSYSTEMS ENGINEERING
·
2023
·
IF 3.8
Jia Dong-Xu,Yu Hai,Wang Fan,Jin Li-Qun,Liu Zhi-Qiang,Zheng Yu-Guo
Cellobiose 2-epimerase (CE) is ideally suited to synthesize lactulose from lactose, but the poor thermostability and catalytic efficiency restrict enzymatic application. Herein, a non-characterized CE originating from Caldicellulosiruptor morganii (CmCE) was discovered in the NCBI database. Then, a smart mutation library was constructed based on FoldX ΔΔG calculation and modeling structure analysis, from which a positive mutant D226G located within the α 8 /α 9 loop exhibited longer half-lives at 65–75 °C as well as lower K m and higher k cat / K m values compared with CmCE. Molecular modeling demonstrated that the improvement of D226G was largely attributed to the rigidification of the flexible loop, the compactness of the catalysis pocket and the increment of substrate-binding capability. Finally, the yield of synthesizing lactulose catalyzed by D226G reached 45.5%, higher than the 35.9% achieved with CmCE. The disclosed effect of the flexible loop on enzymatic stability and catalysis provides insight to redesign efficient CEs to biosynthesize lactulose. Graphical abstract
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Analytical Methods
·
2023
·Vol. 16
·期 4
·576-582
·
IF 3.1
Fangfang Yang,Shuang Li,Jialiang Wu,Shufeng Liu
Reversible structural changes in DNA nanomachines have great potential in the field of bioanalysis. Here, we demonstrate an assembly strategy for quencher-free and tunable DNA tweezers based on 2-aminopurine (2-AP), avoiding the tedious fluorescence labelling step. The conformational state of the tweezers could be controlled by specific oligonucleotides (fuel or anti-fuel). Taking advantage of the local environmental sensitivity of 2-AP, the structural changes of the tweezers were easily tracked, and multiple cyclic switching of the tweezers between the open and closed states was achieved. In addition, the influence of oligonucleotide structure on the fluorescence properties of 2-AP was deeply explored. We figured out that the fluorescence of 2-AP was highly quenched by the base-stacking of natural bases in DNA oligonucleotides. Moreover, by comprehensively regulating the type of bases surrounding the inserted 2-AP site, a sensitive fluorescence response towards dynamic change can be obtained. This principle of quencher-free nanodevices based on 2-AP provides a convenient method for monitoring the structural changes of DNA nanomachines.
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POLYMER
·
2023
·
IF 4.6
Jiani Gao,Yilong Chu,Yuyang Yan,Shuangshuang Zhou,Xiaowei Li,Cheng-Bo Li
Here, poly(1,3,5-tri(thiophene-2-yl)benzene) (PTTB) membrane electrodes with porous surface structures were prepared by using an electropolymerization method. Firstly, a series of PTTB film electrodes with different morphologies are obtained, including open nanotubes , stacked flocs, dispersed cauliflower-like, and aggregated spheres, by separately depositing the PTTB films on different conductive substrates (GCE, silicon wafers, ITO , FTO). Secondly, this study explored the factors affecting the photoelectric properties and stability of PTTB film electrodes by varying the solvent, electrochemical method, scan rate, and number of scan cycles. Finally, the CV method and DCM/ACN mixed solvent were used in this experiment, and the best photoelectric effect of 3.2 μA was obtained under 3 scan cycles. In this study, the factors influencing the properties of PTTB by electrochemical polymerization methods are obtained through the exploration of PTTB film electrodes, providing a reference value for further combining PTTB films with other materials to prepare composite photoelectrodes .
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TALANTA
·
2023
·
IF 6.1
Ying Li,Jian Xue,Rongjun Yu,Siling Chen,Xiangyu Deng,Anyi Chen,Jingfu Qiu
Herein, a ternary PdPtRu nanodendrite as novel trimetallic nanozyme was reported, which possessed excellent peroxidase-like activity as well as electro-catalytic activity on account of the synergistic effect between the three metals. Based on the excellent electro-catalytic activity of trimetallic PdPtRu nanozyme toward the reduction of H 2 O 2 , the trimetallic nanozyme was applied to construct a brief electrochemical immunosensor for SARS-COV-2 antigen detection. Concretely, trimetallic PdPtRu nanodendrite was used to modify electrode surface, which not only generated high reduction current of H 2 O 2 for signal amplification, but also provided massive active sites for capture antibody (Ab 1 ) immobilization to construct immunosensor. In the presence of target SARS-COV-2 antigen, SiO 2 nanosphere labeled detection antibody (Ab 2 ) composites were introduced on the electrode surface according sandwich immuno-reaction. Due to the inhibitory effect of SiO 2 nanosphere on the current signal, the current signal was decreased with the increasing target SARS-COV-2 antigen concentration. As a result, the proposed electrochemical immunosensor presented sensitive detection of SARS-COV-2 antigen with linear range from 1.0 pg/mL to 1.0 μg/mL and limit of detection down to 51.74 fg/mL. The proposed immunosensor provide a brief but sensitive antigen detection tool for rapid diagnosis of COVID-19.
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ACS Catalysis
·
2023
·
IF 12.9
Zhen Chen,Haixin Chen,Kun Wang,Jian Chen,Ming Li,Yi Wang,Panagiotis Tsiakaras,Shuqin Song
The photocatalytic oxygen reduction reaction (ORR) is a promising strategy that generates H2O2 with a lower energy input. Although great progress has been made in the development of photocatalysts, poor accessibility of O2 in photocatalysts interfacial microenvironment is the rate-limiting factor for the photocatalytic 2e– ORR and still little explored. Here, we design a simple method to regulate the hydrophobicity and O2 accessibility at a controllable crystal facet ratio of TiO2 photocatalyst by a facile stearic acid (SA) modification. The adsorption structure of SA bonding with TiO2 has been investigated in detail by Raman spectra, X-ray photoelectron spectroscopy, Fourier transform infrared spectra, and density functional theory calculations. It has been found that the stable ester bond is formed between SA molecules and the TiO2 surface, thus leading to the enhanced hydrophobicity with the increase of SA loading. The highest photocatalytic H2O2 production rate from 2e− ORR on SA-modified TiO2 can reach up to 3160 μM h–1 g–1, which is 1.69 times that of the corresponding pure TiO2 sample. From the results of electrochemical impedance spectroscopy and molecular dynamics simulation, the increase of the O2 concentration in the interfacial microenvironment benefiting from the SA modification is responsible for the enhancement of 2e– ORR activity rather than the increase of hydrophobicity.
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ANALYTICAL CHEMISTRY
·
2023
·
IF 7.4
Yidan Wang,Yunlei Xianyu
The coordination chemistry between phosphorylated molecules and metal ions has been reported, while few studies focus on its sensing capability. Herein, we report a colorimetric sensing strategy through the coordination chemistry between ascorbic acid 2-phosphate (AAP) and copper ions. The phosphate group-containing AAP can coordinate with copper ions to induce a visible color change from blue to green in a rapid way, which can be easily read by the naked eye or a smartphone based on the blue-to-green (B/G) ratio. This coordination chemistry provides a facile and convenient strategy for designing colorimetric assays. Alkaline phosphatase can catalyze the hydrolysis of AAP to ascorbic acid (AA), thus modulating the AAP/AA transformation and the AAP-mediated coordination, offering a straightforward way for monitoring the enzymatic activity. This colorimetric sensing strategy shows good performances in stability, sensitivity, cost, and scale-up production, holding great promise as a point-of-care technique for diagnostic applications.
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BIOLOGY AND FERTILITY OF SOILS
·
2023
·Vol. 59
·期 6
·679-696
·
IF 6.5
Hu Ruiwen,Liu Songfeng,Zhao Haiming,Wang Zhigang,Shu Longfei,Zeng Jiaxiong,Cai Quanying,Mo Cehui,He Zhili,Wang Cheng
Di(2-ethylhexyl) phthalate (DEHP), one of the most important plasticizers, is considered a typical endocrine disruptor. Soil contains high levels of DEHP, and acts as the main medium for its migration into food chain, presenting potential risks to human health. Although soil indigenous microbial communities hold a great potential to degrade DEHP, the kinetics and mechanism of microbial biodegradation for soil DEHP on the long-time scale remain unclear. Here, we analyzed microbial communities from time-series (up to 90 days) samples of laboratory microcosms by sequencing of 16S and ITS rRNA gene amplicons. We found that the kinetics processes of DEHP biodegradation were well fitted by a biphasic model with two independent kinetic phases: phase I as a first-order kinetics process (0–10 days, r 2 = 0.975), and phase II as a fractional power kinetics process (11–90 days, r 2 = 0.967). Linear discriminant and partial least square regression analyses showed that bacterial genera Clostridium , Sporotomaculum , Mycoplana , and Hyphomicrobium were involved in DEHP biodegradation during phase I, and genera Bacillus and Nannocystis were responsible for DEHP biodegradation during phase II. Moreover, we observed transition in microbial co-occurrence patterns: closer inter-taxa connections between bacterial degrader and fungal genera Aspergillus , Fusarium , and Pleurotus in phase I. Such divergence in the composition of potential DEHP-degrading bacteria and their interactions with fungi may induce the decreased degradation rates from phase I to phase II. This study systematically deciphers the bacterially driven DEHP biodegradation kinetics, and provides fundamental basis for developing strategies for efficient DEHP removal in soil.
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