GREEN CHEMISTRY
·
2023
·Vol. 25
·期 21
·8633-8644
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IF 9.8
Anqiu Liu,Xixi Liu,Yaping She,Xiaoqiang Hu,Miao Hu,Zehui Zhang,Xiaochen Wang,Bing Liu
Selective hydrodeoxygenation transformations constitute the most pivotal industrial processes in chemistry and catalysis. Herein, we have rationally designed a heterogeneous Co/CoOx catalytic system with metallic Co and oxygen vacancies in CoOx for selective hydrodeoxygenation of structurally diverse ketones and nitro compounds under mild conditions (80–100 °C and 10 bar H2), which shows a superior performance compared to state-of-the-art noble-metal catalysts. Experimental results and DFT calculation revealed that oxygen vacancies not only promote the adsorption and activation of substrates and the intermediates via electronic interactions, but also enable the hydrodeoxygenation reactions in a low-energy pathway via the direct hydrogenolysis process, instead of the dehydration–hydrogenation process. Given its generality and efficiency, it is believed that this method can serve as a practical, economically viable approach for selective hydrodeoxygenation reactions, which should impact both the chemical industry and scientific research.
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REACTIVE & FUNCTIONAL POLYMERS
·
2023
·
IF 5.1
Yanqing Wang,Sikai Wang,Pengcheng Li,Shuting Cao,Yuetao Liu,Chuanhui Gao
Broadening the range of practical applications of self-healing materials has become a research hotspot for the development of durable and smart materials. This study the development of a hydrogen bond-rich of self-healing elastomer , formed by the combination of disulfide and diazolidinyl urea (DU) cross-linked polyurethane polymers (PDD). The prepared polyurethane elastomer material possessed extremely high mechanical properties (including a stress of 25 MPa and high toughness of 306 MJ/m 3 ). Besides, PDD exhibited an excellent self-healing performance. Even if it is subjected to long-term tensile deformation or extreme strain, it could recover almost completely to its initial state within 12 h in a 60 °C environment. In addition, the synergistic effect of diazolidinylurea and element S on the polymer film gave the material excellent antimicrobial properties. Finally, we added carbon nanotubes into the polyurethane system and assembled them into smart sensors for applications in flexible electronic devices. The versatility of this sensor has been demonstrated in human motion applications.
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APPLIED MICROBIOLOGY AND BIOTECHNOLOGY
·
2023
·
IF 5
Zhang Xiaohan,Zhang Dong,Ding Yan,Li Zilong,Wang Chenchen,Ye Shuhong
Abstract Resveratrol (RES) is a secondary metabolite synthesized by plants in response to environmental stress and pathogen infection, which is of great significance for the industrial production of RES by fermentation culture. In this study, we aimed to explore the biosynthesis pathway of RES and its key enzymes in the Priestia megaterium PH3, which was isolated and screened from peanut fruit. Through Liquid Chromatography-Mass Spectrometry (LC-MS) analysis, we quantified the RES content and distribution in the culture medium and determined that Priestia megaterium PH3 mainly secreted RES extracellularly. Furthermore, the highest production of RES was observed in YPD, yielding an impressive 127.46 ± 6.11 μg/L. By optimizing the fermentation conditions, we achieved a remarkable RES yield of 946.82 ± 24.74 μg/L within just 2 days, which represents the highest reported yield for a natural isolate produced in such a short time frame. Our investigation revealed that the phenylpropane pathway is responsible for RES synthesis in this bacterium, with cinnamate 4-hydroxylase (C4H) identified as the main rate-limiting enzyme. Overall, our findings highlight the robust RES production capabilities of Priestia megaterium PH3, offering novel insights and potential applications for bacterial fermentation in RES production. Key points
• RES synthesized by the bacterium was confirmed through the phenylpropane pathway.
• The key rate-limiting enzyme for biosynthesis-RES is C4H.
• RES reached 946.82 ± 24.74 μg/L after fermentation for 2 days.
Graphical Abstract
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Nature Energy
·
2023
·
IF 56.7
Lei Jiafeng,Zhang Yaqin,Yao Yanxin,Shi Yang,Leung Ka Lok,Fan Jun,Lu Yi-Chun
Aqueous redox flow battery (RFB) is one of the most promising technologies for grid-scale energy storage systems. Polysulfides are particularly attractive active materials owing to their low cost and high capacity, but the low energy efficiency and low operating current density limit their practical applications. Here we report an active and durable molecule catalyst, riboflavin sodium phosphate (FMN-Na), to transform sluggish polysulfide reduction reactions to fast redox reactions of FMN-Na via homogeneous catalysis. The FMN-Na catalyst substantially reduces the overpotential of a polysulfide–ferrocyanide RFB (S-Fe RFB) from more than 800 mV to 241 mV at 30 mA cm − 2 . A catalysed S-Fe flow cell was demonstrated for 2,000 cycles at 40 mA cm − 2 with a low decay rate of 0.00004% per cycle (0.0017% per day). A catalysed polysulfide–iodide RFB operated for 1,300 cycles under 40 mA cm − 2 without capacity decay. This work addresses the bottleneck of polysulfide-based RFBs for long-duration energy storage applications.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Nannan Shao,Jingke Yao,Yanxin Qi,Yubin Huang
Applying hydrogels as medical dressing in treating wounds has become a research hotspot in recent years. Photothermal hydrogels with antibacterial properties and favorable biocompatibility offer great potential for treating infected wounds. However, the risks associated with photosensitizer leakage and excessive heat cause edema and vascular damage, cutting off the nutrients and oxygen supply and slowing the wound healing rate. Herein, a bilayer hydrogel (AuDG 2 ) containing the photothermal and heat-absorbing hydrogel layers is developed to generate adequate heat for quick bacteria removal and tissue protection. In this system, Au nanoparticles are firmly fixed to the nano-hydroxyapatite and coated in the photothermal hydrogel layer, effectively avoiding the leakage of the photosensitizer. Near-infrared imaging shows AuDG 2 hydrogel maintains 48–50 °C at the wound by heat exchange between the two layers of it. This property enables AuDG 2 to have an 89.68 % clearance rate against Staphylococcus aureus ( S. aureus ) and a 73.03 % removal efficiency of Escherichia coli ( E. coli ) within 5 min, increasing the healing area of infected wounds by 26.45 % compared to the normal saline treatment group, without adverse effects from burns, and evaporate water from the blood to stop blooding in a very short time. This anti-scald photothermal hydrogel structure is simple in preparation, offering the possibility to mitigate the side effects of photothermal therapy.
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FOOD CHEMISTRY
·
2023
·
IF 8.8
Yiyan Liu,Hongru Chen,Shufan Chen,Yuehan Zhang,Jingkai Zhang,Xiaoqi Zhu,Wenxuan Li,Jialu Liu,Yang Jiang,Dapeng Li
Pectin extraction is generally an energy-intensive industrial process, while on the other hand their extraction methods vary from different sources. Starting with that perspective, pectin (WSP) containing ultra-low degree of methylation (31.08 ± 1.27%) from dragon fruit peel (DFP) was extracted by using pure water at room temperature. WSP, dominant in DFP (17.13 ± 1.01%), showed both a high molecular weight and a wide molecular weight distribution, while the yield of the rest acid-soluble pectin (HAP) from DFP residue was only 5.22 ± 0.76%. Furthermore, WSP can stabilize emulsions over a wide range of concentrations and oil phases, especially HIPE. Therefore, the hypothesis was verified that the pectin-rich extract from dragon fruit peel with excellent emulsifying properties could be simply extracted by pure water. This environmentally-friendly and energy-saving extraction method provides a new insight to increase the additional value of dragon fruit peel produced in food processing.
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ADVANCED FUNCTIONAL MATERIALS
·
2023
·Vol. 33
·期 48
·2305423
·
IF 19
Yanyu Deng,Zhiguo Zhang,Guanhua Ren,Zhiqi Li,Chunyu Liu,Wenbin Guo
The surface treatment for solution-processed perovskite films using molecular passivation agents has been reported to be critical for improving the performance of perovskite light-emitting diodes (PeLEDs). Generally, most studies emphasized the binding effect between passivation molecules and perovskite surface, while halide perovskites are dominated by multiple defects and need more comprehensive passivation, which is often neglected. Here, a molecule of 5-ammonium valeric acid trifluoroacetate (5-AVATFA) with multi-functional groups is rationally developed to modify the interface of advanced PeLEDs. Combining experimental and density functional theory analysis, the synergism effects of reduced surface defects and increased steric hindrance of 5-AVATFA, which can greatly suppress the ion migration of PeLEDs, are demonstarated. Because of the passivation effect of multi-functional 5-AVATFA, an optimal device with an external quantum efficiency of 22.32%, a radiance of 558.46 W sr −1 m −2 , and an extended half-lifetime of 103.3 h is obtained.
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ACS Sustainable Chemistry & Engineering
·
2023
·
IF 8.4
Ningxia Gu,Lixin Song,Pengyun Zhang,Ye Feng,Pingfan Du,Yongjun Zhu,Lei Ning,Zeyuan Sun,Hua Jiang,Jie Xiong
Electron transport layer (ETL)-free perovskite solar cells (PSCs) have garnered significant attention due to their simple manufacturing process. However, containing ETL results in blocking holes and suppressing charge recombination. Herein, the titanium dioxide (TiO2)-doped carbon nanofibers (TiO2/C NFs) via electrospinning were introduced into the perovskite absorber layer. The one-dimensional TiO2/C NFs provided an additional charge transport channel to promote the carrier transfer and suppress nonradiative recombination. Carbon nanofibers with high conductivity could also improve the electrical conductivity of perovskite. Moreover, TiO2/C NFs functioned as the nucleation sites to regulate the preferred orientation of perovskite crystals. Finally, the power conversion efficiency (PCE) of rigid PSCs with TiO2/C NFs was significantly improved from 18.07 to 19.81%, with an enhanced stability of only 11% degradation after exposure to an ambient environment for 300 h. In addition, the TiO2/C NFs-optimized flexible devices exhibited a PCE of 17.61%. Highly flexible TiO2/C NFs incorporating effectively improved the bending stability, wherein the flexible PSCs without and with TiO2/C NFs retained 84.27 and 48.33% of the original PCE after 6000 bending cycles (radius: 3 mm), respectively. This work highlights a significant application of TiO2/C NFs in developing high-efficiency and well-stability minimalist PSCs.
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Advanced Materials Technologies
·
2023
·
IF 6.8
Shengbin Dai,Jiangqi Zhu,Xingchen Yan,Shun Wu,Yang Liu,Xiang Gao,Hamish Fraser,Peter Hodgson,Yuman Zhu,Martin Heilmaier,Aijun Huang
Oxide dispersion strengthened (ODS) nickel (Ni)-based superalloys are advanced materials known for their outstanding tensile and creep performance at temperatures exceeding 1000 °C. Nevertheless, their conventional synthesis presents a longstanding challenge in cost-effectively producing intricate components for critical applications. In this work, electrostatic self-assembly (ESA) of powders with the laser powder bed fusion (LPBF) process have been successfully combined to produce yttria ODS Inconel 718 (IN718) alloy for the first time. The approach has demonstrated a significant contribution of yttria to the strength of IN718 after the solid solution heat treatment, as evidenced by ≈50% improvement in room temperature yield strength with a 0.5 wt.% yttria addition. The addition of yttria by this process leads to a heterogeneous microstructure. This heterogeneous microstructure comprises two distinct grain areas with varying amounts of yttria nanoparticles and dislocation storage. It has been shown that the yield strength increase can be predicted by the combination of both Y 2 O 3 dispersion strengthening and dislocation strengthening mechanisms. These findings offer an effective approach to tailor heterogeneous microstructures, unlocking new opportunities for cost-effectively producing high-performance ODS Ni-based superalloy products with excellent mechanical properties.
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ANALYST
·
2023
·Vol. 148
·期 18
·4339-4345
·
IF 4.2
Zhong-Xia Wang,Kai-Qi Liu,Xiang-Ying Meng,Feng Li,Heng-Ye Li,Hang Gao,Wei Wang
Meloxicam (Mel), as a powerful and effective anti-inflammatory drug, is commonly employed for the treatment of various inflammatory diseases; however, the use of Mel at high doses or for extended periods could cause severe side effects in human visceral organs. Therefore, a simple, rapid, and reliable method is urgently needed to monitor Mel in biological samples. Herein, novel water-soluble luminescent nano-carbon dots (nano-Cdots) with outstanding physicochemical properties were prepared by a one-pot high-temperature hydrothermal process of ellagic acid and guanidine. The nano-Cdots were further used as an optical probe for the sensitive detection of Mel in serum samples through the cooperative mechanisms of the inner filter effect and photoelectron transfer. By employing this sensor, an excellent linear correlation was achieved between the relative luminescent intensity [(PL0 − PL)/PL0] and the concentration of Mel in the range of 0.1 to 200 μM, with a limit of detection of 34.68 nM (3σ/k). This sensor was effectively employed for the analysis of Mel in real serum samples, implying its potential development prospects for the advancement of drug analysis with carbon-based probes.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2023
·
IF 4.2
Zhenfeng Xiong,Ying Huang,Nan Li,Chaozhi Zhang,Yonghua Li,Zhuo Yang,Weidong Zhou,Kemei Zhou,Rong Zha,Changdong Sheng
Recovery of rare-earth elements (REEs), especially those of Dy and Nd, from Nd–Fe–B permanent magnets is crucial for sustainable development. Herein, an unsymmetrical pentanediamide extractant, N,N′-dimethyl-N,N′-didecyl-3-oxapentanediamide (DMDDOPDA), was synthesized and characterized for the effective extraction of Dy(III) and Nd(III). DMDDOPDA can form coordination bonds with metal ions because of the strong electron-donating abilities of the N and O atoms. The coordination sites might be inclined toward one side during the extraction. DMDDOPDA exhibited superior extraction performance in the HNO3 system than it did in the HCl system. The highest extraction efficiencies of Dy(III) and Nd(III) under optimal conditions were 99.9% and 99.5%, respectively, while their optimum stripping efficiencies were 100% and 85.3%, respectively. DMDDOPDA extraction of Dy(III) and Nd(III) in the four investigated diluents involved the formation of a neutral coordination complex. This study provides new insights into REE extraction using pentanediamide extractants.
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Acta Biomaterialia
·
2023
·
IF 9.7
Chong Zhang,Fen Zeng,Zhengyang Fan,Zhen He,Liang Tai,Qiang Peng,Yixin Zhang,Zhenhua Chao,Wenning Jiang,Lingyun Jia,Lulu Han
Inflammatory bowel disease (IBD) is a global public health challenge that affects millions of people. Current medical treatments for IBD are not fully effective and may cause undesirable side effects on patients. Thus, there is an urgent need for safe, simple, and efficacious strategies to treat IBD in clinical settings. Here, we develop an oral polyphenol nanoparticle (PDT) by assembling dexamethasone sodium phosphate (DSP)-loaded poly-β-cyclodextrin with tannic acid via host-guest interactions for treating IBD. This one-step assembly process is rapid (within 10 s), reproducible, and free of harmful chemical agents, which can facilitate its clinical translation. PDT is negatively charged due to the three components, which enable it to specifically target the positively charged inflamed colonic mucosa through electrostatic attraction, thus localizing the drug at the inflamed site to reduce systemic exposure and side effects. Furthermore, PDT exhibits a strong reactive oxygen species (ROS)-scavenging ability derived from the tannic acid component, which can alleviate ROS-mediated inflammatory responses and ameliorate IBD symptoms. Compared with free DSP, PDT demonstrates sustained DSP release behavior in vitro and in vivo , as well as enhanced therapeutic efficacy in a colitis mouse model. These results suggest that PDT might be a potential therapeutic agent for the treatment of IBD. Moreover, this facile polyphenol host-guest assembly strategy may provide a promising drug-delivery platform for treating various diseases Statement of significance To develop safe and effective treatments for inflammatory bowel disease (IBD), we have designed an oral polyphenol nanoparticle (PDT) using the host-guest assembly of dexamethasone sodium phosphate (DSP)-loaded poly-β-cyclodextrin with tannic acid. Through in vitro and in vivo experiments, PDT has demonstrated remarkable inflammation-targeting, ROS-scavenging, and anti-inflammatory properties, along with sustained release of DSP. Moreover, in an IBD mouse model, PDT has shown significantly improved therapeutic efficacy compared to free DSP. The host-guest assembly strategy employed for PDT is noteworthy for its rapidity, reproducibility, and safety due to the absence of harmful chemicals, holding great promise for designing a diverse range of nanomedicines customized for treating various diseases.
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