ENVIRONMENTAL RESEARCH
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2025
·
IF 7.7
Lina Xiao,Qiuping Zhang,Xinzhi Wang,Huan Zhang,Wenxuan Li,Hao Zhang,Bowen Li
Efficient solar energy storage via light-driven hydrogen (H 2 ) production presents a promising and attractive strategy for addressing the global energy crisis. The integration of platinum (Pt) co-catalyst into metal-organic frameworks (MOFs) to enhance photoinduced charge separation and transfer remains a significant challenge. Herein, a platinum–porphyrin zirconium metal-organic framework (MOF) PCN-223(Pt) is reported, and synthesized using a facile two-solvent strategy. The prepared PCN-223(Pt) is self-sensitized and contains a platinum (Pt) electron-trapping center, which confers excellent visible-light catalytic activity. Under visible-light irradiation, PCN-223(Pt) produced 732 μmol g −1 h −1 of H 2 , a 7.6-fold increase compared to the isostructural PCN-223, which lacks Pt coordination in its porphyrin rings. This improvement results from the photogenerated electrons' efficient transport to the Pt electron-trapping centers, which improves charge carrier separation. Density functional theory calculations demonstrate the positive role that Pt in PCN-223(Pt) play in optimizing the corresponding hydrogen binding energy. PCN-223(Pt) exhibits excellent recyclability, maintaining its catalytic performance across five cycles without significant degradation. These results offer a new approach for designing MOF-based highly efficient visible-light active catalysts.
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EUROPEAN POLYMER JOURNAL
·
2025
·
IF 6.3
Rongli Zhang,Lingran Liu,Zhuo Ge,Hanyu Ren,Wentang Wang,Maiyong Zhu,Chunhui Luo
Gel-based electronic sensors have wide applications in wearable sensors and soft devices, but serious swelling issues and performance degradation over time greatly hinder their functions in underwater environments. Herein, a coordination-driven strategy for preparing a conductive hydrogel via aqueous solution radical polymerization of methyl acrylamide (MAm) and L-serinyl acrylate copper complex (LSA) was proposed to address this issue. Owing to the dual hydrophobic/hydrophilic network of PMAm as well as the strong interaction between L-serinyl acrylate and Cu 2+ , the PMAm-L hydrogel maintained its robustness (with a swelling ratio of approximately 3 %, a tensile stress of 113 kPa, and a tensile strain of 183 %) and sensing performance (electric conductivity of 0.5 S/m, and gauge factor of 2.1) even after immersion in water for one month, indicating excellent stability. Reversible rupture/reformation of coordinate bonds under deformation confers self-healing properties to the material. Furthermore, a highly sensitive underwater mechanical sensor based on this gel was developed for precise monitoring of subtle human movements, and underwater communication using Morse code was achieved, thereby significantly expanding the functional applications in water environments.
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BIOTECHNOLOGY AND BIOENGINEERING
·
2025
·
IF 3.6
Dong-Xu Jia,Lei Zang,Chi-De Ni,Jia-Le Wang,Hai Yu,Zhi-Qiang Liu,Yu-Guo Zheng
Transaminase (TA)-catalyzed asymmetric amination is considered as a green chemistry approach to synthesize pharmaceutical analogs, but their ability to accept substrate for catalyzing sterically hindered ketones remains a challenge. Sitagliptin is an antihyperglycemic drug to treat type II diabetes. Herein, we exploited an efficient ( R )-selective TA to biosynthesize sitagliptin analog ( R )-3-amino-1-morpholino-4-(2,4,5-trifluorophenyl)butan-1-one. Starting from a previously constructed ( R )-ATA5, two rounds of directed evolution were performed through combining error-prone PCR, site-directed saturation and combinatorial mutagenesis. The resultant variant ATA5/F189H/S236T/M121H showed a 10.2-fold higher activity and a 4-fold improved half-life at 45°C. Crucially, the variant was able to either catalyze the amination of 700 mM substrate with a conversion up to 93.1% and product e.e .> 99% in a cosolvent reaction system, or biotransform 200 mM substrate with a conversion of 97.6% and product e.e .> 99% in a cosolvent-free system. Furthermore, the structural analysis gave insight into how the mutations affected enzymatic activity and thermostability. This study, which consists of constructing a robust ( R )-selective TA and the new synthesis route with the highest conversion ever reported, provides a reference for industrial manufacturing sitagliptin analog.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2025
·
IF 3.9
Songlin Wang,Yu Guo,Qi Liu,Peng Yang,Huabo Li,Lei Liang,Hongying Niu,Qiying Zhang,Yanyan Liu,Jianji Wang
The synthesis of carbonates by using nontoxic feedstocks and ecofriendly heterogeneous catalysts has received great attention but remains a significant challenge. Herein, a series of Mg/Al-codoped porous carbons (MgAl@CM) were developed and applied for transesterification to synthesize methyl phenyl carbonate (MPC). The results showed that MgAl@CM possessed abundant mesopores, large amounts of N/O-containing groups, and dispersed Mg/Al species. And 1Mg5Al@CM-700 exhibited the highest catalytic activity with a diphenyl carbonate conversion of 80.2% and MPC selectivity of 99.6% due to its unique structure and acidic–basic properties, indicating a highly efficient acid–base synergistic catalysis process. Moreover, the catalyst presented good stability and reusability for six recycles without a substantial activity loss. The mechanism based on the synergistic catalysis was investigated. This work provides a novel perspective for the design of heteroatom-doped carbon catalysts to accomplish an efficient MPC synthesis.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Yubo Wang,Lixuan Zeng,Jian Lin,Yongqiang Qian,Zhiling Luo,Feng Huang,Luzhuo Chen
Transparent actuators have significant potential in invisible and camouflage robots. However, traditional transparent actuators are typically unprogrammable and used in a single environment (on-land or in-water), which limits their working abilities in complex environments. Herein, we propose transparent actuators and robots that integrate amphibious actuations, programmable motions, self-healing function and camouflage function together. The actuator is composed of MXene polymer composites, including bone glue, gelatin, MXene (BGGM) and polyethylene terephthalate (PET). The transmittance of BGGM/PET actuator is >80 % at 600 nm wavelength, exhibiting high transparency. On one hand, the actuator shows a light-driven bending deformation on land due to the photothermal effect. Synergistic combination of the self-healing of BGGM and the shape-fixing of PET allows the spatial-programming of actuator to demonstrate light-driven complex deformations. On the other hand, the actuator can be driven by Marangoni effect on water by using BGGM composite as fuels. Adding functional modules enables the spatial-temporal programming of the actuator, so the actuator can showcase time-varying trajectories. Finally, we demonstrate a transparent swimming robot with dual-actuation modes and a transparent actuator that conveys invisible information stealthily while moving through a complex maze on water. This research offers a promising approach to camouflage amphibious robots.
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CATALYSIS LETTERS
·
2019
·Vol. 149
·期 11
·2973-2983
·
IF 2.372
Luo Wei,Du Hui-Jun,Bonku Emmanuel Mintah,Hou Ya-Li,Li Ling-Ling,Wang Xiao-Qiang,Yang Zhong-Hua
Abstract Enantiopure alcohols have received much attention due to their widespread use as pharmaceutical intermediates. In the asymmetric biosynthesis of enantiopure alcohols, the excellent performance of carbonyl reductase makes it be the best choice as the biocatalysts. In this work, an alkali-tolerant carbonyl reductase ( Bs CR, encoded by yueD ) from Bacillus subtilis (strain 168) was obtained through gene mining, and successfully heterologously expressed in Escherichia coli with pET-32a. Bs CR showed excellent alkali resistance and even can keep more than 70% of its peak activity after incubation in Tris–HCl buffer at pH 9.0 for 40 h. The Michaelis constants and maximal velocity of the Bs CR to NADPH (A) and ethyl 4-chloroacetoacetate (B) are \(K_{m}^{A}\) = 5.390 × 10 −2 mmol/L, \(K_{m}^{B}\) = 1.855 mmol/L, and \(V_{max}\) = 147.3 μmol·min −1 ·mg −1 , respectively. Applying the E. coli BL21(DE3)/pET-32a-yueD to catalyze asymmetric reduction of ethyl 4-chloroacetoacetate and acetophenone, the yield of S -CHBE reached 89.9% and S -1-phenyl ethanol reached 66.7%, and e.e. of both products reached more than 99%. This work provides a novel CR for asymmetric reduction. Graphic Abstract A carbonyl reductase ( Bs CR) and its gene were identified through gene mining, and overexpressed in Escherichia coli BL21(DE3) for whole-cell biocatalytic asymmetric reduction
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INTERNATIONAL JOURNAL OF PHARMACEUTICS
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2020
·
IF 4.845
Yang Mai,Diane A.I. Ashiru-Oredope,Zhicheng Yao,Liu Dou,Christine M. Madla,Farhan Taherali,Sudaxshina Murdan,Abdul W. Basit
Active pharmaceutical ingredients are routinely formulated with a range of excipients in the manufacture of drug products. Excipients are considered to be inert components of the formulations, although recent research has contested its inactive behaviour. This study investigated the effect of the excipient polyethylene glycol 400 (PEG 400) on the oral bioavailability and intestinal permeability of cimetidine in male and female human volunteers. Aqueous solutions of cimetidine with pharmaceutically relevant concentrations of PEG 400 at 0% w/v (control), 0.3% w/v, 0.5% w/v, 0.7% w/v and 1.0% w/v were orally administered to both sexes. Urine samples were then collected and assayed for the determination of cimetidine which reflected oral bioavailability. This human study showed that PEG 400 at 0.3% w/v, 0.5% w/v and 0.7% w/v concentrations significantly increased cimetidine bioavailability by 34%, 58% and 41% respectively, although this enhancement was only demonstrated in men and not women (p < 0.05). Ussing chamber transport studies with male human jejunal tissues revealed that cimetidine permeability increased by 26%, 48% and 29% with PEG 400 at 0.3% w/v, 0.5% w/v and 0.7% w/v respectively (p < 0.05). No such enhancement was demonstrated in female tissues (p > 0.05). We have shown that PEG 400 interacts with intestinal P-glycoprotein (P-gp) expression differently in males and females. The mechanistic action of PEG 400 at gut level was further investigated on human jejunal tissues following the pre-treatment of the P-gp inhibitor PSC 833 (valspodar) on the transport of cimetidine. When intestinal P-gp was inhibited, the sex- and dose-dependent modulatory effect of PEG 400 with cimetidine was completely eradicated, thus confirming that PEG 400 has a modulatory – rather than inhibitory – effect on P-gp. In sum, the widely used excipient PEG 400 is not inert at pharmaceutically relevant concentrations and its modulatory effect is demonstrated at a human clinical level. Such pharmacological effects, however, are sex- and dose-dependent via its modulation on intestinal P-gp, as evidenced by the boost in cimetidine bioavailability only in male human volunteers. As such, these findings should be carefully considered towards the co-formulation of PEG 400 with drugs that are P-gp substrates.
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CARBON
·
2012
·
IF 5.378
Dong Ma,Jiantao Lin,Yuyun Chen,Wei Xue,Li-Ming Zhang
Graphene oxide nanosheets were used to induce the in situ gelation of doxorubicin hydrochloride as an antitumor drug. When a very small amount of the graphene oxide was introduced into an aqueous solution of doxorubicin hydrochloride at room temperature, a strong and thixotropic gel was rapidly formed without any polymers or chemical additives. The gelation mechanism was investigated by fluorescence spectroscopy, X-ray diffraction and scanning electron microscopy. The encapsulated doxorubicin hydrochloride was found to show sustained release and antitumor efficacy.
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ACS Catalysis
·
2022
·
IF 13.7
Xiangze Du,Xiaomei Lei,Linyuan Zhou,Yong Peng,Yan Zeng,Huiru Yang,Dan Li,Changwei Hu,Hermenegildo Garcia
In the context of the preparation of liquid fuels derived from biomass with zero CO2 footprint, fatty acids appear as suitable feedstocks. However, reduction of carboxylic acid groups usually requires harsh reaction conditions and the development of efficient solid catalysts. Herein, bimetallic Ni–Mo nitrides have been obtained by a procedure not involving nitridation of the corresponding oxide, but reductive decomposition of the tris(ethylenediamine)nickel molybdate at temperatures between 550 and 700 °C. Successful formation of the Ni3Mo3N nitride is confirmed by X-ray diffraction. Ni3Mo3N samples are found to be efficient catalysts for the hydrodeoxygenation of palmitic acid to C15/C16 alkanes with a combined selectivity over 90 and 100% palmitic acid conversion and higher activity than analogous Ni–Mo nitrides obtained by NH3 nitridation of NiMoO4. Ni3Mo3N is found recyclable with only a slight decay in the catalytic activity upon consecutive reuses attributable to the neutralization of acid sites. The present results show an opportunity that bimetallic nitrides offer as robust advanced solid catalysts for reactions of biomass conversion requiring harsh conditions.
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Inorganic Chemistry Frontiers
·
2023
·Vol. 10
·期 16
·4869-4880
·
IF 7
Ruiting Zhang,Yahong Jin,Yanmei Li,Haoyi Wu,Yihua Hu
Inorganic photochromic materials hold great scientific and technological promise in the field of optical information storage due to their numerous advantages, including an extended color change duration, exceptional fatigue resistance, and robust thermal stability. However, their practical application has been hindered by relatively slow coloring and bleaching rates. In this study, we present a P-type photochromic perovskite material, LiTaO3:Bi3+/Sm3+, with an ultra-fast optical response. LiTaO3:Bi3+/Sm3+ exhibits a rapid coloring time of approximately 25 seconds and an ultra-fast bleaching time of approximately 1 second, achieved through alternating 254 nm and 365 nm light irradiation. Notably, the photobleaching rate of LiTaO3:Bi3+/Sm3+ is currently the fastest among all reported inorganic photochromic materials. The prepared LiTaO3:Bi3+/Sm3+ material exhibits a maximum color change contrast of 26.49% and excellent fatigue resistance. The codopant Bi3+ plays a critical role in creating traps within the host lattice, which greatly enhances photochromism contrast and enables efficient long afterglow luminescence. These dual properties make the material suitable for dual-mode optical information storage in both bright and dark fields. Finally, the excellent optical properties of LiTaO3:Bi3+/Sm3+ are demonstrated in its application for erasable optical information storage vividly.
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PHARMACEUTICAL DEVELOPMENT AND TECHNOLOGY
·
2013
·
IF 1.333
Lin Gu,Zheng hong Wu,Xiaole Qi,Huan He,Xiaoli Ma,Xiaohua Chou,Xiaoguang Wen,Miao Zhang,Fang Jiao
The potential of polyamidoamine (PAMAM) dendrimers as solubility enhancers and oral drug delivery system was well known. Herein, we investigated the possibility of PAMAM dendrimers for promoting the solubility and oral bioavailability of puerarin. In the present study, the effect of PAMAM dendrimers with different generations (G1.5, G2, G2.5, and G3) on the solubility of puerarin was evaluated at different concentrations and pH conditions. Further more, the puerarin–G2 dendrimer complex was conducted for the in vitro hemolytic toxicity studies and pharmacokinetics studies in rats. The solubility of puerarin was significantly higher in the presence of the full generation dendrimers (e.g. G2 and G3). No significant hemolysis was observed on erythrocytes (G2, 0–2.5 mg/mL) in the hemolytic toxicity studies. The pharmacokinetics parameters Tmax, Cmax, and AUC0–8 h of puerarin suspension solution and puerarin–G2 dendrimer complex solution were 0.76 h, 1.50 µg/mL, 7.33 µg·h/mL and 0.33 h, 6.49 µg/mL, 14.02 µg·h/mL, respectively. These studies demonstrate that PAMAM dendrimers may be a promising strategy for peroral delivery of puerarin.
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Chemical Engineering and Processing-Process Intensification
·
2019
·
IF 3.031
Suqi Zhang,Jie Zhang,Jian Sun,Zhiyong Tang
A novel capillary microphotoreactor (MPR) packed with TiO 2 -coated glass beads was developed in this work and its photocatalytic performance was evaluated using degradation of methylene blue (MB) as a model reaction. As compared to conventional wall-coated MPR, the use of glass beads as packing material not only provides a larger surface area for catalyst immobilization and shortens the mass transfer route, but also introduces flow perturbation. An appropriate size of glass beads should be chosen for packing because there is a tradeoff between increased catalysts coating area and decreased light penetration. It was found out that nearly 100 % degradation efficiency could be achieved in 80# glass beads packed MPR within short residence time (20 s), which was more than 2 orders of magnitude larger than value obtained in wall-coated MPR under the same operational conditions. Moreover, the packed MPR showed good durability, which declined by about 17 % after 6 h of operation and then remained stable for next 19.5 h.
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