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ACS Applied Materials & Interfaces · 2018 · IF 8.097

Bioinspired Dual-Enzyme Colloidosome Reactors for High-Performance Biphasic Catalysis

Zhenning Liu,Bingdi Wang,Shenghui Jin,Zhida Wang,Lei Wang,Song Liang

In this paper, a novel method for the construction of colloidosomes as a microreactor for dual-enzyme cascade biphasic reaction has been reported. A lipase–glucose oxidase (GOx) enzyme pair is employed in this system. A water-soluble enzyme GOx is compartmentalized inside the colloidosomes. A hydrophobic environment-favored enzyme Candida Antarctica lipase B (CalB) is adsorbed on the outer surfaces of the colloidosomes. The catalysis system is set up by introducing these dual-enzyme-immobilized microcapsules into acetic ether. H2O2 is produced in the aqueous phase by the doped GOx, and then H2O2 diffused out of the microcapsules is utilized by CalB to catalyze the oxidation of ethyl acetate. Finally, the formed peracids oxidized N-heteroaromatic in situ. Furthermore, no obvious yield decline is observed in four reaction cycles. Thus, our work provides a new strategy for the design of high-performance biomimicking reactors for multiple enzyme cascade reactions and further expands the potential application area of colloidosomes.

研究领域: 生物化学 · 材料科学
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS · 2020 · IF 3.99

Study in the experimental manipulation of Janus particle synthesis via emulsion-based method

Zhenxin Chu,Bin Zhong,Wanrong Zhou,Pengcheng Cui,Jiale Gu,Bingbing Tian,Oluseyi S. Olasoju,Xiaohua Zhang,Wei Sun

This study focused on the investigation in the influencing factors of the Granick’s method for Janus particle synthesis , in which selective modification of colloidosome made from a Pickering emulsion-based process was the essential strategy. Homogenizer with high shearing forces was introduced to make stable emulsion. With increased stirring speed of the homogenizer, the sizes of the colloidosomes decrease. And the stirring time of the homogenizer and the paraffin melting point have also been proved to have influence on the size distribution of colloidosomes as well as on the assembly morphology of the silica particles on the surface of the wax sphere. 160 s of the working time and the melting point of 53−57 °C were tested respectively to be the optimal condition for making the ideal colloidosomes. By using the optimized experimental conditions, silica particles with diameters of 200, 400, and 600 nm all had success in making fine colloidosomes. The Janus character were characterized by demonstrating the abilities of interfacial assembly and anisotropic structural growth of the resultant products from the optimized procedure. The research provides the conclusions of optimal experimental conditions as references for achieving scalable synthesis of Janus particles with satisfactory quality. This research could serve as a guidance to effective implementation of Granick’s method of Janus particle synthesis.

CAS / MDL: 112-04-9
研究领域: 材料科学 · 化学工程
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Inorganic Chemistry Frontiers · 2024 · IF 6.1

Bioinspired electron carrier mediated transmembrane photocatalytic hydrogen evolution in silica colloidosomes

Chengkun Bai,Bingdi Wang,Zhengshun Jiang,Chunying Lv,Zhenning Liu,Shiyu Wang,Song Liang,Hongying Zang

Inspired by the ordered processes of chloroplasts in photosynthesis involving coordinative linkages and efficient compartmentalization, a bioinspired compartmentalized photocatalytic system (BCPS) with an inorganic compartment is designed for photocatalytic hydrogen evolution with light driven electron carrier mediated cross-membrane energy transport. A typical BCPS comprises silica colloidosomes containing co-catalysts as microreactors, where positively charged N-methyl-4-cyanopyridinium (MCP+) serves as the electron carrier. The MCP+ molecules harvest energy from photoexcited g-C3N4, and transit to electrically neutral species MCP0, which can pass the colloidosome. Driven by light, the MCP0 diffuse across the membrane and transport electrons to H+ for hydrogen evolution, in which Pt particles are employed as co-catalysts. Analogous to natural photosynthesis, hydrogen evolution occurs within compartments, separating light and dark reactions, protecting the dark reaction from interference during light harvesting and minimizing potential side effects. The system enables sustained evolution of hydrogen with a higher yield than that with the control catalysis in a bulk catalyst suspension. The dramatic influence of SDS on the hydrogen evolution was revealed, and a possible mechanism of electron carrier amount buffering was proposed.

研究领域: 化学 · 材料科学 · 仿生学
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ACS Applied Materials & Interfaces · 2024 · IF 8.3

Multifunctional ZnO-Loaded Colloidosomes with Multiple Synergies as a UV Filter

Jia Jia,Rong-Kun Liu,Qian Sun,Jie-Xin Wang

ZnO nanoparticles with high safety and stability are often used as active ingredients in sunscreens to protect the skin from ultraviolet rays. However, ZnO nanoparticles are easy to agglomerate, which will significantly affect the ultraviolet absorption and bacteriostatic properties, and the reactive oxygen species induced by the photocatalytic activity may result in irreversible secondary damage to the skin. Herein, the ZnO nanoparticles are dispersed uniformly on the surface of latex particles, and these composite particles are used as shell materials to construct self-assembled colloidosomes by high-gravity technology, which can improve the application properties with synergistic enrichment of the hollow structure. The ultraviolet resistance of colloidosomes is significantly higher than that of the pure ZnO nanoparticles. The higher the loading capacity, the more obvious the inhibition effect of colloidosomes on the growth of Gram bacteria. Furthermore, the antioxidant anthocyanin is in situ encapsulated in colloidosomes, and at a concentration of 2 g/L, the high free radical scavenging rate of 78% can be achieved. The construction of multifunctional colloidosomes provides a route for sunscreen and cosmetics applications.

研究领域: 材料科学 · 生物学 · 化妆品科学
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ACS Applied Materials & Interfaces · 2022 · IF 10.383

Lipase-Entrapped Colloidosomes with Tunable Positioning at the Oil–Water Interface for Pickering Emulsion-Enhanced Biocatalysis

Qi Zeng,Mengmeng Sun,Xin Xie,Yuli Zhang,Haoyue Hou,Xingyuan Fang,Ting Guo,Hao Yuan,Tao Meng

Pickering interfacial biocatalysis (PIB) paves the way for efficient enzymatic catalysis in the biphasic system. However, the Pickering interfacial biocatalysts located on the oil–water interface still face the inevitable deactivation when one of the phases contains the reactant that inactivates the enzyme. Herein, the positioning of lipase-entrapped colloidosomes (LECs) at the emulsion interface is rationally designed by physically tuning the wettability, which allows LECs to protrude into the selected phase to protect the lipase away from the damage of the reactant. As a proof of concept, LECs with different positioning at the interface are used as Pickering interfacial biocatalysts to produce biodiesel by esterification of lauric acid and methanol. Impressively, the LECs that protrude into the oil phase possess an optimal catalytic performance to protect more lipases away from the damage of the reactant of short-chain alcohol, which shows an 8.18-fold enhancement in specific activity relative to the free lipase, reach a biodiesel yield of 80.37% after 8 h, and retain the 96.44% of relative activity after 10 cycles. This study provides a novel and robust platform for Pickering emulsion-enhanced biocatalysis.

研究领域: 生物化学 · 材料科学 · 催化工程
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CHEMICAL ENGINEERING JOURNAL · 2017 · IF 6.216

Construction of biocatalytic colloidosome using lipase-containing dendritic mesoporous silica nanospheres for enhanced enzyme catalysis

Jing Gao,Yun Wang,Yingjie Du,Liya Zhou,Ying He,Li Ma,Luyan Yin,Weixi Kong,Yanjun Jiang

The synthesis of silica-based colloidosome with a magnetic solid core via Pickering emulsification and its use as an immobilized enzyme system is described in this work. Lipase B from Candida antarctica (CALB) was physically adsorbed on the material to form the immobilized enzyme (LP@colloidosome) and the enzyme loading was 166.3   mg/g support . The specific hydrolytic activity of LP@colloidosome was 209.6   U/g support and its immobilization yield was 22.08%. The stability test indicated that LP@colloidosome can retain 49% of original activity after incubation at 50   °C for 6   h and 105.6% of original activity after incubation in t -butanol for 96   h, while the free lipase lost most the initial activity under the same condition. These findings showed that LP@colloidosome had the enhanced thermal stability and tolerance in organic solvents. Meanwhile, LP@colloidosome can be easily recovered by magnet due to the addition of modified Fe 3 O 4 nanoparticles in the solid core. LP@colloidosome was successfully used to catalyze the esterification of fatty acids and alcohols with different length in organic solvent. The yields of the corresponding esters that catalyzed by LP@colloidosome were significantly higher than those catalyzed by free lipase. Additionally, the versatility of LP@colloidosome was also verified in the synthesis of glycerol carbonate through transesterification. The results indicated that biosynthesis of glycerol carbonate from glycerol using the LP@colloidosome (6.1   wt%) as catalyst afforded 85.20% of conversion rate at 60   °C. This work offers insight into the design of colloidosome for efficient immobilization of lipase as well as improvement of the lipase’s properties.

CAS / MDL: 77-73-6 87-61-6
研究领域: 生物化学 · 材料科学 · 酶工程
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ADVANCED FUNCTIONAL MATERIALS · 2025 · IF 19

Rotating Liquid Marble Microreactors for Enhanced Enzymatic Reactions

Weijie Jiang,Xin Guan,Wei Liu,Yunxing Li,Hang Jiang,To Ngai

Droplet-based microreactors hold great promise for enzymatic reactions, but their efficiency is often hindered by static operation and poor mass transfer. This study tackles these limitations through the innovative application of dynamic rotating magnetic liquid marbles (LMs) stabilized by proteinaceous colloidosomes. The colloidosomes feature an outer layer of densely-packed hydrophobic silica nanoparticles and an inner zein layer that integrates magnetic particles and enzymes, enhancing hydrophobicity, magnetic responsiveness, and enzyme immobilization. As proof of the concept, glucose oxidase (GOx) is encapsulated within the colloidosomes and horseradish peroxidase (HRP) inside the LMs, respectively. The results demonstrate that the rotating LMs significantly accelerated enzymatic cascade reactions when exposed to an external magnetic field. Moreover, by applying this approach to biphasic enzymatic systems, positioning the LMs at the water/toluene interface yields a 2.2-fold increase in conversion rate compared to static systems, as shown in lipase-driven esterification reactions. This advancement not only broadens the potential applications of LMs but also offers a promising strategy for enhancing catalytic processes in heterogeneous systems.

研究领域: 生物化学 · 材料科学 · 化学工程
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Science China-Chemistry · 2020 ·Vol. 63 ·期 10 ·1507-1514 · IF 6.356

Crosstalk-free colloidosomes for high throughput single-molecule protein analysis

Yin Kun,Zeng Xi,Liang Xuan,Wei Haopai,Zeng Huimin,Qi Wei,Ruan Weidong,Song Yanling,Yang Chaoyong,Zhu Zhi

Droplet microfluidics is a powerful platform for high-throughput single-molecule protein analysis. However, the issues of coalescence and crosstalk of droplets compromise the accuracy of detection and hinder its wide application. To address these limitations, a novel colloidosome-based method was presented by combining a Pickering emulsion with droplet microfluidics for single-molecule protein analysis. Utilizing the self-assembly of easily synthesized colloidal surfactant F-SiO 2 NPs at the water/oil interface, the colloidosomes are rigidly stabilized and can effectively avoid the leakage of fluorescent molecules. The crosstalk-free colloidosomes enable high-throughput single-molecule protein analysis, including heterogenous dynamic studies and digital detection. As a robust and accurate method, colloidosome-based microfluidics is promising as a powerful tool for a wide variety of applications, such as directed enzyme evolution, digital enzyme-linked immunosorbent assay (ELISA), and screening of antibiotics.

CAS / MDL: 101947-16-4
研究领域: 生物技术 · 分析化学 · 材料科学
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ANALYTICAL CHEMISTRY · 2019 · IF 6.35

Ultrasensitive Electrochemical Immunoassay Based on Cargo Release from Nanosized PbS Colloidosomes

Xiujuan Han,Hongfang Zhang,Jianbin Zheng

Colloidosome is a novel nanostructure composed of millions of colloid particles. In this work, nanosized PbS colloidosomes were initially prepared and applied as nanoprobes for an ultrasensitive immunoassay. The colloidosomes were simply prepared in mild conditions by assembling the elementary approximately 8 nm PbS nanoparticles at the water-in-oil interface of emulsion droplets. To enhance the rigidity and biocompatibility of the colloidosomes, interfacial polymer was introduced by utilizing self-polymerization of dopamine. By treating with dilute nitric acid, a bursting release of lead ions from the colloidosomes occurred and the lead ions can be detected easily by anodic stripping voltammetry. In this way, a colloidosome-based electrochemical immunoassay was developed by using the nanosized PbS colloidosomes as electroactive labels. The proposed method featured a linear calibration range from 10 fg·mL–1 to 100 ng·mL–1 with a low detection limit of 3.4 fg·mL–1 for the detection of human epididymis protein 4. This work introduced a new member for the family of colloidosomes and offered a novel perspective for the rational implementation of various colloidosomes for novel low-abundance cancer biomarkers analysis.

研究领域: 纳米技术 · 分析化学 · 生物标志物检测
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ACS Applied Materials & Interfaces · 2013 · IF 5.008

Preparation of Cell-Embedded Colloidosomes in an Oil-in-Water Emulsion

Yi Gong,Ai Mei Zhu,Qiu Gen Zhang,Mei Ling Ye,Hai Tao Wang,Qing Lin Liu

Cell encapsulation by locking the interfacial microgels in a water-in-oil Pickering emulsion has currently been attracting intensive attention because of the biofriendly reaction condition. Various kinds of functional microgels can only stabilize an oil-in-water Pickering emulsion, and it is thus difficult to encapsulate cells in the emulsion where the cells are usually dispersed in the continuous phase. Herein, we introduce a facile method for preparing cell-embedded colloidosomes in an oil-in-water emulsion via polyelectrolyte complexation. Escherichia coli (E. coli) was chosen as a model cell and embedded in the thin shell of chitosan/poly(N-isopropylacrylamide-co-acrylic acid) (P(NIPAM-co-AAc)) microcapsules. This is beneficial for expressing cell function because of the little resistance of mass exchange between the embedded cells and the external environment. Cells can be used in biocatalysis or biomedicine and our product will hold great promises to improve the performance in those fields. The synthesis route presents a platform to prepare cell-embedded microcapsules in an oil-in-water Pickering emulsion in a facile and biocompatible way. First, an emulsion stabilized by P(NIPAM-co-AAc) microgels was prepared. Then, the interfacial microgels in the emulsion were locked by chitosan to form colloidosomes. The mechanism of cell encapsulation in this system was studied via fluorescent labeling. The viability of E. coli after encapsulation is ca. 90%. Encapsulated E. coli is able to metabolize glucose from solution, and exhibits a slower rate than free E. coli. This demonstrates a diffusion constraint through the colloidosome shell.

CAS / MDL: 9012-76-4
研究领域: 生物技术 · 材料科学 · 化学工程
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Bioactive Materials · 2022 · IF 16.874

Microcluster colloidosomes for hemostat delivery into complex wounds: A platform inspired by the attack action of torpedoes

Bitao Lu,Enling Hu,Ruiqi Xie,Kun Yu,Fei Lu,Rong Bao,Chenhui Wang,Guangqian Lan,Fangyin Dai

Complex yet lethal wounds with uncontrollable bleeding hinder conventional hemostats from clotting blood at the source or deep sites of injury vasculature, thereby causing massive blood loss and significantly increased mortality. Inspired by the attack action of torpedoes, we synthesized microcluster (MC) colloidosomes equipped with magnetic-mediated navigation and “blast” systems to deliver hemostats into the cavity of vase-type wounds. CaCO 3 /Fe 2 O 3 (CF) microparticles functionalized with Arg-Gly-Asp (RGD) modified polyelectrolyte multilayers were co-assembled with oppositely charged zwitterionic carbon dots (CDs) to form MC colloidosomes, which were loaded with thrombin and protonated tranexamic acid (TXA-NH 3 + ). The composite microparticles moved against blood flow under magnetic mediation and simultaneously disassembled for the burst release of thrombin stimulated by TXA-NH 3 + . The CO 2 bubbles generated during disassembly produced a “blast” that propelled thrombin into the wound cavity. Severe bleeding in a vase-type hemorrhage model in the rabbit liver was rapidly controlled within ∼60 s. Furthermore, in vivo subcutaneous muscle and liver implantation models demonstrated excellent biodegradability of MC colloidosomes. This study is the first to propose a novel strategy based on the principle of torpedoes for transporting hemostats into vase-type wounds to achieve rapid hemostasis, creating a new paradigm for combating trauma treatment.

研究领域: 生物医学工程 · 材料科学 · 止血 · 伤口愈合
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Research · 2024 · IF 8.5

pH-Responsive Theranostic Colloidosome Drug Carriers Enable Real-Time Imaging of Targeted Thrombolytic Process with Near-Infrared-II for Deep Venous Thrombosis

Yaxin Ye,Zhechang Chen,Shengzhang Zhang,Paul Slezak,Fei Lu,Ruiqi Xie,Dongwon Lee,Guangqian Lan,Enling Hu

Thrombosis can cause life-threatening disorders. Unfortunately, current therapeutic methods for thrombosis using injecting thrombolytic medicines systemically resulted in unexpected bleeding complications. Moreover, the absence of practical imaging tools for thrombi raised dangers of undertreatment and overtreatment. This study develops a theranostic drug carrier, Pkr(IR-Ca/Pda-uPA)-cRGD, that enables real-time monitoring of the targeted thrombolytic process of deep vein thrombosis (DVT). Pkr(IR-Ca/Pda-uPA)-cRGD, which is prepared from a Pickering-emulsion-like system, encapsulates both near-infrared-II (NIR-II) contrast agent (IR-1048 dye, loading capacity: 28%) and urokinase plasminogen activators (uPAs, encapsulation efficiency: 89%), pioneering the loading of multiple drugs with contrasting hydrophilicity into one single-drug carrier. Upon intravenous injection, Pkr(IR-Ca/Pda-uPA)-cRGD considerably targets to thrombi selectively (targeting rate: 91%) and disintegrates in response to acidic thrombi to release IR-1048 dye and uPA for imaging and thrombolysis, respectively. Investigations indicate that Pkr(IR-Ca/Pda-uPA)-cRGD enabled real-time visualization of targeted thrombolysis using NIR-II imaging in DVT models, in which thrombi were eliminated (120 min after drug injection) without bleeding complications. This may be the first study using convenient NIR-II imaging for real-time visualization of targeted thrombolysis. It represents the precision medicine that enables rapid response to acquire instantaneous medical images and make necessary real-time adjustments to diagnostic and therapeutic protocols during treatment.

研究领域: 药学 · 生物医学工程 · 治疗诊断学 · 医学影像
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