INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2025
·
IF 8.5
Qingqing Liu,Yue Tang,Mingming Xiong,Yunting Yang,Yanting Liu,Zhengping Duan,Wei Luo,Yisha Xie,Yongjun Yuan
Lipase is widely used in the food industry, but its catalytic efficiency is limited by the insufficient enzyme-substrate contact. To address this issue, chitosan-zein complex particles immobilized lipase (CZPs-lipase) and the corresponding Pickering emulsion catalytic system (PEC) were fabricated. The results showed that the incorporation of zein increased the three-phase contact angle of the particles and decreased the particle size, facilitating lipase immobilization. However, the reduced ζ-potential of the particles was unfavorable for the lipase immobilization by electrostatic adsorption. As a compromise, the maximum immobilized lipase activity was obtained at a chitosan:zein mass ratio of 1:2 (CZPs 1:2 -lipase). In addition, the PEC stabilized by CZPs-lipase had a significantly ( P < 0.05) smaller particle size than that stabilized by chitosan-lipase particles. Consequently, after 120 min of reaction, the hydrolysis rate of p-nitrophenol palmitate in the PEC stabilized by CZPs 1:2 -lipase was 1.66 and 3.67 times that of the free lipase emulsion and the free lipase biphasic catalytic system, respectively. Meanwhile, after 180 min of reaction, the hydrolysis rate of corn oil and soybean oil in the PEC reached 75.68 ± 1.85 % and 96.27 ± 2.26 %, respectively, significantly ( P < 0.05) higher than that in the free lipase emulsion. After five cycles, the relative hydrolysis rate remained at approximately 85 %. This efficient and PEC has considerable potential for applications in the food industry.
研究领域:
食品科学
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生物技术
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产品关联
DOI
PubMed
高影响因子
Surfaces and Interfaces
·
2024
·
IF 5.7
Hao Zhang,Zhengyuan Tao,Ziqi Yu,Tiantian Zhu,Hanlin Rao,Badusha Mohamad Ali,Jianli Wang
Pickering interfacial catalysts (PICs) have emerged as a promising solution for simultaneously enhancing and catalyzing liquid-liquid biphasic reactions. In this study, we successfully synthesized dumbbell-shaped Janus structured polymeric nanoparticles with one side anchored imidazolium-TEMPO (im-C 4 -TEMPO@JPP) as Pickering interfacial catalyst for the oxidation of alcohols using the Anelli-Montanari reaction system. In the Pickering emulsion system, the im-C 4 -TEMPO@JPPs particles are assembled at the W/O interface due to the hydrophilicity of imidazolium-TEMPO anchored lobe which enables excellent amphiphilic character of the polymeric Janus dumbbell. Moreover, the im-C 4 -TEMPO@JPPs particles reduce the interfacial tension from 27.82 to 18.43 mN/m. This excellent interfacial adsorption capacity of im-C 4 -TEMPO@JPPs strongly stabilizes the water/dichloromethane Pickering emulsion over two months (emulsion volume fraction >90 %), thus providing an efficient reaction platform for liquid-liquid biphasic reactions. As a result, the constructed Pickering emulsion system efficiently catalyzes the oxidation of cinnamyl alcohol to cinnamaldehyde under static conditions. After 1 hour of reaction, the conversion of cinnamyl alcohol achieved 97.1 % with a selectivity of 99 %, nearly the same level relative to stirring intensified biphasic reaction. Hence, this novel PIC effectively improves the efficiency and sustainability of liquid-liquid biphasic catalytic reactions .
研究领域:
化学工程
·
材料科学
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产品关联
DOI
高影响因子
Journal of Physical Chemistry C
·
2019
·
IF 4.309
Kecheng Hu,Jun Tang,Shixiong Cao,Qi Zhang,Jianli Wang,Zhibin Ye
We report in this paper the design and synthesis of a pH-responsive polymeric interfacial catalyst (PIC) via one-step grafting of 2,2,6,6-tetramethylpiperidine-N-oxyl (TEMPO) onto a polyaryletherketone having pendant benzimidazole groups (SCBI-PAEK-6F). The TEMPO-functionalized polymer has been systematically characterized with 1H nuclear magnetic resonance, Fourier-transform infrared spectroscopy, elemental analysis, contact angle, and transmission electron microscopy. Moreover, this well-designed polymer has been applied in the oxidation of alcohols under Montanari conditions. It is found that the functionalized polymer can aggregate at the water–oil interface and act as an efficient stabilizer to facilitate the formation of a stable Pickering emulsion, which shows outstanding catalytic activity for alcohol oxidation through the microreactor mechanism. Moreover, the PIC is featured with desirable high pH responsiveness due to the valuable benzimidazole groups. De-emulsification of the Pickering emulsion reaction system can be conveniently triggered by simply tuning the system pH value to 3, thus facilitating the facile recovery of the PIC. In addition, the sustainable catalyst can be reused for subsequent cycles of alcohol oxidation without appreciable loss in catalytic activity or selectivity.
研究领域:
材料化学
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催化化学
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有机合成
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产品关联
DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2023
·Vol. 33
·期 30
·2300589
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IF 19
Chao Sun,Bing Zhao,Jing Mao,Ke-Hua Dai,Zhen-yu Wang,Lin-bo Tang,He-zhang Chen,Xia-hui Zhang,Jun-chao Zheng
LiCoO 2 plays a key role in energy storage devices due to its high energy density. And the volumetric energy density of LiCoO 2 cathode can be significantly improved by increasing the charging cut-off voltage to 4.6 V. However, the increase in resistance at the LiCoO 2 interface, and the damage to the LiCoO 2 from the outside to the inside by the HF generated that caused by the decomposition of the organic electrolyte and LiPF 6 under 4.6 V conditions are not conducive to structural stability during cycling. Here, it is shown that the decomposition of electrolyte and LiPF 6 is effectively mitigated by inhibiting the interfacial catalytic activity of LiCoO 2 using an atomically thin layer of MXenes as a interlayer. Density functional theory results suggest that the decomposition energy of LiPF 6 is 1.13 and 3.21 eV at the interface of LiCoO 2 and MXenes, respectively. Time of Flight Secondary Ion Mass Spectrometry results further indicate that the decomposition products of the organic electrolyte and LiPF 6 have a thinner thickness at the interface of MXenes (5 nm) than LiCoO 2 (10 nm). This study provides a new and universal strategy for stabilizing the cathode interface to support the development of high energy density lithium-ion batteries.
研究领域:
材料科学
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电化学
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能源存储
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DOI
高影响因子
ACS Applied Materials & Interfaces
·
2020
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IF 8.758
Hang Jiang,Liangdong Liu,Yunxing Li,Shouwei Yin,To Ngai
Water-in-oil (w/o) Pickering emulsions have received considerable attention in biphasic enzymatic catalysis for their advantages of good stability, large interfacial area, and ease of product separation. However, enzymes are commonly encapsulated in the interior of aqueous droplets, which inevitably increases the diffusional resistance to catalysis. Alternatively, enzymes are immobilized or trapped into Pickering stabilizers. Often, however, these approaches suffer from leaching and a decrease of enzyme activity during the chemical treatments. We report here a new Pickering interfacial biocatalysis platform with efficient enzyme encapsulation, binary particle composition, and high catalytic performance. Our approach is based on w/o Pickering emulsions stabilized by binary particles consisting of hard silica and soft, pH-responsive microgel particles. We demonstrate that pH-responsive microgels can simultaneously stabilize a w/o Pickering emulsion, encapsulate enzymes, and catalyze reactions at the water/oil interface. In addition, we show that the coordination with rigid silica nanoparticles as additional stabilizers markedly improves the emulsion structure and will provide a new avenue for the preparation of w/o Pickering emulsion and concept of biphasic catalysis.
研究领域:
化学工程
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生物催化
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
LANGMUIR
·
2024
·
IF 3.7
Zhuoxue Li,Yunlei Shi,Yimian Ding,Dazhen Xiong,Zhiyong Li,Huiyong Wang,Jikuan Qiu,Xiaopeng Xuan,Jianji Wang
A Pickering emulsion is a natural microreactor for interfacial catalysis in which an emulsifier is critical. Recently, a metal–organic framework (MOF) has attracted attention to emulsify water–organic mixtures for constructing a Pickering emulsion. However, a few stimuli-responsive Pickering emulsions based on MOFs have been reported, and the MOF emulsifiers cannot be regenerated at room temperature. Herein, the Zr-MOF with a rodlike morphology is synthesized using ionic liquid as a modulator and then modified with n-(trimethoxysilylpropyl)imidazole (C3im) to prepare a series of functionalized Zr-MOFs (MOF-C3im). It is found that MOF-C3im is an excellent emulsifier to construct stable and CO2-responsive Pickering emulsions even at low content (>0.20 wt %). Notably, the emulsification and demulsification of the emulsions can be easily and reversibly switched by bubbling of CO2 and N2 alternatively at room temperature because CO2 and imidazole molecules anchored on the Zr-MOF underwent a reversible acid–base reaction, resulting in an obvious change in the wettability of the emulsifier. As a proof of concept, the reduction reactions of nitrobenzene have been successfully carried out in these Pickering emulsions, demonstrating the efficient integration as a microreactor for chemical reaction, product separation, and emulsifier recycling under ambient conditions. This strategy provides an innovative option to develop stimulus-responsive Pickering emulsions for sustainable chemical processes.
研究领域:
材料科学
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化学工程
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催化反应
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Advanced Materials Interfaces
·
2022
·Vol. 9
·期 28
·2200802
·
IF 6.389
Yan Liu,Yanyan Li,Meiqi Gao,Chenyi Yuan,Yuan Ren,Wenhe Xie,Xuanyu Yang,Yaozu Liao,Yidong Zou,Yonghui Deng
The emerging combination of Internet of Things requires the development of intelligent gas sensor, and semiconductor gas sensors based on metal oxides have been widely applied in industrial production, environmental monitoring, and food safety. Although versatile nanomaterials have been exploited as gas sensitive materials, restricted gas sensing performance including sensitivity, selectivity and stability, is still the fatal problem of practical applications. Herein, inspired by heteratomic doping engineering, unique rare earth erbium (Er)-doped mesoporous tungsten oxide (Er/mWO 3 ) has been synthesized via one-step collaborative coassembly strategy, and Er ion-doped mWO 3 exhibited peculiarly hexagonal mesostructure ( P6 3 /mmc ), tunable specific surface area (58.1–78.3 m 2 g –1 ), uniform mesoporous size and highly crystallized framework with heteroatomic pore wall doping. The introduction of Er can significantly adjust the micro/nano structure and band characteristics, and 1.5 wt% Er-doped mWO 3 displays superior acetone sensing performance, including high response values (107 for 50 ppm), rapid response–recovery dynamics (9/56 s), prominent acetone selectivity, low concentration detection (125 ppb), anti-humidity property and excellent long-term stability. Such an excellent sensing performance is mainly attributed to unique interfaces catalytic sites induced by heteroatom interstitial doping. This finding opens a door for the design of smart gas sensors for environmental monitoring and industrial safety.
研究领域:
材料科学
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传感器技术
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环境监测
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产品关联
DOI
高影响因子
JOURNAL OF CATALYSIS
·
2024
·
IF 6.5
Lei Wang,Badusha Mohamad Ali,Siyang Yu,Sheng Liang,Qingqing Huang,Hao Zhang,Lingyu Zhu,Jianli Wang
Pickering interfacial catalysts incorporated with amphiphilic architecture significantly expand the sustainability of green catalysis systems. In this work, we present precise and well-designed dumbbell-shaped Janus-structured polymeric nanoparticles with one-side anchored palladium clusters (DB-JPP-Pd) as Pickering interfacial catalyst for static hydrogenations. The large wettability difference of each lobe renders the prominent amphiphilicity of the dumbbell-shaped DB-JPP-Pd. The amphiphilic Janus catalyst displays excellent interfacial activity and extensively reduces the interfacial tension from 34.06 ± 0.13 to 20.54 ± 0.31 mN/m, promoting the formation of a more stable Pickering emulsion than that of the bulk PS-Pd catalyst, which can continuously provide a large interfacial area and shorten the molecular mass transfer distance during the reaction process. As a result, the DB-JPP-Pd catalyzed nitroarene reduction reaction exhibits a normalized reaction rate constant (k nor ) of 3.39 min −1 ⋅g −1 ⋅L under static conditions, which is 56.5 times higher than that of bulk PS-Pd. The constructed Pickering interfacial catalysis (PIC) system converts all the nitrobenzene into aniline within three minutes and possesses excellent selectivity in hydrogenations of different nitro aromatics. In addition, the emulsion catalytic system was conveniently recycled for ten consecutive runs. Hence, this unique amphiphilic dumbbell-shaped catalyst effectively develops an efficient static biphasic catalysis system.
研究领域:
材料科学
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催化化学
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环境科学
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产品关联
DOI
高影响因子
GREEN CHEMISTRY
·
2019
·Vol. 21
·期 9
·2412-2427
·
IF 9.405
Liang Qi,Zhigang Luo,Xuanxuan Lu
In this work, maize starch (MS) was successively modified via an esterification reaction with acetic anhydride (AA) and phthalic anhydride (PTA). Combined with the gelatinization–precipitation process, the formed starch nanoparticles at an AA/PTA ratio of 2 (MS-AP (2)) and 3 (MS-AP (3)) had similar regular spheres but distinct surface characteristics. In order to enhance the activity of lipase B from Candida antarctica (CALB) in an organic solvent, we designed an oil-in-water (o/w) and a water-in-oil (w/o) Pickering interfacial catalytic system simultaneously by utilizing MS-AP (2) and MS-AP (3) as robust Pickering emulsion stabilizers. Impressively, during the esterification of 1-butanol and vinyl acetate, the specific activity of CALB in the o/w (0.0843 U μL−1) or w/o (0.0724 U μL−1) Pickering interfacial catalytic system was much higher than that of free enzymes in the monophasic (0.0198 U μL−1) and biphasic (0.0282 U μL−1) system. Moreover, after preliminarily elaborating mass transfer discrepancies between the o/w and w/o Pickering interfacial catalytic systems and calculating their mass transfer resistance, we clarified the effects of the location of these two phases on the catalytic capacity of the Pickering emulsion. Impressively, both Pickering interfacial catalytic systems exhibited high effectiveness in product separation. It was found that the w/o Pickering emulsion enabled the organic product to be facilely isolated through a simple decantation, while the o/w Pickering emulsion achieved similar results after adjusting the system temperature. The bio-based nanomaterials and simple protocol, in conjunction with the stability to simultaneously achieve high catalysis efficiency and excellent recyclability, makes us believe that this starch nanoparticle-based Pickering interfacial catalytic system is a promising system for meeting the requirements of green and sustainable chemistry.
研究领域:
生物化学
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材料科学
·
绿色化学
✓ 已验证
产品关联
DOI
高影响因子
Processes
·
2023
·Vol. 11
·期 4
·1070
·
IF 3.5
Huihui Lv,Zebo Wang,Jialong An,Zhanfeng Li,Lei Shi,Yuanyuan Shan
Water is increasingly being used as a solvent in place of organic solvent in order to meet the demand for green chemical synthesis. Nevertheless, many of the reaction substrates are organic matter, which have low water solubility, resulting in a low reaction interface and limiting the development of organic-water biphasic systems. A surfactant is typically added to the two-phase system to form an emulsion to increase the contact area between the organic phase and the water. Compared to ordinary emulsion stabilized with the surfactant, Pickering emulsion offers better adhesion resistance, biocompatibility, and environmental friendliness. It possesses unrivaled benefits as an emulsifier and catalyst in a two-phase interfacial catalysis system (PIC). In this study, the amine group (NNDB) was employed to alter the surface of graphene oxide (GO). A stable Pickering emulsion was created by adsorbing GO-NNDB on the toluene–water interface. It was determined that the emulsion system had good stability by analyzing digital photographs and microscope images of droplets at various temperatures, and fluorescence microscopy images of emulsion droplets created by both newly added and recovered emulsifiers. This work provided the groundwork for future applications of Pickering emulsion in interfacial catalysis.
研究领域:
化学工程
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Rongrui Deng,Shuangshuang Tan,Zhongting Wang,Rong Li,Guanjie Lu,Baihua Qu,Le Tong,Ronghua Wang,Chaohe Xu,Guangsheng Huang,Jingfeng Wang,Aitao Tang,Xiaoyuan Zhou,Fusheng Pan
Magnesium-ion batteries (MIBs) have great potential in large-scale energy storage field with high capacity, excellent safety, and low cost. However, the strong solvation effect of Mg2+ will lead to the formation of solvated ions in electrolytes with larger size and sluggish diffusion/reaction kinetics. Here, the concept of interfacial catalytic bond breaking is first introduced into the cathode design of MIBs by hybriding MoS2 quantum dots with VS4 (VS4@MQDs) as the cathode. The “in situ dynamic catalysis and re-equilibration” effects can catalyze the Cl–Mg bond breaking and trigger single Mg2+ insertion/extraction chemistries, which can significantly accelerate the diffusion and reaction kinetics, as verified by the decreased diffusion energy barriers (0.26 eV for Mg2+ vs 2.47 eV for MgCl+) and fast diffusion coefficient. Benefitting from these dynamic catalysis effects, the constructed VS4@MQD-based MIBs deliver a high discharge capacity of ∼120 mA h g–1 at 200 mA g–1 and a long-term cyclic stability of 1000 cycles at 1 A g–1. The improved performance and detailed characterizations well prove that the active ions in MIBs change from MgCl+/Mg2Cl3+ to Mg2+ with fast kinetics.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
Journal of Oleo Science
·
2023
·
IF 1.5
Siyuan Zou,Hao Zhang,Jianli Wang
Recently, Pickering interfacial catalyst (PIC) was widely applied for liquid-liquid reactions, in view of not only intensifying the mass transfer through significant reducing both the drop sizes and the diffusion distance, but also supplying a flexible platform for the immobilization of valuable active sites. However, the restriction of the mobility of catalyst somehow decreases the activity of a catalyst. To obtain a promise reaction efficiency, we firstly report a synergistic method to enhance the biphasic reaction by Pickering emulsion and ultrasound concepts, targeted at efficient production of biodiesel. Response surface methodology based on Box-Behnken design was applied to optimize the reaction conditions, such as composition of catalyst, reaction temperature, ultrasound power, methanol to oil molar ratio and catalyst amount. An over 98% yield of biodiesel could be achieved within 2.5 hours by ultrasound assisted Pickering interfacial catalysis, which is over two times higher than that of ultrasound assisted homogeneous transesterification system. Besides, the ultrasound assisted Pickering emulsion shortened the reaction time by 3.6 fold when compared to mechanical stirring assisted Pickering emulsion system.
研究领域:
化学工程
·
可再生能源
·
催化科学
✓ 已验证
DOI
PubMed
高影响因子
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