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CELLULOSE · 2022 ·Vol. 29 ·期 16 ·8919-8935 · IF 6.123

Stretchable and bendable textile matrix based on cellulose fibers for wearable self-powered glucose biosensors

Fan Shuang,Chang Wei,Fei Cheng,Zhang Zhongguo,Hou Bingbing,Shi Zhuxuan,Wang Huixin,Hui Yuchen

A wearable self-powered biosensor, fabricated from a stretchable and bendable textile matrix, senses glucose in urine. This textile matrix is made of cellulose fibers. A porous three-dimensional electrode with high flexibility, conductivity, and electroactive surface area is obtained by coating multi-wall carbon nanotubes and reduced graphene oxides onto a textile matrix based on cellulose fibers. After immobilizing glucose oxidase and laccase by the polymer embed method, the bioelectrodes show good enzymatic loading density and high electrocatalytic efficiency. The relative self-powered biosensor has a good linear response to glucose in the concentration range from 0 to 40 mM (R 2  = 0.995), with a satisfactory limit of detection at 3.95 mM, owing to the high electrocatalytic efficiency of the bioelectrodes. The biosensors have good selectivity, repeatability, and long-term storage stability, exhibit excellent stretching and bending performance, and show stability to a variety of pH, because of the catalytic specificity and tolerance of enzymes, the reasonable design of the biosensor, and the stable catalytic microenvironment. The recovery of the biosensor integrated with a diaper for glucose in artificial urine samples is between 95.6 and 105.9%, suggesting a promising determination for real samples. Graphical abstract

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Coatings · 2022 ·Vol. 12 ·期 11 ·1734 · IF 3.236

Nanocellulose and Cellulose Making with Bio-Enzymes from Different Particle Sizes of Neosinocalamus Affinis

Jiaxin Zhao,Xiaoxiao Wu,Xushuo Yuan,Xinjie Yang,Haiyang Guo,Wentao Yao,Decai Ji,Xiaoping Li,Lianpeng Zhang

Cellulose is one of the most abundant, widely distributed and abundant polysaccharides on earth, and is the most valuable natural renewable resource for human beings. In this study, three different particle sizes (250, 178, and 150 μm) of Neosinocalamus affinis cellulose were extracted from Neosinocalamus affinis powder using bio-enzyme digestion and prepared into nanocellulose (CNMs). The cellulose contents of 250, 178, and 150 μm particle sizes were 53.44%, 63.38%, and 74.08%, respectively; the crystallinity was 54.21%, 56.03% and 63.58%, respectively. The thermal stability of cellulose increased gradually with smaller particle sizes. The yields of CNMs for 250, 178, and 150 μm particle sizes were 14.27%, 15.44%, and 16.38%, respectively. The results showed that the Neosinocalamus affinis powder was successfully removed from lignin, hemicellulose, and impurities (pectin, resin, etc.) by the treatment of bio-enzyme A (ligninase:hemicellulose:pectinase = 1:1:1) combined with NH3·H2O and H2O2/CH3COOH. Extraction of cellulose from Neosinocalamus affinis using bio-enzyme A, the smaller the particle size of Neosinocalamus affinis powder, the more cellulose content extracted, the higher the crystallinity, the better the thermal stability, and the higher the purity. Subsequently, nanocellulose (CNMs) were prepared by using bio-enzyme B (cellulase:pectinase = 1:1). The CNMs prepared by bio-enzyme B showed a network structure and fibrous bundle shape. Therefore, the ones prepared in this study belong to cellulose nanofibrils (CNFs). This study provides a reference in the extraction of cellulose from bamboo using bio-enzymes and the preparation of nanocellulose. To a certain extent, the utilization of bamboo as a biomass material was improved.Keywords:Neosinocalamus affinis;cellulose;nanocellulose;bio-enzymes;particle size

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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2021 · IF 5.816

Spider nest shaped multi-scale three-dimensional enzymatic electrodes for glucose/oxygen biofuel cells

Yuchen Hui,Huixin Wang,Wei Zuo,Xiaoyan Ma

A spider nest shaped multi-scale three-dimensional substrate consisting of reduced graphene oxide (RGO) and nickel foam is fabricated for enzymatic electrodes and biofuel cells. According to the excellent conductivity and large electroactive surface area of this special structure, the enzymatic electrodes show large enzymatic loading density, low electron transfer resistance and high electrocatalytic efficiency. The strong forces in the spider nest shaped structure and the excellent enzymatic embedding method ensure the stability of the glucose oxidase bioanodes and laccase biocathodes. The Michaelis–Menten constant value for the bioanodes to glucose is calculated to be 2.24 mM, which is close to the Michaelis–Menten constant for free glucose oxidase, implying a remarkably high enzymatic activity . Employed the obtained bioelectrodes with great properties, the relative glucose/oxygen biofuel cell has an open-circuit voltage of 0.70 V, with a high output power performance, and a maximum output power of 7.05 ± 0.05 mW cm −2 , owe to the high enzyme loading and low electron transfer resistance of the electrode based on the spider nest shaped structure. After 60 days of periodic storage experiments, the performance of the biofuel cell still maintained 84.2%, showing a good long-term stability.

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JOURNAL OF APPLIED ELECTROCHEMISTRY · 2023 · IF 2.9

Wearable cellulose textile matrix self-powered biosensor sensing lactate in human sweat

Xia Zunbin,Zuo Wei,Li Haiying,Qiu Liewei,Mu Ruihua,Wang Qian,Liu Hongchen,Wang Huixin,Hui Yuchen

Herein, a self-powered lactate biosensor (SPLBs) was assembled to detect lactate in sweat based on flexible textile matrix enzymatic electrodes. A porous three-dimensional electrode with high flexibility and electrical conductivity was obtained by decorating composites of reduced graphene oxide and carboxylate multiwalled carbon nanotubes onto a cellulose fabric substrate. The excellent enzyme embedding method using a gel electrolyte showed a Michaelis–Menten constant of 1.46 mM, indicating the high enzymatic activity of lactate dehydrogenase. Moreover, the assembled (SPLBs) displayed a sensitivity of 3.16 µW mM −1  cm −2 with a linear range of 0–10 mM and a detection limit of 9.49 µM. Additionally, the biosensor has good tensile flexural stability, selectivity, and long-term stability. When integrated into clothing, the (SPLBs) recovered 91.5–102.3% of lactate from real sweat, with a relative standard deviation of less than 4.16%. This biosensor is promising for sensing lactate in human sweat. Graphical abstract

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CHEMICAL ENGINEERING JOURNAL · 2023 · IF 15.1

Near-infrared light-enhanced enzymatic activity of laccase-platinum nanoparticles as a biosensor for colorimetric and visible detection of ascorbic acid

Guolin Zheng,Zhe Jiang,Yifan Cui,Man Zhou,Yuanyuan Yu,Ping Wang,Qiang Wang

Enzymes, as green catalysts with high activity and substrate specificity, have attracted extensive interest in contrast to chemical catalysts with non-selectivity. However, the enzymes' activities are sensitive to external environments. Therefore, highly efficient strategies are encouraged to modulate the enzymatic activity and stability at the molecular level. Compared with conventional magnetic field, temperature, and pH-responsive enzymatic activities, the near-infrared (NIR) light-controlled activities have noninvasive and convenient controllability advantages, which remains a significant challenge. Besides, NIR light also possesses intense penetration and low phototoxicity compared with UV and blue lights. Herein, the supersmall platinum nanoparticles (Pt-NPs) were for the first time deposited on the laccase body (labelled as laccase-Pt), with the reduction of chloroplatinic acid hexahydrate by sodium borohydride. Fortunately, the synergetic catalysis between laccase and Pt-NPs was demonstrated. Moreover, with and without NIR light irradiation, laccase-Pt activities are 2.439 and 2.258 times of free laccase, respectively. NIR laser could also manipulate the reversible enzyme activity of laccase-Pt. Notably, the laccase-Pt displays a significant advance in three-dimensional structure compared with conventional immobilized and encapsulated enzymes. Then, the high-performance laccase-Pt was used as a sensitive biosensor to detect ascorbic acid, with a detection limit of 3.7 μM obtained by colorimetric approach and smartphone. Briefly, this work provides a novel and feasible idea for manipulating laccase activity by NIR laser, inspiring more scholars to control other natural enzyme activities. Simultaneously, it also gives clear proof for a better understanding of the component-activity relationship of the enzymes-metal nano-bio hybrid catalysts.

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Nano-Micro Letters · 2020 ·Vol. 12 ·期 1 ·1-12 · IF 12.264

Tuning Atomically Dispersed Fe Sites in Metal–Organic Frameworks Boosts Peroxidase-Like Activity for Sensitive Biosensing

Xu Weiqing,Kang Yikun,Jiao Lei,Wu Yu,Yan Hongye,Li Jinli,Gu Wenling,Song Weiyu,Zhu Chengzhou

The two functional groups (nitro and amino) were introduced into MIL-101(Fe) for tuning the atomically dispersed metal active sites. Benefiting from both geometric and electronic effects, the nitro-functionalized MIL-101(Fe) shows a superior electronic structure of active sites and low reaction energy barrier for the HO* formation. Nitro-functionalized MIL-101(Fe)-based biosensor was successfully employed to detect acetylcholinesterase activity and organophosphorus pesticide.

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NEW JOURNAL OF CHEMISTRY · 2020 ·Vol. 44 ·期 17 ·7042-7050 · IF 3.288

Enzymatic deposition of PPy onto cPEG-grafted silk fibroin membrane to achieve conductivity

Jingjing Yuan,Lin Wang,Bo Xu,Ping Wang,Jiugang Yuan,Yuanyuan Yu,Chao Deng,Qiang Wang

Silk fibroins (SFs) have many attractive properties; however, the practical applications of pure fibroin materials are severely restricted by their low elasticity. To improve flexibility of regenerated SF membranes, carboxyl-terminated polyethylene glycol (cPEG) was introduced into fibroin chains using 1-ethyl-3-(3-dimethylaminopropyl)carbodiimide hydrochloride (EDC) and N-hydroxysuccinimide (NHS). Subsequently, laccase-mediated graft polymerization of polypyrrole (PPy) onto the SF-g-cPEG membrane was performed to achieve electrical conductivity. The results implied that cPEG was successfully grafted onto the SF chains; the elongation at break of the SF-g-cPEG membrane increased by three times compared to that of the untreated one. Meanwhile, the introduced cPEG promoted the binding of pyrrole radical cations onto fibroin membrane, resulting in an efficient deposition of a PPy conductive layer during the laccase treatment. Conductivity of the membrane of SF-g-cPEG/PPy meets the standard of conductive materials even after 48 cycles of bending testing. In addition, the composite membrane has acceptable in vitro biocompatibility. The present work provides a novel alternative for fabrication of flexible and conductive SF biomaterials, which would expand the applications of fibroin materials in wearable electronics.

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JOURNAL OF SOLID STATE ELECTROCHEMISTRY · 2018 ·Vol. 23 ·期 1 ·169-178 · IF 2.509

Flexible glucose/oxygen enzymatic biofuel cells based on three-dimensional gold-coated nickel foam

Hui Yuchen,Ma Xiaoyan,Qu Fengjin

A high-efficiency, stable, and flexible glucose/oxygen enzymatic biofuel cell is fabricated based on three-dimensional gold-coated nickel foam. The gold-coated layer makes the skeleton of nickel foam rougher, enhancing the relative apparent surface area of nickel foam and decreasing the electron transfer resistance. With the gold-coated nickel foam as substrate, the bioanode and biocathode exhibit good electrocatalysis activity and stability. By assembling the bioanode and biocathode with agarose gel electrolyte, cellulose acetate membrane, and silicone rubber layer-by-layer, the flexible biofuel cell is obtained. As per the results, the three-dimensional gold-coated nickel foam enlarges the enzymatic loading density to 5.68 × 10 −7  mol cm −2 , increasing the short circuit current density to 9.04 mA cm −2 . The maximum power density of this flexible biofuel cell reaches 2.32 ± 0.07 mW cm −2 with excellent stability for retaining 84.6% of its performance after 60 days. Additionally, the flexible biofuel cell can be very stable in and after 1000 times of bending.

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JOURNAL OF THE ELECTROCHEMICAL SOCIETY · 2017 ·Vol. 164 ·期 13 ·G112 · IF 3.259

Three-Dimensional Nickel Foam Based Enzymatic Electrode and Its Glucose/O2 Biofuel Cell with High Power Density

Yuchen Hui,Xiaoyan Ma,Fengjin Qu,Fang Chen,Ying Chen

A practical strategy is developed to fabricate stable glucose/O2 biofuel cells with high power density assembled by enzymatic bio-electrodes based on three-dimensional nickel foam. The porous three-dimensional nickel foam is used as a substrate to enhance the enzyme loading, while the reduced graphene oxide and gold nanoparticles decorating on the nickel foam are employed as the direct electron transfer system for bio-anodes and bio-cathodes. The ferrocenecarboxylic acid serves for the mediated electron transfer to further increase electron transfer rate for glucose oxidase electrodes. Covalent bond is employed to immobilize the mediator and enzymes for improving the stability of bio-electrodes and biofuel cells. As the results, the surface glucose oxidase loading reaches to 4.03 × 10−7 mol cm−2 with good enzymatic activity. Additionally, the obtained glucose/O2 biofuel cells exhibit an outstanding maximum power density of 2.84 ± 0.09 mW cm−2, with a remarkable long-term operational stability for retaining 85.5% of its performance after 70 days. In human blood, the biofuel cell shows a favorable output performance of 0.39 ± 0.04 mW cm−2, implying the appropriateness for practical applications.

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Journal of Physical Chemistry C · 2016 · IF 4.509

Biomimetic Copper-Based Inorganic–Protein Nanoflower Assembly Constructed on the Nanoscale Fibrous Membrane with Enhanced Stability and Durability

Mufang Li,Mengying Luo,Fei Li,Wenwen Wang,Ke Liu,Qiongzhen Liu,Yuedan Wang,Zhentan Lu,Dong Wang

Copper-based inorganic–protein hybrid nanoflowers were constructed on the surface of a nanofiber membrane, creating a highly biocompatible, biomimetic, and multilevel surface. The inorganic–enzyme nanoflowers exhibited enhanced durability and stability arising in part from the protection of the enzyme by the inorganic crystals. The high specific surface area and abundant functional groups of Cu2+ on the nanofiber membrane enable the dense and compact growth of Cu3(PO4)2·3H2O–protein nanoflowers. The structure, morphology, and crystallization of the copper-based inorganic–protein nanoflowers were analyzed, which led us to propose a formation mechanism of the hybrid nanoflower. The composition and structure of the copper-based inorganic–protein nanoflowers on the nanofiber membrane could be controlled by varying the structure of the nanofiber membrane, formulation of mineralizing solutions, concentration of protein, and growing time. Different structures of protein, such as BSA, papain, laccase, and HRP, show different morphologies. The construction of copper-based inorganic–protein nanoflowers on nanoscale fibrous membrane opens new possibilities for preparing biomimetic multilevel structured materials and makes them an ideal material for biosensor, biocatalysis, bioengineering, and biodevices.

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CURRENT ISSUES IN MOLECULAR BIOLOGY · 2024 ·Vol. 46 ·期 4 ·3694-3712 · IF 2.8

Effects of Lignin-Diverted Reductant with Polyphenol Oxidases on Cellulose Degradation by Wild and Mutant Types of Lytic Polysaccharide Monooxygenase

Kai Li,Yuan Wang,Xiao Guo,Bo Wang

Establishing a multi-enzyme synergistic lignocellulosic biodegradation system using lytic polysaccharide monooxygenase (LPMO) and polyphenol oxidases is vital for efficiently utilizing plant biomass waste, ultimately benefiting the carbon cycle and promoting environmental protection. Single-residue mutations of LPMO can improve the efficiency of lignocellulosic biomass degradation. However, the activity of mutant-type LPMO in relation to lignin-diverted reducing agents has not been sufficiently explored. In this study, laccase and tyrosinase were initially investigated and their optimal conditions and impressive thermal stability were revealed, indicating their potential synergistic abilities with LPMO in lignocellulose biodegradation. When utilizing gallic acid as a reducing agent, the activities of LPMOs were increased by over 10%, which was particularly evident in mutant-type LPMOs after the addition of polyphenol oxidases. In particular, the combination of tyrosinase with either 4-hydroxy-3-methoxyphenylacetone orp-coumaric acid was shown to enhance the efficacy of LPMOs. Furthermore, the highest activity levels of wild-type LPMOs were observed with the addition of laccase and 3-methylcatechol. The similarities between wild and mutant LPMOs regarding their activities in lignin-diverted phenolic compounds and reducing agents are almost identical, suggesting that the single-residue mutation of LPMO does not have a detrimental effect on its performance. Above all, this study indicates that understanding the performance of both wild and mutant types of LPMOs in the presence of polyphenol oxidases and various reducing agents constitutes a key link in the industrialization of the multi-enzyme degradation of lignocellulose.

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JOURNAL OF SOLID STATE ELECTROCHEMISTRY · 2024 · IF 2.6

Flexible and washable self-powered biosensors based on textile bioelectrodes for sensing glucose in sweat

Hui Yuchen,Fei Cheng,Zhang Zhongguo,Fan Shuang,Wang Huixin,Fan Wei,Chang Wei

This study fabricated a flexible and washable self-powered biosensor—based on cellulose textiles—for sensing glucose in sweat. The sensor is integrated with T-shirts for practical use. The cellulose fiber was modified with carbon nanotubes and reduced oxide graphene to decrease its electron transfer resistance and ohmic resistance. Due to their low resistance, the bioelectrodes display high electrocatalytic efficiency of glucose oxidation and oxygen reduction. The biosensors are assembled by packaging the bioanodes and gel electrolytes together. The assembled biosensors have a low limit of detection (6.7 µM) and a wide linear range (0.02–0.5 mM). The great sensing performances are strongly associated with the location of bioanodes and biocathodes. The outer biocathode protects the central bioanode that comes from oxygen and ensures the structural integrity of the device during bending cycles. It also reduces the damage caused by the washing. The biosensor also exhibited selectivity, repeatability, and great stability in different pHs and during long-term storage. Finally, the average recoveries in real sweat are 104.9 to 106.0%. Thus, the flexible and washable self-powered biosensors have great potential for diabetes diagnosis at an early stage by sensing glucose in sweat. Graphical abstract

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