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- Héraly, Frédéric, 1995-, et al.
(author)
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Capacitive CO2 sensor made of aminated cellulose nanofibrils : development and optimization
- 2024
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In: New Journal of Chemistry. - 1144-0546 .- 1369-9261. ; 48:14, s. 6064-6070
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Journal article (peer-reviewed)abstract
- CO2 sensors are very important; however, their performance is limited by stability and selectivity. This study unveils a capacitive CO2 sensor with a dielectric layer comprised of amine-functionalized cellulose nanofibril (CNF) foam, significantly enhanced by the addition of 1,8-diazabicyclo[5.4.0]undec-7-ene (DBU). The core innovation of this research lies in the strategic use of CNF-based foam, which leads to a substantial increase in sensor capacitance, setting a new standard in CO2 monitoring technologies. The sensor showcases exceptional performance under ambient conditions, with marked improvements in sensitivity towards CO2. The advancements are attributed to the chemisorption properties of the aminated CNFs combined with the DBU enhancement, facilitating more effective CO2 capture. By integrating these materials, we present a sensor that opens new avenues for environmental monitoring, healthcare diagnostics, and industrial safety, establishing a new benchmark for capacitive CO2 sensors in efficiency and environmental sustainability.
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- Héraly, Frédéric, 1995-, et al.
(author)
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Humidity-responsive fiber actuators based on cellulose nanofibrils
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Other publication (other academic/artistic)abstract
- Fiber actuators, particularly valuable in soft robotics and environmental sensing, are at the forefront of smart materials and materials innovation. Torsional and tensile biofiber actuators, notable for their cost-effectiveness and biodegradability, mark a critical gap in the development of next-generation functional materials and devices. To address this gap, this study showcases moisture-responsive actuators made from cellulose nanofibrils (CNFs). It introduces a pioneering torsional actuator, leveraging the hydrophilic nature of CNFs filaments produced through wet-spinning processes. These robust filaments exhibit a mechanical strength of 237.0 MPa, and are twisted to form the high-performance torsional actuator. This torsional actuator demonstrates rapid rotations, achieving up to 1180 revolutions per minute (rpm) within merely 10 seconds of moisture exposure and being durable across multiple cycles. The research here further explores critical factors such as filament morphology and twist density, which significantly impact the performance of this torsional actuator. Additionally, a sheath-run tensile actuator is unveiled, ingeniously combining a moisture-sensitive CNFs layer with a supercoiled nylon core to enhance structural support.
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- Lu, Yahua, et al.
(author)
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Heterostructure membranes of high permeability and stability assembled from MXene and modified layered double hydroxide nanosheets
- 2023
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In: Journal of Membrane Science. - 0376-7388 .- 1873-3123. ; 688
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Journal article (peer-reviewed)abstract
- Two-dimensional (2D) MXene-based lamellar membranes play transformative roles in membrane filtration technology. Their practical use in water treatment is however hindered by several hurdles, e.g., unfavorable swelling due to weak interactions between adjacent MXene nanosheets, tortuous diffusion pathways of layered stacking, and the intrinsic aquatic oxidation-prone nature of MXene. Herein, nanoporous 2D/2D heterostructure membranes are elaborately constructed via solution-phase assembly of oppositely charged MXene and modified layered double hydroxide (MLDH) nanosheets. As a multifunctional component, positively charged holey MLDH nanosheets were first tailor-made to serve simultaneously as a binder, spacer and surface-modifier; next they were intercalated into negatively charged MXene lamella to enhance structural stability and mass transfer of membranes. As a result, the as-prepared MLDH@MXene heterostructure membranes successfully break the persistent trade-off between high permeability and selectivity while mitigating the common drawbacks in 2D MXene-based lamellar membranes, e.g., swelling issues, restacking problems, and vulnerable chemical stability. Noticeably, at an operating pressure of 4 bar and a feed solution of 100 ppm of Congo red, the heterostructure membranes enable a threefold jump in permeability (332.7 +/- 20 L m(-2) h(-1 )bar(-1)) when compared to the pristine MXene membrane (119.3 +/- 18 L m(-2 )h(-1) bar(-1)), and better operational stability without compromising the rejection.
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5. |
- Pang, Kanglei, 1993-, et al.
(author)
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Redirecting configuration of atomically dispersed selenium catalytic sites for efficient hydrazine oxidation
- 2024
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In: Matter. - 2590-2393 .- 2590-2385. ; 7:2, s. 655-667
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Journal article (peer-reviewed)abstract
- Understanding the reconstruction of surface sites is crucial for gaining insights into the true active sites and catalytic mechanisms. While extensive research has been conducted on reconstruction behaviors of atomically dispersed metallic catalytic sites, limited attention has been paid to non-metallic ones despite their potential catalytic activity comparable or even superior to their noble-metal counterpart. Herein, we report a carbonaceous, atomically dispersed non-metallic selenium catalyst that displayed exceptional catalytic activity in the hydrazine oxidation reaction (HzOR) in alkaline media, outperforming the noble-metal Pt catalysts. In situ X-ray absorption spectroscopy (XAS) and Fourier transform infrared spectroscopy revealed that the pristine SeC4 site pre-adsorbs an ∗OH ligand, followed by HzOR occurring on the other side of the OH–SeC4. Theoretical calculations proposed that the pre-adsorbed ∗OH group pulls electrons from the Se site, resulting in a more positively charged Se and a higher polarity of Se–C bonds, thereby enhancing surface reactivity toward HzO/R.
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6. |
- Saeedi Garakani, Sadaf, 1993-, et al.
(author)
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Facile Fabrication of Wood-Derived Porous Fe3C/Nitrogen-Doped Carbon Membrane for Colorimetric Sensing of Ascorbic Acid
- 2023
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In: Nanomaterials. - 2079-4991. ; 13:20
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Journal article (peer-reviewed)abstract
- Fe3C nanoparticles hold promise as catalysts and nanozymes, but their low activity and complex preparation have hindered their use. Herein, this study presents a synthetic alternative toward efficient, durable, and recyclable, Fe3C-nanoparticle-encapsulated nitrogen-doped hierarchically porous carbon membranes (Fe3C/N–C). By employing a simple one-step synthetic method, we utilized wood as a renewable and environmentally friendly carbon precursor, coupled with poly(ionic liquids) as a nitrogen and iron source. This innovative strategy offers sustainable, high-performance catalysts with improved stability and reusability. The Fe3C/N–C exhibits an outstanding peroxidase-like catalytic activity toward the oxidation of 3,3′,5,5′-tetramethylbenzidine in the presence of hydrogen peroxide, which stems from well-dispersed, small Fe3C nanoparticles jointly with the structurally unique micro-/macroporous N–C membrane. Owing to the remarkable catalytic activity for mimicking peroxidase, an efficient and sensitive colorimetric method for detecting ascorbic acid over a broad concentration range with a low limit of detection (~2.64 µM), as well as superior selectivity, and anti-interference capability has been developed. This study offers a widely adaptable and sustainable way to synthesize an Fe3C/N–C membrane as an easy-to-handle, convenient, and recoverable biomimetic enzyme with excellent catalytic performance, providing a convenient and sensitive colorimetric technique for potential applications in medicine, biosensing, and environmental fields.
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- Saeedi Garakani, Sadaf, 1993-, et al.
(author)
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Poly(ionic liquid)-derived metal-free heteroatom co-doped porous carbons with peroxidase-like activity
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In: Applied materials today. - 2352-9407.
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Journal article (peer-reviewed)abstract
- Development of affordable, efficacious and metal-free heterogeneous catalytic systems has been a persistent challenge in academia and industry. Heteroatom-doped metal-free carbon materials are increasingly recognized as valuable heterogeneous catalysts, and if well-designed, can present comparable performance to, or even surpass transition metal-containing catalysts. Their physicochemical properties and structural characteristics are tunable in a wide range, plus being free of leakage of transition metal species into the environment. Herein, three types of hierarchically porous N/X co-doped carbon materials (X denotes B, P or S) were synthesized via using poly(ionic liquid)s (PILs) as carbon precursors and source of heteroatom dopants. The incorporation of sacrificial pore-inducing templating agents which created abundant edge defects, in combination with a heteroatom co-doping strategy enhanced the number of active sites and their peroxidase-like catalytic activities. Comparison with only nitrogen single-doped porous carbons as reference demonstrated that co-doping with nitrogen and another heteroatom exhibits higher peroxidase-like activity and affinity towards substrates. Among the three types of heteroatom co-doped porous carbonaceous artificial enzymes, the N/B co-doped carbonaceous catalyst displayed the highest specific activities and Vmax values. These observations suggest a synergistic effect of the co-dopants, here N and B in the enzyme that holds a promising potential to further enhance peroxidase-like activity.
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8. |
- Saeedi Garakani, Sadaf, 1993-, et al.
(author)
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Poly(ionic liquid)-derived metal-free heteroatom co-doped porous carbons with peroxidase-like activity
- 2024
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In: Applied Materials Today. - 2352-9407. ; 37
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Journal article (peer-reviewed)abstract
- Development of affordable, efficient and metal-free heterogeneous catalytic systems has been a persistent challenge in academia and industry. Heteroatom-doped metal-free carbon materials are increasingly recognized as valuable heterogeneous catalysts, and if well-designed, can present comparable performance to, or even surpass transition metal-containing catalysts. Their physicochemical properties and structural characteristics are tunable in a wide range, plus being free of leakage problems of transition metal species into the environment. Herein, three types of hierarchically porous N/X co-doped carbon materials (X denotes B, P or S) were synthesized via using poly(ionic liquid)s (PILs) as carbon precursors and source of heteroatom dopants. The incorporation of sacrificial pore-inducing templating agents which created abundant edge defects, in combination with a heteroatom co-doping strategy, enhanced the number of active sites and their peroxidase-like catalytic activities. Comparison with only nitrogen single-doped porous carbons as reference demonstrated that co-doping with nitrogen and another heteroatom exhibits higher peroxidase-like activity and affinity towards substrates. Among the three types of heteroatom co-doped porous carbonaceous artificial enzymes, the N/B co-doped carbonaceous catalyst displayed the highest specific activities and Vmax values. These observations suggest a synergistic effect of the co-dopants, here N and B in the enzyme that holds a promising potential to further enhance peroxidase-like activity.
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10. |
- Sikdar, Anirban, 1991-, et al.
(author)
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Hierarchically Porous 3D Freestanding Holey-MXene Framework via Mild Oxidation of Self-Assembled MXene Hydrogel for Ultrafast Pseudocapacitive Energy Storage
- 2024
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In: ACS Nano. - 1936-0851 .- 1936-086X. ; 18:4, s. 3707-3719
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Journal article (peer-reviewed)abstract
- The true promise of MXene as a practical supercapacitor electrode hinges on the simultaneous advancement of its three-dimensional (3D) assembly and the engineering of its nanoscopic architecture, two critical factors for facilitating mass transport and enhancing an electrode’s charge-storage performance. Herein, we present a straightforward strategy to engineer robust 3D freestanding MXene (Ti3C2Tx) hydrogels with hierarchically porous structures. The tetraamminezinc(II) complex cation ([Zn(NH3)4]2+) is selected to electrostatically assemble colloidal MXene nanosheets into a 3D interconnected hydrogel framework, followed by a mild oxidative acid-etching process to create nanoholes on the MXene surface. These hierarchically porous, conductive holey-MXene frameworks facilitate 3D transport of both electrons and electrolyte ions to deliver an excellent specific capacitance of 359.2 F g–1 at 10 mV s–1 and superb capacitance retention of 79% at 5000 mV s–1, representing a 42.2% and 15.3% improvement over pristine MXene hydrogel, respectively. Even at a commercial-standard mass loading of 10.1 mg cm–2, it maintains an impressive capacitance retention of 52% at 1000 mV s–1. This rational design of an electrode by engineering nanoholes on MXene nanosheets within a 3D porous framework dictates a significant step forward toward the practical use of MXene and other 2D materials in electrochemical energy storage systems.
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